Forensic investigation of plutonium metal: a case study of CRM 126

DOE PAGES

Byerly, Benjamin L.; Stanley, Floyd; Spencer, Khal; ...

2016-11-01

In our study, a certified plutonium metal reference material (CRM 126) with a known production history is examined using analytical methods that are commonly employed in nuclear forensics for provenancing and attribution. Moreover, the measured plutonium isotopic composition and actinide assay are consistent with values reported on the reference material certificate. Model ages from U/Pu and Am/Pu chronometers agree with the documented production timeline. Finally, these results confirm the utility of these analytical methods and highlight the importance of a holistic approach for forensic study of unknown materials.

The instrumental method of plutonium determination

NASA Astrophysics Data System (ADS)

Knyazev, B. B.; Kazachevskiy, I. V.; Solodukhin, V. P.; Lukashenko, S. N.; Knatova, M. K.; Kashirskiy, V. V.

2003-01-01

A method of direct instrumental determination of plutonium isotopes in soil samples is described. For the method a special program of spectra processing and activity calculation had to be prepared. The detection limit of 239+240Pu in absence of interfering radiation is about 200 Bq/kg (by 3.3σ criteria). Examples are given of the method application for the study of radionuclide soil composition in separate objects of Semipalatinsk Nuclear Test Site (SNTS). It is shown that for different objects under study the correlation degree between plutonium and americium activities may change rather substantially.

The plutonium isotopic composition of marine biota on Enewetak Atoll: a preliminary assessment.

PubMed

Hamilton, Terry F; Martinelli, Roger E; Kehl, Steven R; McAninch, Jeffrey E

2008-10-01

We have determined the level and distribution of gamma-emitting radionuclides, plutonium activity concentrations, and 240Pu/239Pu atom ratios in tissue samples of giant clam (Tridacna gigas and Hippopus hippopus), a top snail (Trochus nilaticas) and sea cucumber (Holothuria atra) collected from different locations around Enewetak Atoll. The plutonium isotopic measurements were performed using ultra-high sensitivity accelerator mass spectrometry (AMS). Elevated levels of plutonium were observed in the stomachs (includes the stomach lining) of Tridacna clam (0.62 to 2.98 Bq kg(-1), wet wt.), in the soft parts (edible portion) of top snails (0.25 to 1.7 Bq kg(-1)), wet wt.) and, to a lesser extent, in sea cucumber (0.015 to 0.22 Bq kg(-1), wet wt.) relative to muscle tissue concentrations in clam (0.006 to 0.021 Bq kg(-1), wet wt.) and in comparison with previous measurements of plutonium in fish. These data and information provide a basis for re-evaluating the relative significance of dietary intakes of plutonium from marine foods on Enewetak Atoll and, perhaps most importantly, demonstrate that discrete 240Pu239Pu isotope signatures might well provide a useful investigative tool to monitor source-term attribution and consequences on Enewetak Atoll. One potential application of immediate interest is to monitor and assess the health and ecological impacts of leakage of plutonium (as well as other radionuclides) from a low-level radioactive waste repository on Runit Island relative to background levels of fallout contamination in Enewetak Atoll lagoon.

Isotope ratio analysis of individual sub-micrometer plutonium particles with inductively coupled plasma mass spectrometry.

PubMed

Esaka, Fumitaka; Magara, Masaaki; Suzuki, Daisuke; Miyamoto, Yutaka; Lee, Chi-Gyu; Kimura, Takaumi

2010-12-15

Information on plutonium isotope ratios in individual particles is of great importance for nuclear safeguards, nuclear forensics and so on. Although secondary ion mass spectrometry (SIMS) is successfully utilized for the analysis of individual uranium particles, the isobaric interference of americium-241 to plutonium-241 makes difficult to obtain accurate isotope ratios in individual plutonium particles. In the present work, an analytical technique by a combination of chemical separation and inductively coupled plasma mass spectrometry (ICP-MS) is developed and applied to isotope ratio analysis of individual sub-micrometer plutonium particles. The ICP-MS results for individual plutonium particles prepared from a standard reference material (NBL SRM-947) indicate that the use of a desolvation system for sample introduction improves the precision of isotope ratios. In addition, the accuracy of the (241)Pu/(239)Pu isotope ratio is much improved, owing to the chemical separation of plutonium and americium. In conclusion, the performance of the proposed ICP-MS technique is sufficient for the analysis of individual plutonium particles. Copyright © 2010 Elsevier B.V. All rights reserved.

Improved sample utilization in thermal ionization mass spectrometry isotope ratio measurements: refined development of porous ion emitters for nuclear forensic applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baruzzini, Matthew Louis

The precise and accurate determination of isotopic composition in nuclear forensic samples is vital for assessing origin, intended use and process history. Thermal ionization mass spectrometry (TIMS) is widely accepted as the gold standard for high performance isotopic measurements and has long served as the workhorse in the isotopic ratio determination of nuclear materials. Nuclear forensic and safeguard specialists have relied heavily on such methods for both routine and atypical e orts. Despite widespread use, TIMS methods for the assay of actinide systems continue to be hindered by poor ionization e ciency, often less than tenths of a percent; themore » majority of a sample is not measured. This represents a growing challenge in addressing nextgeneration nuclear detection needs by limiting the ability to analyze ultratrace quantities of high priority elements that could potentially provide critical nuclear forensic signatures. Porous ion emitter (PIE) thermal ion sources were developed in response to the growing need for new TIMS ion source strategies for improved ionization e ciency, PIEs have proven to be simple to implement, straightforward approach to boosting ion yield. This work serves to expand the use of PIE techniques for the analysis of trace quantities of plutonium and americium. PIEs exhibited superior plutonium and americium ion yields when compared to direct lament loading and the resin bead technique, one of the most e cient methods for actinide analysis, at similar mass loading levels. Initial attempts at altering PIE composition for the analysis of plutonium proved to enhance sample utilization even further. Preliminary investigations of the instrumental fractionation behavior of plutonium and uranium analyzed via PIE methods were conducted. Data collected during these initial trial indicate that PIEs fractionate in a consistent, reproducible manner; a necessity for high precision isotope ratio measurements. Ultimately, PIEs methods were applied for the age determination of various uranium isotopic standards. PIEs did not exhibit signi cant advantages for the determination of model ages when compared to traditional laments; however, this trial was able to provide valuable insight for guiding future investigations.« less

Dissolution of aerosol particles collected from nuclear facility plutonium production process

DOE PAGES

Xu, Ning; Martinez, Alexander; Schappert, Michael Francis; ...

2015-08-14

Here, a simple, robust analytical chemistry method has been developed to dissolve plutonium containing particles in a complex matrix. The aerosol particles collected on Marple cascade impactor substrates were shown to be dissolved completely with an acid mixture of 12 M HNO 3 and 0.1 M HF. A pressurized closed vessel acid digestion technique was utilized to heat the samples at 130 °C for 16 h to facilitate the digestion. The dissolution efficiency for plutonium particles was 99 %. The resulting particle digestate solution was suitable for trace elemental analysis and isotope composition determination, as well as radiochemistry measurements.

Measurements of actinides in soil, sediments, water and vegetation in Northern New Mexico

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gallaher, B. M.; Efurd, D. W.

2002-01-01

This study was undertaken during 1991 - 1998 to identify the origin of plutonium uranium in northern New Mexico Rio Grande and tributary stream sediments. Isotopic fingerprinting techniques help distinguish radioactivity from Los Alamos National Laboratory (LANL) and from global fallout or natural sources. The geographic area covered by the study extended from the headwaters of the Rio Grande in southern Colorado to Elephant Butte Reservoir in southern New Mexico. Over 100 samples of stream channel and reservoir bottom sediments were analyzed for the atom ratios of plutonium and uranium isotopes using thermal ionization mass spectrometry (TIMS). Comparison of thesemore » ratios against those for fallout or natural sources allowed for quantification of the Laboratory impact. Of the seven major drainages crossing LANL, movement of LANL plutonium into the Rio Grande can only be traced via Los Alamos Canyon. The majority of sampled locations within and adjacent to LANL have little or no input of plutonium from the Laboratory. Samples collected upstream and distant to L A N show an average (+ s.d.) fallout 240Pu/239Pauto m ratio of 0.169 + 0.012, consistent with published worldwide global fallout values. These regional background ratios differ significantly from the 240Pu/239Pu atom ratio of 0.015 that is representative of LANL-derived plutonium entering the Rio Grande at Los Alamos Canyon. Mixing calculations of these sources indicate that the largest proportion (60% to 90%) of the plutonium in the Rio Grande sediments is from global atmospheric fallout, with an average of about 25% from the Laboratory. The LANL plutonium is identifiable intermittently along the 35-km reach of the Rio Grande to Cochiti Reservoir. The source of the LANL-derived plutonium in the Rio Grande was traced primarily to pre-1960 discharges of liquid effluents into a canyon bottom at a distance approximately 20 km upstream of the river. Plutonium levels decline exponentially with distance downstream after mixing with cleaner sediments, yet the LANL isotopic fingerprint remains distinct for at least 55 km from the effluent source. Plutonium isotopes in Rio Grande and Pajarito Plateau sediments are not at levels known to adversely affect public health. Activities of 239+240pwui thin this sample set ranged from 0.001- 0.046 pCUg in the Rio Grande to 3.7 pCi/g near the effluent discharge point. Levels in the Rio Grande are usually more than 1000 times. lower than prescribed cleanup standards. Uranium in stream and reservoir sediments is predominantly within natural concentration ranges and is of natural uranium isotopic composition. None of the sediments from the Rio Grande show identifiable Laboratory uranium, using the isotopic ratios. These results suggest that the mass of Laboratory-derived uranium entering the Rio Grande is small relative to the natural load carried with river sediments.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Byerly, Benjamin L.; Stanley, Floyd; Spencer, Khal

In our study, a certified plutonium metal reference material (CRM 126) with a known production history is examined using analytical methods that are commonly employed in nuclear forensics for provenancing and attribution. Moreover, the measured plutonium isotopic composition and actinide assay are consistent with values reported on the reference material certificate. Model ages from U/Pu and Am/Pu chronometers agree with the documented production timeline. Finally, these results confirm the utility of these analytical methods and highlight the importance of a holistic approach for forensic study of unknown materials.

Uranium daughter growth must not be neglected when adjusting plutonium materials for assay and isotopic contents

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marsh, S.F.; Spall, W.D.; Abernathey, R.M.

1976-11-01

Relationships are provided to compute the decreasing plutonium content and changing isotopic distribution of plutonium materials for the radioactive decay of /sup 238/Pu, /sup 239/Pu, /sup 240/Pu and /sup 242/Pu to long-lived uranium daughters and of /sup 241/Pu to /sup 241/Am. This computation is important to the use of plutonium reference materials to calibrate destructive and nondestructive methods for assay and isotopic measurements, as well as to accountability inventory calculations.

Determination of plutonium isotopes (238,239,240Pu) and strontium (90Sr) in seafood using alpha spectrometry and liquid scintillation spectrometry.

PubMed

Shin, Choonshik; Choi, Hoon; Kwon, Hye-Min; Jo, Hye-Jin; Kim, Hye-Jeong; Yoon, Hae-Jung; Kim, Dong-Sul; Kang, Gil-Jin

2017-10-01

The present study was carried out to survey the levels of plutonium isotopes ( 238 , 239 , 240 Pu) and strontium ( 90 Sr) in domestic seafood in Korea. In current, regulatory authorities have analyzed radionuclides, such as 134 Cs, 137 Cs and 131 I, in domestic and imported food. However, people are concerned about contamination of other radionuclides, such as plutonium and strontium, in food. Furthermore, people who live in Korea have much concern about safety of seafood. Accordingly, in this study, we have investigated the activity concentrations of plutonium and strontium in seafood. For the analysis of plutonium isotopes and strontium, a rapid and reliable method developed from previous study was used. Applicability of the test method was verified by examining recovery, minimum detectable activity (MDA), analytical time, etc. Total 40 seafood samples were analyzed in 2014-2015. As a result, plutonium isotopes ( 238 , 239 , 240 Pu) and strontium ( 90 Sr) were not detected or below detection limits in seafood. The detection limits of plutonium isotopes and strontium-90 were 0.01 and 1 Bq/kg, respectively. Copyright © 2017 Elsevier Ltd. All rights reserved.

EPA Method: Rapid Radiochemical Method for Americium-241, Radium-226, Plutonium-238/-239, Radiostronium, and Isotopic Uranium in Water for Environmental Restoration Following Homeland Security Events

EPA Pesticide Factsheets

SAM lists this method for the qualitative determination of Americium-241, Radium-226, Plutonium-238, Plutonium-239 and isotopic uranium in drinking water samples using alpha spectrometry and radiostrontium using beta counting.

Uncertainty propagation for the coulometric measurement of the plutonium concentration in MOX-PU4.

DOE Office of Scientific and Technical Information (OSTI.GOV)

None, None

This GUM WorkbenchTM propagation of uncertainty is for the coulometric measurement of the plutonium concentration in a Pu standard material (C126) supplied as individual aliquots that were prepared by mass. The C126 solution had been prepared and as aliquoted as standard material. Samples are aliquoted into glass vials and heated to dryness for distribution as dried nitrate. The individual plutonium aliquots were not separated chemically or otherwise purified prior to measurement by coulometry in the F/H Laboratory. Hydrogen peroxide was used for valence adjustment. The Pu assay measurement results were corrected for the interference from trace iron in the solutionmore » measured for assay. Aliquot mass measurements were corrected for air buoyancy. The relative atomic mass (atomic weight) of the plutonium from X126 certoficate was used. The isotopic composition was determined by thermal ionization mass spectrometry (TIMS) for comparison but not used in calculations.« less

An MS-DOS-based program for analyzing plutonium gamma-ray spectra

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ruhter, W.D.; Buckley, W.M.

1989-09-07

A plutonium gamma-ray analysis system that operates on MS-DOS-based computers has been developed for the International Atomic Energy Agency (IAEA) to perform in-field analysis of plutonium gamma-ray spectra for plutonium isotopics. The program titled IAEAPU consists of three separate applications: a data-transfer application for transferring spectral data from a CICERO multichannel analyzer to a binary data file, a data-analysis application to analyze plutonium gamma-ray spectra, for plutonium isotopic ratios and weight percents of total plutonium, and a data-quality assurance application to check spectral data for proper data-acquisition setup and performance. Volume 3 contains the software listings for these applications.

Plutonium in the arctic marine environment--a short review.

PubMed

Skipperud, Lindis

2004-06-18

Anthropogenic plutonium has been introduced into the environment over the past 50 years as the result of the detonation of nuclear weapons and operational releases from the nuclear industry. In the Arctic environment, the main source of plutonium is from atmospheric weapons testing, which has resulted in a relatively uniform, underlying global distribution of plutonium. Previous studies of plutonium in the Kara Sea have shown that, at certain sites, other releases have given rise to enhanced local concentrations. Since different plutonium sources are characterised by distinctive plutonium-isotope ratios, evidence of a localised influence can be supported by clear perturbations in the plutonium-isotope ratio fingerprints as compared to the known ratio in global fallout. In Kara Sea sites, such perturbations have been observed as a result of underwater weapons tests at Chernaya Bay, dumped radioactive waste in Novaya Zemlya, and terrestrial runoff from the Ob and Yenisey Rivers. Measurement of the plutonium-isotope ratios offers both a means of identifying the origin of radionuclide contamination and the influence of the various nuclear installations on inputs to the Arctic, as well as a potential method for following the movement of water and sediment loads in the rivers.

Natural Transmutation of Actinides via the Fission Reaction in the Closed Thorium-Uranium-Plutonium Fuel Cycle

NASA Astrophysics Data System (ADS)

Marshalkin, V. Ye.; Povyshev, V. M.

2017-12-01

It is shown for a closed thorium-uranium-plutonium fuel cycle that, upon processing of one metric ton of irradiated fuel after each four-year campaign, the radioactive wastes contain 54 kg of fission products, 0.8 kg of thorium, 0.10 kg of uranium isotopes, 0.005 kg of plutonium isotopes, 0.002 kg of neptunium, and "trace" amounts of americium and curium isotopes. This qualitatively simplifies the handling of high-level wastes in nuclear power engineering.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.

A new rapid fusion method for the determination of plutonium in large rice samples has been developed at the Savannah River National Laboratory (Aiken, SC, USA) that can be used to determine very low levels of plutonium isotopes in rice. The recent accident at Fukushima Nuclear Power Plant in March, 2011 reinforces the need to have rapid, reliable radiochemical analyses for radionuclides in environmental and food samples. Public concern regarding foods, particularly foods such as rice in Japan, highlights the need for analytical techniques that will allow very large sample aliquots of rice to be used for analysis so thatmore » very low levels of plutonium isotopes may be detected. The new method to determine plutonium isotopes in large rice samples utilizes a furnace ashing step, a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a column separation process with TEVA Resin cartridges. The method can be applied to rice sample aliquots as large as 5 kg. Plutonium isotopes can be determined using alpha spectrometry or inductively-coupled plasma mass spectrometry (ICP-MS). The method showed high chemical recoveries and effective removal of interferences. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory plutonium particles are effectively digested. The MDA for a 5 kg rice sample using alpha spectrometry is 7E-5 mBq g{sup -1}. The method can easily be adapted for use by ICP-MS to allow detection of plutonium isotopic ratios.« less

Analysis of plutonium isotope ratios including 238Pu/239Pu in individual U-Pu mixed oxide particles by means of a combination of alpha spectrometry and ICP-MS.

PubMed

Esaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki

2017-04-01

Isotope ratio analysis of individual uranium-plutonium (U-Pu) mixed oxide particles contained within environmental samples taken from nuclear facilities is proving to be increasingly important in the field of nuclear safeguards. However, isobaric interferences, such as 238 U with 238 Pu and 241 Am with 241 Pu, make it difficult to determine plutonium isotope ratios in mass spectrometric measurements. In the present study, the isotope ratios of 238 Pu/ 239 Pu, 240 Pu/ 239 Pu, 241 Pu/ 239 Pu, and 242 Pu/ 239 Pu were measured for individual Pu and U-Pu mixed oxide particles by a combination of alpha spectrometry and inductively coupled plasma mass spectrometry (ICP-MS). As a consequence, we were able to determine the 240 Pu/ 239 Pu, 241 Pu/ 239 Pu, and 242 Pu/ 239 Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of plutonium with UTEVA resins. Furthermore, 238 Pu/ 239 Pu isotope ratios were able to be calculated by using both the 238 Pu/( 239 Pu+ 240 Pu) activity ratios that had been measured through alpha spectrometry and the 240 Pu/ 239 Pu isotope ratios determined through ICP-MS. Therefore, the combined use of alpha spectrometry and ICP-MS is useful in determining plutonium isotope ratios, including 238 Pu/ 239 Pu, in individual U-Pu mixed oxide particles. Copyright © 2016 Elsevier B.V. All rights reserved.

Static, Mixed-Array Total Evaporation for Improved Quantitation of Plutonium Minor Isotopes in Small Samples

NASA Astrophysics Data System (ADS)

Stanley, F. E.; Byerly, Benjamin L.; Thomas, Mariam R.; Spencer, Khalil J.

2016-06-01

Actinide isotope measurements are a critical signature capability in the modern nuclear forensics "toolbox", especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10-6) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Results are presented for small sample (~20 ng) applications involving a well-known plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods.

Static, Mixed-Array Total Evaporation for Improved Quantitation of Plutonium Minor Isotopes in Small Samples.

PubMed

Stanley, F E; Byerly, Benjamin L; Thomas, Mariam R; Spencer, Khalil J

2016-06-01

Actinide isotope measurements are a critical signature capability in the modern nuclear forensics "toolbox", especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10(-6)) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Results are presented for small sample (~20 ng) applications involving a well-known plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods. Graphical Abstract ᅟ.

Isotopic fractionation studies of uranium and plutonium using porous ion emitters as thermal ionization mass spectrometry sources

DOE PAGES

Baruzzini, Matthew L.; Hall, Howard L.; Spencer, Khalil J.; ...

2018-04-22

Investigations of the isotope fractionation behaviors of plutonium and uranium reference standards were conducted employing platinum and rhenium (Pt/Re) porous ion emitter (PIE) sources, a relatively new thermal ionization mass spectrometry (TIMS) ion source strategy. The suitability of commonly employed, empirically developed mass bias correction laws (i.e., the Linear, Power, and Russell's laws) for correcting such isotope ratio data was also determined. Corrected plutonium isotope ratio data, regardless of mass bias correction strategy, were statistically identical to that of the certificate, however, the process of isotope fractionation behavior of plutonium using the adopted experimental conditions was determined to be bestmore » described by the Power law. Finally, the fractionation behavior of uranium, using the analytical conditions described herein, is also most suitably modeled using the Power law, though Russell's and the Linear law for mass bias correction rendered results that were identical, within uncertainty, to the certificate value.« less

Isotopic fractionation studies of uranium and plutonium using porous ion emitters as thermal ionization mass spectrometry sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baruzzini, Matthew L.; Hall, Howard L.; Spencer, Khalil J.

Investigations of the isotope fractionation behaviors of plutonium and uranium reference standards were conducted employing platinum and rhenium (Pt/Re) porous ion emitter (PIE) sources, a relatively new thermal ionization mass spectrometry (TIMS) ion source strategy. The suitability of commonly employed, empirically developed mass bias correction laws (i.e., the Linear, Power, and Russell's laws) for correcting such isotope ratio data was also determined. Corrected plutonium isotope ratio data, regardless of mass bias correction strategy, were statistically identical to that of the certificate, however, the process of isotope fractionation behavior of plutonium using the adopted experimental conditions was determined to be bestmore » described by the Power law. Finally, the fractionation behavior of uranium, using the analytical conditions described herein, is also most suitably modeled using the Power law, though Russell's and the Linear law for mass bias correction rendered results that were identical, within uncertainty, to the certificate value.« less

Plutonium release from Fukushima Daiichi fosters the need for more detailed investigations

NASA Astrophysics Data System (ADS)

Schneider, Stephanie; Walther, Clemens; Bister, Stefan; Schauer, Viktoria; Christl, Marcus; Synal, Hans-Arno; Shozugawa, Katsumi; Steinhauser, Georg

2013-10-01

The contamination of Japan after the Fukushima accident has been investigated mainly for volatile fission products, but only sparsely for actinides such as plutonium. Only small releases of actinides were estimated in Fukushima. Plutonium is still omnipresent in the environment from previous atmospheric nuclear weapons tests. We investigated soil and plants sampled at different hot spots in Japan, searching for reactor-borne plutonium using its isotopic ratio 240Pu/239Pu. By using accelerator mass spectrometry, we clearly demonstrated the release of Pu from the Fukushima Daiichi power plant: While most samples contained only the radionuclide signature of fallout plutonium, there is at least one vegetation sample whose isotope ratio (0.381 +/- 0.046) evidences that the Pu originates from a nuclear reactor (239+240Pu activity concentration 0.49 Bq/kg). Plutonium content and isotope ratios differ considerably even for very close sampling locations, e.g. the soil and the plants growing on it. This strong localization indicates a particulate Pu release, which is of high radiological risk if incorporated.

Static, mixed-array total evaporation for improved quantitation of plutonium minor isotopes in small samples

DOE PAGES

Stanley, F. E.; Byerly, Benjamin L.; Thomas, Mariam R.; ...

2016-03-31

Actinide isotope measurements are a critical signature capability in the modern nuclear forensics “toolbox”, especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10 -6) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Furthermore, results are presented for small sample (~20 ng) applications involving a well-knownmore » plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods.« less

Preserving Plutonium-244 as a National Asset

DOE Office of Scientific and Technical Information (OSTI.GOV)

Patton, Bradley D; Alexander, Charles W; Benker, Dennis

Plutonium-244 (244 Pu) is an extremely rare and long-lived isotope of plutonium with a half-life of 80 million years. Measureable amounts of 244 Pu are found in neither reactor-grade nor weapons-grade plutonium. Production of this isotope requires a very high thermal flux to permit the two successive neutron captures that convert 242 Pu to 243 Pu to 244 Pu, particularly given the short (about 5 hour) half-life of 243 Pu. Such conditions simply do not exist in plutonium production processes. Therefore, 244 Pu is ideal for precise radiochemical analyses measuring plutonium material properties and isotopic concentrations in items containing plutonium.more » Isotope dilution mass spectrometry is about ten times more sensitive when using 244 Pu rather than 242 Pu for determining plutonium isotopic content. The isotope can also be irradiated in small quantities to produce superheavy elements. The majority of the existing global inventory of 244 Pu is contained in the outer housing of Mark-18A targets at the Savannah River Site (SRS). The total inventory is about 20 grams of 244 Pu in about 400 grams of plutonium distributed among the 65 targets. Currently, there are no specific plans to preserve these targets. Although the cost of separating and preserving this material would be considerable, it is trivial in comparison to new production costs. For all practical purposes, the material is irreplaceable, because new production would cost billions of dollars and require a series of irradiation and chemical separation cycles spanning up to 50 years. This paper will discuss a set of options for overcoming the significant challenges to preserve the 244 Pu as a National Asset: (1) the need to relocate the material from SRS in a timely manner, (2) the need to reduce the volume of material to the extent possible for storage, and (3) the need to establish an operational capability to enrich the 244 Pu in significant quantities. This paper suggests that if all the Mark-18A plutonium is separated, it would occupy a small volume and would be inexpensive to store while an enrichment capability is developed. Very small quantities could be enriched in existing mass separators to support critical needs.« less

Improved plutonium identification and characterization results with NaI(Tl) detector using ASEDRA

NASA Astrophysics Data System (ADS)

Detwiler, R.; Sjoden, G.; Baciak, J.; LaVigne, E.

2008-04-01

The ASEDRA algorithm (Advanced Synthetically Enhanced Detector Resolution Algorithm) is a tool developed at the University of Florida to synthetically enhance the resolved photopeaks derived from a characteristically poor resolution spectra collected at room temperature from scintillator crystal-photomultiplier detector, such as a NaI(Tl) system. This work reports on analysis of a side-by-side test comparing the identification capabilities of ASEDRA applied to a NaI(Tl) detector with HPGe results for a Plutonium Beryllium (PuBe) source containing approximately 47 year old weapons-grade plutonium (WGPu), a test case of real-world interest with a complex spectra including plutonium isotopes and 241Am decay products. The analysis included a comparison of photopeaks identified and photopeak energies between the ASEDRA and HPGe detector systems, and the known energies of the plutonium isotopes. ASEDRA's performance in peak area accuracy, also important in isotope identification as well as plutonium quality and age determination, was evaluated for key energy lines by comparing the observed relative ratios of peak areas, adjusted for efficiency and attenuation due to source shielding, to the predicted ratios from known energy line branching and source isotopics. The results show that ASEDRA has identified over 20 lines also found by the HPGe and directly correlated to WGPu energies.

Isotope ratio measurements of pg-size plutonium samples using TIMS in combination with "multiple ion counting" and filament carburization

NASA Astrophysics Data System (ADS)

Jakopic, Rozle; Richter, Stephan; Kühn, Heinz; Benedik, Ljudmila; Pihlar, Boris; Aregbe, Yetunde

2009-01-01

A sample preparation procedure for isotopic measurements using thermal ionization mass spectrometry (TIMS) was developed which employs the technique of carburization of rhenium filaments. Carburized filaments were prepared in a special vacuum chamber in which the filaments were exposed to benzene vapour as a carbon supply and carburized electrothermally. To find the optimal conditions for the carburization and isotopic measurements using TIMS, the influence of various parameters such as benzene pressure, carburization current and the exposure time were tested. As a result, carburization of the filaments improved the overall efficiency by one order of magnitude. Additionally, a new "multi-dynamic" measurement technique was developed for Pu isotope ratio measurements using a "multiple ion counting" (MIC) system. This technique was combined with filament carburization and applied to the NBL-137 isotopic standard and samples of the NUSIMEP 5 inter-laboratory comparison campaign, which included certified plutonium materials at the ppt-level. The multi-dynamic measurement technique for plutonium, in combination with filament carburization, has been shown to significantly improve the precision and accuracy for isotopic analysis of environmental samples with low-levels of plutonium.

Composition of Radioactive Aerosols in the Shelter Construction of the Chernobyl Nuclear Power Plant in 2000-2015

NASA Astrophysics Data System (ADS)

Ogorodnikov, B. I.

2018-06-01

The results of the physicochemical studies of radioactive aerosols inside and outside the Shelter construction at the Arch construction stage of the Chernobyl Nuclear Power Plant (ChNPP) in 2000-2015 were presented. The dominant isotopes were shown to be cesium, strontium, americium, plutonium, and uranium. They are carried by disperse particles of 2-7 μm. In subreactor rooms, in particular, 012/7, the composition of aerosols is affected by the erosion of the fuel-containing mass formed in 1986. Submicron cesium carrier aerosols appear as a result of evaporation and condensation during fires and welding works. Radiocesium is a well-soluble component of aerosols, while plutonium isotopes are not readily soluble components. In several rooms, the contents of radon, thoron, and their daughter products exceeded the permissible values. In April-June 2011, the intake of radionuclides from the accident at the Japanese Fukushima-1 NPP, which had AMAD of 0.5 μm, was detected and tracked using Petryanov multilayer filters. The productivity of filtration units under the dusty conditions in the exclusion zone of ChNPP and in fogs and haze was investigated. Hydrophilic prefilters with 7-10 μm fibers were recommended.

Determination of ultra-low level plutonium isotopes (239Pu, 240Pu) in environmental samples with high uranium.

PubMed

Xing, Shan; Zhang, Weichao; Qiao, Jixin; Hou, Xiaolin

2018-09-01

In order to measure trace plutonium and its isotopes ratio ( 240 Pu/ 239 Pu) in environmental samples with a high uranium, an analytical method was developed using radiochemical separation for separation of plutonium from matrix and interfering elements including most of uranium and ICP-MS for measurement of plutonium isotopes. A novel measurement method was established for extensively removing the isobaric interference from uranium ( 238 U 1 H and 238 UH 2 + ) and tailing of 238 U, but significantly improving the measurement sensitivity of plutonium isotopes by employing NH 3 /He as collision/reaction cell gases and MS/MS system in the triple quadrupole ICP-MS instrument. The results show that removal efficiency of uranium interference was improved by more than 15 times, and the sensitivity of plutonium isotopes was increased by a factor of more than 3 compared to the conventional ICP-MS. The mechanism on the effective suppress of 238 U interference for 239 Pu measurement using NH 3 -He reaction gases was explored to be the formation of UNH + and UNH 2 + in the reactions of UH + and U + with NH 3 , while no reaction between NH 3 and Pu + . The detection limits of this method were estimated to be 0.55 fg mL -1 for 239 Pu, 0.09 fg mL -1 for 240 Pu. The analytical precision and accuracy of the method for Pu isotopes concentration and 240 Pu/ 239 Pu atomic ratio were evaluated by analysis of sediment reference materials (IAEA-385 and IAEA-412) with different levels of plutonium and uranium. The developed method were successfully applied to determine 239 Pu and 240 Pu concentrations and 240 Pu/ 239 Pu atomic ratios in soil samples collected in coastal areas of eastern China. Copyright © 2018 Elsevier B.V. All rights reserved.

Estimation of Plutonium-240 Mass in Waste Tanks Using Ultra-Sensitive Detection of Radioactive Xenon Isotopes from Spontaneous Fission

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bowyer, Theodore W.; Gesh, Christopher J.; Haas, Daniel A.

This report details efforts to develop a technique which is able to detect and quantify the mass of 240Pu in waste storage tanks and other enclosed spaces. If the isotopic ratios of the plutonium contained in the enclosed space is also known, then this technique is capable of estimating the total mass of the plutonium without physical sample retrieval and radiochemical analysis of hazardous material. Results utilizing this technique are reported for a Hanford Site waste tank (TX-118) and a well-characterized plutonium sample in a laboratory environment.

Measurements of extinct fission products in nuclear bomb debris: Determination of the yield of the Trinity nuclear test 70 y later

DOE PAGES

Hanson, Susan Kloek; Pollington, Anthony Douglas; Waidmann, Christopher Russell; ...

2016-07-05

This study describes an approach to measuring extinct fission products that would allow for the characterization of a nuclear test at any time. The isotopic composition of molybdenum in five samples of glassy debris from the 1945 Trinity nuclear test has been measured. Nonnatural molybdenum isotopic compositions were observed, reflecting an input from the decay of the short-lived fission products 95Zr and 97Zr. By measuring both the perturbation of the 95Mo/ 96Mo and 97Mo/ 96Mo isotopic ratios and the total amount of molybdenum in the Trinity nuclear debris samples, it is possible to calculate the original concentrations of the 95Zrmore » and 97Zr isotopes formed in the nuclear detonation. Together with a determination of the amount of plutonium in the debris, these measurements of extinct fission products allow for new estimates of the efficiency and yield of the historic Trinity test.« less

Measurements of extinct fission products in nuclear bomb debris: Determination of the yield of the Trinity nuclear test 70 y later

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hanson, Susan Kloek; Pollington, Anthony Douglas; Waidmann, Christopher Russell

This study describes an approach to measuring extinct fission products that would allow for the characterization of a nuclear test at any time. The isotopic composition of molybdenum in five samples of glassy debris from the 1945 Trinity nuclear test has been measured. Nonnatural molybdenum isotopic compositions were observed, reflecting an input from the decay of the short-lived fission products 95Zr and 97Zr. By measuring both the perturbation of the 95Mo/ 96Mo and 97Mo/ 96Mo isotopic ratios and the total amount of molybdenum in the Trinity nuclear debris samples, it is possible to calculate the original concentrations of the 95Zrmore » and 97Zr isotopes formed in the nuclear detonation. Together with a determination of the amount of plutonium in the debris, these measurements of extinct fission products allow for new estimates of the efficiency and yield of the historic Trinity test.« less

Measurements of extinct fission products in nuclear bomb debris: Determination of the yield of the Trinity nuclear test 70 y later

PubMed Central

Hanson, Susan K.; Pollington, Anthony D.; Waidmann, Christopher R.; Kinman, William S.; Wende, Allison M.; Miller, Jeffrey L.; Berger, Jennifer A.; Oldham, Warren J.; Selby, Hugh D.

2016-01-01

This paper describes an approach to measuring extinct fission products that would allow for the characterization of a nuclear test at any time. The isotopic composition of molybdenum in five samples of glassy debris from the 1945 Trinity nuclear test has been measured. Nonnatural molybdenum isotopic compositions were observed, reflecting an input from the decay of the short-lived fission products 95Zr and 97Zr. By measuring both the perturbation of the 95Mo/96Mo and 97Mo/96Mo isotopic ratios and the total amount of molybdenum in the Trinity nuclear debris samples, it is possible to calculate the original concentrations of the 95Zr and 97Zr isotopes formed in the nuclear detonation. Together with a determination of the amount of plutonium in the debris, these measurements of extinct fission products allow for new estimates of the efficiency and yield of the historic Trinity test. PMID:27382169

[Rapid analysis of the radionuclides plutonium and americium-241 in soils].

PubMed

Egorov, A V; Klochkova, N V

2009-01-01

The paper shows it possible to perform a rapid analysis of the isotopes of plutomium and americium-241. The basis of the developed rapid analysis is X-spectrometric determination of the amount of plutonium isotopes and gamma-spectrometric determination of the radionuclide 241AM.

Sources of plutonium in the atmosphere and stratosphere-troposphere mixing

PubMed Central

Hirose, Katsumi; Povinec, Pavel P.

2015-01-01

Plutonium isotopes have primarily been injected to the stratosphere by the atmospheric nuclear weapon tests and the burn-up of the SNAP-9A satellite. Here we show by using published data that the stratospheric plutonium exponentially decreased with apparent residence time of 1.5 ± 0.5 years, and that the temporal variations of plutonium in surface air followed the stratospheric trends until the early 1980s. In the 2000s, plutonium and its isotope ratios in the atmosphere varied dynamically, and sporadic high concentrations of 239,240Pu reported for the lower stratospheric and upper tropospheric aerosols may be due to environmental events such as the global dust outbreaks and biomass burning. PMID:26508010

The scheme for evaluation of isotopic composition of fast reactor core in closed nuclear fuel cycle

NASA Astrophysics Data System (ADS)

Saldikov, I. S.; Ternovykh, M. Yu; Fomichenko, P. A.; Gerasimov, A. S.

2017-01-01

The PRORYV (i.e. «Breakthrough» in Russian) project is currently under development. Within the framework of this project, fast reactors BN-1200 and BREST-OD-300 should be built to, inter alia, demonstrate possibility of the closed nuclear fuel cycle technologies with plutonium as a main source of power. Russia has a large inventory of plutonium which was accumulated in the result of reprocessing of spent fuel of thermal power reactors and conversion of nuclear weapons. This kind of plutonium will be used for development of initial fuel assemblies for fast reactors. To solve the closed nuclear fuel modeling tasks REPRORYV code was developed. It simulates the mass flow for nuclides in the closed fuel cycle. This paper presents the results of modeling of a closed nuclear fuel cycle, nuclide flows considering the influence of the uncertainty on the outcome of neutron-physical characteristics of the reactor.

Implementation of Microcalorimeter Array Technology for Safeguards of Nuclear Material

NASA Astrophysics Data System (ADS)

Kossmann, Shannon; Mateju, Klara; Koehler, Katrina; Croce, Mark

2018-03-01

Safeguards of nuclear materials depend on both destructive and nondestructive assay (DA and NDA, respectively). Ultra-high-resolution microcalorimeter gamma spectroscopy has the potential to substantially reduce the performance gap between NDA and DA methods in determination of plutonium isotopic composition. This paper details the setup of a cryostat and microwave readout system for microcalorimeter gamma spectroscopy, the functionality of which has been successfully demonstrated.

Flammability Analysis For Actinide Oxides Packaged In 9975 Shipping Containers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Laurinat, James E.; Askew, Neal M.; Hensel, Steve J.

2013-03-21

Packaging options are evaluated for compliance with safety requirements for shipment of mixed actinide oxides packaged in a 9975 Primary Containment Vessel (PCV). Radiolytic gas generation rates, PCV internal gas pressures, and shipping windows (times to reach unacceptable gas compositions or pressures after closure of the PCV) are calculated for shipment of a 9975 PCV containing a plastic bottle filled with plutonium and uranium oxides with a selected isotopic composition. G-values for radiolytic hydrogen generation from adsorbed moisture are estimated from the results of gas generation tests for plutonium oxide and uranium oxide doped with curium-244. The radiolytic generation ofmore » hydrogen from the plastic bottle is calculated using a geometric model for alpha particle deposition in the bottle wall. The temperature of the PCV during shipment is estimated from the results of finite element heat transfer analyses.« less

The iodine-plutonium-xenon age of the Moon-Earth system revisited.

PubMed

Avice, G; Marty, B

2014-09-13

Iodine-plutonium-xenon isotope systematics have been used to re-evaluate time constraints on the early evolution of the Earth-atmosphere system and, by inference, on the Moon-forming event. Two extinct radionuclides ((129)I, T1/2=15.6 Ma and (244)Pu, T1/2=80 Ma) have produced radiogenic (129)Xe and fissiogenic (131-136)Xe, respectively, within the Earth, the related isotope fingerprints of which are seen in the compositions of mantle and atmospheric Xe. Recent studies of Archaean rocks suggest that xenon atoms have been lost from the Earth's atmosphere and isotopically fractionated during long periods of geological time, until at least the end of the Archaean eon. Here, we build a model that takes into account these results. Correction for Xe loss permits the computation of new closure ages for the Earth's atmosphere that are in agreement with those computed for mantle Xe. The corrected Xe formation interval for the Earth-atmosphere system is [Formula: see text] Ma after the beginning of Solar System formation. This time interval may represent a lower limit for the age of the Moon-forming impact. © 2014 The Author(s) Published by the Royal Society. All rights reserved.

Plutonium isotopes offer an alternative approach to establishing chronological profiles in coarse sediments

NASA Astrophysics Data System (ADS)

Pondell, C.; Kuehl, S. A.; Canuel, E. A.

2016-12-01

There are several methodologies used to determine chronologies for sediments deposited within the past 100 years, including 210Pb and 137Cs radioisotopes and organic and inorganic contaminants. These techniques are quite effective in fine sediments, which generally have a high affinity for metals and organic compounds. However, the application of these chronological tools becomes limited in systems where coarse sediments accumulate. Englebright Lake is an impoundment in northern California where sediment accumulation is characterized by a combination of fine and coarse sediments. This combination of sediment grain size complicated chronological analysis using the more traditional 137Cs chronological approach. This study established a chronology of these sediments using 239+240Pu isotopes. While most of the 249+240Pu activity was measured in the fine grain size fraction (<63 microns), up to 25% of the plutonium activity was detected in the coarse size fractions of sediments from Englebright Lake. Profiles of 239+240Pu were similar to available 137Cs profiles, verifying the application of plutonium isotopes for determining sediment chronologies and expanding the established geochronology for Englebright Lake sediments. This study of sediment accumulation in Englebright Lake demonstrates the application of plutonium isotopes in establishing chronologies in coarse sediments and highlights the potential for plutonium to offer new insights into patterns of coarse sediment accumulation.

Selection of Russian Plutonium Beryllium Sources for Inclusion in the Nuclear Mateirals Information Program Archive

DOE Office of Scientific and Technical Information (OSTI.GOV)

Narlesky, Joshua E; Padilla, Dennis D; Watts, Joe

2009-01-01

Throughout the 1960s and 1970s, the former Soviet Union produced and exported Plutonium-Beryllium (PuBe) neutron sources to various Eastern European countries. The Russian sources consist of an intermetallic compound of plutonium and beryllium encapsulated in an inner welded, sealed capsule and consisting of a body and one or more covers. The amount of plutonium in the sources ranges from 0.002 g up to 15 g. A portion of the sources was originally exported to East Germany. A portion of these sources were acquired by Los Alamos National Laboratory (LANL) in the late 1990s for destruction in the Offsite Source Recoverymore » Program. When the OSRP was canceled, the remaining 88 PuBe neutron sources were packaged and stored in a 55-gal drum at T A-55. This storage configuration is no longer acceptable for PuBe sources, and the sources must either be repackaged or disposed of. Repackaging would place the sources into Hagan container, and depending on the dose rates, some sources may be packaged individually increasing the footprint and cost of storage. In addition, each source will be subject to leak-checking every six months. Leaks have already been detected in some of the sources, and due to the age of these sources, it is likely that additional leaks may be detected over time, which will increase the overall complexity of handling and storage. Therefore, it was decided that the sources would be disposed of at the Waste Isolation Pilot Plant (WIPP) due to the cost and labor associated with continued storage at TA-55. However, the plutonium in the sources is of Russian origin and needs to be preserved for research purposes. Therefore, it is important that a representative sample of the sources retained and archived for future studies. This report describes the criteria used to obtain a representative sample of the sources. Nine Russian PuBe neutron sources have been selected out of a collection of 77 sources for inclusion in the NMIP archive. Selection criteria were developed so that the largest sources that are representative of the collection are included. One representative source was chosen for every 20 sources in the collection, and effort was made to preserve sources unique to the collection. In total, four representative sources and five unique sources were selected for the archive. The archive samples contain 40 grams of plutonium with an isotopic composition similar to that of weapon grade material and three grams of plutonium with an isotopic composition similar to that of reactor grade plutonium.« less

Isotopic Analysis of Plutonium by Optical Spectroscopy; ANALYSE ISOTOPIQUE DU PLUTONIUM PAR SPECTROSCOPIE OPTIQUE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Artaud, J.; Chaput, M.; Gerstenkorn, S.

1961-01-01

Isotopic analyses of mixtures of plutonium-239 and -240 were carried out by means of the photoelectric spectrometer, the source being a hollow cathode cooled by liquid nitrogen. The relative precision is of the order of 2%, for samples containieg 3% of Pu/sup 240/. The study of the reproductibility of the measurements should make it possible to increase the precision; the relative precision which can be expected from the method should be 1% for mixtures containing 1% of Pu/sup 240/. (auth)

LWR First Recycle of TRU with Thorium Oxide for Transmutation and Cross Sections

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andrea Alfonsi; Gilles Youinou; Sonat Sen

2013-02-01

Thorium has been considered as an option to uranium-based fuel, based on considerations of resource utilization (thorium is approximately three times more plentiful than uranium) and as a result of concerns about proliferation and waste management (e.g. reduced production of plutonium, etc.). Since the average composition of natural Thorium is dominated (100%) by the fertile isotope Th-232, Thorium is only useful as a resource for breeding new fissile materials, in this case U-233. Consequently a certain amount of fissile material must be present at the start-up of the reactor in order to guarantee its operation. The thorium fuel can bemore » used in both once-through and recycle options, and in both fast and thermal spectrum systems. The present study has been aimed by the necessity of investigating the option of using reprocessed plutonium/TRU, from a once-through reference LEU scenario (50 GWd/ tIHM), mixed with natural thorium and the need of collect data (mass fractions, cross-sections etc.) for this particular fuel cycle scenario. As previously pointed out, the fissile plutonium is needed to guarantee the operation of the reactor. Four different scenarios have been considered: • Thorium – recycled Plutonium; • Thorium – recycled Plutonium/Neptunium; • Thorium – recycled Plutonium/Neptunium/Americium; • Thorium – recycled Transuranic. The calculations have been performed with SCALE6.1-TRITON.« less

LWR First Recycle of TRU with Thorium Oxide for Transmutation and Cross Sections

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andrea Alfonsi; Gilles Youinou

2012-07-01

Thorium has been considered as an option to uranium-based fuel, based on considerations of resource utilization (thorium is approximately three times more plentiful than uranium) and as a result of concerns about proliferation and waste management (e.g. reduced production of plutonium, etc.). Since the average composition of natural Thorium is dominated (100%) by the fertile isotope Th-232, Thorium is only useful as a resource for breeding new fissile materials, in this case U-233. Consequently a certain amount of fissile material must be present at the start-up of the reactor in order to guarantee its operation. The thorium fuel can bemore » used in both once-through and recycle options, and in both fast and thermal spectrum systems. The present study has been aimed by the necessity of investigating the option of using reprocessed plutonium/TRU, from a once-through reference LEU scenario (50 GWd/ tIHM), mixed with natural thorium and the need of collect data (mass fractions, cross-sections etc.) for this particular fuel cycle scenario. As previously pointed out, the fissile plutonium is needed to guarantee the operation of the reactor. Four different scenarios have been considered: • Thorium – recycled Plutonium; • Thorium – recycled Plutonium/Neptunium; • Thorium – recycled Plutonium/Neptunium/Americium; • Thorium – recycled Transuranic. The calculations have been performed with SCALE6.1-TRITON.« less

Using Nitrogen and Oxygen Isotope Compositions of Nitrate to Distinguish Contaminant Sources in Hanford Soil and Groundwater

DOE Office of Scientific and Technical Information (OSTI.GOV)

Conrad, Mark; Bill, Markus

2008-08-01

The nitrogen ({delta}{sup 15}N) and oxygen ({delta}{sup 18}O) isotopic compositions of nitrate in the environment are primarily a function of the source of the nitrate. The ranges of isotopic compositions for nitrate resulting from common sources are outlined in Figure 1 from Kendall (1998). As noted on Figure 1, processes such as microbial metabolism can modify the isotopic compositions of the nitrate, but the effects of these processes are generally predictable. At Hanford, nitrate and other nitrogenous compounds were significant components of most of the chemical processes used at the site. Most of the oxygen in nitrate chemicals (e.g., nitricmore » acid) is derived from atmospheric oxygen, giving it a significantly higher {delta}{sup 18}O value (+23.5{per_thousand}) than naturally occurring nitrate that obtains most of its oxygen from water (the {delta}{sup 18}O of Hanford groundwater ranges from -14{per_thousand} to -18{per_thousand}). This makes it possible to differentiate nitrate from Hanford site activities from background nitrate at the site (including most fertilizers that might have been used prior to the Department of Energy plutonium production activities at the site). In addition, the extreme thermal and chemical conditions that occurred during some of the waste processing procedures and subsequent waste storage in select single-shell tanks resulted in unique nitrate isotopic compositions that can be used to identify those waste streams in soil and groundwater at the site (Singleton et al., 2005; Christensen et al., 2007). This report presents nitrate isotope data for soil and groundwater samples from the Hanford 200 Areas and discusses the implications of that data for potential sources of groundwater contamination.« less

Multi-isotopic determination of plutonium (239Pu, 240Pu, 241Pu and 242Pu) in marine sediments using sector-field inductively coupled plasma mass spectrometry.

PubMed

Donard, O F X; Bruneau, F; Moldovan, M; Garraud, H; Epov, V N; Boust, D

2007-03-28

Among the transuranic elements present in the environment, plutonium isotopes are mainly attached to particles, and therefore they present a great interest for the study and modelling of particle transport in the marine environment. Except in the close vicinity of industrial sources, plutonium concentration in marine sediments is very low (from 10(-4) ng kg(-1) for (241)Pu to 10 ng kg(-1) for (239)Pu), and therefore the measurement of (238)Pu, (239)Pu, (240)Pu, (241)Pu and (242)Pu in sediments at such concentration level requires the use of very sensitive techniques. Moreover, sediment matrix contains huge amounts of mineral species, uranium and organic substances that must be removed before the determination of plutonium isotopes. Hence, an efficient sample preparation step is necessary prior to analysis. Within this work, a chemical procedure for the extraction, purification and pre-concentration of plutonium from marine sediments prior to sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS) analysis has been optimized. The analytical method developed yields a pre-concentrated solution of plutonium from which (238)U and (241)Am have been removed, and which is suitable for the direct and simultaneous measurement of (239)Pu, (240)Pu, (241)Pu and (242)Pu by SF-ICP-MS.

Actinides in deer tissues at the rocky flats environmental technology site.

PubMed

Todd, Andrew S; Sattelberg, R Mark

2005-11-01

Limited hunting of deer at the future Rocky Flats National Wildlife Refuge has been proposed in U.S. Fish and Wildlife planning documents as a compatible wildlife-dependent public use. Historically, Rocky Flats site activities resulted in the contamination of surface environmental media with actinides, including isotopes of americium, plutonium, and uranium. In this study, measurements of actinides [Americium-241 (241Am); Plutonium-238 (238Pu); Plutonium-239,240 (239,240Pu); uranium-233,244 (233,234U); uranium-235,236 (235,236U); and uranium-238 (238U)] were completed on select liver, muscle, lung, bone, and kidney tissue samples harvested from resident Rocky Flats deer (N = 26) and control deer (N = 1). In total, only 17 of the more than 450 individual isotopic analyses conducted on Rocky Flats deer tissue samples measured actinide concentrations above method detection limits. Of these 17 detects, only 2 analyses, with analytical uncertainty values added, exceeded threshold values calculated around a 1 x 10(-6) risk level (isotopic americium, 0.01 pCi/g; isotopic plutonium, 0.02 pCi/g; isotopic uranium, 0.2 pCi/g). Subsequent, conservative risk calculations suggest minimal human risk associated with ingestion of these edible deer tissues. The maximum calculated risk level in this study (4.73 x 10(-6)) is at the low end of the U.S. Environmental Protection Agency's acceptable risk range.

Multiple recycle of REMIX fuel at VVER-1000 operation in closed fuel cycle

NASA Astrophysics Data System (ADS)

Alekseev, P. N.; Bobrov, E. A.; Chibinyaev, A. V.; Teplov, P. S.; Dudnikov, A. A.

2015-12-01

The basic features of loading the VVER-1000 core with a new variant of REMIX fuel (REgenerated MIXture of U-Pu oxides) are considered during its multiple recycle in a closed nuclear fuel cycle. The fuel composition is produced on the basis of the uranium-plutonium regenerate extracted at processing the spent nuclear fuel (SNF) from a VVER-1000, depleted uranium, and the fissionable material: 235U as a part of highly enriched uranium (HEU) from warheads superfluous for defense purposes or 233U accumulated in thorium blankets of fusion (electronuclear) neutron sources or fast reactors. Production of such a fuel assumes no use of natural uranium in addition. When converting a part of the VVER-1000 reactors to the closed fuel cycle based on the REMIX technology, the consumption of natural uranium decreases considerably, and there is no substantial degradation of the isotopic composition of plutonium or change in the reactor-safety characteristics at the passage from recycle to recycle.

Multiple recycle of REMIX fuel at VVER-1000 operation in closed fuel cycle

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alekseev, P. N.; Bobrov, E. A., E-mail: evgeniybobrov89@rambler.ru; Chibinyaev, A. V.

2015-12-15

The basic features of loading the VVER-1000 core with a new variant of REMIX fuel (REgenerated MIXture of U–Pu oxides) are considered during its multiple recycle in a closed nuclear fuel cycle. The fuel composition is produced on the basis of the uranium–plutonium regenerate extracted at processing the spent nuclear fuel (SNF) from a VVER-1000, depleted uranium, and the fissionable material: {sup 235}U as a part of highly enriched uranium (HEU) from warheads superfluous for defense purposes or {sup 233}U accumulated in thorium blankets of fusion (electronuclear) neutron sources or fast reactors. Production of such a fuel assumes no usemore » of natural uranium in addition. When converting a part of the VVER-1000 reactors to the closed fuel cycle based on the REMIX technology, the consumption of natural uranium decreases considerably, and there is no substantial degradation of the isotopic composition of plutonium or change in the reactor-safety characteristics at the passage from recycle to recycle.« less

The efficacy of denaturing actinide elements as a means of decreasing materials attractiveness

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hase, K.R.; Bathke, C.G.; Ebbinghaus, B.B.

2013-07-01

This study considers the concept of denaturing as applied to the actinide elements present in spent fuel as a means to reduce materials attractiveness. Highly attractive materials generally have low values of bare critical mass, heat content, and dose. To denature an attractive element, its spent-fuel isotopic composition (isotopic vector) is intentionally modified by introducing sufficient quantities of a significantly less attractive isotope to dilute the concentration of a highly attractive isotope so that the overall attractiveness of the element is reduced. The authors used FOM (Figure of Merit) formula as the material attractiveness metric for their parametric determination ofmore » the attractiveness of the Pu and U. Materials attractiveness needs to be considered in three distinct phases in the process to construct a nuclear explosive device (NED): the acquisition phase, processing phase, and utilization phase. The results show that denaturing uranium with {sup 238}U is actually an effective means of reducing the attractiveness. For uranium with a large minority of {sup 235}U, a mixture of 80% {sup 238}U to 20% {sup 235}U is required to reduce the attractiveness to low. For uranium with a large concentration of {sup 233}U, a mixture of 88% {sup 238}U to 12% {sup 233}U is required to reduce the attractiveness to low. The results also show that denaturing plutonium with {sup 238}Pu is less effective than denaturing uranium with {sup 238}U. Using {sup 238}Pu as the denaturing agent would require 80% or more by mass in order to reduce the attractiveness to low. No amount of {sup 240}Pu is enough to reduce the plutonium attractiveness below medium. The combination of {sup 238}Pu and {sup 240}Pu would require approximately 70% {sup 238}Pu and 25% {sup 240}Pu by mass to reduce the plutonium attractiveness to low.« less

Determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using radiochemical separation combined with radiometric and mass spectrometric measurements.

PubMed

Xu, Yihong; Qiao, Jixin; Hou, Xiaolin; Pan, Shaoming; Roos, Per

2014-02-01

This paper reports an analytical method for the determination of plutonium isotopes ((238)Pu, (239)Pu, (240)Pu, (241)Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation counting and alpha spectrometry) and inductively coupled plasma mass spectrometry (ICP-MS) were applied for the measurement of plutonium isotopes. The decontamination factors for uranium were significantly improved up to 7.5 × 10(5) for 20 g soil compared to the level reported in the literature, this is critical for the measurement of plutonium isotopes using mass spectrometric technique. Although the chemical yield of Pu in the entire procedure is about 55%, the analytical results of IAEA soil 6 and IAEA-367 in this work are in a good agreement with the values reported in the literature or reference values, revealing that the developed method for plutonium determination in environmental samples is reliable. The measurement results of (239+240)Pu by alpha spectrometry agreed very well with the sum of (239)Pu and (240)Pu measured by ICP-MS. ICP-MS can not only measure (239)Pu and (240)Pu separately but also (241)Pu. However, it is impossible to measure (238)Pu using ICP-MS in environmental samples even a decontamination factor as high as 10(6) for uranium was obtained by chemical separation. © 2013 Elsevier B.V. All rights reserved.

Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study

DOE PAGES

Armstrong, Christopher R.; Nuessle, Patterson R.; Brant, Heather A.; ...

2015-01-16

This work presents the findings of a long term plutonium study at Savannah River Site (SRS) conducted between 2003 and 2013. Terrestrial environmental samples were obtained at Savannah River National Laboratory (SRNL) in A-area. Plutonium content and isotopic abundances were measured over this time period by alpha spectrometry and three stage thermal ionization mass spectrometry (3STIMS). Here we detail the complete sample collection, radiochemical separation, and measurement procedure specifically targeted to trace plutonium in bulk environmental samples. Total plutonium activities were determined to be not significantly above atmospheric global fallout. However, the 238Pu/ 239+240Pu activity ratios attributed to SRS aremore » above atmospheric global fallout ranges. The 240Pu/ 239Pu atom ratios are reasonably consistent from year to year and are lower than fallout, while the 242Pu/ 239Pu atom ratios are higher than fallout values. Overall, the plutonium signatures obtained in this study reflect a mixture of weapons-grade, higher burn-up, and fallout material. This study provides a blue print for long term low level monitoring of plutonium in the environment.« less

Evaluation of isotopic composition of fast reactor core in closed nuclear fuel cycle

NASA Astrophysics Data System (ADS)

Tikhomirov, Georgy; Ternovykh, Mikhail; Saldikov, Ivan; Fomichenko, Peter; Gerasimov, Alexander

2017-09-01

The strategy of the development of nuclear power in Russia provides for use of fast power reactors in closed nuclear fuel cycle. The PRORYV (i.e. «Breakthrough» in Russian) project is currently under development. Within the framework of this project, fast reactors BN-1200 and BREST-OD-300 should be built to, inter alia, demonstrate possibility of the closed nuclear fuel cycle technologies with plutonium as a main source of energy. Russia has a large inventory of plutonium which was accumulated in the result of reprocessing of spent fuel of thermal power reactors and conversion of nuclear weapons. This kind of plutonium will be used for development of initial fuel assemblies for fast reactors. The closed nuclear fuel cycle concept of the PRORYV assumes self-supplied mode of operation with fuel regeneration by neutron capture reaction in non-enriched uranium, which is used as a raw material. Operating modes of reactors and its characteristics should be chosen so as to provide the self-sufficient mode by using of fissile isotopes while refueling by depleted uranium and to support this state during the entire period of reactor operation. Thus, the actual issue is modeling fuel handling processes. To solve these problems, the code REPRORYV (Recycle for PRORYV) has been developed. It simulates nuclide streams in non-reactor stages of the closed fuel cycle. At the same time various verified codes can be used to evaluate in-core characteristics of a reactor. By using this approach various options for nuclide streams and assess the impact of different plutonium content in the fuel, fuel processing conditions, losses during fuel processing, as well as the impact of initial uncertainties on neutron-physical characteristics of reactor are considered in this study.

Development and Attestation of Gamma-Ray Measurement Methodologies for use by Rostekhnadzor Inspectors in the Russian Federation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jeff Sanders

2006-09-01

Development and attestation of gamma-ray non-destructive assay measurement methodologies for use by inspectors of the Russian Federal Service for Environmental, Technological, and Nuclear Oversight (Rostekhnadzor, formerly Gosatomnadzor or GAN), as well as for use by Russian nuclear facilities, has been completed. Specifically, a methodology utilizing the gamma-ray multi group analysis (MGA) method for determining plutonium isotopic composition has been developed, while existing methodologies to determining uranium enrichment and isotopic composition have been revised to make them more appropriate to the material types and conditions present in nuclear facilities in the Russian Federation. This paper will discuss the development and revisionmore » of these methodologies, the metrological characteristics of the final methodologies, as well as the limitations and concerns specific to the utilization of these analysis methods in the Russian Federation.« less

Second NBL measurement evaluation program meeting: A summary

DOE Office of Scientific and Technical Information (OSTI.GOV)

Spaletto, M.I.; Clapper, M.; Tolbert, M.E.M.

New Brunswick Laboratory (NBL), the US government`s nuclear materials measurements and reference materials laboratory, administers interlaboratory measurement evaluation programs to evaluate the quality and adequacy of safeguards measurements. The NBL Measurement Evaluation Program covers several types of safeguards analytical measurements. The Safeguards Measurement Evaluation (SME) program distributes test materials destructive measurements of uranium for both elemental concentration and isotopic abundances, and of plutonium for isotopic abundances. The Calorimetry Exchange (CalEx) Program tests the quality of nondestructive measurements of plutonium isotopic abundances by gamma spectroscopy and plutonium concentration by calorimetry. In May 1997, more than 30 representatives from the Department ofmore » Energy (DOE), its contractor laboratories, and Nuclear Regulatory Commission licensees met at NBL in Argonne, Illinois, for the annual meeting of the Measurement Evaluation Program. The summary which follows details key points that were discussed or presented at the meeting.« less

Plutonium in the atmosphere: A global perspective.

PubMed

Thakur, P; Khaing, H; Salminen-Paatero, S

2017-09-01

A number of potential source terms have contributed plutonium isotopes to the atmosphere. The atmospheric nuclear weapon tests conducted between 1945 and 1980 and the re-entry of the burned SNAP-9A satellite in 1964, respectively. It is generally believed that current levels of plutonium in the stratosphere are negligible and compared with the levels generally found at surface-level air. In this study, the time trend analysis and long-term behavior of plutonium isotopes ( 239+240 Pu and 238 Pu) in the atmosphere were assessed using historical data collected by various national and international monitoring networks since 1960s. An analysis of historical data indicates that 239+240 Pu concentration post-1984 is still frequently detectable, whereas 238 Pu is detected infrequently. Furthermore, the seasonal and time-trend variation of plutonium concentration in surface air followed the stratospheric trends until the early 1980s. After the last Chinese test of 1980, the plutonium concentrations in surface air dropped to the current levels, suggesting that the observed concentrations post-1984 have not been under stratospheric control, but rather reflect the environmental processes such as resuspension. Recent plutonium atmospheric air concentrations data show that besides resuspension, other environmental processes such as global dust storms and biomass burning/wildfire also play an important role in redistributing plutonium in the atmosphere. Copyright © 2017 Elsevier Ltd. All rights reserved.

Measurement of 240Pu/239Pu isotopic ratios in soils from the Marshall Islands using ICP-MS.

PubMed

Muramatsu, Y; Hamilton, T; Uchida, S; Tagami, K; Yoshida, S; Robison, W

2001-10-20

Nuclear weapons tests conducted by the United States in the Marshall Islands produced significant quantities of regional or tropospheric fallout contamination. Here we report on some preliminary inductively coupled plasma-mass spectrometry (ICP-MS) measurements of plutonium isolated from seven composite soil samples collected from Bikini, Enewetak and Rongelap Atolls in the northern Marshall Islands. These data show that 240Pu/239Pu isotopic signatures in surface soils from the Marshall Island vary significantly and could potentially be used to help quantify the range and extent of fallout deposition (and associated impacts) from specific weapons tests. 137Cs and 60Co were also determined on the same set of soil samples for comparative purposes.

Sensitivity and Uncertainty Analysis of Plutonium and Cesium Isotopes in Modeling of BR3 Reactor Spent Fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Conant, Andrew; Erickson, Anna; Robel, Martin

Nuclear forensics has a broad task to characterize recovered nuclear or radiological material and interpret the results of investigation. One approach to isotopic characterization of nuclear material obtained from a reactor is to chemically separate and perform isotopic measurements on the sample and verify the results with modeling of the sample history, for example, operation of a nuclear reactor. The major actinide plutonium and fission product cesium are commonly measured signatures of the fuel history in a reactor core. This study investigates the uncertainty of the plutonium and cesium isotope ratios of a fuel rod discharged from a research pressurizedmore » water reactor when the location of the sample is not known a priori. A sensitivity analysis showed overpredicted values for the 240Pu/ 239Pu ratio toward the axial center of the rod and revealed a lower probability of the rod of interest (ROI) being on the periphery of the assembly. The uncertainty analysis found the relative errors due to only the rod position and boron concentration to be 17% to 36% and 7% to 15% for the 240Pu/ 239Pu and 137Cs/ 135Cs ratios, respectively. Lastly, this study provides a method for uncertainty quantification of isotope concentrations due to the location of the ROI. Similar analyses can be performed to verify future chemical and isotopic analyses.« less

Sensitivity and Uncertainty Analysis of Plutonium and Cesium Isotopes in Modeling of BR3 Reactor Spent Fuel

DOE PAGES

Conant, Andrew; Erickson, Anna; Robel, Martin; ...

2017-02-03

Nuclear forensics has a broad task to characterize recovered nuclear or radiological material and interpret the results of investigation. One approach to isotopic characterization of nuclear material obtained from a reactor is to chemically separate and perform isotopic measurements on the sample and verify the results with modeling of the sample history, for example, operation of a nuclear reactor. The major actinide plutonium and fission product cesium are commonly measured signatures of the fuel history in a reactor core. This study investigates the uncertainty of the plutonium and cesium isotope ratios of a fuel rod discharged from a research pressurizedmore » water reactor when the location of the sample is not known a priori. A sensitivity analysis showed overpredicted values for the 240Pu/ 239Pu ratio toward the axial center of the rod and revealed a lower probability of the rod of interest (ROI) being on the periphery of the assembly. The uncertainty analysis found the relative errors due to only the rod position and boron concentration to be 17% to 36% and 7% to 15% for the 240Pu/ 239Pu and 137Cs/ 135Cs ratios, respectively. Lastly, this study provides a method for uncertainty quantification of isotope concentrations due to the location of the ROI. Similar analyses can be performed to verify future chemical and isotopic analyses.« less

Plutonium segregation in glassy aerodynamic fallout from a nuclear weapon test

DOE PAGES

Holliday, K. S.; Dierken, J. M.; Monroe, M. L.; ...

2017-01-11

Our study combines electron microscopy equipped with energy dispersive spectroscopy to probe major element composition and autoradiography to map plutonium in order to examine the spatial relationships between plutonium and fallout composition in aerodynamic glassy fallout from a nuclear weapon test. We interrogated a sample set of 48 individual fallout specimens in order to reveal that the significant chemical heterogeneity of this sample set could be described compositionally with a relatively small number of compositional endmembers. Furthermore, high concentrations of plutonium were never associated with several endmember compositions and concentrated with the so-called mafic glass endmember. Our result suggests thatmore » it is the physical characteristics of the compositional endmembers and not the chemical characteristics of the individual component elements that govern the un-burnt plutonium distribution with respect to major element composition in fallout.« less

Multirecycling of Plutonium from LMFBR Blanket in Standard PWRs Loaded with MOX Fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sonat Sen; Gilles Youinou

2013-02-01

It is now well-known that, from a physics standpoint, Pu, or even TRU (i.e. Pu+M.A.), originating from LEU fuel irradiated in PWRs can be multirecycled also in PWRs using MOX fuel. However, the degradation of the isotopic composition during irradiation necessitates using enriched U in conjunction with the MOX fuel either homogeneously or heterogeneously to maintain the Pu (or TRU) content at a level allowing safe operation of the reactor, i.e. below about 10%. The study is related to another possible utilization of the excess Pu produced in the blanket of a LMFBR, namely in a PWR(MOX). In this casemore » the more Pu is bred in the LMFBR, the more PWR(MOX) it can sustain. The important difference between the Pu coming from the blanket of a LMFBR and that coming from a PWR(LEU) is its isotopic composition. The first one contains about 95% of fissile isotopes whereas the second one contains only about 65% of fissile isotopes. As it will be shown later, this difference allows the PWR fed by Pu from the LMFBR blanket to operate with natural U instead of enriched U when it is fed by Pu from PWR(LEU)« less

15. VIEW OF LABORATORY EQUIPMENT IN THE BUILDING 771 ANALYTICAL ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

15. VIEW OF LABORATORY EQUIPMENT IN THE BUILDING 771 ANALYTICAL LABORATORY. THE LAB ANALYZED SAMPLES FOR PLUTONIUM, AMERICIUM, URANIUM, NEPTUNIUM, AND OTHER RADIOACTIVE ISOTOPES. (9/25/62) - Rocky Flats Plant, Plutonium Recovery & Fabrication Facility, North-central section of plant, Golden, Jefferson County, CO

Plutonium Story

DOE R&D Accomplishments Database

Seaborg, G. T.

1981-09-01

The first nuclear synthesis and identification (i.e., the discovery) of the synthetic transuranium element plutonium (isotope /sup 238/Pu) and the demonstration of its fissionability with slow neutrons (isotope /sup 239/Pu) took place at the University of California, Berkeley, through the use of the 60-inch and 37-inch cyclotrons, in late 1940 and early 1941. This led to the development of industrial scale methods in secret work centered at the University of Chicago's Metallurgical Laboratory and the application of these methods to industrial scale production, at manufacturing plants in Tennessee and Washington, during the World War II years 1942 to 1945. The chemical properties of plutonium, needed to devise the procedures for its industrial scale production, were studied by tracer and ultramicrochemical methods during this period on an extraordinarily urgent basis. This work, and subsequent investigations on a worldwide basis, have made the properties of plutonium very well known. Its well studied electronic structure and chemical properties give it a very interesting position in the actinide series of inner transition elements.

SPRAY CALCINATION REACTOR

DOEpatents

Johnson, B.M.

1963-08-20

A spray calcination reactor for calcining reprocessin- g waste solutions is described. Coaxial within the outer shell of the reactor is a shorter inner shell having heated walls and with open regions above and below. When the solution is sprayed into the irner shell droplets are entrained by a current of gas that moves downwardly within the inner shell and upwardly between it and the outer shell, and while thus being circulated the droplets are calcined to solids, whlch drop to the bottom without being deposited on the walls. (AEC) H03 H0233412 The average molecular weights of four diallyl phthalate polymer samples extruded from the experimental rheometer were redetermined using the vapor phase osmometer. An amine curing agent is required for obtaining suitable silver- filled epoxy-bonded conductive adhesives. When the curing agent was modified with a 47% polyurethane resin, its effectiveness was hampered. Neither silver nor nickel filler impart a high electrical conductivity to Adiprenebased adhesives. Silver filler was found to perform well in Dow-Corning A-4000 adhesive. Two cascaded hot-wire columns are being used to remove heavy gaseous impurities from methane. This purified gas is being enriched in the concentric tube unit to approximately 20% carbon-13. Studies to count low-level krypton-85 in xenon are continuing. The parameters of the counting technique are being determined. The bismuth isotopes produced in bismuth irradiated for polonium production are being determined. Preliminary data indicate the presence of bismuth207 and bismuth-210m. The light bismuth isotopes are probably produced by (n,xn) reactions bismuth-209. The separation of uranium-234 from plutonium-238 solutions was demonstrated. The bulk of the plutonium is removed by anion exchange, and the remainder is extracted from the uranium by solvent extraction techniques. About 99% of the plutonium can be removed in each thenoyltrifluoroacetone extraction. The viscosity, liquid density, and selfdiffusion coefficient for lanthanum, cerium, and praseodymium were determined. The investigation of phase relationships in the plutonium-cerium-copper ternary system was continued on samples containing a high concentration of copper. These analyses indicate that complete solid solution exists between the binary compounds CeCu/sub 2/ and PuCu/sub 2/, thus forming a quasi-binary system. The study of high temperature ceramic fuel materials has continued with the homogenization and microspheroidization of binary mixtures of plutonium dioxide and zirconium dioxide. Sintering a die-pressed pellet of the mixed powders for one hour at 1450 deg C was not sufficient to completely react the constituents. Complete homogenization was obtained when the pellet was melted in the plasma flame. In addition to the plutonium dioxide-zirconium dioxide microspheres, pure beryllium oxide microspheres were produced in the plasma torch. The electronic distribution functions for the 10% by weight PuO/sub 2/ dissolved in a silicate glass were determined. The plutonium-oxygen interaction at about 2.2A is less than the plutonium-oxygen distance for the 5% PuO/sub 2/. The decrease in the interionic distance is indicative of a stronger plutonium-oxygen association for the more concentrated composition. Potassium plutonium sulfate is being evaluated as a reagent to quantitatively separate plutonium from aqueous solutions. The compound containing two waters of hydration was prepared for thermogravimetric studies using analytically pure plutonium-239. Because of the stability of this compound, it is being evaluated as a calorimetric standard for plutonium-238. (auth)

Assessment of the radionuclide composition of "hot particles" sampled in the Chernobyl nuclear power plant fourth reactor unit.

PubMed

Bondarkov, Mikhail D; Zheltonozhsky, Viktor A; Zheltonozhskaya, Maryna V; Kulich, Nadezhda V; Maksimenko, Andrey M; Farfán, Eduardo B; Jannik, G Timothy; Marra, James C

2011-10-01

Fuel-containing materials sampled from within the Chernobyl Nuclear Power Plant (ChNPP) Unit 4 Confinement Shelter were spectroscopically studied for gamma and alpha content. Isotopic ratios for cesium, europium, plutonium, americium, and curium were identified, and the fuel burn-up in these samples was determined. A systematic deviation in the burn-up values based on the cesium isotopes in comparison with other radionuclides was observed. The studies conducted were the first ever performed to demonstrate the presence of significant quantities of 242Cm and 243Cm. It was determined that there was a systematic underestimation of activities of transuranic radionuclides in fuel samples from inside of the ChNPP Confinement Shelter, starting from 241Am (and going higher) in comparison with the theoretical calculations.

Chemical Disposition of Plutonium in Hanford Site Tank Wastes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Delegard, Calvin H.; Jones, Susan A.

2015-05-07

This report examines the chemical disposition of plutonium (Pu) in Hanford Site tank wastes, by itself and in its observed and potential interactions with the neutron absorbers aluminum (Al), cadmium (Cd), chromium (Cr), iron (Fe), manganese (Mn), nickel (Ni), and sodium (Na). Consideration also is given to the interactions of plutonium with uranium (U). No consideration of the disposition of uranium itself as an element with fissile isotopes is considered except tangentially with respect to its interaction as an absorber for plutonium. The report begins with a brief review of Hanford Site plutonium processes, examining the various means used tomore » recover plutonium from irradiated fuel and from scrap, and also examines the intermediate processing of plutonium to prepare useful chemical forms. The paper provides an overview of Hanford tank defined-waste–type compositions and some calculations of the ratios of plutonium to absorber elements in these waste types and in individual waste analyses. These assessments are based on Hanford tank waste inventory data derived from separately published, expert assessments of tank disposal records, process flowsheets, and chemical/radiochemical analyses. This work also investigates the distribution and expected speciation of plutonium in tank waste solution and solid phases. For the solid phases, both pure plutonium compounds and plutonium interactions with absorber elements are considered. These assessments of plutonium chemistry are based largely on analyses of idealized or simulated tank waste or strongly alkaline systems. The very limited information available on plutonium behavior, disposition, and speciation in genuine tank waste also is discussed. The assessments show that plutonium coprecipitates strongly with chromium, iron, manganese and uranium absorbers. Plutonium’s chemical interactions with aluminum, nickel, and sodium are minimal to non-existent. Credit for neutronic interaction of plutonium with these absorbers occurs only if they are physically proximal in solution or the plutonium present in the solid phase is intimately mixed with compounds or solutions of these absorbers. No information on the potential chemical interaction of plutonium with cadmium was found in the technical literature. Definitive evidence of sorption or adsorption of plutonium onto various solid phases from strongly alkaline media is less clear-cut, perhaps owing to fewer studies and to some well-attributed tests run under conditions exceeding the very low solubility of plutonium. The several studies that are well-founded show that only about half of the plutonium is adsorbed from waste solutions onto sludge solid phases. The organic complexants found in many Hanford tank waste solutions seem to decrease plutonium uptake onto solids. A number of studies show plutonium sorbs effectively onto sodium titanate. Finally, this report presents findings describing the behavior of plutonium vis-à-vis other elements during sludge dissolution in nitric acid based on Hanford tank waste experience gained by lab-scale tests, chemical and radiochemical sample characterization, and full-scale processing in preparation for strontium-90 recovery from PUREX sludges.« less

Stability of zinc stearate under alpha irradiation in the manufacturing process of SFR nuclear fuels

NASA Astrophysics Data System (ADS)

Gracia, J.; Vermeulen, J.; Baux, D.; Sauvage, T.; Venault, L.; Audubert, F.; Colin, X.

2018-03-01

The manufacture of new fuels for sodium-cooled fast reactors (SFRs) will involve powders derived from recycling existing fuels in order to keep on producing electricity while saving natural resources and reducing the amount of waste produced by spent MOX fuels. Using recycled plutonium in this way will significantly increase the amount of 238Pu, a high energy alpha emitter, in the powders. The process of shaping powders by pressing requires the use of a solid lubricant, zinc stearate, to produce pellets with no defects compliant with the standards. The purpose of this study is to determine the impact of alpha radiolysis on this additive and its lubrication properties. Experiments were conducted on samples in contact with PuO2, as well as under external helium ion beam irradiation, in order to define the kinetics of radiolytic gas generation. The yield results relating to the formation of these gases (G0) show that the alpha radiation of plutonium can be simulated using external helium ion beam irradiation. The isotopic composition of plutonium has little impact on the yield. However, an increased yield was globally observed with increasing the mean linear energy transfer (LET). A radiolytic degradation process is proposed.

Determination of Plutonium Isotope Ratios at Very Low Levels by ICP-MS using On-Line Electrochemically Modulated Separations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liezers, Martin; Lehn, Scott A; Olsen, Khris B

2009-10-01

Electrochemically modulated separations (EMS) are shown to be a rapid and selective means of extracting and concentrating Pu from complex solutions prior to isotopic analysis by inductively coupled plasma mass spectrometry (ICP-MS). This separation is performed in a flow injection mode, on-line with the ICP-MS. A three-electrode, flow-by electrochemical cell is used to accumulate Pu at an anodized glassy carbon electrode by redox conversion of Pu(III) to Pu (IV&VI). The entire process takes place in 2% v/v (0.46M) HNO 3. No redox chemicals or acid concentration changes are required. Plutonium accumulation and release is redox dependent and controlled by themore » applied cell potential. Thus large transient volumetric concentration enhancements can be achieved. Based on more negative U(IV) potentials relative to Pu(IV), separation of Pu from uranium is efficient, thereby eliminating uranium hydride interferences. EMS-ICP-MS isotope ratio measurement performance will be presented for femtogram to attogram level plutonium concentrations.« less

Plutonium isotopes in the Hungarian environment.

PubMed

Varga, Beata; Tarján, Sandor; Vajda, Nora

2008-04-01

More than 50 soil samples were analysed from different parts of the country, the activity concentration of 239+240Pu was in the range of 0.01-0.84 Bq/kg dry soil with the average of 0.10 Bq/kg. 238Pu could be detected only in few moss samples and 238Pu/239+240Pu ratio determines the origin of plutonium. 241Pu was determined by liquid scintillation spectrometry. The activity concentration of this isotope in the soil is between 0.04 and 3.74 Bq/kg with the average of 0.82 Bq/kg, while in the moss is also similar 0.01-2.07 Bq/kg fresh mass with the average of 0.43 Bq/kg. Significant difference could not be observed between the different types of soils occurring in the country, but the results could be sorted according to the sampling carried out on undisturbed or cultivated area. The isotope ratios 241Pu/239+240Pu prove that the origin of the plutonium in Hungary is the global fallout determined by the atmospheric nuclear weapon tests.

AMS of the Minor Plutonium Isotopes

NASA Astrophysics Data System (ADS)

Steier, P.; Hrnecek, E.; Priller, A.; Quinto, F.; Srncik, M.; Wallner, A.; Wallner, G.; Winkler, S.

2013-01-01

VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure 239Pu, 240Pu, 241Pu, 242Pu and 244Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of 244Pu/239Pu = (5.7 ± 1.0) × 10-5 based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the 242Pu/240Pu ratio as an estimate of the initial 241Pu/239Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method.

Determining the dissolution rates of actinide glasses: A time and temperature Product Consistency Test study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Daniel, W.E.; Best, D.R.

1995-12-01

Vitrification has been identified as one potential option for the e materials such as Americium (Am), Curium (Cm), Neptunium (Np), and Plutonium (Pu). A process is being developed at the Savannah River Site to safely vitrify all of the highly radioactive Am/Cm material and a portion of the fissile (Pu) actinide materials stored on site. Vitrification of the Am/Cm will allow the material to be transported and easily stored at the Oak Ridge National Laboratory. The Am/Cm glass has been specifically designed to be (1) highly durable in aqueous environments and (2) selectively attacked by nitric acid to allow recoverymore » of the valuable Am and Cm isotopes. A similar glass composition will allow for safe storage of surplus plutonium. This paper will address the composition, relative durability, and dissolution rate characteristics of the actinide glass, Loeffler Target, that will be used in the Americium/Curium Vitrification Project at Westinghouse Savannah River Company near Aiken, South Carolina. The first part discusses the tests performed on the Loeffler Target Glass concerning instantaneous dissolution rates. The second part presents information concerning pseudo-activation energy for the one week glass dissolution process.« less

Radioisotope contaminations from releases of the Tomsk-Seversk nuclear facility (Siberia, Russia).

PubMed

Gauthier-Lafaye, F; Pourcelot, L; Eikenberg, J; Beer, H; Le Roux, G; Rhikvanov, L P; Stille, P; Renaud, Ph; Mezhibor, A

2008-04-01

Soils have been sampled in the vicinity of the Tomsk-Seversk facility (Siberia, Russia) that allows us to measure radioactive contaminations due to atmospheric and aquatic releases. Indeed soils exhibit large inventories of man-made fission products including 137Cs (ranging from 33,000 to 68,500 Bq m(-2)) and actinides such as plutonium (i.e. 239+240Pu from 420 to 5900 Bq m(-2)) or 241Am (160-1220 Bq m(-2)). Among all sampling sites, the bank of the Romashka channel exhibits the highest radioisotope concentrations. At this site, some short half-life gamma emitters were detected as well indicating recent aquatic discharge in the channel. In comparison, soils that underwent atmospheric depositions like peat and forest soils exhibit lower activities of actinides and 137Cs. Soil activities are too high to be related solely to global fallout and thus the source of plutonium must be discharges from the Siberian Chemical Combine (SCC) plant. This is confirmed by plutonium isotopic ratios measured by ICP-MS; the low 241Pu/239Pu and 240Pu/239Pu atomic ratios with respect to global fallout ratio or civil nuclear fuel are consistent with weapons grade signatures. Up to now, the influence of Tomsk-Seversk plutonium discharges was speculated in the Ob River and its estuary. Isotopic data from the present study show that plutonium measured in SCC probably constitutes a significant source of plutonium in the aquatic environment, together with plutonium from global fallout and other contaminated sites including Tomsk, Mayak (Russia) and Semipalatinsk (Republic of Kazakhstan). It is estimated that the proportion of plutonium from SCC source can reach 45% for 239Pu and 60% for 241Pu in the sediments.

Effect of Americium-241 Content on Plutonium Radiation Source Terms

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rainisch, R.

1998-12-28

The management of excess plutonium by the US Department of Energy includes a number of storage and disposition alternatives. Savannah River Site (SRS) is supporting DOE with plutonium disposition efforts, including the immobilization of certain plutonium materials in a borosilicate glass matrix. Surplus plutonium inventories slated for vitrification include materials with elevated levels of Americium-241. The Am-241 content of plutonium materials generally reflects in-growth of the isotope due to decay of plutonium and is age-dependent. However, select plutonium inventories have Am-241 levels considerably above the age-based levels. Elevated levels of americium significantly impact radiation source terms of plutonium materials andmore » will make handling of the materials more difficult. Plutonium materials are normally handled in shielded glove boxes, and the work entails both extremity and whole body exposures. This paper reports results of an SRS analysis of plutonium materials source terms vs. the Americium-241 content of the materials. Data with respect to dependence and magnitude of source terms on/vs. Am-241 levels are presented and discussed. The investigation encompasses both vitrified and un-vitrified plutonium oxide (PuO2) batches.« less

A Graphical Examination of Uranium and Plutonium Fissility

ERIC Educational Resources Information Center

Reed, B. Cameron

2008-01-01

The issue of why only particular isotopes of uranium and plutonium are suitable for use in nuclear weapons is analyzed with the aid of graphs and semiquantitative discussions of parameters such as excitation energies, fission barriers, reaction cross-sections, and the role of processes such as [alpha]-decay and spontaneous fission. The goal is to…

10 CFR 150.14 - Commission regulatory authority for physical protection.

Code of Federal Regulations, 2012 CFR

2012-01-01

... significance in quantities greater than 15 grams of plutonium or uranium-233 or uranium-235 (enriched to 20 percent or more in the U-235 isotope) or any combination greater than 15 grams when computed by the equation grams=grams uranium-235+grams plutonium+grams uranium-233 shall meet the physical protection...

10 CFR 150.14 - Commission regulatory authority for physical protection.

Code of Federal Regulations, 2010 CFR

2010-01-01

... significance in quantities greater than 15 grams of plutonium or uranium-233 or uranium-235 (enriched to 20 percent or more in the U-235 isotope) or any combination greater than 15 grams when computed by the equation grams=grams uranium-235+grams plutonium+grams uranium-233 shall meet the physical protection...

10 CFR 150.14 - Commission regulatory authority for physical protection.

Code of Federal Regulations, 2011 CFR

2011-01-01

... significance in quantities greater than 15 grams of plutonium or uranium-233 or uranium-235 (enriched to 20 percent or more in the U-235 isotope) or any combination greater than 15 grams when computed by the equation grams=grams uranium-235+grams plutonium+grams uranium-233 shall meet the physical protection...

10 CFR 150.14 - Commission regulatory authority for physical protection.

Code of Federal Regulations, 2013 CFR

2013-01-01

... significance in quantities greater than 15 grams of plutonium or uranium-233 or uranium-235 (enriched to 20 percent or more in the U-235 isotope) or any combination greater than 15 grams when computed by the equation grams=grams uranium-235+grams plutonium+grams uranium-233 shall meet the physical protection...

10 CFR 150.14 - Commission regulatory authority for physical protection.

Code of Federal Regulations, 2014 CFR

2014-01-01

... significance in quantities greater than 15 grams of plutonium or uranium-233 or uranium-235 (enriched to 20 percent or more in the U-235 isotope) or any combination greater than 15 grams when computed by the equation grams=grams uranium-235+grams plutonium+grams uranium-233 shall meet the physical protection...

Plutonium Bioassay Testing of U.S. Atmospheric Nuclear Test Participants and U.S. Occupation Forces of Hiroshima and Nagasaki, Japan

DTIC Science & Technology

2015-10-30

with nuclear weapons testing or plutonium work. The results for the 100 atomic veterans were compared to those of the unexposed population, and...as a marker for significant internal intakes of other associated radionuclides in nuclear weapons debris due to its low natural background. However...isotope in weapons grade plutonium, is important from a health perspective, its presence within a given urine sample being analyzed by FTA can only

Some neutron and gamma radiation characteristics of plutonium cermet fuel for isotopic power sources

NASA Technical Reports Server (NTRS)

Neff, R. A.; Anderson, M. E.; Campbell, A. R.; Haas, F. X.

1972-01-01

Gamma and neutron measurements on various types of plutonium sources are presented in order to show the effects of O-17, O-18 F-19, Pu-236, age of the fuel, and size of the source on the gamma and neutron spectra. Analysis of the radiation measurements shows that fluorine is the main contributor to the neutron yields from present plutonium-molybdenum cermet fuel, while both fluorine and Pu-236 daughters contribute significantly to the gamma ray intensities.

ASSESSMENT OF THE RADIONUCLIDE COMPOSITION OF "HOT PARTICLES" SAMPLED IN THE CHERNOBYL NUCLEAR POWER PLANT FOURTH REACTOR UNIT

DOE Office of Scientific and Technical Information (OSTI.GOV)

Farfan, E.; Jannik, T.; Marra, J.

2011-10-01

Fuel-containing materials sampled from within the Chernobyl Nuclear Power Plant (ChNPP) 4th Reactor Unit Confinement Shelter were spectroscopically studied for gamma and alpha content. Isotopic ratios for cesium, europium, plutonium, americium, and curium were identified and the fuel burnup in these samples was determined. A systematic deviation in the burnup values based on the cesium isotopes, in comparison with other radionuclides, was observed. The conducted studies were the first ever performed to demonstrate the presence of significant quantities of {sup 242}Cm and {sup 243}Cm. It was determined that there was a systematic underestimation of activities of transuranic radionuclides in fuelmore » samples from inside of the ChNPP Confinement Shelter, starting from {sup 241}Am (and going higher), in comparison with the theoretical calculations.« less

Certified reference materials and reference methods for nuclear safeguards and security.

PubMed

Jakopič, R; Sturm, M; Kraiem, M; Richter, S; Aregbe, Y

2013-11-01

Confidence in comparability and reliability of measurement results in nuclear material and environmental sample analysis are established via certified reference materials (CRMs), reference measurements, and inter-laboratory comparisons (ILCs). Increased needs for quality control tools in proliferation resistance, environmental sample analysis, development of measurement capabilities over the years and progress in modern analytical techniques are the main reasons for the development of new reference materials and reference methods for nuclear safeguards and security. The Institute for Reference Materials and Measurements (IRMM) prepares and certifices large quantities of the so-called "large-sized dried" (LSD) spikes for accurate measurement of the uranium and plutonium content in dissolved nuclear fuel solutions by isotope dilution mass spectrometry (IDMS) and also develops particle reference materials applied for the detection of nuclear signatures in environmental samples. IRMM is currently replacing some of its exhausted stocks of CRMs with new ones whose specifications are up-to-date and tailored for the demands of modern analytical techniques. Some of the existing materials will be re-measured to improve the uncertainties associated with their certified values, and to enable laboratories to reduce their combined measurement uncertainty. Safeguards involve the quantitative verification by independent measurements so that no nuclear material is diverted from its intended peaceful use. Safeguards authorities pay particular attention to plutonium and the uranium isotope (235)U, indicating the so-called 'enrichment', in nuclear material and in environmental samples. In addition to the verification of the major ratios, n((235)U)/n((238)U) and n((240)Pu)/n((239)Pu), the minor ratios of the less abundant uranium and plutonium isotopes contain valuable information about the origin and the 'history' of material used for commercial or possibly clandestine purposes, and have therefore reached high level of attention for safeguards authorities. Furthermore, IRMM initiated and coordinated the development of a Modified Total Evaporation (MTE) technique for accurate abundance ratio measurements of the "minor" isotope-amount ratios of uranium and plutonium in nuclear material and, in combination with a multi-dynamic measurement technique and filament carburization, in environmental samples. Currently IRMM is engaged in a study on the development of plutonium reference materials for "age dating", i.e. determination of the time elapsed since the last separation of plutonium from its daughter nuclides. The decay of a radioactive parent isotope and the build-up of a corresponding amount of daughter nuclide serve as chronometer to calculate the age of a nuclear material. There are no such certified reference materials available yet. Copyright © 2013 Elsevier Ltd. All rights reserved.

Preparation, certification and validation of a stable solid spike of uranium and plutonium coated with a cellulose derivative for the measurement of uranium and plutonium content in dissolved nuclear fuel by isotope dilution mass spectrometry.

PubMed

Surugaya, Naoki; Hiyama, Toshiaki; Verbruggen, André; Wellum, Roger

2008-02-01

A stable solid spike for the measurement of uranium and plutonium content in nitric acid solutions of spent nuclear fuel by isotope dilution mass spectrometry has been prepared at the European Commission Institute for Reference Materials and Measurements in Belgium. The spike contains about 50 mg of uranium with a 19.838% (235)U enrichment and 2 mg of plutonium with a 97.766% (239)Pu abundance in each individual ampoule. The dried materials were covered with a thin film of cellulose acetate butyrate as a protective organic stabilizer to resist shocks encountered during transportation and to eliminate flaking-off during long-term storage. It was found that the cellulose acetate butyrate has good characteristics, maintaining a thin film for a long time, but readily dissolving on heating with nitric acid solution. The solid spike containing cellulose acetate butyrate was certified as a reference material with certified quantities: (235)U and (239)Pu amounts and uranium and plutonium amount ratios, and was validated by analyzing spent fuel dissolver solutions of the Tokai reprocessing plant in Japan. This paper describes the preparation, certification and validation of the solid spike coated with a cellulose derivative.

Release of plutonium isotopes into the environment from the Fukushima Daiichi Nuclear Power Plant accident: what is known and what needs to be known.

PubMed

Zheng, Jian; Tagami, Keiko; Uchida, Shigeo

2013-09-03

The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has caused serious contamination in the environment. The release of Pu isotopes renewed considerable public concern because they present a large risk for internal radiation exposure. In this Critical Review, we summarize and analyze published studies related to the release of Pu from the FDNPP accident based on environmental sample analyses and the ORIGEN model simulations. Our analysis emphasizes the environmental distribution of released Pu isotopes, information on Pu isotopic composition for source identification of Pu releases in the FDNPP-damaged reactors or spent fuel pools, and estimation of the amounts of Pu isotopes released from the FDNPP accident. Our analysis indicates that a trace amount of Pu isotopes (∼2 × 10(-5)% of core inventory) was released into the environment from the damaged reactors but not from the spent fuel pools located in the reactor buildings. Regarding the possible Pu contamination in the marine environment, limited studies suggest that no extra Pu input from the FDNPP accident could be detected in the western North Pacific 30 km off the Fukushima coast. Finally, we identified knowledge gaps remained on the release of Pu into the environment and recommended issues for future studies.

Heterogeneous sodium fast reactor designed for transmuting minor actinide waste isotopes into plutonium fuel

NASA Astrophysics Data System (ADS)

Bays, Samuel Eugene

2008-10-01

In the past several years there has been a renewed interest in sodium fast reactor (SFR) technology for the purpose of destroying transuranic waste (TRU) produced by light water reactors (LWR). The utility of SFRs as waste burners is due to the fact that higher neutron energies allow all of the actinides, including the minor actinides (MA), to contribute to fission. It is well understood that many of the design issues of LWR spent nuclear fuel (SNF) disposal in a geologic repository are linked to MAs. Because the probability of fission for essentially all the "non-fissile" MAs is nearly zero at low neutron energies, these isotopes act as a neutron capture sink in most thermal reactor systems. Furthermore, because most of the isotopes produced by these capture reactions are also non-fissile, they too are neutron sinks in most thermal reactor systems. Conversely, with high neutron energies, the MAs can produce neutrons by fast fission. Additionally, capture reactions transmute the MAs into mostly plutonium isotopes, which can fission more readily at any energy. The transmutation of non-fissile into fissile atoms is the premise of the plutonium breeder reactor. In a breeder reactor, not only does the non-fissile "fertile" U-238 atom contribute fast fission neutrons, but also transmutes into fissile Pu-239. The fissile value of the plutonium produced by MA transmutation can only be realized in fast neutron spectra. This is due to the fact that the predominate isotope produced by MA transmutation, Pu-238, is itself not fissile. However, the Pu-238 fission cross section is significantly larger than the original transmutation parent, predominately: Np-237 and Am-241, in the fast energy range. Also, Pu-238's fission cross section and fission-to-capture ratio is almost as high as that of fissile Pu-239 in the fast neutron spectrum. It is also important to note that a neutron absorption in Pu-238, that does not cause fission, will instead produce fissile Pu-239. Given this fast fissile quality and also the fact that Pu-238 is transmuted from Np-237 and Am-241, these MAs are regarded as fertile material in the SFR design proposed by this dissertation. This dissertation demonstrates a SFR design which is dedicated to plutonium breeding by targeting Am-241 transmutation. This SFR design uses a moderated axial transmutation target that functions primarily as a pseudo-blanket fuel, which is reprocessed with the active driver fuel in an integrated recycling strategy. This work demonstrates the cost and feasibility advantages of plutonium breeding via MA transmutation by adopting reactor, reprocessing and fuel technologies previously demonstrated for traditional breeder reactors. The fuel cycle proposed seeks to find a harmony between the waste management advantages of transuranic burning SFRs and the resource sustainability of traditional plutonium breeder SFRs. As a result, the enhanced plutonium conversion from MAs decreases the burner SFR's fuel costs, by extracting more fissile value from the initial TRU purchased through SNF reprocessing.

Historical review of californium-252 discovery and development

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stoddard, D.H.

1985-01-01

This paper discusses the discovery and history of californium 252. This isotope may be synthesized by irradiating plutonium 239, plutonium 242, americium 243, or curium 244 with neutrons in a nuclear reactor. Various experiments and inventions involving /sup 252/Cf conducted at the Savannah River Plant are discussed. The evolution of radiotherapy using californium 252 is reviewed. (PLG)

Historical Review of Californium-252 Discovery and Development

DOE R&D Accomplishments Database

Stoddard, D. H.

1985-01-01

This paper discusses the discovery and history of californium 252. This isotope may be synthesized by irradiating plutonium 239, plutonium 242, americium 243, or curium 244 with neutrons in a nuclear reactor. Various experiments and inventions involving Cf conducted at the Savannah River Plant are discussed. The evolution of radiotherapy using californium 252 is reviewed. (PLG)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Savina, Joseph A.; Steeb, Jennifer L.; Savina, Michael R.

A plutonium alpha standard dating from 1948 was discovered at Argonne National Laboratory and characterized using a number of non-destructive analytical techniques. The principle radioactive isotope was found to be 239Pu and unique ring structures were found across the surface of the deposition area. Due to chronological constraints on possible sources and its high isotopic purity, the plutonium in the sample was likely produced by the Oak Ridge National Lab X-10 Reactor. As a result, it is proposed that the rings are resultant through a combination of polishing and electrodeposition, though the hypothesis fails to address a few key featuresmore » of the ring structures.« less

Determination of 240Pu/239Pu isotopic ratios in human tissues collected from areas around the Semipalatinsk Nuclear Test Site by sector-field high resolution ICP-MS.

PubMed

Yamamoto, M; Oikawa, S; Sakaguchi, A; Tomita, J; Hoshi, M; Apsalikov, K N

2008-09-01

Information on the 240Pu/239Pu isotope ratios in human tissues for people living around the Semipalatinsk Nuclear Test Site (SNTS) was deduced from 9 sets of soft tissues and bones, and 23 other bone samples obtained by autopsy. Plutonium was radiochemically separated and purified, and plutonium isotopes (239Pu and 240Pu) were determined by sector-field high resolution inductively coupled plasma-mass spectrometry. For most of the tissue samples from the former nine subjects, low 240Pu/239Pu isotope ratios were determined: bone, 0.125 +/- 0.018 (0.113-0.145, n = 4); lungs, 0.063 +/- 0.010 (0.051-0.078, n = 5); and liver, 0.148 +/- 0.026 (0.104-0.189, n = 9). Only 239Pu was detected in the kidney samples; the amount of 240Pu was too small to be measured, probably due to the small size of samples analyzed. The mean 240Pu/239Pu isotope ratio for bone samples from the latter 23 subjects was 0.152 +/- 0.034, ranging from 0.088 to 0.207. A significant difference (a two-tailed Student's t test; 95% significant level, alpha = 0.05) between mean 240Pu/239Pu isotope ratios for the tissue samples and for the global fallout value (0.178 +/- 0.014) indicated that weapons-grade plutonium from the atomic bombs has been incorporated into the human tissues, especially lungs, in the residents living around the SNTS. The present 239,240Pu concentrations in bone, lung, and liver samples were, however, not much different from ranges found for human tissues from other countries that were due solely to global fallout during the 1970's-1980's.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carmack, Jon; Hayes, Steven; Walters, L. C.

This document explores startup fuel options for a proposed test/demonstration fast reactor. The fuel options considered are the metallic fuels U-Zr and U-Pu-Zr and the ceramic fuels UO 2 and UO 2-PuO 2 (MOX). Attributes of the candidate fuel choices considered were feedstock availability, fabrication feasibility, rough order of magnitude cost and schedule, and the existing irradiation performance database. The reactor-grade plutonium bearing fuels (U-Pu-Zr and MOX) were eliminated from consideration as the initial startup fuels because the availability and isotopics of domestic plutonium feedstock is uncertain. There are international sources of reactor grade plutonium feedstock but isotopics and availabilitymore » are also uncertain. Weapons grade plutonium is the only possible source of Pu feedstock in sufficient quantities needed to fuel a startup core. Currently, the available U.S. source of (excess) weapons-grade plutonium is designated for irradiation in commercial light water reactors (LWR) to a level that would preclude diversion. Weapons-grade plutonium also contains a significant concentration of gallium. Gallium presents a potential issue for both the fabrication of MOX fuel as well as possible performance issues for metallic fuel. Also, the construction of a fuel fabrication line for plutonium fuels, with or without a line to remove gallium, is expected to be considerably more expensive than for uranium fuels. In the case of U-Pu-Zr, a relatively small number of fuel pins have been irradiated to high burnup, and in no case has a full assembly been irradiated to high burnup without disassembly and re-constitution. For MOX fuel, the irradiation database from the Fast Flux Test Facility (FFTF) is extensive. If a significant source of either weapons-grade or reactor-grade Pu became available (i.e., from an international source), a startup core based on Pu could be reconsidered.« less

Validation of Electrochemically Modulated Separations Performed On-Line with MC-ICP-MS for Uranium and Plutonium Isotopic Analyses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liezers, Martin; Olsen, Khris B.; Mitroshkov, Alexandre V.

2010-08-11

The most time consuming process in uranium or plutonium isotopic analyses is performing the requisite chromatographic separation of the actinides. Filament preparation for thermal ionization (TIMS) adds further delays, but is generally accepted due to the unmatched performance in trace isotopic analyses. Advances in Multi-Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICP-MS) are beginning to rival the performance of TIMS. Methods, such as Electrochemically Modulated Separations (EMS) can efficiently pre-concentrate U or Pu quite selectively from small solution volumes in a matrix of 0.5 M nitric acid. When performed in-line with ICP-MS, the rapid analyte release from the electrode is fast,more » and large transient analyte signal enhancements of >100 fold can be achieved as compared to more conventional continuous nebulization of the original starting solution. This makes the approach ideal for very low level isotope ratio measurements. In this paper, some aspects of EMS performance are described. These include low level Pu isotope ratio behavior versus concentration by MC-ICP-MS and uranium rejection characteristics that are also important for reliable low level Pu isotope ratio determinations.« less

LANL robotics site overview

DOE Office of Scientific and Technical Information (OSTI.GOV)

Beugelsdijk, T.J.

1990-11-01

This paper reports on robotics applications at the Los Alamos National Laboratory. The topics of the paper include the ROBOCAL project to assay all nuclear materials entering and leaving the process floor at the Los Alamos Plutonium Facility, the isotope detector fabrication project, a plutonium dissolution robotic system, a safeguards waste automated measurement instrument, and DNA filter array construction. This report consists of overheads only.

Age determination of single plutonium particles after chemical separation

NASA Astrophysics Data System (ADS)

Shinonaga, T.; Donohue, D.; Ciurapinski, A.; Klose, D.

2009-01-01

Age determination of single plutonium particles was demonstrated using five particles of the standard reference material, NBS 947 (Plutonium Isotopic Standard. National Bureau of Standards, Washington, D.C. 20234, August 19, 1982, currently distributed as NBL CRM-137) and the radioactive decay of 241Pu into 241Am. The elemental ratio of Am/Pu in Pu particles found on a carbon planchet was measured by wavelength dispersive X-ray spectrometry (WDX) coupled to a scanning electron microscope (SEM). After the WDX measurement, each plutonium particle, with an average size of a few μm, was picked up and relocated to a silicon wafer inside the SEM chamber using a micromanipulator. The silicon wafer was then transferred to a quartz tube for dissolution in an acid solution prior to chemical separation. After the Pu was chemically separated from Am and U, the isotopic ratios of Pu ( 240Pu/ 239Pu, 241Pu/ 239Pu and 242Pu/ 239Pu) were measured with a thermal ionization mass spectrometer (TIMS) for the calculation of Pu age. The age of particles determined in this study was in good agreement with the expected age (35.9 a) of NBS 947 within the measurement uncertainty.

Characteristics of Chernobyl-derived radionuclides in particulate form in surface waters in the exclusion zone around the Chernobyl Nuclear Power Plant

NASA Astrophysics Data System (ADS)

Matsunaga, Takeshi; Ueno, Takashi; Amano, Hikaru; Tkatchenko, Y.; Kovalyov, A.; Watanabe, Miki; Onuma, Yoshikazu

1998-12-01

The distribution of Chernobyl-derived radionuclides in river and lake water bodies at 6-40 km from the Chernobyl Nuclear Power Plant was studied. Current levels of radionuclides (Cesium-137, Strontium-90, Plutonium, Americium and Curium isotopes) in water bodies and their relation to the ground contamination are presented. The investigation of the radionuclide composition of aqueous and ground contamination revealed that radionuclides on suspended solids (particulate form) originate mainly from the erosion of the contaminated surface soil layer in the zone. Apparent distribution ratios between particulate and dissolved forms are compared to known distribution coefficients.

METHOD OF PREPARING URANIUM, THORIUM, OR PLUTONIUM OXIDES IN LIQUID BISMUTH

DOEpatents

Davidson, J.K.; Robb, W.L.; Salmon, O.N.

1960-11-22

A method is given for forming compositions, as well as the compositions themselves, employing uranium hydride in a liquid bismuth composition to increase the solubility of uranium, plutonium and thorium oxides in the liquid bismuth. The finely divided oxide of uranium, plutonium. or thorium is mixed with the liquid bismuth and uranium hydride, the hydride being present in an amount equal to about 3 at. %, heated to about 5OO deg C, agitated and thereafter cooled and excess resultant hydrogen removed therefrom.

Source-dependent and source-independent controls on plutonium oxidation state and colloid associations in groundwater.

PubMed

Buesseler, Ken O; Kaplan, Daniel I; Dai, Minhan; Pike, Steven

2009-03-01

Plutonium (Pu) was characterized for its isotopic composition, oxidation states, and association with colloids in groundwater samples near disposal basins in F-Area of the Savannah River Site and compared to similar samples collected six years earlier. Two sources of Pu were identified, the disposal basins, which contained a 24Pu/l39Pu isotopic signature consistent with weapons grade Pu, and 244Cm, a cocontaminant that is a progenitor radionuclide of 24Pu. 24Pu that originated primarily from 244Cm tended to be appreciably more oxidized (Pu(V/VI)), less associated with colloids (approximately 1 kDa - 0.2 microm), and more mobile than 239Pu, as suggested by our prior studies at this site. This is not evidence of isotope fractionation but rather "source-dependent" controls on 240Pu speciation which are processes that are not at equilibrium, i.e., processes that appear kinetically hindered. There were also "source-independent" controls on 239Pu speciation, which are those processes that follow thermodynamic equilibrium with their surroundings. For example, a groundwater pH increase in one well from 4.1 in 1998 to 6.1 in 2004 resulted in an order of magnitude decrease in groundwater 239Pu concentrations. Similarly, the fraction of 239Pu in the reduced Pu(III/IV) and colloidal forms increased systematically with decreases in redox condition in 2004 vs 1998. This research demonstrates the importance of source-dependent and source-independent controls on Pu speciation which would impact Pu mobility during changes in hydrological, chemical, or biological conditions on both seasonal and decadal time scales, and over short spatial scales. This implies more dynamic shifts in Pu speciation, colloids association, and transport in groundwater than commonly believed.

Investigation into the Feasibility of Highly Enriched Uranium Detection by External Neutron Stimulation (Expanded Study)

DTIC Science & Technology

2006-05-01

26 1.10.1 Radiation Isotope Detector Operation ...... 27 1.10.2 HEU Counts in Radioisotope with 1 kg HEU.. 27 1.10.3 Radiation Isotope ...REACTOR GRADE PLUTONIUM ........... 173 10.2 GAMMA EMITTING ISOTOPES IN CARGO MATERIAL ............. 177 10.3 MCNP ANALYSIS OF GAMMA TRANSPORT FROM A...experiment at USNA using a germanium detector .......................... 31 1-13 Counts in the radiation isotope detector versus counting time for 1

History of MET Lab Section C-I, April 1942--April 1943

DOE Office of Scientific and Technical Information (OSTI.GOV)

Seaborg, G.T.

A day-to-day account of the work done at the University of Chicago Metallurgical Laboratory from April 1942 to April 1943 is given. The work concerned the development of chemical procedures for the extraction of plutonium, for the purification of plutonium, and, in the later phases, for research on the isotopes of other heavy elements including other transuranium elements. (LK)

Volatile Impurities in the Plutonium Immobilization Ceramic Wasteform

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cozzi, A.D.

1999-10-15

Approximately 18 of the 50 metric tons of plutonium identified for disposition contain significant quantities of impurities. A ceramic waste form is the chosen option for immobilization of the excess plutonium. The impurities associated with the stored plutonium have been identified (CaCl2, MgF2, Pb, etc.). For this study, only volatile species are investigated. The impurities are added individually. Cerium is used as the surrogate for plutonium. Three compositions, including the baseline composition, were used to verify the ability of the ceramic wasteform to accommodate impurities. The criteria for evaluation of the effect of the impurities were the apparent porosity andmore » phase assemblage of sintered pellets.« less

APPROACHING CRYOGENIC GE PERFORMANCE WITH PELTIER COOLED CDTE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Khusainov, A. K.; Iwanczyk, J. S.; Patt, B. E.

A new class of hand-held, portable spectrometers based on large area (lcm2) CdTe detectors of thickness up to 3mm has been demonstrated to produce energy resolution of between 0.3 and 0.5% FWHM at 662 keV. The system uses a charge loss correction circuit for improved efficiency, and detector temperature stabilization to ensure consistent operation of the detector during field measurements over a wide range of ambient temperature. The system can operate continuously for up to 8hrs on rechargeable batteries. The signal output from the charge loss corrector is compatible with most analog and digital spectroscopy amplifiers and multi channel analyzers.more » Using a detector measuring 11.2 by 9.1 by 2.13 mm3, we have recently been able to obtain the first wide-range plutonium gamma-ray isotopic analysis with other than a cryogenically cooled germanium spectrometer. The CdTe spectrometer is capable of measuring small plutonium reference samples in about one hour, covering the range from low to high burnup. The isotopic analysis software used to obtain these results was FRAM, Version 4 from LANL. The new spectrometer is expected to be useful for low-grade assay, as well as for some in-situ plutonium gamma-ray isotopics in lieu of cryogenically cooled Ge.« less

Method of isotope separation by chemi-ionization

DOEpatents

Wexler, Sol; Young, Charles E.

1977-05-17

A method for separating specific isotopes present in an isotopic mixture by aerodynamically accelerating a gaseous compound to form a jet of molecules, and passing the jet through a stream of electron donor atoms whereby an electron transfer takes place, thus forming negative ions of the molecules. The molecular ions are then passed through a radiofrequency quadrupole mass filter to separate the specific isotopes. This method may be used for any compounds having a sufficiently high electron affinity to permit negative ion formation, and is especially useful for the separation of plutonium and uranium isotopes.

Development of Metallic Magnetic Calorimeters for Nuclear Safeguards Applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bates, Cameron Russell

2015-03-11

Many nuclear safeguards applications could benefit from high-resolution gamma-ray spectroscopy achievable with metallic magnetic calorimeters. This dissertation covers the development of a system for these applications based on gamma-ray detectors developed at the University of Heidelberg. It demonstrates new calorimeters of this type, which achieved an energy resolution of 45.5 eV full-width at half-maximum at 59.54 keV, roughly ten times better than current state of the art high purity germanium detectors. This is the best energy resolution achieved with a gamma-ray metallic magnetic calorimeter at this energy to date. In addition to demonstrating a new benchmark in energy resolution, anmore » experimental system for measuring samples with metallic magnetic calorimeters was constructed at Lawrence Livermore National Laboratory. This system achieved an energy resolution of 91.3 eV full-width at half-maximum at 59.54 keV under optimal conditions. Using this system it was possible to characterize the linearity of the response, the count-rate limitations, and the energy resolution as a function of temperature of the new calorimeter. With this characterization it was determined that it would be feasible to measure 242Pu in a mixed isotope plutonium sample. A measurement of a mixed isotope plutonium sample was performed over the course of 12 days with a single two-pixel metallic magnetic calorimeter. The relative concentration of 242Pu in comparison to other plutonium isotopes was determined by direct measurement to less than half a percent accuracy. This is comparable with the accuracy of the best-case scenario using traditional indirect methods. The ability to directly measure the relative concentration of 242Pu in a sample could enable more accurate accounting and detection of indications of undeclared activities in nuclear safeguards, a better constraint on source material in forensic samples containing plutonium, and improvements in verification in a future plutonium disposition treaty.« less

Conversion electron spectrometry of Pu isotopes with a silicon drift detector.

PubMed

Pommé, S; Paepen, J; Peräjärvi, K; Turunen, J; Pöllänen, R

2016-03-01

An electron spectrometry set-up was built at IRMM consisting of a vacuum chamber with a moveable source holder and windowless Peltier-cooled silicon drift detector (SDD). The SDD is well suited for measuring low-energy x rays and electrons emitted from thin radioactive sources with low self-absorption. The attainable energy resolution is better than 0.5keV for electrons of 30keV. It has been used to measure the conversion electron spectra of three plutonium isotopes, i.e. (238)Pu, (239)Pu, (240)Pu, as well as (241)Am (being a decay product of (241)Pu). The obtained mixed x-ray and electron spectra are compared with spectra obtained with a close-geometry set-up using another SDD in STUK and spectra measured with a Si(Li) detector at IRMM. The potential of conversion electron spectrometry for isotopic analysis of mixed plutonium samples is investigated. With respect to the (240)Pu/(239)Pu isotopic ratio, the conversion electron peaks of both isotopes are more clearly separated than their largely overlapping peaks in alpha spectra. Copyright © 2015 The Authors. Published by Elsevier Ltd.. All rights reserved.

Variants of Regenerated Fissile Materials Usage in Thermal Reactors as the First Stage of Fuel Cycle Closing

NASA Astrophysics Data System (ADS)

Andrianova, E. A.; Tsibul'skiy, V. F.

2017-12-01

At present, 240 000 t of spent nuclear fuel (SF) has been accumulated in the world. Its long-term storage should meet safety conditions and requires noticeable finances, which grow every year. Obviously, this situation cannot exist for a long time; in the end, it will require a final decision. At present, several variants of solution of the problem of SF management are considered. Since most of the operating reactors and those under construction are thermal reactors, it is reasonable to assume that the structure of the nuclear power industry in the near and medium-term future will be unchanged, and it will be necessary to utilize plutonium in thermal reactors. In this study, different strategies of SF management are compared: open fuel cycle with long-term SF storage, closed fuel cycle with MOX fuel usage in thermal reactors and subsequent long-term storage of SF from MOX fuel, and closed fuel cycle in thermal reactors with heterogeneous fuel arrangement. The concept of heterogeneous fuel arrangement is considered in detail. While in the case of traditional fuel it is necessary to reprocess the whole amount of spent fuel, in the case of heterogeneous arrangement, it is possible to separate plutonium and 238U in different fuel rods. In this case, it is possible to achieve nearly complete burning of fissile isotopes of plutonium in fuel rods loaded with plutonium. These fuel rods with burned plutonium can be buried after cooling without reprocessing. They would contain just several percent of initially loaded plutonium, mainly even isotopes. Fuel rods with 238U alone should be reprocessed in the usual way.

Plutonium weathering on Johnston Atoll

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wolf, S.E.; Bates, J.K.; Buck, E.C.

1995-12-31

Johnston Atoll was contaminated with transuranic elements, particularly plutonium, by atmospheric nuclear weapons tests and aborted nuclear devices. Initial cleanup operations and and an extensive soil remediation program were performed. However, many areas contained a low-level continuum of activity, and subsurface contamination has been detected. Discrete hot particles and contaminated soil were characterized to determine whether the spread of activity was caused by weathering. Analytical techniques included gamma spectrometry, alpha spectrometry, and inductively coupled plasma-mass spectrometry to determine transuranic elemental and isotopic composition. Ultrafiltration and small-particle handling techniques were employed to isolate individual particles. Optical microscopy, scanning electron microscopy, analyticalmore » transmission electron microscopy, energy dispersive X-ray spectroscopy, and electron energy loss spectroscopy were used to characterize individual particles. Analyses of the hot particles showed that they are aborted nuclear warhead fragments that been melted and weathered in the presence of water and CaCO{sub 3}. It was concluded that the formation of aqueous ionic (Pu/Am)-CO{sub 3} coordinated complexes, during environmental exposure to large volumes of rainwater and carbonate-satured seawater, enhanced the solubility of transuranic elements. The (Pu/Am)-CO{sub 3} complexes sorbed onto colloidal CaCO{sub 3} and coral soil surfaces as they were exposed to rain and seawater. This mechanism led to greater dispersal of plutonium and americium than would be expected by physical transport of discrete hot particles alone.« less

METHOD FOR OBTAINING PLUTONIUM METAL AND ALLOYS OF PLUTONIUM FROM PLUTONIUM TRICHLORIDE

DOEpatents

Reavis, J.G.; Leary, J.A.; Maraman, W.J.

1962-11-13

A process is given for both reducing plutonium trichloride to plutonium metal using cerium as the reductant and simultaneously alloying such plutonium metal with an excess of cerium or cerium and cobalt sufficient to yield the desired nuclear reactor fuel composition. The process is conducted at a temperature from about 550 to 775 deg C, at atmospheric pressure, without the use of booster reactants, and a substantial decontamination is effected in the product alloy of any rare earths which may be associated with the source of the plutonium. (AEC)

A non-destructive internal nuclear forensic investigation at Argonne: discovery of a Pu planchet from 1948

DOE PAGES

Savina, Joseph A.; Steeb, Jennifer L.; Savina, Michael R.; ...

2016-06-02

A plutonium alpha standard dating from 1948 was discovered at Argonne National Laboratory and characterized using a number of non-destructive analytical techniques. The principle radioactive isotope was found to be 239Pu and unique ring structures were found across the surface of the deposition area. Due to chronological constraints on possible sources and its high isotopic purity, the plutonium in the sample was likely produced by the Oak Ridge National Lab X-10 Reactor. As a result, it is proposed that the rings are resultant through a combination of polishing and electrodeposition, though the hypothesis fails to address a few key featuresmore » of the ring structures.« less

Analysis of IAEA Environmental Samples for Plutonium and Uranium by ICP/MS in Support Of International Safeguards

DOE Office of Scientific and Technical Information (OSTI.GOV)

Farmer, Orville T.; Olsen, Khris B.; Thomas, May-Lin P.

2008-05-01

A method for the separation and determination of total and isotopic uranium and plutonium by ICP-MS was developed for IAEA samples on cellulose-based media. Preparation of the IAEA samples involved a series of redox chemistries and separations using TRU® resin (Eichrom). The sample introduction system, an APEX nebulizer (Elemental Scientific, Inc), provided enhanced nebulization for a several-fold increase in sensitivity and reduction in background. Application of mass bias (ALPHA) correction factors greatly improved the precision of the data. By combining the enhancements of chemical separation, instrumentation and data processing, detection levels for uranium and plutonium approached high attogram levels.

Plutonium isotopes in the atmosphere of Central Europe: Isotopic composition and time evolution vs. circulation factors.

PubMed

Kierepko, Renata; Mietelski, Jerzy W; Ustrnul, Zbigniew; Anczkiewicz, Robert; Wershofen, Herbert; Holgye, Zoltan; Kapała, Jacek; Isajenko, Krzysztof

2016-11-01

This paper reports evidence of Pu isotopes in the lower part of the troposphere of Central Europe. The data were obtained based on atmospheric aerosol fraction samples collected from four places in three countries (participating in the informal European network known as the Ring of Five (Ro5)) forming a cell with a surface area of about 200,000km(2). We compared our original data sets from Krakow (Poland, 1990-2007) and Bialystok (Poland, 1991-2007) with the results from two other locations, Prague (Czech Republic; 1997-2004) and Braunschweig (Germany; 1990-2003) to find time evolution of the Pu isotopes. The levels of the activity concentration for (238)Pu and for ((239+240))Pu were estimated to be a few and some tens of nBqm(-3), respectively. However, we also noted some results were much higher (even about 70 times higher) than the average concentration of (238)Pu in the atmosphere. The achieved complex data sets were used to test a new approach to the problem of solving mixing isotopic traces from various sources (here up to three) in one sample. Results of our model, supported by mesoscale atmospheric circulation parameters, suggest that Pu from nuclear weapon accidents or tests and nuclear burnt-up fuel are present in the air. Copyright © 2016 Elsevier B.V. All rights reserved.

Concentrations of plutonium and americium in plankton from the western Mediterranean Sea.

PubMed

Sanchez-Cabeza, Joan-Albert; Merino, Juan; Masqué, Pere; Mitchell, Peter I; Vintró, L León; Schell, William R; Cross, Lluïsa; Calbet, Albert

2003-07-20

Understanding the transfer of radionuclides through the food chain leading to man and in particular, the uptake of transuranic nuclides by plankton, is basic to assess the potential radiological risk of the consumption of marine products by man. The main sources of transuranic elements in the Mediterranean Sea in the past were global fallout and the Palomares accident, although at present smaller amounts are released from nuclear establishments in the northwestern region. Plankton from the western Mediterranean Sea was collected and analyzed for plutonium and americium in order to study their biological uptake. The microplankton fractions accounted for approximately 50% of the total plutonium contents in particulate form. At Garrucha (Palomares area), microplankton showed much higher 239,240 Pu activity, indicating the contamination with plutonium from the bottom sediments. Concentration factors were within the range of the values recommended by the International Atomic Energy Agency. Continental shelf mesoplankton was observed to efficiently concentrate transuranics. In open seawaters, concentrations were much lower. We speculate that sediments might play a role in the transfer of transuranics to mesoplankton in coastal waters, although we cannot discard that the difference in species composition may also play a role. In Palomares, both 239,240 Pu and 241Am showed activities five times higher than the mean values observed in continental shelf mesoplankton. As the plutonium isotopic ratios in the contaminated sample were similar to those found in material related to the accident, the contamination was attributed to bomb debris from the Palomares accident. Concentration factors in mesoplankton were also in relatively good agreement with the ranges recommended by IAEA. In the Palomares station the highest concentration factor was observed in the sample that showed predominance of the dynoflagellate Ceratium spp. Mean values of the enrichment factors showed, on average, discrimination rather than enrichment in the primary producer trophic chain.

Destructive analysis capabilities for plutonium and uranium characterization at Los Alamos National Laboratory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tandon, Lav; Kuhn, Kevin J; Drake, Lawrence R

Los Alamos National Laboratory's (LANL) Actinide Analytical Chemistry (AAC) group has been in existence since the Manhattan Project. It maintains a complete set of analytical capabilities for performing complete characterization (elemental assay, isotopic, metallic and non metallic trace impurities) of uranium and plutonium samples in different forms. For a majority of the customers there are strong quality assurance (QA) and quality control (QC) objectives including highest accuracy and precision with well defined uncertainties associated with the analytical results. Los Alamos participates in various international and national programs such as the Plutonium Metal Exchange Program, New Brunswick Laboratory's (NBL' s) Safeguardsmore » Measurement Evaluation Program (SME) and several other inter-laboratory round robin exercises to monitor and evaluate the data quality generated by AAC. These programs also provide independent verification of analytical measurement capabilities, and allow any technical problems with analytical measurements to be identified and corrected. This presentation will focus on key analytical capabilities for destructive analysis in AAC and also comparative data between LANL and peer groups for Pu assay and isotopic analysis.« less

Boeing Michigan Aeronautical Research Center (BOMARC) Missile Shelters and Bunkers Scoping Survey Workplan

DTIC Science & Technology

2007-08-01

Characterization (OHM 1998). From the plot, it is clear that the HEU dominates DU in the overall isotopic characteristic. Among the three uranium ... isotopes , 234U comprised about 90 % of the total activity, including naturally-occurring background sources. However, in comparison to the WGP, uranium ...listed for a few sampling locations that had isotopic plutonium analysis of wipe samples. Figure A-19 contains a scatterplot of the paired Table 4-13

Assessment of Non-traditional Isotopic Ratios by Mass Spectrometry for Analysis of Nuclear Activities. Annual Report 2011

DOE Office of Scientific and Technical Information (OSTI.GOV)

Biegalski, Steven R.; Buchholz, Bruce A.

2011-08-24

The objective of this work is to identify isotopic ratios suitable for analysis via mass spectrometry that distinguish between commercial nuclear reactor fuel cycles, fuel cycles for weapons grade plutonium, and products from nuclear weapons explosions. Methods will also be determined to distinguish the above from medical and industrial radionuclide sources. Mass spectrometry systems will be identified that are suitable for field measurement of such isotopes in an expedient manner.

A prototype experiment for cooperative monitoring of nuclear reactors with cubic meter scale antineutrino detectors

NASA Astrophysics Data System (ADS)

Bernstein, A.; Allen, M.; Bowden, N.; Brennan, J.; Carr, D. J.; Estrada, J.; Hagmann, C.; Lund, J. C.; Madden, N. W.; Winant, C. D.

2005-09-01

Our Lawrence Livermore National Laboratory/Sandia National Laboratories collaboration has deployed a cubic-meter-scale antineutrino detector to demonstrate non-intrusive and automatic monitoring of the power levels and plutonium content of a nuclear reactor. Reactor monitoring of this kind is required for all non-nuclear weapons states under the Nuclear Nonproliferation Treaty (NPT), and is implemented by the International Atomic Energy Agency (IAEA). Since the antineutrino count rate and energy spectrum depend on the relative yields of fissioning isotopes in the reactor core, changes in isotopic composition can be observed without ever directly accessing the core. Data from a cubic meter scale antineutrino detector, coupled with the well-understood principles that govern the core's evolution in time, can be used to determine whether the reactor is being operated in an illegitimate way. Our group has deployed a detector at the San Onofre reactor site in California to demonstrate this concept. This paper describes the concept and shows preliminary results from 8 months of operation.

PLUTONIUM-ZIRCONIUM ALLOYS

DOEpatents

Schonfeld, F.W.; Waber, J.T.

1960-08-30

A series of nuclear reactor fuel alloys consisting of from about 5 to about 50 at.% zirconium (or higher zirconium alloys such as Zircaloy), balance plutonium, and having the structural composition of a plutonium are described. Zirconium is a satisfactory diluent because it alloys readily with plutonium and has desirable nuclear properties. Additional advantages are corrosion resistance, excellent fabrication propenties, an isotropie structure, and initial softness.

Determination of uranium isotopic composition and 236U content of soil samples and hot particles using inductively coupled plasma mass spectrometry.

PubMed

Boulyga, S F; Becker, J S

2001-07-01

As a result of the accident at the Chernobyl nuclear power plant (NPP) the environment was contaminated with spent nuclear fuel. The 236U isotope was used in this study to monitor the spent uranium from nuclear fallout in soil samples collected in the vicinity of the Chernobyl NPP. Nuclear track radiography was applied for the identification and extraction of hot radioactive particles from soil samples. A rapid and sensitive analytical procedure was developed for uranium isotopic ratio measurement in environmental samples based on double-focusing inductively coupled plasma mass spectrometry (DF-ICP-MS) with a MicroMist nebulizer and a direct injection high-efficiency nebulizer (DIHEN). The performance of the DF-ICP-MS with a quartz DIHEN and plasma shielded torch was studied. Overall detection efficiencies of 4 x 10(-4) and 10(-3) counts per atom were achieved for 238U in DF-ICP-QMS with the MicroMist nebulizer and DIHEN, respectively. The rate of formation of uranium hydride ions UH+/U+ was 1.2 x 10(-4) and 1.4 x 10(-4), respectively. The precision of short-term measurements of uranium isotopic ratios (n = 5) in 1 microg L(-1) NBS U-020 standard solution was 0.11% (238U/235U) and 1.4% (236U/238U) using a MicroMist nebulizer and 0.25% (235U/238U) and 1.9% (236U/P38U) using a DIHEN. The isotopic composition of all investigated Chernobyl soil samples differed from those of natural uranium; i.e. in these samples the 236U/238U ratio ranged from 10(-5) to 10(-3). Results obtained with ICP-MS, alpha- and gamma-spectrometry showed differences in the migration properties of spent uranium, plutonium, and americium. The isotopic ratio of uranium was also measured in hot particles extracted from soil samples.

Process chemistry of americium-241

DOE Office of Scientific and Technical Information (OSTI.GOV)

Navratil, J.D.

1983-01-01

Americium-241, one of the most useful actinide isotopes, is produced as a by-product of plutonium scrap recovery operations. Rocky Flats has supplied high purity americium oxide to the US Department of Energy's Isotope Pool since 1962. Over the years, the evolving separation and purification processes have included such diverse operations as ion exchange, aqueous precipitation, and both molten-salt and organic-solvent extraction.

Improvements in the MGA Code Provide Flexibility and Better Error Analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ruhter, W D; Kerr, J

2005-05-26

The Multi-Group Analysis (MGA) code is widely used to determine nondestructively the relative isotopic abundances of plutonium by gamma-ray spectrometry. MGA users have expressed concern about the lack of flexibility and transparency in the code. Users often have to ask the code developers for modifications to the code to accommodate new measurement situations, such as additional peaks being present in the plutonium spectrum or expected peaks being absent. We are testing several new improvements to a prototype, general gamma-ray isotopic analysis tool with the intent of either revising or replacing the MGA code. These improvements will give the user themore » ability to modify, add, or delete the gamma- and x-ray energies and branching intensities used by the code in determining a more precise gain and in the determination of the relative detection efficiency. We have also fully integrated the determination of the relative isotopic abundances with the determination of the relative detection efficiency to provide a more accurate determination of the errors in the relative isotopic abundances. We provide details in this paper on these improvements and a comparison of results obtained with current versions of the MGA code.« less

Photochemical isotope separation

DOEpatents

Robinson, C. Paul; Jensen, Reed J.; Cotter, Theodore P.; Greiner, Norman R.; Boyer, Keith

1987-01-01

A process for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium.

Isotope separation by laser means

DOEpatents

Robinson, C. Paul; Jensen, Reed J.; Cotter, Theodore P.; Greiner, Norman R.; Boyer, Keith

1982-06-15

A process for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium.

Clues in the rare gas isotopes to early solar system history

NASA Technical Reports Server (NTRS)

Reynolds, J. H.

1974-01-01

Rare gases in meteorites and lunar samples are discussed stimulating the discovery of the solar wind. Radioactive isotopes are examined, making a correlation to the origin of the solar system. It is shown that the heights of the peaks above the horizontal lines represent the spectrum of the fissiogenic sample. Nuclear tracks of iodine, xenon, and plutonium detected in lunar rocks are also explained.

The Manhattan Project

NASA Astrophysics Data System (ADS)

Reed, B. Cameron

2014-10-01

The Manhattan Project was the United States Army’s program to develop and deploy nuclear weapons during World War II. In these devices, which are known popularly as ‘atomic bombs’, energy is released not by a chemical explosion but by the much more violent process of fission of nuclei of heavy elements via a neutron-mediated chain-reaction. Three years after taking on this project in mid-1942, the Army’s Manhattan Engineer District produced three nuclear bombs of two different designs. Two of these devices were fueled with the 239 isotope of the synthetic element plutonium, while the third employed the rare 235 isotope of uranium. One of the plutonium devices, code-named Trinity, was detonated in a test in southern New Mexico on 16 July 1945; this was the world’s first nuclear explosion. Three weeks later, on 6 August, the uranium bomb, Little Boy, was dropped on the Japanese city of Hiroshima. On 9 August the second plutonium device, Fat Man, was dropped on Nagasaki. Together, the two bombings killed over 100 000 people and were at least partially responsible for the Japanese government’s 14 August decision to surrender. This article surveys, at an undergraduate level, the science and history of the Manhattan Project.

Photochemical isotope separation

DOEpatents

Robinson, C.P.; Jensen, R.J.; Cotter, T.P.; Greiner, N.R.; Boyer, K.

1987-04-28

A process is described for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium. 8 figs.

Digital pile-up rejection for plutonium experiments with solution-grown stilbene

NASA Astrophysics Data System (ADS)

Bourne, M. M.; Clarke, S. D.; Paff, M.; DiFulvio, A.; Norsworthy, M.; Pozzi, S. A.

2017-01-01

A solution-grown stilbene detector was used in several experiments with plutonium samples including plutonium oxide, mixed oxide, and plutonium metal samples. Neutrons from different reactions and plutonium isotopes are accompanied by numerous gamma rays especially by the 59-keV gamma ray of 241Am. Identifying neutrons correctly is important for nuclear nonproliferation applications and makes neutron/gamma discrimination and pile-up rejection necessary. Each experimental dataset is presented with and without pile-up filtering using a previously developed algorithm. The experiments were simulated using MCNPX-PoliMi, a Monte Carlo code designed to accurately model scintillation detector response. Collision output from MCNPX-PoliMi was processed using the specialized MPPost post-processing code to convert neutron energy depositions event-by-event into light pulses. The model was compared to experimental data after pulse-shape discrimination identified waveforms as gamma ray or neutron interactions. We show that the use of the digital pile-up rejection algorithm allows for accurate neutron counting with stilbene to within 2% even when not using lead shielding.

Americium-Curium Stabilization - 5'' Cylindrical Induction Melter System Design Basis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Witt, D.C.

1999-11-08

Approximately 11,000 liters (3,600) gallons of solution containing isotopes of Am and Cm are currently stored in F-Canyon Tank 17.1. These isotopes were recovered during plutonium-242 production campaigns in the mid- and late-1970s. Experimental work for the project began in 1995 by the Savannah River Technology Center (SRTC). Details of the process are given in the various sections of this document.

Investigating Pu and U isotopic compositions in sediments: a case study in Lake Obuchi, Rokkasho Village, Japan using sector-field ICP-MS and ICP-QMS.

PubMed

Zheng, Jian; Yamada, Masatoshi

2005-08-01

The objectives of the present work were to study isotope ratios and the inventory of plutonium and uranium isotope compositions in sediments from Lake Obuchi, which is in the vicinity of several nuclear fuel facilities in Rokkasho, Japan. Pu and its isotopes were determined using sector-field ICP-MS and U and its isotopes were determined with ICP-QMS after separation and purification with a combination of ion-exchange and extraction chromatography. The observed (240)Pu/(239)Pu atom ratio (0.186 +/- 0.016) was similar to that of global fallout, indicating that the possible early tropospheric fallout Pu did not deliver Pu from the Pacific Proving Ground to areas above 40 degrees N. The previously reported higher Pu inventory in the deep water area of Lake Obuchi could be attributed to the lateral transportation of Pu deposited in the shallow area which resulted from the migration of deposited global fallout Pu from the land into the lake by river runoff and from the Pacific Ocean by tide movement and sea water scavenging, as well as from direct soil input by winds. The (235)U/(238)U atom ratios ranged from 0.00723 to 0.00732, indicating the natural origin of U in the sediments. The average (234)U/(238)U activity ratio of 1.11 in a sediment core indicated a significant sea water U contribution. No evidence was found for the release of U containing wastes from the nearby nuclear facilities. These results will serve as a reference baseline on the levels of Pu and U in the studied site so that any further contamination from the spent nuclear fuel reprocessing plants, the radioactive waste disposal and storage facilities, and the uranium enrichment plant can be identified, and the impact of future release can be rapidly assessed.

Fission fragment mass and total kinetic energy distributions of spontaneously fissioning plutonium isotopes

NASA Astrophysics Data System (ADS)

Pomorski, K.; Nerlo-Pomorska, B.; Bartel, J.; Schmitt, C.

2018-03-01

The fission-fragment mass and total kinetic energy (TKE) distributions are evaluated in a quantum mechanical framework using elongation, mass asymmetry, neck degree of freedom as the relevant collective parameters in the Fourier shape parametrization recently developed by us. The potential energy surfaces (PES) are calculated within the macroscopic-microscopic model based on the Lublin-Strasbourg Drop (LSD), the Yukawa-folded (YF) single-particle potential and a monopole pairing force. The PES are presented and analysed in detail for even-even Plutonium isotopes with A = 236-246. They reveal deep asymmetric valleys. The fission-fragment mass and TKE distributions are obtained from the ground state of a collective Hamiltonian computed within the Born-Oppenheimer approximation, in the WKB approach by introducing a neck-dependent fission probability. The calculated mass and total kinetic energy distributions are found in good agreement with the data.

Area G perimeter surface-soil and single-stage water sampling: Environmental surveillance for fiscal year 95. Progress report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Childs, M.; Conrad, R.

1997-09-01

ESH-19 personnel collected soil and single-stage water samples around the perimeter of Area G at Los Alamos National Laboratory (LANL) during FY 95 to characterize possible radionuclide movement out of Area G through surface water and entrained sediment runoff. Soil samples were analyzed for tritium, total uranium, isotopic plutonium, americium-241, and cesium-137. The single-stage water samples were analyzed for tritium and plutonium isotopes. All radiochemical data was compared with analogous samples collected during FY 93 and 94 and reported in LA-12986 and LA-13165-PR. Six surface soils were also submitted for metal analyses. These data were included with similar data generatedmore » for soil samples collected during FY 94 and compared with metals in background samples collected at the Area G expansion area.« less

The production and certification of a plutonium equal-atom reference material: NBL CRM 128

DOE Office of Scientific and Technical Information (OSTI.GOV)

Crawford, D.W.; Gradle, C.G.; Soriano, M.D.

This report describes the design, production, and certification of the New Brunswick Laboratory plutonium equal-atom certified reference material (CRM), NBL CRM 128. The primary use of this CRM is for the determination of bias corrections encountered in the operation of a mass spectrometer. This reference material is available to the US Department of Energy contractor-operated and government-operated laboratories, as well as to the international nuclear safeguards community. The absolute, or unbiased, certified value for the CRM's Pu-242/Pu-239 ratio is 1.00063 {plus minus} 0.00026 (95% confidence interval) as of October 1, 1984. This value was obtained through the quantitative blending ofmore » high-purity, chemically and isotopically characterized separated isotopes, as well as through intercomparisons of CRM samples with calibration mixtures using thermal ionization mass spectrometry. 32 tabs.« less

PROCESS OF REMOVING PLUTONIUM VALUES FROM SOLUTION WITH GROUP IVB METAL PHOSPHO-SILICATE COMPOSITIONS

DOEpatents

Russell, E.R.; Adamson, A.W.; Schubert, J.; Boyd, G.E.

1957-10-29

A process for separating plutonium values from aqueous solutions which contain the plutonium in minute concentrations is described. These values can be removed from an aqueous solution by taking an aqueous solution containing a salt of zirconium, titanium, hafnium or thorium, adding an aqueous solution of silicate and phosphoric acid anions to the metal salt solution, and separating, washing and drying the precipitate which forms when the two solutions are mixed. The aqueous plutonium containing solution is then acidified and passed over the above described precipi-tate causing the plutonium values to be adsorbed by the precipitate.

Spatially resolved analysis of plutonium isotopic signatures in environmental particle samples by laser ablation-MC-ICP-MS.

PubMed

Konegger-Kappel, Stefanie; Prohaska, Thomas

2016-01-01

Laser ablation-multi-collector-inductively coupled plasma mass spectrometry (LA-MC-ICP-MS) was optimized and investigated with respect to its performance for determining spatially resolved Pu isotopic signatures within radioactive fuel particle clusters. Fuel particles had been emitted from the Chernobyl nuclear power plant (ChNPP) where the 1986 accident occurred and were deposited in the surrounding soil, where weathering processes caused their transformation into radioactive clusters, so-called micro-samples. The size of the investigated micro-samples, which showed surface alpha activities below 40 mBq, ranged from about 200 to 1000 μm. Direct single static point ablations allowed to identify variations of Pu isotopic signatures not only between distinct fuel particle clusters but also within individual clusters. The resolution was limited to 100 to 120 μm as a result of the applied laser ablation spot sizes and the resolving power of the nuclear track radiography methodology that was applied for particle pre-selection. The determined (242)Pu/(239)Pu and (240)Pu/(239)Pu isotope ratios showed a variation from low to high Pu isotope ratios, ranging from 0.007(2) to 0.047(8) for (242)Pu/(239)Pu and from 0.183(13) to 0.577(40) for (240)Pu/(239)Pu. In contrast to other studies, the applied methodology allowed for the first time to display the Pu isotopic distribution in the Chernobyl fallout, which reflects the differences in the spent fuel composition over the reactor core. The measured Pu isotopic signatures are in good agreement with the expected Pu isotopic composition distribution that is typical for a RBMK-1000 reactor, indicating that the analyzed samples are originating from the ill-fated Chernobyl reactor. The average Pu isotope ratios [(240)Pu/(239)Pu = 0.388(86), (242)Pu/(239)Pu = 0.028(11)] that were calculated from all investigated samples (n = 48) correspond well to previously published results of Pu analyses in contaminated samples from the vicinity of the Chernobyl NPP [e.g. (240)Pu/(239)Pu = 0.394(2) and (242)Pu/(239)Pu = 0.027(1); Nunnemann et al. (J Alloys Compd 271-273:45-48, 1998)].

Chondritic xenon in the Earth’s mantle

NASA Astrophysics Data System (ADS)

Caracausi, Antonio; Avice, Guillaume; Burnard, Peter G.; Füri, Evelyn; Marty, Bernard

2016-05-01

Noble gas isotopes are powerful tracers of the origins of planetary volatiles, and the accretion and evolution of the Earth. The compositions of magmatic gases provide insights into the evolution of the Earth’s mantle and atmosphere. Despite recent analytical progress in the study of planetary materials and mantle-derived gases, the possible dual origin of the planetary gases in the mantle and the atmosphere remains unconstrained. Evidence relating to the relationship between the volatiles within our planet and the potential cosmochemical end-members is scarce. Here we show, using high-precision analysis of magmatic gas from the Eifel volcanic area (in Germany), that the light xenon isotopes identify a chondritic primordial component that differs from the precursor of atmospheric xenon. This is consistent with an asteroidal origin for the volatiles in the Earth’s mantle, and indicates that the volatiles in the atmosphere and mantle originated from distinct cosmochemical sources. Furthermore, our data are consistent with the origin of Eifel magmatism being a deep mantle plume. The corresponding mantle source has been isolated from the convective mantle since about 4.45 billion years ago, in agreement with models that predict the early isolation of mantle domains. Xenon isotope systematics support a clear distinction between mid-ocean-ridge and continental or oceanic plume sources, with chemical heterogeneities dating back to the Earth’s accretion. The deep reservoir now sampled by the Eifel gas had a lower volatile/refractory (iodine/plutonium) composition than the shallower mantle sampled by mid-ocean-ridge volcanism, highlighting the increasing contribution of volatile-rich material during the first tens of millions of years of terrestrial accretion.

Chondritic xenon in the Earth's mantle.

PubMed

Caracausi, Antonio; Avice, Guillaume; Burnard, Peter G; Füri, Evelyn; Marty, Bernard

2016-05-05

Noble gas isotopes are powerful tracers of the origins of planetary volatiles, and the accretion and evolution of the Earth. The compositions of magmatic gases provide insights into the evolution of the Earth's mantle and atmosphere. Despite recent analytical progress in the study of planetary materials and mantle-derived gases, the possible dual origin of the planetary gases in the mantle and the atmosphere remains unconstrained. Evidence relating to the relationship between the volatiles within our planet and the potential cosmochemical end-members is scarce. Here we show, using high-precision analysis of magmatic gas from the Eifel volcanic area (in Germany), that the light xenon isotopes identify a chondritic primordial component that differs from the precursor of atmospheric xenon. This is consistent with an asteroidal origin for the volatiles in the Earth's mantle, and indicates that the volatiles in the atmosphere and mantle originated from distinct cosmochemical sources. Furthermore, our data are consistent with the origin of Eifel magmatism being a deep mantle plume. The corresponding mantle source has been isolated from the convective mantle since about 4.45 billion years ago, in agreement with models that predict the early isolation of mantle domains. Xenon isotope systematics support a clear distinction between mid-ocean-ridge and continental or oceanic plume sources, with chemical heterogeneities dating back to the Earth's accretion. The deep reservoir now sampled by the Eifel gas had a lower volatile/refractory (iodine/plutonium) composition than the shallower mantle sampled by mid-ocean-ridge volcanism, highlighting the increasing contribution of volatile-rich material during the first tens of millions of years of terrestrial accretion.

Determination of origin and intended use of plutonium metal using nuclear forensic techniques.

PubMed

Rim, Jung H; Kuhn, Kevin J; Tandon, Lav; Xu, Ning; Porterfield, Donivan R; Worley, Christopher G; Thomas, Mariam R; Spencer, Khalil J; Stanley, Floyd E; Lujan, Elmer J; Garduno, Katherine; Trellue, Holly R

2017-04-01

Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials' properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% 240 Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modeling feedback and trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. Based on this investigation, the most likely intended use for these plutonium foils was 239 Pu fission foil targets for physics experiments, such as cross-section measurements, etc. Copyright © 2017 Elsevier B.V. All rights reserved.

Determination of origin and intended use of plutonium metal using nuclear forensic techniques

DOE PAGES

Rim, Jung H.; Kuhn, Kevin J.; Tandon, Lav; ...

2017-04-01

Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials’ properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% 240Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modelling feedback andmore » trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. In conclusion, based on this investigation, the most likely intended use for these plutonium foils was 239Pu fission foil targets for physics experiments, such as cross-section measurements, etc.« less

Assessment of the global fallout of plutonium isotopes and americium-241 in the soil of the central region of Saudi Arabia.

PubMed

Shabana, E I; Al-Shammari, H L

2001-01-01

A radiochemical technique for determination of plutonium isotopes and 241Am in soil samples is tested against IAEA-standard reference materials to determine its accuracy and precision for reliable results. The technique is then used in the investigation of topsoil samples, collected from the natural environment of the central region of Saudi Arabia, to assess the effect of fallout accumulation of these radionuclides in the region. Plutonium and americium were sequentially separated from all other components of the sample by anion-exchange chromatography and co-precipitated with Nd3+ as fluorides. The precipitates were mounted on membrane filters and measured using a high-resolution alpha-spectrometer. The results of the analysis of the reference materials showed satisfactory sensitivity and precision of the technique. The results of the analyzed soil samples show activity levels ranging from < LLD to 0.089 and from

Analysis of actinides in an ombrotrophic peat core - evidence of post-depositional migration of fallout radionuclides

NASA Astrophysics Data System (ADS)

Quinto, Francesca; Hrnecek, Erich; Krachler, Michael; Shotyk, William; Steier, Peter; Winkler, Stephan R.

2013-04-01

Plutonium (239Pu, 240Pu, 241Pu, 242Pu) and uranium (236U, 238U) isotopes were analyzed in an ombrotrophic peat core from the Black Forest, Germany, representing the last 80 years of atmospheric deposition. The reliable determination of these isotopes at ultra-trace levels was possible using ultra-clean laboratory procedures and accelerator mass spectrometry. The 240Pu/239Pu isotopic ratios are constant along the core with a mean value of 0.19 ±0.02 (N = 32). This result is consistent with the acknowledged average 240Pu/239Pu isotopic ratio from global fallout in the Northern Hemisphere. The global fallout origin of Pu is confirmed by the corresponding 241Pu/239Pu (0.0012 ±0.0005) and 242Pu/239Pu (0.004 ± 0.001) isotopic ratios. The identification of the Pu isotopic composition characteristic for global fallout in peat layers pre-dating the period of atmospheric atom bomb testing (AD 1956 - AD 1980) is a clear evidence of the migration of Pu downwards the peat profile. The maximum of global fallout derived 236U is detected in correspondence to the age/depth layer of maximum stratospheric fallout (AD 1963). This finding demonstrates that the 236U bomb peak can be successfully used as an independent chronological marker complementing the 210Pb dating of peat cores. The profiles of the global fallout derived 236U and 239Pu are compared with those of 137Cs and 241Am. As typical of ombrothrophic peat, the temporal fallout pattern of 137Cs is poorly retained. Similarly like for Pu, post-depositional migration of 241Am in peat layers preceding the era of atmospheric nuclear tests is observed.

Comparisons of the skeletal locations of putative plutonium-induced osteosarcomas in humans with those in beagle dogs and with naturally occurring tumors in both species.

PubMed

Miller, Scott C; Lloyd, Ray D; Bruenger, Fred W; Krahenbuhl, Melinda P; Polig, Erich; Romanov, Sergey A

2003-11-01

Osteosarcomas occur from exposures to bone-seeking, alpha-particle-emitting isotopes, particularly plutonium. The skeletal distribution of putative 239Pu-induced osteosarcomas reported in Mayak Metallurgical and Radiochemical Plutonium Plant workers is compared with those observed in canine studies, and these are compared with distributions of naturally occurring osteosarcomas in both species. In the Mayak workers, 29% and 71% of the osteosarcomas were in the peripheral and central skeleton, respectively, with the spine having the most tumors (36%). An almost identical distribution of plutonium-induced osteosarcomas was reported for dogs injected with 239Pu as young adults. This distribution of osteosarcomas is quite different from the distributions of naturally occurring osteosarcomas for both species. In the Cooperative Osteosarcoma Study Group in humans (1,736 osteosarcomas from all ages), over 91% of the tumors occurred in the peripheral skeleton. In the Mayo Clinic group of older individuals (>40 years old), over 60% of the osteosarcomas appeared in the peripheral skeleton. The distribution of naturally occurring osteosarcomas in the canine is similar to that in the adult human. The similarities of the distributions of plutonium-associated osteosarcomas in the Mayak workers with those found in experimental studies suggest that many of the reported osteosarcomas may have been associated with plutonium exposures. These results also support the experimental paradigm that plutonium osteosarcomas have a preference for well vascularized cancellous bone sites. These sites have a greater initial deposition of plutonium, but also greater turnover due to elevated bone remodeling rates.

PROCESS OF MAKING A NEUTRONIC REACTOR FUEL ELEMENT COMPOSITION

DOEpatents

Alter, H.W.; Davidson, J.K.; Miller, R.S.; Mewherter, J.L.

1959-01-13

A process is presented for making a ceramic-like material suitable for use as a nuclear fuel. The material consists of a solid solution of plutonium dioxide in uranium dioxide and is produced from a uranyl nitrate -plutonium nitrate solution containing uraniunm and plutonium in the desired ratio. The uranium and plutonium are first precipitated from the solution by addition of NH/ sub 4/OH and the dried precipitate is then calcined at 600 C in a hydrogen atmosphere to yield the desired solid solution of PuO/sub 2/ in UO/sub 2/.

Simulation of uranium and plutonium oxides compounds obtained in plasma

NASA Astrophysics Data System (ADS)

Novoselov, Ivan Yu.; Karengin, Alexander G.; Babaev, Renat G.

2018-03-01

The aim of this paper is to carry out thermodynamic simulation of mixed plutonium and uranium oxides compounds obtained after plasma treatment of plutonium and uranium nitrates and to determine optimal water-salt-organic mixture composition as well as conditions for their plasma treatment (temperature, air mass fraction). Authors conclude that it needs to complete the treatment of nitric solutions in form of water-salt-organic mixtures to guarantee energy saving obtainment of oxide compounds for mixed-oxide fuel and explain the choice of chemical composition of water-salt-organic mixture. It has been confirmed that temperature of 1200 °C is optimal to practice the process. Authors have demonstrated that condensed products after plasma treatment of water-salt-organic mixture contains targeted products (uranium and plutonium oxides) and gaseous products are environmental friendly. In conclusion basic operational modes for practicing the process are showed.

Production and recovery of Americium-241

DOE Office of Scientific and Technical Information (OSTI.GOV)

Navratil, J.D.

1984-01-01

Americium-241, one of the most useful actinide isotopes, is produced as a by-product of plutonium scrap recovery operations. Rocky Flats (RF) has supplied high-purity americium oxide to the US Department of Energy's Isotope Pool since 1962. Over the years, the evolving separation and purification processes have included such diverse operations as aqueous precipitation, ion exchange, and both molten-salt and organic-solvent extraction. A review is presented of the production and recovery processes of americium-241. 5 references.

[Interest and limits of inductively coupled plasma mass spectrometry (ICP-MS) for urinary diagnosis of radionuclide internal contamination].

PubMed

Lecompte, Yannick; Bohand, Sandra; Laroche, Pierre; Cazoulat, Alain

2013-01-01

After a review of radiometric reference methods used in radiotoxicology, analytical performance of inductively coupled plasma mass spectrometry (ICP-MS) for the workplace urinary diagnosis of internal contamination by radionuclides are evaluated. A literature review (covering the period from 2000 to 2012) is performed to identify the different applications of ICP-MS in radiotoxicology for urine analysis. The limits of detection are compared to the recommendations of the International commission on radiological protection (ICRP 78: "Individual monitoring for internal exposure of workers"). Except one publication describing the determination of strontium-90 (β emitter), all methods using ICP-MS reported in the literature concern actinides (α emitters). For radionuclides with a radioactive period higher than 10(4) years, limits of detection are most often in compliance with ICRP publication 78 and frequently lower than radiometric methods. ICP-MS allows the specific determination of plutonium-239 + 240 isotopes which cannot be discriminated by α spectrometry. High resolution ICP-MS can also measure uranium isotopic ratios in urine for total uranium concentrations lower than 20 ng/L. The interest of ICP-MS in radiotoxicology concerns essentially the urinary measurement of long radioactive period actinides, particularly for uranium isotope ratio determination and 239 and 240 plutonium isotopes discrimination. Radiometric methods remain the most efficient for the majority of other radionuclides.

Continuous transport of Pacific-derived anthropogenic radionuclides towards the Indian Ocean

PubMed Central

Pittauer, Daniela; Tims, Stephen G.; Froehlich, Michaela B.; Fifield, L. Keith; Wallner, Anton; McNeil, Steven D.; Fischer, Helmut W.

2017-01-01

Unusually high concentrations of americium and plutonium have been observed in a sediment core collected from the eastern Lombok Basin between Sumba and Sumbawa Islands in the Indonesian Archipelago. Gamma spectrometry and accelerator mass spectrometry data together with radiometric dating of the core provide a high-resolution record of ongoing deposition of anthropogenic radionuclides. A plutonium signature characteristic of the Pacific Proving Grounds (PPG) dominates in the first two decades after the start of the high yield atmospheric tests in 1950’s. Approximately 40–70% of plutonium at this site in the post 1970 period originates from the PPG. This sediment record of transuranic isotopes deposition over the last 55 years provides evidence for the continuous long-distance transport of particle-reactive radionuclides from the Pacific Ocean towards the Indian Ocean. PMID:28304374

10 CFR 110.41 - Executive Branch review.

Code of Federal Regulations, 2011 CFR

2011-01-01

.... (6) An export involving assistance to end uses related to isotope separation, chemical reprocessing, heavy water production, advanced reactors, or the fabrication of nuclear fuel containing plutonium... equipment to a foreign reactor. (8) An export involving radioactive waste. (9) An export to any country...

The New Element Curium (Atomic Number 96)

DOE R&D Accomplishments Database

Seaborg, G. T.; James, R. A.; Ghiorso, A.

1948-01-01

Two isotopes of the element with atomic number 96 have been produced by the helium-ion bombardment of plutonium. The name curium, symbol Cm, is proposed for element 96. The chemical experiments indicate that the most stable oxidation state of curium is the III state.

The Inglorious Death of Jumbo

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meade, Roger Allen

In the summer of 1944, J. Robert Oppenheimer and Los Alamos faced a crisis. An isotopic impurity in Plutonium rendered the metal unusable in a gun-assembled atomic bomb (i.e., Little Boy). Making this situation worse was a shortage of Uranium. The combination of these two problems threatened the entire wartime project. The answer to this dilemma, in part, was to develop a novel assembly method for Plutonium using the supersonic shock waves created by several tons of high explosives to compress a ball of Plutonium into a supercritical state. Since this method, implosion, was not much more than a theoreticalmore » construct, the Trinity test was devised to proof test the process. Given the speculative nature of implosion, Trinity was a gamble of sorts. If the test failed (i.e., little or no nuclear yield), the blast of the high explosives would scatter the scarce and expensive Plutonium over the surrounding desert. Since the probability of failure remained high into the early summer of 1945, some method of containing a failed nuclear explosion was needed. Jumbo was the answer.« less

Minimizing Glovebox Glove Breaches, Part III: Deriving Service Lifetimes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cournoyer, M.E.; Wilson, K.V.; Maestas, M.M.

At the Los Alamos Plutonium Facility, various isotopes of plutonium along with other actinides are handled in a glove box environment. Weapons-grade plutonium consists mainly in Pu-239. Pu-238 is another isotope used for heat sources. The Pu-238 is more aggressive regarding gloves due to its higher alpha-emitting characteristic ({approx}300 times more active than Pu-239), which modifies the change-out intervals for gloves. Optimization of the change-out intervals for gloves is fundamental since Nuclear Materials Technology (NMT) Division generates approximately 4 m{sup 3}/yr of TRU waste from the disposal of glovebox gloves. To reduce the number of glovebox glove failures, the NMTmore » Division pro-actively investigates processes and procedures that minimize glove failures. Aging studies have been conducted that correlate changes in mechanical (physical) properties with degradation chemistry. This present work derives glovebox glove change intervals based on mechanical data of thermally aged Hypalon{sup R}, and Butasol{sup R} glove samples. Information from this study represent an important baseline in gauging the acceptable standards for polymeric gloves used in a laboratory glovebox environment and will be used later to account for possible presence of dose-rate or synergistic effects in 'combined-environment'. In addition, excursions of contaminants into the operator's breathing zone and excess exposure to the radiological sources associated with unplanned breaches in the glovebox are reduced. (authors)« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rim, Jung H.; Kuhn, Kevin J.; Tandon, Lav

Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials’ properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% 240Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modelling feedback andmore » trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. In conclusion, based on this investigation, the most likely intended use for these plutonium foils was 239Pu fission foil targets for physics experiments, such as cross-section measurements, etc.« less

A simple model for the critical mass of a nuclear weapon

NASA Astrophysics Data System (ADS)

Reed, B. Cameron

2018-07-01

A probability-based model for estimating the critical mass of a fissile isotope is developed. The model requires introducing some concepts from nuclear physics and incorporating some approximations, but gives results correct to about a factor of two for uranium-235 and plutonium-239.

10 CFR 110.41 - Executive Branch review.

Code of Federal Regulations, 2010 CFR

2010-01-01

... export involving assistance to end uses related to isotope separation, chemical reprocessing, heavy water production, advanced reactors, or the fabrication of nuclear fuel containing plutonium, except for exports of... foreign reactor. (8) An export involving radioactive waste. (9) An export to any country listed in § 110...

Americium, plutonium and uranium contamination and speciation in well waters, streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site, Kazakhstan.

PubMed

León Vintró, L; Mitchell, P I; Omarova, A; Burkitbayev, M; Jiménez Nápoles, H; Priest, N D

2009-04-01

New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel'kem 1 and Tel'kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that (241)Am, (239,240)Pu and (238)U concentrations in well waters within the study area are in the range 0.04-87mBq dm(-3), 0.7-99mBq dm(-3), and 74-213mBq dm(-3), respectively, and for (241)Am and (239,240)Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01mBq dm(-3), 0.08mBq dm(-3) and 0.32mBq dm(-3) for (241)Am, (239,240)Pu and (238)U, respectively. The (235)U/(238)U isotopic ratio in almost all well and stream waters is slightly elevated above the 'best estimate' value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53-85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11-42microSv (mean 21microSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel'kem explosions.

Critical Need for Plutonium and Uranium Isotopic Standards with Lower Uncertainties

DOE PAGES

Mathew, Kattathu Joseph; Stanley, Floyd E.; Thomas, Mariam R.; ...

2016-09-23

Certified reference materials (CRMs) traceable to national and international safeguards database are a critical prerequisite for ensuring that nuclear measurement systems are free of systematic biases. CRMs are used to validate measurement processes associated with nuclear analytical laboratories. Diverse areas related to nuclear safeguards are impacted by the quality of the CRM standards available to analytical laboratories. These include: nuclear forensics, radio-chronometry, national and international safeguards, stockpile stewardship, nuclear weapons infrastructure and nonproliferation, fuel fabrication, waste processing, radiation protection, and environmental monitoring. For the past three decades the nuclear community is confronted with the strange situation that improvements in measurementmore » data quality resulting from the improved accuracy and precision achievable with modern multi-collector mass spectrometers could not be fully exploited due to large uncertainties associated with CRMs available from New Brunswick Laboratory (NBL) that are used for instrument calibration and measurement control. Similar conditions prevail for both plutonium and uranium isotopic standards and for impurity element standards in uranium matrices. Herein, the current status of U and Pu isotopic standards available from NBL is reviewed. Critical areas requiring improvement in the quality of the nuclear standards to enable the U. S. and international safeguards community to utilize the full potential of modern multi-collector mass spectrometer instruments are highlighted.« less

Critical Need for Plutonium and Uranium Isotopic Standards with Lower Uncertainties

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mathew, Kattathu Joseph; Stanley, Floyd E.; Thomas, Mariam R.

Certified reference materials (CRMs) traceable to national and international safeguards database are a critical prerequisite for ensuring that nuclear measurement systems are free of systematic biases. CRMs are used to validate measurement processes associated with nuclear analytical laboratories. Diverse areas related to nuclear safeguards are impacted by the quality of the CRM standards available to analytical laboratories. These include: nuclear forensics, radio-chronometry, national and international safeguards, stockpile stewardship, nuclear weapons infrastructure and nonproliferation, fuel fabrication, waste processing, radiation protection, and environmental monitoring. For the past three decades the nuclear community is confronted with the strange situation that improvements in measurementmore » data quality resulting from the improved accuracy and precision achievable with modern multi-collector mass spectrometers could not be fully exploited due to large uncertainties associated with CRMs available from New Brunswick Laboratory (NBL) that are used for instrument calibration and measurement control. Similar conditions prevail for both plutonium and uranium isotopic standards and for impurity element standards in uranium matrices. Herein, the current status of U and Pu isotopic standards available from NBL is reviewed. Critical areas requiring improvement in the quality of the nuclear standards to enable the U. S. and international safeguards community to utilize the full potential of modern multi-collector mass spectrometer instruments are highlighted.« less

10 CFR 150.11 - Critical mass.

Code of Federal Regulations, 2013 CFR

2013-01-01

... uranium enriched in the isotope U-235 in quantities not exceeding 350 grams of contained U-235; uranium-233 in quantities not exceeding 200 grams; plutonium in quantities not exceeding 200 grams; or any... not exceed the limitation and are within the formula, as follows: (175 (grams contained U-235/350)+(50...

10 CFR 150.11 - Critical mass.

Code of Federal Regulations, 2011 CFR

2011-01-01

... uranium enriched in the isotope U-235 in quantities not exceeding 350 grams of contained U-235; uranium-233 in quantities not exceeding 200 grams; plutonium in quantities not exceeding 200 grams; or any... not exceed the limitation and are within the formula, as follows: (175 (grams contained U-235/350)+(50...

10 CFR 150.11 - Critical mass.

Code of Federal Regulations, 2010 CFR

2010-01-01

... uranium enriched in the isotope U-235 in quantities not exceeding 350 grams of contained U-235; uranium-233 in quantities not exceeding 200 grams; plutonium in quantities not exceeding 200 grams; or any... not exceed the limitation and are within the formula, as follows: (175 (grams contained U-235/350)+(50...

10 CFR 150.11 - Critical mass.

Code of Federal Regulations, 2014 CFR

2014-01-01

... uranium enriched in the isotope U-235 in quantities not exceeding 350 grams of contained U-235; uranium-233 in quantities not exceeding 200 grams; plutonium in quantities not exceeding 200 grams; or any... not exceed the limitation and are within the formula, as follows: (175 (grams contained U-235/350)+(50...

10 CFR 150.11 - Critical mass.

Code of Federal Regulations, 2012 CFR

2012-01-01

... uranium enriched in the isotope U-235 in quantities not exceeding 350 grams of contained U-235; uranium-233 in quantities not exceeding 200 grams; plutonium in quantities not exceeding 200 grams; or any... not exceed the limitation and are within the formula, as follows: (175 (grams contained U-235/350)+(50...

An anti-neutrino detector to monitor nuclear reactor's power and fuel composition

NASA Astrophysics Data System (ADS)

Battaglieri, M.; DeVita, R.; Firpo, G.; Neuhold, P.; Osipenko, M.; Piombo, D.; Ricco, G.; Ripani, M.; Taiuti, M.

2010-05-01

In this contribution, we present the expected performance of a new detector to measure the absolute energy-integrated flux and the energy spectrum of anti-neutrinos emitted by a nuclear power plant. The number of detected anti-neutrino is a direct measure of the power while from the energy spectrum is possible to infer the evolution in time of the core isotopic composition. The proposed method should be sensitive to a sudden change in the core burn-up as caused, for instance, by a fraudulent subtraction of plutonium. The detector, a 130×100×100 cm3 cube with 1 m3 active volume, made by plastic scintillator wrapped in thin Gd foils, is segmented in 50 independent optical channels read, side by side, by a pair of 3 in. photomultipliers. Anti-neutrino interacts with hydrogen contained in the plastic scintillator via the neutron inverse β- decay ( ν¯p→e+n). The high segmentation of the detector allows to reduce the background from other reactions by detecting independent hits for the positron, the two photons emitted in the e+e- annihilation and the neutron.

Improved precision and accuracy in quantifying plutonium isotope ratios by RIMS

DOE PAGES

Isselhardt, B. H.; Savina, M. R.; Kucher, A.; ...

2015-09-01

Resonance ionization mass spectrometry (RIMS) holds the promise of rapid, isobar-free quantification of actinide isotope ratios in as-received materials (i.e. not chemically purified). Recent progress in achieving this potential using two Pu test materials is presented. RIMS measurements were conducted multiple times over a period of two months on two different Pu solutions deposited on metal surfaces. Measurements were bracketed with a Pu isotopic standard, and yielded absolute accuracies of the measured 240Pu/ 239Pu ratios of 0.7% and 0.58%, with precisions (95% confidence intervals) of 1.49% and 0.91%. In conclusion, the minor isotope 238Pu was also quantified despite the presencemore » of a significant quantity of 238U in the samples.« less

Fabrication of 12% {sup 240}Pu calorimetry standards

DOE Office of Scientific and Technical Information (OSTI.GOV)

Long, S.M.; Hildner, S.; Gutierrez, D.

1995-08-01

Throughout the DOE complex, laboratories are performing calorimetric assays on items containing high burnup plutonium. These materials contain higher isotopic range and higher wattages than materials previously encountered in vault holdings. Currently, measurement control standards have been limited to utilizing 6% {sup 240}Pu standards. The lower isotopic and wattage value standards do not complement the measurement of the higher burnup material. Participants of the Calorimetry Exchange (CALEX) Program have identified the need for new calorimetric assay standards with a higher wattage and isotopic range. This paper describes the fabrication and verification measurements of the new CALEX standard containing 12% {supmore » 240}Pu oxide with a wattage of about 6 to 8 watts.« less

Experiments and Monte Carlo modeling of a higher resolution Cadmium Zinc Telluride detector for safeguards applications

NASA Astrophysics Data System (ADS)

Borella, Alessandro

2016-09-01

The Belgian Nuclear Research Centre is engaged in R&D activity in the field of Non Destructive Analysis on nuclear materials, with focus on spent fuel characterization. A 500 mm3 Cadmium Zinc Telluride (CZT) with enhanced resolution was recently purchased. With a full width at half maximum of 1.3% at 662 keV, the detector is very promising in view of its use for applications such as determination of uranium enrichment and plutonium isotopic composition, as well as measurement on spent fuel. In this paper, I report about the work done with such a detector in terms of its characterization. The detector energy calibration, peak shape and efficiency were determined from experimental data. The data included measurements with calibrated sources, both in a bare and in a shielded environment. In addition, Monte Carlo calculations with the MCNPX code were carried out and benchmarked with experiments.

Plutonium-239 and americium-241 uptake by plants from soil. Final report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brown, K.W.

1979-03-01

Alfalfa was grown in soil contaminated with plutonium-239 dioxide (239PuO2) at a concentration of 29.7 nanocuries per gram (nCi/g). In addition to alfalfa, radishes, wheat, rye, and tomatoes were grown in soils contaminated with americium-241 nitrate (241Am(NO3)3) at a concentration of 189 nCi/g. The length of exposure varied from 52 days for the radishes to 237 days for the alfalfa. The magnitude of plutonium incorporation by the alfalfa as indicated by the concentration ratio, 0.0000025, was similar to previously reported data using other chemical forms of plutonium. The results did indicate, however, that differences in the biological availability of plutoniummore » isotopes do exist. All of the species exposed to americium-241 assimilated and translocated this radioisotope to the stem, leaf, and fruiting structures. The magnitude of incorporation as signified by the concentration ratios varied from 0.00001 for the wheat grass to 0.0152 for the radishes. An increase in the uptake of americium also occurred as a function of time for four of the five plant species. Evidence indicates that the predominant factor in plutonium and americium uptake by plants may involve the chelation of these elements in soils by the action of compounds such as citric acid and/or other similar chelating agents released from plant roots.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kippen, Karen Elizabeth

This is Los Alamos National Laboratory's (LANL) June 2016 newsletter of the Materials Science and Technology Division. The following are major topics in this newsletter: MST-8 scientists guide national efforts to overcome nuclear energy technical challenges, first-ever scanning probe microscopy capabilities for plutonium, laboratory metallurgists make thorium targets for production of cancer-fighting isotopes, and a spotlight on Veronica Livescu.

Importance of resonance interference effects in multigroup self-shielding calculation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stachowski, R.E.; Protsik, R.

1995-12-31

The impact of the resonance interference method (RIF) on multigroup neutron cross sections is significant for major isotopes in the fuel, indicating the importance of resonance interference in the computation of gadolinia burnout and plutonium buildup. The self-shielding factor method with the RIF method effectively eliminates shortcomings in multigroup resonance calculations.

10 CFR 140.91 - Appendix A-Form of nuclear energy liability policy for facilities.

Code of Federal Regulations, 2010 CFR

2010-01-01

... designed or used for (a) separating the isotopes of uranium or plutonium, (b) processing or utilizing spent... processing, fabricating or alloying of special nuclear material if at any time the total amount of such... operations conducted thereat; Nuclear reactor means any apparatus designed or used to sustain nuclear fission...

10 CFR 140.91 - Appendix A-Form of nuclear energy liability policy for facilities.

Code of Federal Regulations, 2013 CFR

2013-01-01

... designed or used for (a) separating the isotopes of uranium or plutonium, (b) processing or utilizing spent... processing, fabricating or alloying of special nuclear material if at any time the total amount of such... operations conducted thereat; Nuclear reactor means any apparatus designed or used to sustain nuclear fission...

10 CFR 140.91 - Appendix A-Form of nuclear energy liability policy for facilities.

Code of Federal Regulations, 2014 CFR

2014-01-01

... designed or used for (a) separating the isotopes of uranium or plutonium, (b) processing or utilizing spent... processing, fabricating or alloying of special nuclear material if at any time the total amount of such... operations conducted thereat; Nuclear reactor means any apparatus designed or used to sustain nuclear fission...

10 CFR 140.91 - Appendix A-Form of nuclear energy liability policy for facilities.

Code of Federal Regulations, 2012 CFR

2012-01-01

... designed or used for (a) separating the isotopes of uranium or plutonium, (b) processing or utilizing spent... processing, fabricating or alloying of special nuclear material if at any time the total amount of such... operations conducted thereat; Nuclear reactor means any apparatus designed or used to sustain nuclear fission...

10 CFR 140.91 - Appendix A-Form of nuclear energy liability policy for facilities.

Code of Federal Regulations, 2011 CFR

2011-01-01

... designed or used for (a) separating the isotopes of uranium or plutonium, (b) processing or utilizing spent... processing, fabricating or alloying of special nuclear material if at any time the total amount of such... operations conducted thereat; Nuclear reactor means any apparatus designed or used to sustain nuclear fission...

78 FR 1848 - Plutonium-238 Production for Radioisotope Power Systems for National Aeronautics and Space...

Federal Register 2010, 2011, 2012, 2013, 2014

2013-01-09

... for Accomplishing Expanded Civilian Nuclear Energy Research and Development and Isotope Production...-75), Office of Nuclear Energy, U.S. Department of Energy, 1000 Independence Ave. SW., Washington, DC 20585, Phone 301- 903-6062, [email protected]nuclear.energy.gov . For information on NEPA analysis for Pu...

Soil and sediment sample analysis for the sequential determination of natural and anthropogenic radionuclides.

PubMed

Michel, H; Levent, D; Barci, V; Barci-Funel, G; Hurel, C

2008-02-15

A new sequential method for the determination of both natural (U, Th) and anthropogenic (Sr, Cs, Pu, Am) radionuclides has been developed for application to soil and sediment samples. The procedure was optimised using a reference sediment (IAEA-368) and reference soils (IAEA-375 and IAEA-326). Reference materials were first digested using acids (leaching), 'total' acids on hot plate, and acids in microwave in order to compare the different digestion technique. Then, the separation and purification were made by anion exchange resin and selective extraction chromatography: transuranic (TRU) and strontium (SR) resins. Natural and anthropogenic alpha radionuclides were separated by uranium and tetravalent actinide (UTEVA) resin, considering different acid elution medium. Finally, alpha and gamma semiconductor spectrometer and liquid scintillation spectrometer were used to measure radionuclide activities. The results obtained for strontium-90, cesium-137, thorium-232, uranium-238, plutonium-239+240 and americium-241 isotopes by the proposed method for the reference materials provided excellent agreement with the recommended values and good chemical recoveries. Plutonium isotopes in alpha spectrometry planchet deposits could be also analysed by ICPMS.

SEPARATION OF URANIUM, PLUTONIUM AND FISSION PRODUCTS FROM NEUTRON- BOMBARDED URANIUM

DOEpatents

Martin, A.E.; Johnson, I.; Burris, L. Jr.; Winsch, I.O.; Feder, H.M.

1962-11-13

A process is given for removing plutonium and/or fission products from uranium fuel. The fuel is dissolved in molten zinc--magnesium (10 to 18% Mg) alloy, more magnesium is added to obtain eutectic composition whereby uranium precipitates, and the uranium are separated from the Plutoniumand fission-product- containing eutectic. (AEC)

EXTRACTION METHOD FOR SEPARATING URANIUM, PLUTONIUM, AND FISSION PRODUCTS FROM COMPOSITIONS CONTAINING SAME

DOEpatents

Seaborg, G.T.

1957-10-29

Methods for separating plutonium from the fission products present in masses of neutron irradiated uranium are reported. The neutron irradiated uranium is first dissolved in an aqueous solution of nitric acid. The plutonium in this solution is present as plutonous nitrate. The aqueous solution is then agitated with an organic solvent, which is not miscible with water, such as diethyl ether. The ether extracts 90% of the uraryl nitrate leaving, substantially all of the plutonium in the aqueous phase. The aqueous solution of plutonous nitrate is then oxidized to the hexavalent state, and agitated with diethyl ether again. In the ether phase there is then obtained 90% of plutonium as a solution of plutonyl nitrate. The ether solution of plutonyl nitrate is then agitated with water containing a reducing agent such as sulfur dioxide, and the plutonium dissolves in the water and is reduced to the plutonous state. The uranyl nitrate remains in the ether. The plutonous nitrate in the water may be recovered by precipitation.

A METHOD TO IMPROVE DOSE ASSESSMENT BY RECONSTRUCTION OF THE COMPLETE ISOTOPES INVENTORY.

PubMed

Bonin, Alice; Tsilanizara, Aimé

2017-06-01

Radiation shielding assessments may underestimate the expected dose if some isotopes at trace level are not considered in the isotopes inventory of the shielded radioactive materials. Indeed, information about traces is not often available. Nevertheless, the activation of some minor isotopic traces may significantly contribute to the dose build-up. This paper presents a new method (Isotopes Inventory Reconstruction-IIR) estimating the concentration of the minor isotopes in the irradiated material at the beginning of the cooling period. The method requires the solution of the inverse problem describing the irradiated material's decay. In a mixture of an irradiated uranium-plutonium oxide shielded by a set-up made of stainless-steel, porous polyethylene plaster and lead methyl methacrylate, the comparison between different methods proves that the IIR-method allows better assessment of the dose than other approximate methods. © The Author 2016. Published by Oxford University Press. All rights reserved. For Permissions, please email: journals.permissions@oup.com.

Application of isotope-dilution laser ablation ICP-MS for direct determination of Pu concentrations in soils at pg g(-1) levels.

PubMed

Boulyga, Sergei F; Tibi, Markus; Heumann, Klaus G

2004-01-01

The methods available for determination of environmental contamination by plutonium at ultra-trace levels require labor-consuming sample preparation including matrix removal and plutonium extraction in both nuclear spectroscopy and mass spectrometry. In this work, laser-ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) was applied for direct analysis of Pu in soil and sediment samples. Application of a LINA-Spark-Atomizer system (a modified laser ablation system providing high ablation rates) coupled with a sector-field ICP-MS resulted in detection limits as low as 3x10(-13) g g(-1) for Pu isotopes in soil samples containing uranium at a concentration of a few microg g(-1). The isotope dilution (ID) technique was used for quantification, which compensated for matrix effects in LA-ICP-MS. Interferences by UH+ and PbO2+ ions and by the peak tail of 238U+ ions were reduced or separated by use of dry plasma conditions and a mass resolution of 4000, respectively. No other effects affecting measurement accuracy, except sample inhomogeneity, were revealed. Comparison of results obtained for three contaminated soil samples by use of alpha-spectrometry, ICP-MS with sample decomposition, and LA-ICP-IDMS showed, in general, satisfactory agreement of the different methods. The specific activity of (239+240)Pu (9.8 +/- 3.0 mBq g(-1)) calculated from LA-ICP-IDMS analysis of SRM NIST 4357 coincided well with the certified value of 10.4 +/- 0.2 mBq g(-1). However, the precision of LA-ICP-MS for determination of plutonium in inhomogeneous samples, i.e. if "hot" particles are present, is limited. As far as we are aware this paper reports the lowest detection limits and element concentrations yet measured in direct LA-ICP-MS analysis of environmental samples.

Determination of the 240Pu/ 239Pu atomic ratio in soils from Palomares (Spain) by low-energy accelerator mass spectrometry

NASA Astrophysics Data System (ADS)

Chamizo, E.; García-León, M.; Synal, H.-A.; Suter, M.; Wacker, L.

2006-08-01

In 1966, the nuclear fuel of two thermonuclear bombs was released over the Spanish region of Palomares, due to a B52 bomber accident during a refuelling operation. Since then, much effort has been made to assess its impact to the different environmental compartments of this area in South-East Spain, mostly by measuring the 239+240Pu activity concentration and the 238Pu/239+240Pu activity ratio. Nevertheless, these measurements do not give enough information on the problem. In order to recognize unambiguously small traces of the weapon-grade plutonium released in the accident, the ratio of the two major isotopes of plutonium, 240Pu/239Pu, has to be determined. In this work, this ratio has been measured in low- and high-activity samples from Palomares by means of low-energy accelerator mass spectrometry (AMS). That way, we will show the potential of the new generation of compact AMS facilities in terms of plutonium characterization at ultra-trace levels.

Microprobe Analysis of Pu-Ga Standards

DOE PAGES

Wall, Angélique D.; Romero, Joseph P.; Schwartz, Daniel

2017-08-04

In order to obtain quantitative analysis using an Electron Scanning Microprobe it is essential to have a standard of known composition. Most elemental and multi-elemental standards can be easily obtained from places like Elemental Scientific or other standards organizations that are NIST (National Institute of Standards and Technology) traceable. It is, however, more challenging to find standards for plutonium. Past work performed in our group has typically involved using the plutonium sample to be analysed as its own standard as long as all other known components of the sample have standards to be compared to [1,2,3]. Finally, this method worksmore » well enough, but this experiment was performed in order to develop a more reliable standard for plutonium using five samples of known chemistry of a plutonium gallium mix that could then be used as the main plutonium and gallium standards for future experiments.« less

Microprobe Analysis of Pu-Ga Standards

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wall, Angélique D.; Romero, Joseph P.; Schwartz, Daniel

In order to obtain quantitative analysis using an Electron Scanning Microprobe it is essential to have a standard of known composition. Most elemental and multi-elemental standards can be easily obtained from places like Elemental Scientific or other standards organizations that are NIST (National Institute of Standards and Technology) traceable. It is, however, more challenging to find standards for plutonium. Past work performed in our group has typically involved using the plutonium sample to be analysed as its own standard as long as all other known components of the sample have standards to be compared to [1,2,3]. Finally, this method worksmore » well enough, but this experiment was performed in order to develop a more reliable standard for plutonium using five samples of known chemistry of a plutonium gallium mix that could then be used as the main plutonium and gallium standards for future experiments.« less

Characterization and source term assessments of radioactive particles from Marshall Islands using non-destructive analytical techniques

NASA Astrophysics Data System (ADS)

Jernström, J.; Eriksson, M.; Simon, R.; Tamborini, G.; Bildstein, O.; Marquez, R. Carlos; Kehl, S. R.; Hamilton, T. F.; Ranebo, Y.; Betti, M.

2006-08-01

Six plutonium-containing particles stemming from Runit Island soil (Marshall Islands) were characterized by non-destructive analytical and microanalytical methods. Composition and elemental distribution in the particles were studied with synchrotron radiation based micro X-ray fluorescence spectrometry. Scanning electron microscope equipped with energy dispersive X-ray detector and with wavelength dispersive system as well as a secondary ion mass spectrometer were used to examine particle surfaces. Based on the elemental composition the particles were divided into two groups: particles with pure Pu matrix, and particles where the plutonium is included in Si/O-rich matrix being more heterogenously distributed. All of the particles were identified as nuclear fuel fragments of exploded weapon components. As containing plutonium with low 240Pu/ 239Pu atomic ratio, less than 0.065, which corresponds to weapons-grade plutonium or a detonation with low fission yield, the particles were identified to originate from the safety test and low-yield tests conducted in the history of Runit Island. The Si/O-rich particles contained traces of 137Cs ( 239 + 240 Pu/ 137Cs activity ratio higher than 2500), which indicated that a minor fission process occurred during the explosion. The average 241Am/ 239Pu atomic ratio in the six particles was 3.7 × 10 - 3 ± 0.2 × 10 - 3 (February 2006), which indicated that plutonium in the different particles had similar age.

Estimation of the formation rates of polyatomic species of heavy metals in plutonium analyses using a multicollector ICP-MS with a desolvating nebulizer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mitroshkov, Alexandre V.; Olsen, Khris B.; Thomas, Linda M.

2015-01-01

The analyses of IAEA and environmental samples for Plutonium isotopic content are conducted normally at very low concentrations of Pu–usually in the range of part per trillion level and even more often at the parts per quadrillion level. To analyze such low concentrations, the interferences in the analytical solution must be reduced as much as possible. Polyatomic interferences (PIs), formed by the heavy metals (HMs) from Hf to Bi are known to create the problems for Pu isotopic analyses, because even the relatively high resolution of a modern multicollector ICP-MS is not enough to separate Pu isotopes from this PIsmore » in most of the cases. Desolvating nebulizers (DSN) (e.g. APEX and AridusII) reduce significantly the formation of PIs compare to the use of wet plasma. The purpose of this work was to investigate the rate of formation of PIs, produced by HMs, when high resolution MC ICP-MS with desolvating nebulizer was used for Pu isotopic analyses and to estimate the influence of the metals present in the sample on the results of analyses. The NU Plasma HR Multicollector and AridusII desolvating nebulizer were used in this investigation. This investigation was done for all Pu isotopes normally analyzed by ICP-MS, including ²⁴⁴Pu, with the exception of ²³⁸Pu, which most of the time can’t be analyzed by ICP-MS, because of the overwhelming presence of ²³⁸U in the solutions. The PI formation rates were determined and reported for all 12 HMs from Hf to Bi. Selected IAEA samples were scanned for the presence of HMs and the influence of HMs on the results of Pu isotopic analyses was evaluated. It was found that the implemented separation procedure provides sufficient separation of HM from Pu, although the effect of PIs on the measurement of low level isotopes like ²⁴¹Pu and ²⁴²Pu in some cases can still be observed.« less

Analysis of a nuclear accident: fission and activation product releases from the Fukushima Daiichi nuclear facility as remote indicators of source identification, extent of release, and state of damaged spent nuclear fuel.

PubMed

Schwantes, Jon M; Orton, Christopher R; Clark, Richard A

2012-08-21

Researchers evaluated radionuclide measurements of environmental samples taken from the Fukushima Daiichi nuclear facility and reported on the Tokyo Electric Power Co. Website following the 2011 tsunami-initiated catastrophe. This effort identified Units 1 and 3 as the major source of radioactive contamination to the surface soil near the facility. Radionuclide trends identified in the soils suggested that: (1) chemical volatility driven by temperature and reduction potential within the vented reactors' primary containment vessels dictated the extent of release of radiation; (2) all coolant had likely evaporated by the time of venting; and (3) physical migration through the fuel matrix and across the cladding wall were minimally effective at containing volatile species, suggesting damage to fuel bundles was extensive. Plutonium isotopic ratios and their distance from the source indicated that the damaged reactors were the major contributor of plutonium to surface soil at the source, decreasing rapidly with distance from the facility. Two independent evaluations estimated the fraction of the total plutonium inventory released to the environment relative to cesium from venting Units 1 and 3 to be ∼0.002-0.004%. This study suggests significant volatile radionuclides within the spent fuel at the time of venting, but not as yet observed and reported within environmental samples, as potential analytes of concern for future environmental surveys around the site. The majority of the reactor inventories of isotopes of less volatile elements like Pu, Nb, and Sr were likely contained within the damaged reactors during venting.

Sub-micron Hard X-ray Fluorescence Imaging of Synthetic Elements

PubMed Central

Jensen, Mark P.; Aryal, Baikuntha P.; Gorman-Lewis, Drew; Paunesku, Tatjana; Lai, Barry; Vogt, Stefan; Woloschak, Gayle E.

2013-01-01

Synchrotron-based X-ray fluorescence microscopy (SXFM) using hard X-rays focused into sub-micron spots is a powerful technique for elemental quantification and mapping, as well as microspectroscopic measurement such as μ-XANES (X-ray absorption near edge structure). We have used SXFM to image and simultaneously quantify the transuranic element plutonium at the L3 or L2 edge as well as lighter biologically essential elements in individual rat pheochromocytoma (PC12) cells after exposure to the long-lived plutonium isotope 242Pu. Elemental maps reveal that plutonium localizes principally in the cytoplasm of the cells and avoids the cell nucleus, which is marked by the highest concentrations of phosphorus and zinc, under the conditions of our experiments. The minimum detection limit under typical acquisition conditions for an average 202 μm2 cell is 1.4 fg Pu/cell or 2.9 × 10−20 moles Pu/μm2, which is similar to the detection limit of K-edge SXFM of transition metals at 10 keV. Copper electron microscopy grids were used to avoid interference from gold X-ray emissions, but traces of strontium present in naturally occurring calcium can still interfere with plutonium detection using its Lα X-ray emission. PMID:22444530

Physics overview of AVLIS

NASA Astrophysics Data System (ADS)

Solarz, R. W.

1985-02-01

Atomic vapor laster isotope separation (AVLIS) represents the largest-scale potential application of tunable lasers that has received serious attention. The underlying physical principles were identified and optimized, the major technology components were developed, and the integrated enrichment performance of the process was tested. The central physical processes are outlined, progress to date on the technology elements is reviewed, and scaling laws are fomulated. Two primary applications are the production of light-water reactor fuel and the conversion of fuel-grade plutonium to weapons-grade material. A variety of applications exist that all potentially use a common base of AVLIS technology. These include missions such as the enrichment of mercury isotopes to improve fluorescent lamp efficiency, the enrichment of iodine isotopes for medical isotope use, and the cleanup of strontium from defense waste for recovering strontium isotopes for radiothermal mechanical generators. The ability to radidly assess the economic and technical feasibility of each mission is derived from the general applicability of AVLIS physics and AVLIS technology.

Soils element history, sampling, analyses, and recommendations. [Plutonium isotopes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fowler, E.B.; Essington, E.H.

A five year history of the Soils Element of the Nevada Applied Ecology Group (NAEG) is presented. Major projects are reviewed. Emphasis is placed on mound studies and profile studies for the period March 1, 1975, through February 1, 1976. A series of recommendations is made relative to extensions of past efforts of the Soils Element of the NAEG.

Plutonium and americium in the foodchain lichen-reindeer-man

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jaakkola, T.; Hakanen, M.; Keinonen, M.

1977-01-01

The atmospheric nuclear tests have produced a worldwide fallout of transuranium elements. In addition to plutonium measurable concentrations of americium are to be found in terrestrial and aquatic environments. The metabolism of plutonium in reindeer was investigated by analyzing plutonium in liver, bone, and lung collected during 1963-1976. To determine the distribution of plutonium in reindeer all tissues of four animals of different ages were analyzed. To estimate the uptake of plutonium from the gastrointestinal tract in reindeer, the tissue samples of elk were also analyzed. Elk which is of the same genus as reindeer does not feed on lichenmore » but mainly on deciduous plants, buds, young twigs, and leaves of trees and bushes. The composition of its feed corresponds fairly well to that of reindeer during the summer. Studies on behaviour of americium along the foodchain lichen-reindeer-man were started by determining the Am-241 concentrations in lichen and reindeer liver. The Am-241 results were compared with those of Pu-239,240. The plutonium contents of the southern Finns, whose diet does not contain reindeer tissues, were determined by analyzing autopsy tissue samples (liver, lung, and bone). The southern Finns form a control group to the Lapps consuming reindeer tissues. Plutonium analyses of the placenta, blood, and tooth samples of the Lapps were performed.« less

Analysis of the 2H-evaporator scale samples (HTF-17-56, -57)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hay, M.; Coleman, C.; Diprete, D.

Savannah River National Laboratory analyzed scale samples from both the wall and cone sections of the 242-16H Evaporator prior to chemical cleaning. The samples were analyzed for uranium and plutonium isotopes required for a Nuclear Criticality Safety Assessment of the scale removal process. The analysis of the scale samples found the material to contain crystalline nitrated cancrinite and clarkeite. Samples from both the wall and cone contain depleted uranium. Uranium concentrations of 16.8 wt% 4.76 wt% were measured in the wall and cone samples, respectively. The ratio of plutonium isotopes in both samples is ~85% Pu-239 and ~15% Pu-238 bymore » mass and shows approximately the same 3.5 times higher concentration in the wall sample versus the cone sample as observed in the uranium concentrations. The mercury concentrations measured in the scale samples were higher than previously reported values. The wall sample contains 19.4 wt% mercury and the cone scale sample 11.4 wt% mercury. The results from the current scales samples show reasonable agreement with previous 242-16H Evaporator scale sample analysis; however, the uranium concentration in the current wall sample is substantially higher than previous measurements.« less

Quantitative Analysis of Plutonium Content in Particles Collected from a Certified Reference Material by Total Nuclear Reaction Energy (Q Value) Spectroscopy

NASA Astrophysics Data System (ADS)

Croce, M. P.; Hoover, A. S.; Rabin, M. W.; Bond, E. M.; Wolfsberg, L. E.; Schmidt, D. R.; Ullom, J. N.

2016-08-01

Microcalorimeters with embedded radioisotopes are an emerging category of sensor with advantages over existing methods for isotopic analysis of trace-level nuclear materials. For each nuclear decay, the energy of all decay products captured by the absorber (alpha particles, gamma rays, X-rays, electrons, daughter nuclei, etc.) is measured in one pulse. For alpha-decaying isotopes, this gives a measurement of the total nuclear reaction energy (Q value) and the spectra consist of well-separated, narrow peaks. We have demonstrated a simple mechanical alloying process to create an absorber structure consisting of a gold matrix with small inclusions of a radioactive sample. This absorber structure provides an optimized energy thermalization environment, resulting in high-resolution spectra with minimal tailing. We have applied this process to the analysis of particles collected from the surface of a plutonium metal certified reference material (CRM-126A from New Brunswick Laboratory) and demonstrated isotopic analysis by microcalorimeter Q value spectroscopy. Energy resolution from the Gaussian component of a Bortels function fit was 1.3 keV FWHM at 5244 keV. The collected particles were integrated directly into the detector absorber without any chemical processing. The ^{238}Pu/^{239}Pu and ^{240}Pu/^{239}Pu mass ratios were measured and the results confirmed against the certificate of analysis for the reference material. We also demonstrated inter-element analysis capability by measuring the ^{241}Am/^{239}Pu mass ratio.

General statistical considerations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Eberhardt, L L; Gilbert, R O

From NAEG plutonium environmental studies program meeting; Las Vegas, Nevada, USA (2 Oct 1973). The high sampling variability encountered in environmental plutonium studies along with high analytical costs makes it very important that efficient soil sampling plans be used. However, efficient sampling depends on explicit and simple statements of the objectives of the study. When there are multiple objectives it may be difficult to devise a wholly suitable sampling scheme. Sampling for long-term changes in plutonium concentration in soils may also be complex and expensive. Further attention to problems associated with compositing samples is recommended, as is the consistent usemore » of random sampling as a basic technique. (auth)« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reilly, Sean Douglas; Smith, Paul Herrick; Jarvinen, Gordon D.

Understanding the water solubility of plutonium and uranium compounds and residues at TA-55 is necessary to provide a technical basis for appropriate criticality safety, safety basis and accountability controls. Individual compound solubility was determined using published solubility data and solution thermodynamic modeling. Residue solubility was estimated using a combination of published technical reports and process knowledge of constituent compounds. The scope of materials considered includes all compounds and residues at TA-55 as of March 2016 that contain Pu-239 or U-235 where any single item in the facility has more than 500 g of nuclear material. This analysis indicates that themore » following materials are not appreciably soluble in water: plutonium dioxide (IDC=C21), plutonium phosphate (IDC=C66), plutonium tetrafluoride (IDC=C80), plutonium filter residue (IDC=R26), plutonium hydroxide precipitate (IDC=R41), plutonium DOR salt (IDC=R42), plutonium incinerator ash (IDC=R47), uranium carbide (IDC=C13), uranium dioxide (IDC=C21), U 3O 8 (IDC=C88), and uranium filter residue (IDC=R26). This analysis also indicates that the following materials are soluble in water: plutonium chloride (IDC=C19) and uranium nitrate (IDC=C52). Equilibrium calculations suggest that PuOCl is water soluble under certain conditions, but some plutonium processing reports indicate that it is insoluble when present in electrorefining residues (R65). Plutonium molten salt extraction residues (IDC=R83) contain significant quantities of PuCl 3, and are expected to be soluble in water. The solubility of the following plutonium residues is indeterminate due to conflicting reports, insufficient process knowledge or process-dependent composition: calcium salt (IDC=R09), electrorefining salt (IDC=R65), salt (IDC=R71), silica (IDC=R73) and sweepings/screenings (IDC=R78). Solution thermodynamic modeling also indicates that fire suppression water buffered with a commercially-available phosphate buffer would significantly reduce the solubility of PuCl 3 by the precipitation of PuPO 4.« less

Ultra-Low Level Plutonium Isotopes in the NIST SRM 4355A (Peruvian Soil-1)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Inn, Kenneth G.; LaRosa, Jerome; Nour, Svetlana

2009-05-31

For more than 20 years, countries and their agencies which monitor discharge sites and storage facilities have relied on the National Institute of Standards and Technology (NIST) Standard Reference Material (SRM) 4355 Peruvian Soil reference material. Its low fallout contamination makes it an ideal soil blank for measurements associated with terrestrial pathway to man studies. Presently, SRM 4355 is out of stock, and a new batch of the Peruvian soil is currently under development as future NIST SRM 4355A. Both environmental radioanalytical laboratories and mass spectrometry communities will benefit from this SRM. The former must assess their laboratory contamination andmore » measurement detection limits by measurement of blank sample material. The Peruvian Soil is so low in anthropogenic radionuclides that it is a suitable virtual blank. On the other hand, mass spectrometric laboratories have high sensitivity instruments that are capable of quantitative isotopic measurements at low plutonium levels of the SRM 4355 (first Peruvian Soil SRM) that provided the mass spectrometric community with the calibration, quality control, and testing material needed for methods development, and legal defensibility. The quantification of the ultra-low plutonium content in the SRM 4355A was a considerable challenge for the mass spectrometric laboratories. Careful blank control and correction, isobaric interferences, instrument stability, peak assessment, and detection assessment were necessary. Furthermore, a systematic statistical evaluation of the measurement results and considerable discussions with the mass spectroscopy metrologists were needed to derive the certified values and uncertainties. SRM 4355A will provide the mass spectrometric community with the quality control and testing material needed for higher sensitivity methods development, and legal defensibility.« less

Ultra-low level plutonium isotopes in the NIST SRM 4355A (Peruvian Soil-1).

PubMed

Inn, Kenneth G W; LaRosa, Jerome; Nour, Svetlana; Brooks, George; LaMont, Steve; Steiner, Rob; Williams, Ross; Patton, Brad; Bostick, Debbie; Eiden, Gregory; Petersen, Steve; Douglas, Matthew; Beals, Donna; Cadieux, James; Hall, Greg; Goldberg, Steve; Vogt, Stephan

2009-05-01

For more than 20 years, countries and their agencies which monitor radionuclide discharge sites and storage facilities have relied on the National Institute of Standards and Technology (NIST) Standard Reference Material (SRM) 4355 Peruvian Soil. Its low fallout contamination makes it an ideal soil blank for measurements associated with terrestrial-pathway-to-man studies. Presently, SRM 4355 is out of stock, and a new batch of the Peruvian soil is currently under development as future NIST SRM 4355A. Both environmental radioanalytical laboratories and mass spectrometry communities will benefit from the use of this SRM. The former must assess their laboratory procedural contamination and measurement detection limits by measurement of blank sample material. The Peruvian Soil is so low in anthropogenic radionuclide content that it is a suitable virtual blank. On the other hand, mass spectrometric laboratories have high sensitivity instruments that are capable of quantitative isotopic measurements at low plutonium levels in the SRM 4355 (first Peruvian Soil SRM) that provided the mass spectrometric community with the calibration, quality control, and testing material needed for methods development and legal defensibility. The quantification of the ultra-low plutonium content in the SRM 4355A was a considerable challenge for the mass spectrometric laboratories. Careful blank control and correction, isobaric interferences, instrument stability, peak assessment, and detection assessment were necessary. Furthermore, a systematic statistical evaluation of the measurement results and considerable discussions with the mass spectroscopy metrologists were needed to derive the certified values and uncertainties. The one sided upper limit of the 95% tolerance with 95% confidence for the massic (239)Pu content in SRM 4355A is estimated to be 54,000 atoms/g.

Submicron hard X-ray fluorescence imaging of synthetic elements.

PubMed

Jensen, Mark P; Aryal, Baikuntha P; Gorman-Lewis, Drew; Paunesku, Tatjana; Lai, Barry; Vogt, Stefan; Woloschak, Gayle E

2012-04-13

Synchrotron-based X-ray fluorescence microscopy (XFM) using hard X-rays focused into sub-micron spots is a powerful technique for elemental quantification and mapping, as well as microspectroscopic measurements such as μ-XANES (X-ray absorption near edge structure). We have used XFM to image and simultaneously quantify the transuranic element plutonium at the L(3) or L(2)-edge as well as Th and lighter biologically essential elements in individual rat pheochromocytoma (PC12) cells after exposure to the long-lived plutonium isotope (242)Pu. Elemental maps demonstrate that plutonium localizes principally in the cytoplasm of the cells and avoids the cell nucleus, which is marked by the highest concentrations of phosphorus and zinc, under the conditions of our experiments. The minimum detection limit under typical acquisition conditions with an incident X-ray energy of 18 keV for an average 202 μm(2) cell is 1.4 fg Pu or 2.9×10(-20) moles Pu μm(-2), which is similar to the detection limit of K-edge XFM of transition metals at 10 keV. Copper electron microscopy grids were used to avoid interference from gold X-ray emissions, but traces of strontium present in naturally occurring calcium can still interfere with plutonium detection using its L(α) X-ray emission. Copyright © 2012 Elsevier B.V. All rights reserved.

The Association of Inbreeding With Lung Fibrosis Incidence in Beagle Dogs That Inhaled 238PuO2 or 239PuO2.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wilson, Dulaney A.; Brigantic, Andrea M.; Morgan, William F.

Studies of health effects in animals after exposure to internally deposited radionuclides were intended to supplement observational studies in humans. Both nuclear workers and Beagle dogs have exhibited plutonium associated lung fibrosis; however, the dogs smaller gene pool may limit the applicability of findings to humans. Data on Beagles that inhaled either plutonium-238 dioxide (238PuO2) or plutonium-239 dioxide (239PuO2) were analyzed. Wright's Coefficient of Inbreeding was used to measure genetic or familial susceptibility and was assessed as an explanatory variable when modeling the association between lung fibrosis incidence and plutonium exposure. Lung fibrosis was diagnosed in approximately 80% of themore » exposed dogs compared with 23.7% of the control dogs. The maximum degree of inbreeding was 9.4%. Regardless of isotope, the addition of inbreeding significantly improved the model in female dogs but not in males. In female dogs an increased inbreeding coefficient predicted decreased hazard of a lung fibrosis diagnosis. Lung fibrosis was common in these dogs with inbreeding affecting models of lung fibrosis incidence in females but not in males. The apparent protective effect in females predicted by these models of lung fibrosis incidence is likely to be minimal given the small degree of inbreeding in these groups.« less

Solubility of Plutonium (IV) Oxalate During Americium/Curium Pretreatment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rudisill, T.S.

1999-08-11

Approximately 15,000 L of solution containing isotopes of americium and curium (Am/Cm) will undergo stabilization by vitrification at the Savannah River Site (SRS). Prior to vitrification, an in-tank pretreatment will be used to remove metal impurities from the solution using an oxalate precipitation process. Material balance calculations for this process, based on solubility data in pure nitric acid, predict approximately 80 percent of the plutonium in the solution will be lost to waste. Due to the uncertainty associated with the plutonium losses during processing, solubility experiments were performed to measure the recovery of plutonium during pretreatment and a subsequent precipitationmore » process to prepare a slurry feed for a batch melter. A good estimate of the plutonium content of the glass is required for planning the shipment of the vitrified Am/Cm product to Oak Ridge National Laboratory (ORNL).The plutonium solubility in the oxalate precipitation supernate during pretreatment was 10 mg/mL at 35 degrees C. In two subsequent washes with a 0.25M oxalic acid/0.5M nitric acid solution, the solubility dropped to less than 5 mg/mL. During the precipitation and washing steps, lanthanide fission products in the solution were mostly insoluble. Uranium, and alkali, alkaline earth, and transition metal impurities were soluble as expected. An elemental material balance for plutonium showed that greater than 94 percent of the plutonium was recovered in the dissolved precipitate. The recovery of the lanthanide elements was generally 94 percent or higher except for the more soluble lanthanum. The recovery of soluble metal impurities from the precipitate slurry ranged from 15 to 22 percent. Theoretically, 16 percent of the soluble oxalates should have been present in the dissolved slurry based on the dilution effects and volumes of supernate and wash solutions removed. A trace level material balance showed greater than 97 percent recovery of americium-241 (from the beta dec ay of plutonium-241) in the dissolved precipitate, a value consistent with the recovery of europium, the americium surrogate.In a subsequent experiment, the plutonium solubility following an oxalate precipitation to simulate the preparation of a slurry feed for a batch melter was 21 mg/mL at 35 degrees C. The increase in solubility compared to the value measured during the pretreatment experiment was attributed to the increased nitrate concentration and ensuing increase in plutonium complexation. The solubility of the plutonium following a precipitant wash with 0.1M oxalic acid was unchanged. The recovery of plutonium from the precipitate slurry was greater than 97 percent allowing an estimation that approximately 92 percent of the plutonium in Tank 17.1 will report to the glass. The behavior of the lanthanides and soluble metal impurities was consistent with the behavior seen during the pretreatment experiment. A trace level material balance showed that 99.9 percent of the americium w as recovered from the precipitate slurry. The overall recovery of americium from the pretreatment and feed preparation processes was greater than 97 percent, which was consistent with the measured recovery of the europium surrogate.« less

Evaluating bis(2-ethylhexyl) methanediphosphonic acid (H 2DEH[MDP]) based polymer ligand film (PLF) for plutonium and uranium extraction

DOE PAGES

Rim, Jung H.; Armenta, Claudine E.; Gonzales, Edward R.; ...

2015-09-12

This paper describes a new analyte extraction medium called polymer ligand film (PLF) that was developed to rapidly extract radionuclides. PLF is a polymer medium with ligands incorporated in its matrix that selectively and quickly extracts analytes. The main focus of the new technique is to shorten and simplify the procedure for chemically isolating radionuclides for determination through alpha spectroscopy. The PLF system was effective for plutonium and uranium extraction. The PLF was capable of co-extracting or selectively extracting plutonium over uranium depending on the PLF composition. As a result, the PLF and electrodeposited samples had similar alpha spectra resolutions.

Some Thermodynamic Features of Uranium-Plutonium Nitride Fuel in the Course of Burnup

NASA Astrophysics Data System (ADS)

Rusinkevich, A. A.; Ivanov, A. S.; Belov, G. V.; Skupov, M. V.

2017-12-01

Calculation studies on the effect of carbon and oxygen impurities on the chemical and phase compositions of nitride uranium-plutonium fuel in the course of burnup are performed using the IVTANTHERMO code. It is shown that the number of moles of UN decreases with increasing burnup level, whereas UN1.466, UN1.54, and UN1.73 exhibit a considerable increase. The presence of oxygen and carbon impurities causes an increase in the content of the UN1.466, UN1.54 and UN1.73 phases in the initial fuel by several orders of magnitude, in particular, at a relatively low temperature. At the same time, the presence of impurities abruptly reduces the content of free uranium in unburned fuel. Plutonium in the considered system is contained in form of Pu, PuC, PuC2, Pu2C3, and PuN. Plutonium carbides, as well as uranium carbides, are formed in small amounts. Most of the plutonium remains in the form of nitride PuN, whereas unbound Pu is present only in the areas with a low burnup level and high temperatures.

Variability of Fe isotope compositions of hydrothermal sulfides and oxidation products at mid-ocean ridges

NASA Astrophysics Data System (ADS)

Li, Xiaohu; Wang, Jianqiang; Chu, Fengyou; Wang, Hao; Li, Zhenggang; Yu, Xing; Bi, Dongwei; He, Yongsheng

2018-04-01

Significant Fe isotopic fractionation occurs during the precipitation and oxidative weathering of modern seafloor hydrothermal sulfides, which has an important impact on the cycling of Fe isotopes in the ocean. This study reports the Fe-isotope compositions of whole-rock sulfides and single-mineral pyrite collected from hydrothermal fields at the South Mid-Atlantic Ridge (SMAR) and the East Pacific Rise (EPR) and discusses the impacts of precipitation and late-stage oxidative weathering of sulfide minerals on Fe isotopic fractionation. The results show large variation in the Fe-isotope compositions of the sulfides from the different hydrothermal fields on the mid-oceanic ridges, indicating that relatively significant isotope fractionation occurs during the sulfide precipitation and oxidative weathering processes. The Fe-isotope compositions of the sulfides from the study area at the SMAR vary across a relatively small range, with an average value of 0.01‰. This Fe-isotope composition is similar to the Fe-isotope composition of mid-oceanic ridge basalt, which suggests that Fe was mainly leached from basalt. In contrast, the Fe-isotope composition of the sulfides from the study area at the EPR are significantly enriched in light Fe isotopes (average value - 1.63‰), mainly due to the kinetic fractionation during the rapid precipitation process of hydrothermal sulfide. In addition, the pyrite from different hydrothermal fields is enriched in light Fe isotopes, which is consistent with the phenomenon in which light Fe isotopes are preferentially enriched during the precipitation of pyrite. The red oxides have the heaviest Fe-isotope compositions (up to 0.80‰), indicating that heavy Fe isotopes are preferentially enriched in the oxidation product during the late-stage oxidation process. The data obtained from this study and previous studies show a significant difference between the Fe-isotope compositions of the sulfides from the SMAR and EPR. The relatively heavy Fe isotopes compositions of the sulfides from the SMAR may suggest the equilibrium fractionation process under high temperature conditions. The red Fe oxides are enriched in heavy Fe isotopes, indicating that the oxidative weathering processes result in the occurrence of significant Fe-isotope fractionation and the preferential enrichment of heavy Fe isotopes in the oxidation product.

Isotopy of the hydrosphere

NASA Astrophysics Data System (ADS)

Ferronskii, V. I.; Poliakov, V. A.

This book is concerned with the natural relations regarding the distribution of the stable isotopes of hydrogen and oxygen in the hydrosphere, taking into account the most important problems with respect to the dynamics and the origin of waters. The solution of these problems on an isotopic basis is considered. The physicochemical principles of isotope separation are discussed along with the isotopic composition of atmospheric moisture, the isotopic composition of surface continental waters, the hydrogen and oxygen isotopic composition of minerals of magmatic and metamorphic rocks and fluid inclusions, the isotopic composition of groundwaters of modern volcanic regions, and the origin of the earth's hydrosphere in the light of isotopic, cosmochemical, and theoretical studies. Attention is also given to the separation of hydrogen and oxygen isotopes of waters in the underground cycle, the isotopic composition of the deep-formation waters of sedimentary basins, the relationship between surface and ground waters, and the groundwater residence time in an aquifer.

PU-ICE Summary Information.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moore, Michael

The Generator Knowledge Report for the Plutonium Isentropic Compression Experiment Containment Systems (GK Report) provides information for the Plutonium Isentropic Compression Experiment (Pu- ICE) program to support waste management and characterization efforts. Attachment 3-18 presents generator knowledge (GK) information specific to the eighteenth Pu-ICE conducted in August 2015, also known as ‘Shot 18 (Aug 2015) and Pu-ICE Z-2841 (1).’ Shot 18 (Aug 2015) was generated on August 28, 2015 (1). Calculations based on the isotopic content of Shot 18 (Aug 2015) and the measured mass of the containment system demonstrate the post-shot containment system is low-level waste (LLW). Therefore, thismore » containment system will be managed at Sandia National Laboratory/New Mexico (SNL/NM) as LLW. Attachment 3-18 provides documentation of the TRU concentration and documents the concentration of any hazardous constituents.« less

Radiation Detection and Classification of Heavy Oxide Inorganic Scintillator Crystals for Detection of Fast Neutrons

DTIC Science & Technology

2016-06-01

of these three pillars, yet current detectors for fast neutrons from nuclear weapons materials are bulky, expensive, and have low efficiencies, well...passive fast neutron emissions. Similarly, isotopes present in weapons grade Plutonium (which is predominantly Pu-239), especially Pu-240, are... weapons material, and the propensity of the neutrons resulting from their fission to inelastically scatter, defines the interactions of interest

Report on the FY 1986 Activities of the Defense Science Study Group. Volume 1.

DTIC Science & Technology

1987-05-01

Reactors Improved Techniques for Wavefront Sensing and Correction in Adaptive Optics Hypervelocity Launchers Underground Facilities 0 Automated...oceanography and sound propagation in partially coherent media such as the turbulent ocean. There are large fixed arrays such as the Sound Surveillance System...Aircraft Continuous Patrol Aircraft Miscellaneous Studies Review of the Plutonium Special Isotope Separation Program of the DOE 4r Fusion Fission Hybrid

Plutonium isotopes and 241Am in the atmosphere of Lithuania: A comparison of different source terms

NASA Astrophysics Data System (ADS)

Lujanienė, G.; Valiulis, D.; Byčenkienė, S.; Šakalys, J.; Povinec, P. P.

2012-12-01

137Cs, 241Am and Pu isotopes collected in aerosol samples during 1994-2011 were analyzed with special emphasis on better understanding of Pu and Am behavior in the atmosphere. The results from long-term measurements of 240Pu/239Pu atom ratios showed a bimodal frequency distribution with median values of 0.195 and 0.253, indicating two main sources contributing to the Pu activities at the Vilnius sampling station. The low Pu atom ratio of 0.141 could be attributed to the weapon-grade plutonium derived from the nuclear weapon test sites. The frequency of air masses arriving from the North-West and North-East correlated with the Pu atom ratio indicating the input from the sources located in these regions (the Novaya Zemlya test site, Siberian nuclear plants), while no correlation with the Chernobyl region was observed. Measurements carried out during the Fukushima accident showed a negligible impact of this source with Pu activities by four orders of magnitude lower as compared to the Chernobyl accident. The activity concentration of actinides measured in the integrated sample collected in March-April, 2011 showed a small contribution of Pu with unusual activity and atom ratios indicating the presence of the spent fuel of different origin than that of the Chernobyl accident.

Distribution of neptunium and plutonium in New Mexico lichen samples ( Usnea arizonica) contaminated by atmospheric fallout

DOE PAGES

Oldham, Jr., Warren J.; Hanson, Susan K.; Lavelle, Kevin B.; ...

2015-08-30

In this study, the concentrations of 237Np, 239Pu and 240Pu were determined in lichen samples ( Usnea arizonica) that were collected from ten locations in New Mexico between 2011 and 2013 using isotope dilution inductively-coupled plasma mass spectrometry (ID-ICP-MS). The observed isotopic ratios for 237Np/ 239Pu and 240Pu/ 239Pu indicate trace contamination from global and regional fallout (e.g. Trinity test and atmospheric testing at the Nevada Test Site). The fact that actinide contamination is detected in recent lichen collections suggests continuous re-suspension of fallout radionuclides even 50 years after ratification of the Limited Test Ban Treaty.

Preliminary Assessment for CAU 485: Cactus Spring Ranch Pu and Du Site, CAS No. TA-39-001-TAGR: Soil Contamination, Tonapah Test Range, Nevada

DOE Office of Scientific and Technical Information (OSTI.GOV)

ITLV

1998-07-01

Corrective Action Unit 485, Corrective Action Site TA-39-001-TAGR, the Cactus Spring Ranch Soil Contamination Area, is located approximately six miles southwest of the Area 3 Compound at the eastern mouth of Sleeping Column Canyon in the Cactus Range on the Tonopah Test Range. This site was used in conjunction with animal studies involving the biological effects of radionuclides (specifically plutonium) associated with Operation Roller Coaster. According to field records, a hardened layer of livestock feces ranging from 2.54 centimeters (cm) (1 inch [in.]) to 10.2 cm (4 in.) thick is present in each of the main sheds. IT personnel conductedmore » a field visit on December 3, 1997, and noted that the only visible feces were located within the east shed, the previously fenced area near the east shed, and a small area southwest of the west shed. Other historical records indicate that other areas may still be covered with animal feces, but heavy vegetation now covers it. It is possible that radionuclides are present in this layer, given the history of operations in this area. Chemicals of concern may include plutonium and depleted uranium. Surface soil sampling was conducted on February 18, 1998. An evaluation of historical documentation indicated that plutonium should not be and depleted uranium could not be present at levels significantly above background as the result of test animals being penned at the site. The samples were analyzed for isotopic plutonium using method NAS-NS-3058. The results of the analysis indicated that plutonium levels of the feces and surface soil were not significantly elevated above background.« less

Variations in Urine Calcium Isotope: Composition Reflect Changes in Bone Mineral Balance in Humans

NASA Technical Reports Server (NTRS)

Skulan, Joseph; Anbar, Ariel; Bullen, Thomas; Puzas, J. Edward; Shackelford, Linda; Smith, Scott M.

2004-01-01

Changes in bone mineral balance cause rapid and systematic changes in the calcium isotope composition of human urine. Urine from subjects in a 17 week bed rest study was analyzed for calcium isotopic composition. Comparison of isotopic data with measurements of bone mineral density and metabolic markers of bone metabolism indicates the calcium isotope composition of urine reflects changes in bone mineral balance. Urine calcium isotope composition probably is affected by both bone metabolism and renal processes. Calcium isotope. analysis of urine and other tissues may provide information on bone mineral balance that is in important respects better than that available from other techniques, and illustrates the usefulness of applying geochemical techniques to biomedical problems.

Isotopic signatures: An important tool in today`s world

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rokop, D.J.; Efurd, D.W.; Benjamin, T.M.

1995-12-01

High-sensitivity/high-accuracy actinide measurement techniques developed to support weapons diagnostic capabilities at the Los Alamos National Laboratory are now being used for environmental monitoring. The measurement techniques used are Thermal Ionization Mass Spectrometry (TIMS), Alpha Spectrometry(AS), and High Resolution Gamma Spectrometry(HRGS). These techniques are used to address a wide variety of actinide inventory issues: Environmental surveillance, site characterizations, food chain member determination, sedimentary records of activities, and treaty compliance concerns. As little as 10 femtograms of plutonium can be detected in samples and isotopic signatures determined on samples containing sub-100 femtogram amounts. Uranium, present in all environmental samples, can generally yieldmore » isotopic signatures of anthropogenic origin when present at the 40 picogam/gram level. Solid samples (soils, sediments, fauna, and tissue) can range from a few particles to several kilograms in size. Water samples can range from a few milliliters to as much as 200 liters.« less

Leaching of plutonium from a radioactive waste glass by eight groundwaters from the western United States

USGS Publications Warehouse

Rees, T.F.; Cleveland, J.M.; Nash, K.L.

1985-01-01

The leachability of a radioactive waste glass formulated to Battelle Pacific Northwest Laboratory specification 80-270 has been studied using eight actual groundwaters with a range of chemical compositions as leachants. Waters collected from the Grande Ronde Basalt (Washington State) and from alluvial deposits in the Hualapai Valley (Arizona) were the most effective at removing plutonium from this glass. Leaching was shown to be incongruent; plutonium was removed from the glass more slowly than the overall glass matrix. The results of these experiments indicate the need to study the leachability of actual waste forms using the actual projected groundwaters that are most likely to come into contact with the waste should a radioactive waste repository be breached.

Asian dust input in the western Philippine Sea: Evidence from radiogenic Sr and Nd isotopes

NASA Astrophysics Data System (ADS)

Jiang, Fuqing; Frank, Martin; Li, Tiegang; Chen, Tian-Yu; Xu, Zhaokai; Li, Anchun

2013-05-01

The radiogenic strontium (Sr) and neodymium (Nd) isotope compositions of the detrital fraction of surface and subsurface sediments have been determined to trace sediment provenance and contributions from Asian dust off the east coast of Luzon Islands in the western Philippine Sea. The Sr and Nd isotope compositions have been very homogenous near the east coast of the Luzon Islands during the latest Quaternary yielding relatively least radiogenic Sr (87Sr/86Sr = 0.70453 to 0.70491) and more radiogenic Nd isotope compositions (ɛNd(0) = +5.3 to +5.5). These isotope compositions are similar to Luzon rocks and show that these sediments were mainly derived from the Luzon Islands. In contrast, the Sr and Nd isotope compositions of sediments on the Benham Rise and in the Philippine Basin are markedly different in that they are characterized by overall more variable and more radiogenic Sr isotope compositions (87Sr/86Sr = 0.70452 to 0.70723) and less radiogenic Nd isotope compositions (ɛNd(0) = -5.3 to +2.4). The Sr isotope composition in the Huatung Basin is intermediate between those of the east coast of Luzon and Benham Rise, but shows the least radiogenic Nd isotope compositions. The data are consistent with a two end-member mixing relationship between Luzon volcanic rocks and eolian dust from the Asian continent, which is characterized by highly radiogenic Sr and unradiogenic Nd isotope compositions. The results show that Asian continental dust contributes about 10-50% of the detrital fraction of the sediments on Benham Rise in the western Philippine Sea, which offers the potentials to reconstruct the climatic evolution of eastern Asia from these sediments and compare this information to the records from the central and northern Pacific.

Sulfur Isotope Composition of Putative Primary Troilite in Chondrules

NASA Technical Reports Server (NTRS)

Tachibana, Shogo; Huss, Gary R.

2002-01-01

Sulfur isotope compositions of putative primary troilites in chondrules from Bishunpur were measured by ion probe. These primary troilites have the same S isotope compositions as matrix troilites and thus appear to be isotopically unfractionated. Additional information is contained in the original extended abstract.

Device and method for accurately measuring concentrations of airborne transuranic isotopes

DOEpatents

McIsaac, Charles V.; Killian, E. Wayne; Grafwallner, Ervin G.; Kynaston, Ronnie L.; Johnson, Larry O.; Randolph, Peter D.

1996-01-01

An alpha continuous air monitor (CAM) with two silicon alpha detectors and three sample collection filters is described. This alpha CAM design provides continuous sampling and also measures the cumulative transuranic (TRU), i.e., plutonium and americium, activity on the filter, and thus provides a more accurate measurement of airborne TRU concentrations than can be accomplished using a single fixed sample collection filter and a single silicon alpha detector.

Device and method for accurately measuring concentrations of airborne transuranic isotopes

DOEpatents

McIsaac, C.V.; Killian, E.W.; Grafwallner, E.G.; Kynaston, R.L.; Johnson, L.O.; Randolph, P.D.

1996-09-03

An alpha continuous air monitor (CAM) with two silicon alpha detectors and three sample collection filters is described. This alpha CAM design provides continuous sampling and also measures the cumulative transuranic (TRU), i.e., plutonium and americium, activity on the filter, and thus provides a more accurate measurement of airborne TRU concentrations than can be accomplished using a single fixed sample collection filter and a single silicon alpha detector. 7 figs.

Atomic Weights and Isotopic Compositions

National Institute of Standards and Technology Data Gateway

SRD 144 Atomic Weights and Isotopic Compositions (Web, free access)   The atomic weights are available for elements 1 through 111, and isotopic compositions or abundances are given when appropriate.

Magnesium isotopic composition of the Earth and chondrites

NASA Astrophysics Data System (ADS)

Teng, Fang-Zhen; Li, Wang-Ye; Ke, Shan; Marty, Bernard; Dauphas, Nicolas; Huang, Shichun; Wu, Fu-Yuan; Pourmand, Ali

2010-07-01

To constrain further the Mg isotopic composition of the Earth and chondrites, and investigate the behavior of Mg isotopes during planetary formation and magmatic processes, we report high-precision (±0.06‰ on δ 25Mg and ±0.07‰ on δ 26Mg, 2SD) analyses of Mg isotopes for (1) 47 mid-ocean ridge basalts covering global major ridge segments and spanning a broad range in latitudes, geochemical and radiogenic isotopic compositions; (2) 63 ocean island basalts from Hawaii (Kilauea, Koolau and Loihi) and French Polynesia (Society Island and Cook-Austral chain); (3) 29 peridotite xenoliths from Australia, China, France, Tanzania and USA; and (4) 38 carbonaceous, ordinary and enstatite chondrites including 9 chondrite groups (CI, CM, CO, CV, L, LL, H, EH and EL). Oceanic basalts and peridotite xenoliths have similar Mg isotopic compositions, with average values of δ 25Mg = -0.13 ± 0.05 (2SD) and δ 26Mg = -0.26 ± 0.07 (2SD) for global oceanic basalts ( n = 110) and δ 25Mg = -0.13 ± 0.03 (2SD) and δ 26Mg = -0.25 ± 0.04 (2SD) for global peridotite xenoliths ( n = 29). The identical Mg isotopic compositions in oceanic basalts and peridotites suggest that equilibrium Mg isotope fractionation during partial melting of peridotite mantle and magmatic differentiation of basaltic magma is negligible. Thirty-eight chondrites have indistinguishable Mg isotopic compositions, with δ 25Mg = -0.15 ± 0.04 (2SD) and δ 26Mg = -0.28 ± 0.06 (2SD). The constancy of Mg isotopic compositions in all major types of chondrites suggest that primary and secondary processes that affected the chemical and oxygen isotopic compositions of chondrites did not significantly fractionate Mg isotopes. Collectively, the Mg isotopic composition of the Earth's mantle, based on oceanic basalts and peridotites, is estimated to be -0.13 ± 0.04 for δ 25Mg and -0.25 ± 0.07 for δ 26Mg (2SD, n = 139). The Mg isotopic composition of the Earth, as represented by the mantle, is similar to chondrites. The chondritic composition of the Earth implies that Mg isotopes were well mixed during accretion of the inner solar system.

High-precision isotopic characterization of USGS reference materials by TIMS and MC-ICP-MS

NASA Astrophysics Data System (ADS)

Weis, Dominique; Kieffer, Bruno; Maerschalk, Claude; Barling, Jane; de Jong, Jeroen; Williams, Gwen A.; Hanano, Diane; Pretorius, Wilma; Mattielli, Nadine; Scoates, James S.; Goolaerts, Arnaud; Friedman, Richard M.; Mahoney, J. Brian

2006-08-01

The Pacific Centre for Isotopic and Geochemical Research (PCIGR) at the University of British Columbia has undertaken a systematic analysis of the isotopic (Sr, Nd, and Pb) compositions and concentrations of a broad compositional range of U.S. Geological Survey (USGS) reference materials, including basalt (BCR-1, 2; BHVO-1, 2), andesite (AGV-1, 2), rhyolite (RGM-1, 2), syenite (STM-1, 2), granodiorite (GSP-2), and granite (G-2, 3). USGS rock reference materials are geochemically well characterized, but there is neither a systematic methodology nor a database for radiogenic isotopic compositions, even for the widely used BCR-1. This investigation represents the first comprehensive, systematic analysis of the isotopic composition and concentration of USGS reference materials and provides an important database for the isotopic community. In addition, the range of equipment at the PCIGR, including a Nu Instruments Plasma MC-ICP-MS, a Thermo Finnigan Triton TIMS, and a Thermo Finnigan Element2 HR-ICP-MS, permits an assessment and comparison of the precision and accuracy of isotopic analyses determined by both the TIMS and MC-ICP-MS methods (e.g., Nd isotopic compositions). For each of the reference materials, 5 to 10 complete replicate analyses provide coherent isotopic results, all with external precision below 30 ppm (2 SD) for Sr and Nd isotopic compositions (27 and 24 ppm for TIMS and MC-ICP-MS, respectively). Our results also show that the first- and second-generation USGS reference materials have homogeneous Sr and Nd isotopic compositions. Nd isotopic compositions by MC-ICP-MS and TIMS agree to within 15 ppm for all reference materials. Interlaboratory MC-ICP-MS comparisons show excellent agreement for Pb isotopic compositions; however, the reproducibility is not as good as for Sr and Nd. A careful, sequential leaching experiment of three first- and second-generation reference materials (BCR, BHVO, AGV) indicates that the heterogeneity in Pb isotopic compositions, and concentrations, could be directly related to contamination by the steel (mortar/pestle) used to process the materials. Contamination also accounts for the high concentrations of certain other trace elements (e.g., Li, Mo, Cd, Sn, Sb, W) in various USGS reference materials.

Current state of nuclear fuel cycles in nuclear engineering and trends in their development according to the environmental safety requirements

NASA Astrophysics Data System (ADS)

Vislov, I. S.; Pischulin, V. P.; Kladiev, S. N.; Slobodyan, S. M.

2016-08-01

The state and trends in the development of nuclear fuel cycles in nuclear engineering, taking into account the ecological aspects of using nuclear power plants, are considered. An analysis of advantages and disadvantages of nuclear engineering, compared with thermal engineering based on organic fuel types, was carried out. Spent nuclear fuel (SNF) reprocessing is an important task in the nuclear industry, since fuel unloaded from modern reactors of any type contains a large amount of radioactive elements that are harmful to the environment. On the other hand, the newly generated isotopes of uranium and plutonium should be reused to fabricate new nuclear fuel. The spent nuclear fuel also includes other types of fission products. Conditions for SNF handling are determined by ecological and economic factors. When choosing a certain handling method, one should assess these factors at all stages of its implementation. There are two main methods of SNF handling: open nuclear fuel cycle, with spent nuclear fuel assemblies (NFAs) that are held in storage facilities with their consequent disposal, and closed nuclear fuel cycle, with separation of uranium and plutonium, their purification from fission products, and use for producing new fuel batches. The development of effective closed fuel cycles using mixed uranium-plutonium fuel can provide a successful development of the nuclear industry only under the conditions of implementation of novel effective technological treatment processes that meet strict requirements of environmental safety and reliability of process equipment being applied. The diversity of technological processes is determined by different types of NFA devices and construction materials being used, as well as by the composition that depends on nuclear fuel components and operational conditions for assemblies in the nuclear power reactor. This work provides an overview of technological processes of SNF treatment and methods of handling of nuclear fuel assemblies. Based on analysis of modern engineering solutions on SNF regeneration, it has been concluded that new reprocessing technologies should meet the ecological safety requirements, provide a more extensive use of the resource base of nuclear engineering, allow the production of valuable and trace elements on an industrial scale, and decrease radioactive waste release.

MIS High-Purity Plutonium Oxide Metal Oxidation Product TS707001 (SSR123): Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Veirs, Douglas Kirk; Stroud, Mary Ann; Berg, John M.

A high-purity plutonium dioxide material from the Material Identification and Surveillance (MIS) Program inventory has been studied with regard to gas generation and corrosion in a storage environment. Sample TS707001 represents process plutonium oxides from several metal oxidation operations as well as impure and scrap plutonium from Hanford that are currently stored in 3013 containers. After calcination to 950°C, the material contained 86.98% plutonium with no major impurities. This study followed over time, the gas pressure of a sample with nominally 0.5 wt% water in a sealed container with an internal volume scaled to 1/500th of the volume of amore » 3013 container. Gas compositions were measured periodically over a six year period. The maximum observed gas pressure was 138 kPa. The increase over the initial pressure of 80 kPa was primarily due to generation of nitrogen and carbon dioxide gas in the first six months. Hydrogen and oxygen were minor components of the headspace gas. At the completion of the study, the internal components of the sealed container showed signs of corrosion, including pitting.« less

TRANSURANIC ELEMENT, COMPOSITION THEREOF, AND METHODS FOR PRODUCING SEPARATING AND PURIFYING SAME

DOEpatents

Wahl, A.C.

1961-09-19

A process of separating plutonium from fission products contained in an aqueous solution is described. Plutonium, in the tri- or tetravalent state, and the fission products are coprecipitated on lanthanum fluoride, lanthanum oxalate, cerous fluoride, cerous phosphate, ceric iodate, zirconyl phosphate, thorium iodate, or thorium fluoride. The precipitate is dissolved in acid, and the plutonium is oxidized to the hexavalent state. The fission products are selectively precipitated on a carrier of the above group but different from that used for the coprecipitation. The plutonium in the solution, after removal of the fission product precipitate, is reduced to at least the tetravalent state and precipitated on lanthanum fluoride, lanthanum phosphate, lanthanum oxalate, lanthanum hydroxide, cerous fluoride, cerous phosphate, cerous oxalate, cerous hydroxide, ceric iodate, zirconyl phosphate, zirconyl iodate, zirconium hydroxide, thorium fluoride, thorium oxalate, thorium iodate, thorium peroxide, uranium iodate, uranium oxalate, or uranium peroxide, again using a different carrier than that used for the precipitation of the fission products.

Nuclear Archeology in a Bottle: Evidence of Pre-Trinity U.S. Weapons Activities from a Waste Burial Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schwantes, Jon M.; Douglas, Matthew; Bonde, Steven E.

2009-02-15

During World War II, the Hanford Site in Washington was chosen for plutonium production. In 2004, a bottle containing a sample of plutonium was recovered from a Hanford waste trench. Isotopic age dating indicated the sample was separated from the fuel pellet 64 ±2.8 years earlier. Detectable products of secondary nuclear reactions, such as 22Na, proved useful as 1) a detectable analog for alpha emitting actinides, 2) an indicator of sample splitting, and 3) a measure of the time since sample splitting. The sample origin was identified as the X-10 reactor, Oak Ridge, TN. Corroborated by historical documents, we concludedmore » this sample was part of the first batch of Pu separated at T-Plant, Hanford, the world’s first industrial-scale reprocessing facility, on December 9, 1944.« less

Converting isotope ratios to diet composition - the use of mixing models - June 2010

EPA Science Inventory

One application of stable isotope analysis is to reconstruct diet composition based on isotopic mass balance. The isotopic value of a consumer’s tissue reflects the isotopic values of its food sources proportional to their dietary contributions. Isotopic mixing models are used ...

Plutonium Isotopes (239-241Pu) Dissolved in Pacific Ocean Waters Detected by Accelerator Mass Spectrometry: No Effects of the Fukushima Accident Observed.

PubMed

Hain, Karin; Faestermann, Thomas; Fimiani, Leticia; Golser, Robin; Gómez-Guzmán, José Manuel; Korschinek, Gunther; Kortmann, Florian; Lierse von Gostomski, Christoph; Ludwig, Peter; Steier, Peter; Tazoe, Hirofumi; Yamada, Masatoshi

2017-02-21

The concentration of plutonium (Pu) and the isotopic ratios of 240 Pu to 239 Pu and 241 Pu to 239 Pu were determined by accelerator mass spectrometry (AMS) in Pacific Ocean water samples (20 L each) collected in late 2012. The isotopic Pu ratios are important indicators of different contamination sources and were used to identify a possible release of Pu into the ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. In particular, 241 Pu is a well-suited indicator for a recent entry of Pu because 241 Pu from fallout of nuclear weapon testings has already significantly decayed. A total of 10 ocean water samples were prepared at the Radiochemie München of the TUM and analyzed at the Vienna Environmental Research Laboratory (VERA). Several samples showed a slightly elevated 240 Pu/ 239 Pu ratio of up to 0.22 ± 0.02 compared to global fallout ( 240 Pu/ 239 Pu = 0.180 ± 0.007), whereas all measured 241 Pu-to- 239 Pu ratios were consistent with nuclear weapon fallout ( 241 Pu/ 239 Pu < 2.4 × 10 -3 ), which means that no impact from the Fukushima accident was detected. From the average 241 Pu-to- 239 Pu ratio of 8 -2 +3 ×10 -4 at a sampling station located at a distance of 39.6 km to FDNPP, the 1-σ upper limit for the FDNPP contribution to the 239 Pu inventory in the water column was estimated to be 0.2%. Pu, with the signature of weapon-grade Pu was found in a single sample collected around 770 km off the west coast of the United States.

FUSED REACTOR FUELS

DOEpatents

Mayer, S.W.

1962-11-13

This invention relates to a nuciear reactor fuel composition comprising (1) from about 0.01 to about 50 wt.% based on the total weight of said composition of at least one element selected from the class consisting of uranium, thorium, and plutonium, wherein said eiement is present in the form of at least one component selected from the class consisting of oxides, halides, and salts of oxygenated anions, with components comprising (2) at least one member selected from the class consisting of (a) sulfur, wherein the sulfur is in the form of at least one entity selected irom the class consisting of oxides of sulfur, metal sulfates, metal sulfites, metal halosulfonates, and acids of sulfur, (b) halogen, wherein said halogen is in the form of at least one compound selected from the class of metal halides, metal halosulfonates, and metal halophosphates, (c) phosphorus, wherein said phosphorus is in the form of at least one constituent selected from the class consisting of oxides of phosphorus, metal phosphates, metal phosphites, and metal halophosphates, (d) at least one oxide of a member selected from the class consisting of a metal and a metalloid wherein said oxide is free from an oxide of said element in (1); wherein the amount of at least one member selected from the class consisting of halogen and sulfur is at least about one at.% based on the amount of the sum of said sulfur, halogen, and phosphorus atom in said composition; and wherein the amount of said 2(a), 2(b) and 2(c) components in said composition which are free from said elements of uranium, thorium, arid plutonium, is at least about 60 wt.% based on the combined weight of the components of said composition which are free from said elements of uranium, thorium, and plutonium. (AEC)

REACTOR FUEL SCAVENGING MEANS

DOEpatents

Coffinberry, A.S.

1962-04-10

A process for removing fission products from reactor liquid fuel without interfering with the reactor's normal operation or causing a significant change in its fuel composition is described. The process consists of mixing a liquid scavenger alloy composed of about 44 at.% plutoniunm, 33 at.% lanthanum, and 23 at.% nickel or cobalt with a plutonium alloy reactor fuel containing about 3 at.% lanthanum; removing a portion of the fuel and scavenger alloy from the reactor core and replacing it with an equal amount of the fresh scavenger alloy; transferring the portion to a quiescent zone where the scavenger and the plutonium fuel form two distinct liquid layers with the fission products being dissolved in the lanthanum-rich scavenger layer; and the clean plutonium-rich fuel layer being returned to the reactor core. (AEC)

DOE research and development report. Progress report, October 1980-September 1981

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bingham, Carleton D.

The DOE New Brunswick Laboratory (NBL) is the US Government's Nuclear Materials Standards and Measurement Laboratory. NBL is assigned the mission to provide and maintain, as an essential part of federal statutory responsibilities related to national and international safeguards of nuclear materials for USA defense and energy programs, an ongoing capability for: the development, preparation, certification, and distribution of reference materials for the calibration and standardization of nuclear materials measurements; the development, improvement, and evaluation of nuclear materials measurement technology; the assessment and evaluation of the practice and application of nuclear materials measurement technology; expert and reliable specialized nuclear materialsmore » measurement services for the government; and technology exchange and training in nuclear materials measurement and standards. Progress reports for this fiscal year are presented under the following sections: (1) development or evaluation of measurement technology (elemental assay of uranium plutonium; isotope composition); (2) standards and reference materials (NBL standards and reference materials; NBS reference materials); and (3) evaluation programs (safeguards analytical laboratory evaluation; general analytical evaluation program; other evaluation programs).« less

Effects of climatic seasonality on the isotopic composition of evaporating soil waters

NASA Astrophysics Data System (ADS)

Benettin, Paolo; Volkmann, Till H. M.; von Freyberg, Jana; Frentress, Jay; Penna, Daniele; Dawson, Todd E.; Kirchner, James W.

2018-05-01

Stable water isotopes are widely used in ecohydrology to trace the transport, storage, and mixing of water on its journey through landscapes and ecosystems. Evaporation leaves a characteristic signature on the isotopic composition of the water that is left behind, such that in dual-isotope space, evaporated waters plot below the local meteoric water line (LMWL) that characterizes precipitation. Soil and xylem water samples can often plot below the LMWL as well, suggesting that they have also been influenced by evaporation. These soil and xylem water samples frequently plot along linear trends in dual-isotope space. These trend lines are often termed "evaporation lines" and their intersection with the LMWL is often interpreted as the isotopic composition of the precipitation source water. Here we use numerical experiments based on established isotope fractionation theory to show that these trend lines are often by-products of the seasonality in evaporative fractionation and in the isotopic composition of precipitation. Thus, they are often not true evaporation lines, and, if interpreted as such, can yield highly biased estimates of the isotopic composition of the source water.

Baseline shifts in coral skeletal oxygen isotopic composition: a signature of symbiont shuffling?

NASA Astrophysics Data System (ADS)

Carilli, J. E.; Charles, C. D.; Garren, M.; McField, M.; Norris, R. D.

2013-06-01

Decades-long records of the stable isotopic composition of coral skeletal cores were analyzed from four sites on the Mesoamerican Reef. Two of the sites exhibited baseline shifts in oxygen isotopic composition after known coral bleaching events. Changes in pH at the calcification site caused by a change in the associated symbiont community are invoked to explain the observed shift in the isotopic composition. To test the hypothesis that changes in symbiont clade could affect skeletal chemistry, additional coral samples were collected from Belize for paired Symbiodinium identification and skeletal stable isotopic analysis. We found some evidence that skeletal stable isotopic composition may be affected by symbiont clade and suggest this is an important topic for future investigation. If different Symbiodinium clades leave consistent signatures in skeletal geochemical composition, the signature will provide a method to quantify past symbiont shuffling events, important for understanding how corals are likely to respond to climate change.

Managing the Nuclear Fuel Cycle: Policy Implications of Expanding Global Access to Nuclear Power

DTIC Science & Technology

2010-03-05

However, the case of Iran raises perhaps the most critical question in this decade for strengthening the nuclear nonproliferation regime: How can...enrichment process can take advantage of the slight difference in atomic mass between 235U and 238U. The typical enrichment process requires about 10 lbs of...neutrons but can induce fission in all actinides , including all plutonium isotopes. Therefore, nuclear fuel for a fast reactor must have a higher

Characterization of the MVST waste tanks located at ORNL

DOE Office of Scientific and Technical Information (OSTI.GOV)

Keller, J.M.; Giaquinto, J.M.; Meeks, A.M.

During the fall of 1996 there was a major effort to sample and analyze the Active Liquid Low-Level Waste (LLLW) tanks at ORNL which include the Melton Valley Storage Tanks (MVST) and the Bethel Valley Evaporator Service Tanks (BVEST). The characterization data summarized in this report was needed to address waste processing options, address concerns of the performance assessment (PA) data for the Waste Isolation Pilot Plant (WIPP), evaluate the characteristics with respect to the waste acceptance criteria (WAC) for WIPP and Nevada Test Site (NTS), address criticality concerns, and meet DOT requirements for transporting the waste. This report onlymore » discusses the analytical characterization data for the MVST waste tanks. The isotopic data presented in this report support the position that fissile isotopes of uranium and plutonium were ``denatured`` as required by administrative controls. In general, MVST sludge was found to be both hazardous by RCRA characteristics and the transuranic alpha activity was well about the limit for TRU waste. The characteristics of the MVST sludge relative to the WIPP WAC limits for fissile gram equivalent, plutonium equivalent activity, and thermal power from decay heat, were estimated from the data in this report and found to be far below the upper boundary for any of the remote-handled transuranic waste requirements for disposal of the waste in WIPP.« less

Thorium-based mixed oxide fuel in a pressurized water reactor: A feasibility analysis with MCNP

NASA Astrophysics Data System (ADS)

Tucker, Lucas Powelson

This dissertation investigates techniques for spent fuel monitoring, and assesses the feasibility of using a thorium-based mixed oxide fuel in a conventional pressurized water reactor for plutonium disposition. Both non-paralyzing and paralyzing dead-time calculations were performed for the Portable Spectroscopic Fast Neutron Probe (N-Probe), which can be used for spent fuel interrogation. Also, a Canberra 3He neutron detector's dead-time was estimated using a combination of subcritical assembly measurements and MCNP simulations. Next, a multitude of fission products were identified as candidates for burnup and spent fuel analysis of irradiated mixed oxide fuel. The best isotopes for these applications were identified by investigating half-life, photon energy, fission yield, branching ratios, production modes, thermal neutron absorption cross section and fuel matrix diffusivity. 132I and 97Nb were identified as good candidates for MOX fuel on-line burnup analysis. In the second, and most important, part of this work, the feasibility of utilizing ThMOX fuel in a pressurized water reactor (PWR) was first examined under steady-state, beginning of life conditions. Using a three-dimensional MCNP model of a Westinghouse-type 17x17 PWR, several fuel compositions and configurations of a one-third ThMOX core were compared to a 100% UO2 core. A blanket-type arrangement of 5.5 wt% PuO2 was determined to be the best candidate for further analysis. Next, the safety of the ThMOX configuration was evaluated through three cycles of burnup at several using the following metrics: axial and radial nuclear hot channel factors, moderator and fuel temperature coefficients, delayed neutron fraction, and shutdown margin. Additionally, the performance of the ThMOX configuration was assessed by tracking cycle length, plutonium destroyed, and fission product poison concentration.

Archival processes of the water stable isotope signal in East Antarctic ice cores

NASA Astrophysics Data System (ADS)

Casado, Mathieu; Landais, Amaelle; Picard, Ghislain; Münch, Thomas; Laepple, Thomas; Stenni, Barbara; Dreossi, Giuliano; Ekaykin, Alexey; Arnaud, Laurent; Genthon, Christophe; Touzeau, Alexandra; Masson-Delmotte, Valerie; Jouzel, Jean

2018-05-01

The oldest ice core records are obtained from the East Antarctic Plateau. Water isotopes are key proxies to reconstructing past climatic conditions over the ice sheet and at the evaporation source. The accuracy of climate reconstructions depends on knowledge of all processes affecting water vapour, precipitation and snow isotopic compositions. Fractionation processes are well understood and can be integrated in trajectory-based Rayleigh distillation and isotope-enabled climate models. However, a quantitative understanding of processes potentially altering snow isotopic composition after deposition is still missing. In low-accumulation sites, such as those found in East Antarctica, these poorly constrained processes are likely to play a significant role and limit the interpretability of an ice core's isotopic composition. By combining observations of isotopic composition in vapour, precipitation, surface snow and buried snow from Dome C, a deep ice core site on the East Antarctic Plateau, we found indications of a seasonal impact of metamorphism on the surface snow isotopic signal when compared to the initial precipitation. Particularly in summer, exchanges of water molecules between vapour and snow are driven by the diurnal sublimation-condensation cycles. Overall, we observe in between precipitation events modification of the surface snow isotopic composition. Using high-resolution water isotopic composition profiles from snow pits at five Antarctic sites with different accumulation rates, we identified common patterns which cannot be attributed to the seasonal variability of precipitation. These differences in the precipitation, surface snow and buried snow isotopic composition provide evidence of post-deposition processes affecting ice core records in low-accumulation areas.

Compound-specific isotopic analyses: a novel tool for reconstruction of ancient biogeochemical processes

NASA Technical Reports Server (NTRS)

Hayes, J. M.; Freeman, K. H.; Popp, B. N.; Hoham, C. H.

1990-01-01

Patterns of isotopic fractionation in biogeochemical processes are reviewed and it is suggested that isotopic fractionations will be small when substrates are large. If so, isotopic compositions of biomarkers will reflect those of their biosynthetic precursors. This prediction is tested by consideration of results of analyses of geoporphyrins and geolipids from the Greenhorn Formation (Cretaceous, Western Interior Seaway of North America) and the Messel Shale (Eocene, lacustrine, southern Germany). It is shown (i) that isotopic compositions of porphyrins that are related to a common source, but which have been altered structurally, cluster tightly and (ii) that isotopic differences between geolipids and porphyrins related to a common source are equal to those observed in modern biosynthetic products. Both of these observations are consistent with preservation of biologically controlled isotopic compositions during diagenesis. Isotopic compositions of individual compounds can thus be interpreted in terms of biogeochemical processes in ancient depositional environments. In the Cretaceous samples, isotopic compositions of n-alkanes are covariant with those of total organic carbon, while delta values for pristane and phytane are covariant with those of porphyrins. In this unit representing an open marine environment, the preserved acyclic polyisoprenoids apparently derive mainly from primary material, while the extractable, n-alkanes derive mainly from lower levels of the food chain. In the Messel Shale, isotopic compositions of individual biomarkers range from -20.9 to -73.4% vs PDB. Isotopic compositions of specific compounds can be interpreted in terms of origin from methylotrophic, chemautotrophic, and chemolithotrophic microorganisms as well as from primary producers that lived in the water column and sediments of this ancient lake.

Seasonality of Oxygen isotope composition in cow (Bos taurus) hair and its model interpretation

NASA Astrophysics Data System (ADS)

Chen, Guo; Schnyder, Hans; Auerswald, Karl

2017-04-01

Oxygen isotopes in animal and human tissues are expected to be good recorders of geographical origin and migration histories based on the isotopic relationship between hair oxygen and annual precipitation and the well-known spatial pattern of oxygen isotope composition in meteoric water. However, seasonal variation of oxygen isotope composition may diminish the origin information in the tissues. Here the seasonality of oxygen isotope composition in tail hair was investigated in a domestic suckler cow (Bos taurus) that underwent different ambient conditions, physiological states, and keeping and feeding strategies during five years. A detailed mechanistic model involving in ambient conditions, soil properties and animal physiology was built to explain this variation. The measured oxygen isotope composition in hair was significantly related (p<0.05) to the isotope composition in meteoric water in a regression analysis. Modelling suggested that this relation was only partly derived from the direct influence of feed moisture. Ambient conditions (temperature, moisture) did not only influence the isotopic signal of precipitation but also affected the animal itself (drinking water demand, transcutaneous vapor etc.). The clear temporal variation thus resulted from complex interactions with multiple influences. The twofold influence of ambient conditions via the feed and via the animal itself is advantageous for tracing the geographic origin because the oxygen isotope composition is then less influenced by variations in moisture uptake; however, it is unfavorable for indicating the production system, e.g. to distinguish between milk produced from fresh grass or from silage.

Magnesium isotopic composition of the mantle

NASA Astrophysics Data System (ADS)

Teng, F.; Li, W.; Ke, S.; Marty, B.; Huang, S.; Dauphas, N.; Wu, F.; Helz, R. L.

2009-12-01

Studies of Mg isotopic composition of the Earth not only are important for understanding its geochemistry but also can shed light on the accretion history of the Earth as well as the evolution of the Earth-Moon system. However, to date, the Mg isotopic composition of the Earth is still poorly constrained and highly debated. There is uncertainty in the magnitude of Mg isotope fractionation at mantle temperatures and whether the Earth has a chondritic Mg isotopic composition or not. To constrain further the Mg isotopic composition of the mantle and investigate the behavior of Mg isotopes during igneous differentiation, we report >200 high-precision (δ26Mg < 0.1‰, 2SD) analyses of Mg isotopes on 1) global mid-ocean ridge basalts covering major ridge segments of the world and spanning a broad range in latitudes, chemical and radiogenic isotopic compositions; 2) ocean island basalts from Hawaiian (Koolau, Kilauea and Loihi) and French Polynesian volcanoes (Society island and Cook Austral chain); 3) olivine grains from Hawaiian volcanoes (Kilauea, Koolau and Loihi) and 4) peridotite xenoliths from Australia, China, France, Tanzania and USA. Global oceanic basalts and peridotite xenoliths have a limited (<0.2 ‰) variation in Mg isotopic composition, with an average δ26Mg = -0.25 relative to DSM3. Olivines from Hawaiian lavas have δ26Mg ranging from -0.43 to +0.03, with most having compositions identical to basalts and peridotites. Therefore, the mantle’s δ26Mg value is estimated to be ~ -0.25 ± 0.1 (2SD), different from that reported by Wiechert and Halliday (2007; δ26Mg = ~ 0) but similar to more recent studies (δ26Mg = -0.27 to -0.33) (Teng et al. 2007; Handler et al. 2009; Yang et al., 2009). Moreover, we suggest the Earth, as represented by the mantle, has a Mg isotopic composition similar to chondrites (δ26Mg = ~-0.33). The need for a model such as that of Wiechert and Halliday (2007) that involves sorting of chondrules and calcium-aluminum-rich inclusions in the proto planetary disc is thus not required to explain the Mg isotopic composition of the Earth.

ISOTOPE CONVERSION DEVICE

DOEpatents

Wigner, E.P.; Young, G.J.; Ohlinger, L.A.

1957-12-01

This patent relates to nuclear reactors of tbe type utilizing a liquid fuel and designed to convert a non-thermally fissionable isotope to a thermally fissionable isotope by neutron absorption. A tank containing a reactive composition of a thermally fissionable isotope dispersed in a liquid moderator is disposed within an outer tank containing a slurry of a non-thermally fissionable isotope convertible to a thermally fissionable isotope by neutron absorption. A control rod is used to control the chain reaction in the reactive composition and means are provided for circulating and cooling the reactive composition and slurry in separate circuits.

MAST - A mass spectrometer telescope for studies of the isotopic composition of solar, anomalous, and galactic cosmic ray nuclei

NASA Technical Reports Server (NTRS)

Cook, Walter R.; Cummings, Alan C.; Cummings, Jay R.; Garrard, Thomas L.; Kecman, Branislav; Mewaldt, Richard A.; Selesnick, Richard S.; Stone, Edward C.; Von Rosenvinge, T. T.

1993-01-01

The Mass Spectrometer Telescope (MAST) on SAMPEX is designed to provide high resolution measurements of the isotopic composition of energetic nuclei from He to Ni (Z = 2 to 28) over the energy range from about 10 to several hundred MeV/nuc. During large solar flares MAST will measure the isotopic abundances of solar energetic particles to determine directly the composition of the solar corona, while during solar quiet times MAST will study the isotopic composition of galactic cosmic rays. In addition, MAST will measure the isotopic composition of both interplanetary and trapped fluxes of anomalous cosmic rays, believed to be a sample of the nearby interstellar medium.

Long-term data set analysis of stable isotopic composition in German rivers

NASA Astrophysics Data System (ADS)

Reckerth, Anne; Stichler, Willibald; Schmidt, Axel; Stumpp, Christine

2017-09-01

Stable isotopes oxygen-18 (18O) and deuterium (2H) are commonly used to investigate hydrological processes in catchments. However, only a few isotope studies have been conducted on a large scale and rarely over long time periods. The objective of this study was to identify the spatial and seasonal variability of isotopic composition in river water and how it is affected by geographical and hydrological factors. The stable isotopic composition of river water has been measured in nine large river catchments in Germany for a time period of 12 years or 26 years. We conducted time series and correlation analyses to identify spatial and temporal patterns of the isotopic composition in the rivers. Further, we compared it to isotopic composition in local precipitation and catchments characteristics. In the majority of the rivers, the spatial and temporal patterns of precipitation were directly reflected in river water. The isotopic signals of the river water were time shifted and show attenuated amplitudes. Further deviations from isotopic compositions in local precipitation were observed in catchments with complex flow systems. These deviations were attributed to catchment processes and influences like evaporation, damming and storage. The seasonality of the isotopic composition was mainly determined by the discharge regimes of the rivers. We found correlations between isotopic long-term averages and catchment altitude as well as latitude and longitude, resulting in a northwest-southeast gradient. Furthermore, it was shown that long-term averages of d-excess were inversely related to flow length and catchment size, which indicates that evaporation enrichment has an impact on the isotopic composition even in catchments of humid climates. This study showed that isotopic composition in rivers can serve as a proxy for the local precipitation and can be utilized as an indicator for hydrological processes even in large river basins. In future, such long time series will help to also understand the impact of changes in the hydrological cycle on the larger scales. They can also be used for calibration and validation of flow and transport models at catchment and sub-catchment scale.

Application of laser induced breakdown spectroscopy (LIBS) instrumentation for international safeguards

DOE Office of Scientific and Technical Information (OSTI.GOV)

Barefield Ii, James E; Clegg, Samuel M; Lopez, Leon N

2010-01-01

Advanced methodologies and improvements to current measurements techniques are needed to strengthen the effectiveness and efficiency of international safeguards. This need was recognized and discussed at a Technical Meeting on 'The Application of Laser Spectrometry Techniques in IAEA Safeguards' held at IAEA headquarters (September 2006). One of the principal recommendations from that meeting was the need to pursue the development of novel complementary access instrumentation based on Laser Induced Breakdown Spectroscopy (UBS) for the detection of gaseous and solid signatures and indicators of nuclear fuel cycle processes and associated materials'. Pursuant to this recommendation the Department of Safeguards (SG) undermore » the Division of Technical Support (SGTS) convened the 'Experts and Users Advisory Meeting on Laser Induced Breakdown Spectroscopy (LIBS) for Safeguards Applications' also held at IAEA headquarters (July 2008). This meeting was attended by 12 LlBS experts from the Czech Republic, the European Commission, France, the Republic of South Korea, the United States of America, Germany, the United Kingdom of Great Britain, Canada, and Northern Ireland. Following a presentation of the needs of the IAEA inspectors, the LIBS experts agreed that needs as presented could be partially or fully fulfilled using LIBS instrumentation. Inspectors needs were grouped into the following broad categories: (1) Improvements to in-field measurements/environmental sampling; (2) Monitoring status of activities in Hot Cells; (3) Verify status of activity at a declared facility via process monitoring; and (4) Need for pre-screening of environmental samples before analysis. The primary tool employed by the IAEA to detect undeclared processes and activities at special nuclear material facilities and sites is environmental sampling. One of the objectives of the Next Generation Safeguards Initiative (NGSI) Program Plan calls for the development of advanced tools and methodologies to detect and analyze undeclared processing or production of special nuclear material. Los Alamos National Laboratory is currently investigating potential uses of LIBS for safeguards applications, including (1) a user-friendly man-portable LIBS system to characterize samples in real to near-real time (typical analysis time are on the order of minutes) across a wide range of elements in the periodic table from hydrogen up to heavy elements like plutonium and uranium, (2) a LIBS system that can be deployed in harsh environments such as hot cells and glove boxes providing relative compositional analysis of process streams for example ratios like Cm/Up and Cm/U, (3) an inspector field deployable system that can be used to analyze the elemental composition of microscopic quantities of samples containing plutonium and uranium, and (4) a high resolution LIBS system that can be used to determine the isotopic composition of samples containing for example uranium, plutonium... etc. In this paper, we will describe our current development and performance testing results for LIBS instrumentation both in a fixed lab and measurements in field deployable configurations.« less

Biogeochemical cycling in an organic-rich coastal marine basin. 8. A sulfur isotopic budget balanced by differential diffusion across the sediment-water interface

USGS Publications Warehouse

Chanton, J.P.; Martens, C.S.; Goldhaber, M.B.

1987-01-01

The sulfur isotopic composition of the sulfur fluxes occurring in the anoxic marine sediments of Cape Lookout Bight, N.C., U.S.A., was determined, and the result of isotopic mass balance was obtained via the differential diffusion model. Seasonal pore water sulfate ??34S measurements yielded a calculated sulfate input of 0.6%.. Sulfate transported into the sediments via diffusion appeared to be enriched in the lighter isotope because its concentration gradient was steeper, due to the increase in the measured isotopic composition of sulfate with depth. Similarly, the back diffusion of dissolved sulfide towards the sediment-water interface appeared enriched in the heavier isotope. The isotopic composition of this flux was calculated from measurements of the ??34S of dissolved sulfide and was determined to be 15.9%.. The isotopic composition of buried sulfide was determined to be -5.2%. and the detrital sulfur input was estimated to be -6.2%.. An isotope mass balance equation based upon the fluxes at the sediment-water interface successfully predicted the isotopic composition of the buried sulfur flux within 0.5%., thus confirming that isotopes diffuse in response to their individual concentration gradients. ?? 1987.

Flowsheet Analysis of U-Pu Co-Crystallization Process as a New Reprocessing System

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shunji Homma; Jun-ichi Ishii; Jiro Koga

2006-07-01

A new fuel reprocessing system by U-Pu co-crystallization process is proposed and examined by flowsheet analysis. This reprocessing system is based on the fact that hexavalent plutonium in nitric acid solution is co-crystallized with uranyl nitrate, whereas it is not crystallized when uranyl nitrate does not exist in the solution. The system consists of five steps: dissolution of spent fuel, plutonium oxidation, U-Pu co-crystallization as a co-decontamination, re-dissolution of the crystals, and U re-crystallization as a U-Pu separation. The system requires a recycling of the mother liquor from the U-Pu co-crystallization step and the appropriate recycle ratio is determined bymore » flowsheet analysis such that the satisfactory decontamination is achieved. Further flowsheet study using four different compositions of LWR spent fuels demonstrates that the constant ratio of plutonium to uranium in mother liquor from the re-crystallization step is achieved for every composition by controlling the temperature. It is also demonstrated by comparing to the Purex process that the size of the plant based on the proposed system is significantly reduced. (authors)« less

Molybdenum Isotopic Composition of Iron Meteorites, Chondrites and Refractory Inclusions

NASA Technical Reports Server (NTRS)

Becker, H.; Walker, R. J.

2003-01-01

Recent Mo isotopic studies of meteorites reported evidence for differences in isotopic compositions for whole rocks of some primitive and differentiated meteorites relative to terrestrial materials. Enrichments of r- and p-process isotopes of up to 3-4 units (e unit = parts in 10(exp 4) over s-process dominated isotopes are the most prominent features. Certain types of presolar grains show large enrichments in s-process isotopes, however, it was concluded on grounds of mass balance that incomplete digestion of such grains cannot explain the enrichments of r- and p-process isotopes in whole rocks of primitive chondrites. If the reported variability in r- and p-process isotope enrichments reflects the true isotopic characteristics of the whole rocks, the implications are quite profound. It would suggest the presence of large scale Mo isotopic heterogeneity within the solar accretion disk with likely collateral effects for other elements. However, such effects were not found for Ru isotopes, nor for Zr isotopes. Another recent Mo isotopic study by multi collector ICP-MS could not confirm the reported deviations in Allende, Murchison or iron meteorites. Here, we present new results for the Mo isotopic composition of iron meteorites, chondrites and CAIs obtained by negative thermal ionization mass spectrometry (NTIMS). We discuss analytical aspects and the homogeneity of Mo isotopic compositions in solar system materials.

Tags to Track Illicit Uranium and Plutonium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Haire, M. Jonathan; Forsberg, Charles W.

2007-07-01

With the expansion of nuclear power, it is essential to avoid nuclear materials from falling into the hands of rogue nations, terrorists, and other opportunists. This paper examines the idea of detection and attribution tags for nuclear materials. For a detection tag, it is proposed to add small amounts [about one part per billion (ppb)] of {sup 232}U to enriched uranium to brighten its radioactive signature. Enriched uranium would then be as detectable as plutonium and thus increase the likelihood of intercepting illicit enriched uranium. The use of rare earth oxide elements is proposed as a new type of 'attribution'more » tag for uranium and thorium from mills, uranium and plutonium fuels, and other nuclear materials. Rare earth oxides are chosen because they are chemically compatible with the fuel cycle, can survive high-temperature processing operations in fuel fabrication, and can be chosen to have minimal neutronic impact within the nuclear reactor core. The mixture of rare earths and/or rare earth isotopes provides a unique 'bar code' for each tag. If illicit nuclear materials are recovered, the attribution tag can identify the source and lot of nuclear material, and thus help police reduce the possible number of suspects in the diversion of nuclear materials based on who had access. (authors)« less

Do Hf isotopes in magmatic zircons represent those of their host rocks?

NASA Astrophysics Data System (ADS)

Wang, Di; Wang, Xiao-Lei; Cai, Yue; Goldstein, Steven L.; Yang, Tao

2018-04-01

Lu-Hf isotopic system in zircon is a powerful and widely used geochemical tracer in studying petrogenesis of magmatic rocks and crustal evolution, assuming that zircon Hf isotopes can represent initial Hf isotopes of their parental whole rock. However, this assumption may not always be valid. Disequilibrium partial melting of continental crust would preferentially melt out non-zircon minerals with high time-integrated Lu/Hf ratios and generate partial melts with Hf isotope compositions that are more radiogenic than those of its magma source. Dissolution experiments (with hotplate, bomb and sintering procedures) of zircon-bearing samples demonstrate this disequilibrium effect where partial dissolution yielded variable and more radiogenic Hf isotope compositions than fully dissolved samples. A case study from the Neoproterozoic Jiuling batholith in southern China shows that about half of the investigated samples show decoupled Hf isotopes between zircons and the bulk rocks. This decoupling could reflect complex and prolonged magmatic processes, such as crustal assimilation, magma mixing, and disequilibrium melting, which are consistent with the wide temperature spectrum from ∼630 °C to ∼900 °C by Ti-in-zircon thermometer. We suggest that magmatic zircons may only record the Hf isotopic composition of their surrounding melt during crystallization and it is uncertain whether their Hf isotopic compositions can represent the primary Hf isotopic compositions of the bulk magmas. In this regard, using zircon Hf isotopic compositions to trace crustal evolution may be biased since most of these could be originally from disequilibrium partial melts.

Oxygen Isotope Measurements of a Rare Murchison Type A CAI and Its Rim

NASA Technical Reports Server (NTRS)

Matzel, J. E. P.; Simon, J. I.; Hutcheon, I. D.; Jacobsen, B.; Simon, S. B.; Grossman, L.

2013-01-01

Ca-, Al-rich inclusions (CAIs) from CV chondrites commonly show oxygen isotope heterogeneity among different mineral phases within individual inclusions reflecting the complex history of CAIs in both the solar nebula and/or parent bodies. The degree of isotopic exchange is typically mineral-specific, yielding O-16-rich spinel, hibonite and pyroxene and O-16-depleted melilite and anorthite. Recent work demonstrated large and systematic variations in oxygen isotope composition within the margin and Wark-Lovering rim of an Allende Type A CAI. These variations suggest that some CV CAIs formed from several oxygen reservoirs and may reflect transport between distinct regions of the solar nebula or varying gas composition near the proto-Sun. Oxygen isotope compositions of CAIs from other, less-altered chondrites show less intra-CAI variability and 16O-rich compositions. The record of intra-CAI oxygen isotope variability in CM chondrites, which commonly show evidence for low-temperature aqueous alteration, is less clear, in part because the most common CAIs found in CM chondrites are mineralogically simple (hibonite +/- spinel or spinel +/- pyroxene) and are composed of minerals less susceptible to O-isotopic exchange. No measurements of the oxygen isotope compositions of rims on CAIs in CM chondrites have been reported. Here, we present oxygen isotope data from a rare, Type A CAI from the Murchison meteorite, MUM-1. The data were collected from melilite, hibonite, perovskite and spinel in a traverse into the interior of the CAI and from pyroxene, melilite, anorthite, and spinel in the Wark-Lovering rim. Our objectives were to (1) document any evidence for intra-CAI oxygen isotope variability; (2) determine the isotopic composition of the rim minerals and compare their composition(s) to the CAI interior; and (3) compare the MUM-1 data to oxygen isotope zoning profiles measured from CAIs in other chondrites.

Zn isotopes in hydrothermal sulfides and their oxidation products along the south mid-Atlantic ridge: evidence of hydrothermal fluid deposition

NASA Astrophysics Data System (ADS)

Li, Xiaohu; Wang, Jianqiang; Chu, Fengyou; Lei, Jijiang; Wang, Hao; Li, Zhenggang

2018-04-01

Significant Zn isotope fractionation occurs during seafloor hydrothermal activities. Therefore, exploring variations in Zn isotope composition affected by hydrothermal fluids and oxidative processes would help to better understand hydrothermal fluid cycling and sulfide deposition on mid-ocean ridges. In this paper, the Zn isotope compositions of different types of sulfides and their oxidation products obtained from hydrothermal fields on the South Mid-Atlantic Ridge (13-15°S) were analyzed using a Neptune plus MC-ICP-MS. The δ66Zn ratios range from -0.14‰ to +0.38‰, and the average δ66Zn ratio is +0.12±0.06‰ ( n=21, 2 SD) for all the studied sulfides and oxidation products. The Cu-rich sulfides have a slightly heavier Zn isotope composition (average δ66Zn=+0.19±0.07‰, n=6) than the Zn-rich sulfides (average δ66Zn=-0.02±0.06‰, n=5). The Zn isotope compositions of the oxidation products are similar to those of the Cu-rich sulfides, with an average δ66Zn ratio of 0.14±0.06‰ ( n=10, 2 SD). The Zn isotope compositions of all the samples are generally within the ranges of sulfides from hydrothermal fields on other mid-ocean ridges, such as the East Pacific Rise (9°N, 21°N) and the Trans-Atlantic Geotraverse. However, the average Zn isotope composition indicates the presence of significantly lighter Zn isotopes relative to those reported in the literature (average δ66Zn=+0.39‰). The significant enrichment of the Zn-rich sulfides with light Zn isotopes reveals that kinetic fractionation likely occurs during mineral deposition. Furthermore, the Zn isotope compositions of the sulfides and their oxidation products (average δ66Zn=+0.12‰) are significantly lighter than the average Zn isotope composition of the ocean (δ66Zn=+0.5‰), which could further constrain the modern Zn isotope cycle in the ocean by serving as a sink for light Zn isotopes.

Magnesium isotopic evidence for chemical disequilibrium among cumulus minerals in layered mafic intrusion

NASA Astrophysics Data System (ADS)

Chen, Lie-Meng; Teng, Fang-Zhen; Song, Xie-Yan; Hu, Rui-Zhong; Yu, Song-Yue; Zhu, Dan; Kang, Jian

2018-04-01

Magnesium isotopic compositions of olivine, clinopyroxene, and ilmenite from the Baima intrusion, SW China, for the first time, are investigated to constrain the magnitude and mechanisms of Mg isotope fractionation among cumulus minerals in layered mafic intrusions and to evaluate their geological implications. Olivine and clinopyroxene have limited Mg isotope variations, with δ26Mg ranging from -0.33 to +0.05‰ and from -0.29 to -0.13‰, respectively, similar to those of mantle xenolithic peridotites. By contrast, ilmenites display extremely large Mg isotopic variation, with δ26Mg ranging from -0.50 to +1.90‰. The large inter-mineral fractionations of Mg isotopes between ilmenite and silicates may reflect both equilibrium and kinetic processes. A few ilmenites have lighter Mg isotopic compositions than coexisting silicates and contain high MgO contents without compositional zoning, indicating equilibrium fractionation. The implication is that the light Mg isotopic compositions of lunar high-Ti basalts may result from an isotopically light source enriched in cumulate ilmenites. On the other hand, most ilmenites have heavy Mg isotopic compositions, coupled with high MgO concentration and chemical zoning, which can be quantitatively modeled by kinetic Mg isotope fractionations induced by subsolidus Mg-Fe exchange between ilmenite and ferromagnesian silicates during the cooling of the Baima intrusion. The extensive occurrence of kinetic Mg isotope fractionation in ilmenites implies the possibility of widespread compositional disequilibrium among igneous minerals in magma chambers. Consequently, disequilibrium effects need to be considered in studies of basaltic magma evolution, magma chamber processes, and magmatic Fe-Ti oxide ore genesis.

Tracing subducted crustal materials in the mantle by using magnesium isotopes

NASA Astrophysics Data System (ADS)

Teng, F. Z.

2016-12-01

Recent studies show that some continental basalt, mantle-metasomatised peridotite and cratonic eclogite have heterogeneous Mg isotopic compositions. These isotopically distinct Mg isotopic compositions have been explained by the incorporation of subducted materials in their mantle sources though the detailed mechanisms are still not well understood. In particular, how Mg-poor crustal materials can modify Mg isotopic systematics of Mg-rich mantle is unknown. Subduction zones are the most efficient sites for crust and mantle interactions, hence should be where the most prominent Mg isotopic variation occurs. However, to date, little is known on Mg isotope systematics in the subduction factory. Here I first review and report new Mg isotopic data for arc lava, subarc peridotite and the subducted slab (marine sediment, altered basalt and abyssal peridotite), then use them to constrain the origins of mantle Mg isotopic heterogeneity and lay the foundation for using Mg isotopes as new tools for tracing crust-mantle interactions. The main conclusions are 1) fluid-rock interactions can modify Mg isotopic systematics of abyssal peridotites; 2) island arc lavas have non-MORB Mg isotopic compositions, reflecting distinct surbarc mantle Mg isotopic signature; 3) continental arcs have non-MORB Mg isotopic compositions, likely resulting from crustal contamination and 4) the isotopically heterogeneous continental basalts are mainly produced by mixing of isotopically distinct magmas instead of being partial melting products of metasomatised mantle peridotites.

The role of mantle-hybridization and crustal contamination in the petrogenesis of lithospheric mantle-derived alkaline rocks: constraints from Os and Hf isotopes

NASA Astrophysics Data System (ADS)

Mayer, B.; Jung, S.; Brauns, M.; Münker, C.

2018-06-01

The Rhön area as part of the Central European Volcanic Province (CEVP) hosts an unusual suite of Tertiary 24-Ma old hornblende-bearing alkaline basalts that provide insights into melting and fractionation processes within the lithospheric mantle. These chemically primitive to slightly evolved and isotopically (Sr, Nd, Pb) depleted basalts have slightly lower Hf isotopic compositions than respective other CEVP basalts and Os isotope compositions more radiogenic than commonly observed for continental intraplate alkaline basalts. These highly radiogenic initial 187Os/188Os ratios (0.268-0.892) together with their respective Sr-Nd-Pb isotopic compositions are unlikely to result from crustal contamination alone, although a lack of Os data for lower crustal rocks from the area and limited data for CEVP basalts or mantle xenoliths preclude a detailed evaluation. Similarly, melting of the same metasomatized subcontinental lithospheric mantle as inferred for other CEVP basalts alone is also unlikely, based on only moderately radiogenic Os isotope compositions obtained for upper mantle xenoliths from elsewhere in the province. Another explanation for the combined Nd, Sr and Os isotope data is that the lavas gained their highly radiogenic Os isotope composition through a mantle "hybridization", metasomatism process. This model involves a mafic lithospheric component, such as an intrusion of a sublithospheric primary alkaline melt or a melt derived from subducted oceanic material, sometime in the past into the lithospheric mantle where it metasomatized the ambient mantle. Later at 24 Ma, thermal perturbations during rifting forced the isotopically evolved parts of the mantle together with the peridotitic ambient mantle to melt. This yielded a package of melts with highly correlated Re/Os ratios and radiogenic Os isotope compositions. Subsequent movement through the crust may have further altered the Os isotope composition although this effect is probably minor for the majority of the samples based on radiogenic Nd and unradiogenic Sr isotope composition of the lavas. If the radiogenic Os isotope composition can be explained by a mantle-hybridization and metasomatism model, the isotopic compositions of the hornblende basalts can be satisfied by ca. 5-25% addition of the mafic lithospheric component to an asthenospheric alkaline magma. Although a lack of isotope data for all required endmembers make this model somewhat speculative, the results show that the Re-Os isotope system in continental basalts is able to distinguish between crustal contamination and derivation of continental alkaline lavas from isotopically evolved peridotitic lithosphere that was contaminated by mafic material in the past and later remelted during rifting. The Hf isotopic compositions are slightly less radiogenic than in other alkaline basalts from the province and indicate the derivation of the lavas from low Lu-Hf parts of the lithospheric mantle. The new Os and Hf isotope data constrain a new light of the nature of such metasomatizing agents, at least for these particular rocks, which represent within the particular volcanic complex the first product of the volcanism.

The silicon isotope composition of the upper continental crust

NASA Astrophysics Data System (ADS)

Savage, Paul S.; Georg, R. Bastian; Williams, Helen M.; Halliday, Alex N.

2013-05-01

The upper continental crust (UCC) is the major source of silicon (Si) to the oceans and yet its isotopic composition is not well constrained. In an effort to investigate the degree of heterogeneity and provide a robust estimate for the average Si isotopic composition of the UCC, a representative selection of well-characterised, continentally-derived clastic sediments have been analysed using high-precision MC-ICPMS. Analyses of loess samples define a narrow range of Si isotopic compositions (δ30Si = -0.28‰ to -0.15‰). This is thought to reflect the primary igneous mineralogy and predominance of mechanical weathering in the formation of such samples. The average loess δ30Si is -0.22 ± 0.07‰ (2 s.d.), identical to average granite and felsic igneous compositions. Therefore, minor chemical weathering does not resolvably affect bulk rock δ30Si, and loess is a good proxy for the Si isotopic composition of unweathered, crystalline, continental crust. The Si isotopic compositions of shales display much more variability (δ30Si = -0.82‰ to 0.00‰). Shale Si isotope compositions do not correlate well with canonical proxies for chemical weathering, such as CIA values, but do correlate negatively with insoluble element concentrations and Al/Si ratios. This implies that more intensive or prolonged chemical weathering of a sedimentary source, with attendant desilicification, is required before resolvable negative Si isotopic fractionation occurs. Shale δ30Si values that are more positive than those of felsic igneous rocks most likely indicate the presence of marine-derived silica in such samples. Using the data gathered in this study, combined with already published granite Si isotope analyses, a weighted average composition of δ30Si = -0.25 ± 0.16‰ (2 s.d.) for the UCC has been calculated.

Controls on the barium isotope compositions of marine sediments

NASA Astrophysics Data System (ADS)

Bridgestock, Luke; Hsieh, Yu-Te; Porcelli, Donald; Homoky, William B.; Bryan, Allison; Henderson, Gideon M.

2018-01-01

The accumulation of barium (Ba) in marine sediments is considered to be a robust proxy for export production, although this application can be limited by uncertainty in BaSO4 preservation and sediment mass accumulation rates. The Ba isotope compositions of marine sediments could potentially record insights into past changes in the marine Ba cycle, which should be insensitive to these limitations, enabling more robust interpretation of sedimentary Ba as a proxy. To investigate the controls on the Ba isotope compositions of marine sediments and their potential for paleo-oceanographic applications, we present the first Ba isotope compositions results for sediments, as well as overlying seawater depth profiles collected in the South Atlantic. Variations in Ba isotope compositions of the sediments predominantly reflect changes in the relative contributions of detrital and authigenic Ba sources, with open-ocean sediments constraining the isotope composition of authigenic Ba to be δ 138/134Ba ≈ + 0.1 ‰. This value is consistent with the average isotope composition inferred for sinking particulate Ba using simple mass balance models of Ba in the overlying water column and is hypothesized to reflect the removal of Ba from the upper water column with an associated isotopic fractionation of Δ diss-part 138/134Ba ≈ + 0.4 to +0.5. Perturbations to upper ocean Ba cycling, due to changes in export production and the supply of Ba via upwelling, should therefore be recorded by the isotope compositions of sedimentary authigenic Ba. Such insights will help to improve the reliable application of Ba accumulation rates in marine sediments as a proxy for past changes in export production.

Isotopic signals of denitrification in a northern hardwood forested catchment

NASA Astrophysics Data System (ADS)

Wexler, Sarah; Goodale, Christine

2013-04-01

Water samples from streams, groundwater and precipitation were collected during summer from the hydrologic reference watershed (W3) at Hubbard Brook Experimental Forest in the White Mountains, New Hampshire, and analysed for d15N-NO3 and d18O-NO3. Despite very low nitrate concentrations (<0.5 to 8.8 uM NO3-) dual-isotopic signals of sources and processes were clearly distinguishable. The isotopic composition of nitrate from shallow groundwater showed evidence of dual isotopic fractionation in line with denitrification, with a positive relationship between nitrogen and oxygen isotopic composition, a regression line slope of 0.76 (r2 = 0.68), and an empirical isotope enrichment factor of ɛP-S 15N-NO3 -12.7%. The isotopic composition of riparian groundwater nitrate from time-series samples showed variation in processes over a small spatial scale. The expected isotopic composition of nitrate sources in the watershed was used to distinguish nitrate in rain and nitrate from nitrification of both rainfall ammonium and ammonium from mineralised soil organic nitrogen. Evidence of oxygen exchange with water during nitrification was seen in the isotopic composition of stream and shallow groundwater nitrate. The isotopic composition of streamwater nitrate following a period of storms indicated that 25% of nitrate in the streamwater was of atmospheric origin. This suggests rapid infiltration of rainfall via vertical bypass flow to the saturated zone, enabling transport of atmospheric nitrate to the stream channels. Across the Hubbard Brook basin, the isotopic composition of nitrate from paired samples from watersheds 4-7 indicated a switch between a nitrification and assimilation dominated system, to a system influenced by rainfall nitrogen inputs and denitrification. The dual isotope approach has revealed evidence of denitrification of nitrate from different sources at low concentrations at Hubbard Brook during summer. This isotopic evidence deepens our understanding of the significance and spatial variability of denitrification in environments with low levels of nitrate, represented by this northern hardwood forested catchment.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Valysaev, B.M.; Erokhin, V.E.; Grinchenko, Y.I.

A study has been made of the isotopic composition of the carbon in methane and carbon dioxide, as well as hydrogen in the methane, in the gases of mud volcanoes, for all main mud volcano areas in the USSR. The isotopic composition of carbon and hydrogen in methane shows that the gases resemble those of oil and gas deposits, while carbon dioxide of these volcanoes has a heavier isotopic composition with a greater presence of ''ultraheavy'' carbon dioxide. By the chemical and isotopic composition of gases, Azerbaidzhan and South Sakhalin types of mud volcano gases have been identified, as wellmore » as Bulganak subtypes and Akhtala and Kobystan varieties. Correlations are seen between the isotopic composition of gases and the geological build of mud volcano areas.« less

Stable isotopic composition of perchlorate and nitrate accumulated in plants: Hydroponic experiments and field data.

PubMed

Estrada, Nubia Luz; Böhlke, J K; Sturchio, Neil C; Gu, Baohua; Harvey, Greg; Burkey, Kent O; Grantz, David A; McGrath, Margaret T; Anderson, Todd A; Rao, Balaji; Sevanthi, Ritesh; Hatzinger, Paul B; Jackson, W Andrew

2017-10-01

Natural perchlorate (ClO 4 - ) in soil and groundwater exhibits a wide range in stable isotopic compositions (δ 37 Cl, δ 18 O, and Δ 17 O), indicating that ClO 4 - may be formed through more than one pathway and/or undergoes post-depositional isotopic alteration. Plants are known to accumulate ClO 4 - , but little is known about their ability to alter its isotopic composition. We examined the potential for plants to alter the isotopic composition of ClO 4 - in hydroponic and field experiments conducted with snap beans (Phaseolus vulgaris L.). In hydroponic studies, anion ratios indicated that ClO 4 - was transported from solutions into plants similarly to NO 3 - but preferentially to Cl - (4-fold). The ClO 4 - isotopic compositions of initial ClO 4 - reagents, final growth solutions, and aqueous extracts from plant tissues were essentially indistinguishable, indicating no significant isotope effects during ClO 4 - uptake or accumulation. The ClO 4 - isotopic composition of field-grown snap beans was also consistent with that of ClO 4 - in varying proportions from irrigation water and precipitation. NO 3 - uptake had little or no effect on NO 3 - isotopic compositions in hydroponic solutions. However, a large fractionation effect with an apparent ε ( 15 N/ 18 O) ratio of 1.05 was observed between NO 3 - in hydroponic solutions and leaf extracts, consistent with partial NO 3 - reduction during assimilation within plant tissue. We also explored the feasibility of evaluating sources of ClO 4 - in commercial produce, as illustrated by spinach, for which the ClO 4 - isotopic composition was similar to that of indigenous natural ClO 4 - . Our results indicate that some types of plants can accumulate and (presumably) release ClO 4 - to soil and groundwater without altering its isotopic characteristics. Concentrations and isotopic compositions of ClO 4 - and NO 3 - in plants may be useful for determining sources of fertilizers and sources of ClO 4 - in their growth environments and consequently in food supplies. Copyright © 2017 Elsevier B.V. All rights reserved.

Stable isotopic composition of perchlorate and nitrate accumulated in plants: Hydroponic experiments and field data

USGS Publications Warehouse

Estrada, Nubia Luz; Böhlke, John Karl; Sturchio, Neil C.; Gu, Baohua; Harvey, Greg; Burkey, Kent O.; Grantz, David A.; McGrath, Margaret T.; Anderson, Todd A.; Rao, Balaji; Sevanthi, Ritesh; Hatzinger, Paul B.; Jackson, W. Andrew

2017-01-01

Natural perchlorate (ClO4−) in soil and groundwater exhibits a wide range in stable isotopic compositions (δ37Cl, δ18O, and Δ17O), indicating that ClO4− may be formed through more than one pathway and/or undergoes post-depositional isotopic alteration. Plants are known to accumulate ClO4−, but little is known about their ability to alter its isotopic composition. We examined the potential for plants to alter the isotopic composition of ClO4− in hydroponic and field experiments conducted with snap beans (Phaseolus vulgaris L.). In hydroponic studies, anion ratios indicated that ClO4− was transported from solutions into plants similarly to NO3− but preferentially to Cl− (4-fold). The ClO4− isotopic compositions of initial ClO4− reagents, final growth solutions, and aqueous extracts from plant tissues were essentially indistinguishable, indicating no significant isotope effects during ClO4− uptake or accumulation. The ClO4− isotopic composition of field-grown snap beans was also consistent with that of ClO4− in varying proportions from irrigation water and precipitation. NO3− uptake had little or no effect on NO3− isotopic compositions in hydroponic solutions. However, a large fractionation effect with an apparent ε (15N/18O) ratio of 1.05 was observed between NO3− in hydroponic solutions and leaf extracts, consistent with partial NO3− reduction during assimilation within plant tissue. We also explored the feasibility of evaluating sources of ClO4− in commercial produce, as illustrated by spinach, for which the ClO4− isotopic composition was similar to that of indigenous natural ClO4−. Our results indicate that some types of plants can accumulate and (presumably) release ClO4− to soil and groundwater without altering its isotopic characteristics. Concentrations and isotopic compositions of ClO4−and NO3− in plants may be useful for determining sources of fertilizers and sources of ClO4− in their growth environments and consequently in food supplies.

Monte Carlo calculations of the incineration of plutonium and minor actinides of laser fusion inertial confinement fusion fission energy (LIFE) engine

NASA Astrophysics Data System (ADS)

Adem, ACIR; Eşref, BAYSAL

2018-07-01

In this paper, neutronic analysis in a laser fusion inertial confinement fusion fission energy (LIFE) engine fuelled plutonium and minor actinides using a MCNP codes was investigated. LIFE engine fuel zone contained 10 vol% TRISO particles and 90 vol% natural lithium coolant mixture. TRISO fuel compositions have Mod①: reactor grade plutonium (RG-Pu), Mod②: weapon grade plutonium (WG-Pu) and Mod③: minor actinides (MAs). Tritium breeding ratios (TBR) were computed as 1.52, 1.62 and 1.46 for Mod①, Mod② and Mod③, respectively. The operation period was computed as ∼21 years when the reference TBR > 1.05 for a self-sustained reactor for all investigated cases. Blanket energy multiplication values (M) were calculated as 4.18, 4.95 and 3.75 for Mod①, Mod② and Mod③, respectively. The burnup (BU) values were obtained as ∼1230, ∼1550 and ∼1060 GWd tM–1, respectively. As a result, the higher BU were provided with using TRISO particles for all cases in LIFE engine.

MIS High-Purity Plutonium Oxide Hydride Product 5501579 (SSR124): Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Veirs, Douglas Kirk; Stroud, Mary Ann; Berg, John M.

A high-purity plutonium dioxide material from the Material Identification and Surveillance (MIS) Program inventory has been studied with regard to gas generation and corrosion in a storage environment. Sample 5501579 represents process plutonium oxides from hydride oxide from Rocky Flats that are currently stored in 3013 containers. After calcination to 950°C, the material contained 87.42% plutonium with no major impurities. This study followed over time, the gas pressure of a sample with nominally 0.5 wt% water in a sealed container with an internal volume scaled to 1/500th of the volume of a 3013 container. Gas compositions were measured periodically overmore » a six year period. The maximum observed gas pressure was 124 kPa. The increase over the initial pressure of 70 kPa was primarily due to generation of nitrogen and carbon dioxide gas. Hydrogen and oxygen were minor components of the headspace gas. At the completion of the study, the internal components of the sealed container showed signs of corrosion.« less

Tracing Cd, Zn and Pb pollution sources in bivalves using isotopes

NASA Astrophysics Data System (ADS)

Shiel, A. E.; Weis, D. A.; Orians, K. J.

2010-12-01

In a multi-tracer study, Cd, Zn and Pb isotopes (MC-ICP-MS) and elemental concentrations (HR-ICP-MS) are evaluated as tools to distinguish between natural and anthropogenic sources of these metals in bivalves from western Canada (British Columbia), the eastern USA, Hawaii and France. High Cd concentrations found in BC oysters have elicited economic and health concerns. The source of these high Cd levels is unknown but thought to be largely natural. High Cd levels in BC oysters are largely attributed to the natural upwelling of Cd-rich intermediate waters in the North Pacific as the δ114/110Cd (-0.69 to -0.09‰) and δ66/64Zn (0.28 to 0.36‰) values of BC oysters fall within the range reported for North Pacific seawater. Different contributions from anthropogenic sources account for the variability of Cd isotopic compositions of BC oysters; the lightest of these oysters are from the BC mainland. These oysters also have Pb isotopic compositions that reflect primarily anthropogenic sources (e.g., leaded and unleaded automotive gasoline and smelting of Pb ores, potentially historical). On the contrary, USA East Coast bivalves exhibit relatively light Cd isotopic compositions (δ114/110Cd = -1.20 to -0.54‰; lighter than reported for North Atlantic seawater) due to the high prevalence of industry on this coast. The Pb isotopic compositions of these bivalves indicate contributions from the combustion of coal. The large variability of environmental health among coastal areas in France is reflected in the broad range of Cd isotopic compositions exhibited by French bivalves (δ114/110Cd = -1.08 to -0.20‰). Oysters and mussels from the Marennes-Oléron basin and Gironde estuary have the lightest Cd isotopic compositions of the French oysters consistent with significant historical Cd emissions from the now-closed proximal Zn smelter. In these bivalves, significant declines in the Cd levels between 1984/7 and 2004/5 are not accompanied by a significant shift in the Cd isotopic composition toward natural values. The Mediterranean samples have isotopic compositions within error of the lighter end of the range reported for Mediterranean seawater. The Zn isotopic compositions of French oysters and mussels (δ66/64Zn = 0.39 to 0.46‰) are identical to those reported for North Atlantic seawater, with the exception of the much heavier compositions of oysters (δ66/64Zn = 1.03 to 1.15‰) from the polluted Gironde estuary. In agreement with Cd and Zn isotopic compositions, the Pb isotopic compositions of the French bivalves indicate primarily industrial (as opposed to automotive) sources; this is consistent with the collection of most of the French bivalve samples in 2004, after the complete phase-out of leaded gasoline in France. This study demonstrates the effective use of Cd and Zn isotopes to trace anthropogenic sources in the environment and the benefit of combining these tools with Pb isotope “fingerprinting” techniques to identify processes contributing metals. Use of these new geochemical tools requires site-specific knowledge of potential metal sources and their isotopic compositions.

Isotopic evidence of plutonium release into the environment from the Fukushima DNPP accident

PubMed Central

Zheng, Jian; Tagami, Keiko; Watanabe, Yoshito; Uchida, Shigeo; Aono, Tatsuo; Ishii, Nobuyoshi; Yoshida, Satoshi; Kubota, Yoshihisa; Fuma, Shoichi; Ihara, Sadao

2012-01-01

The Fukushima Daiichi nuclear power plant (DNPP) accident caused massive releases of radioactivity into the environment. The released highly volatile fission products, such as 129mTe, 131I, 134Cs, 136Cs and 137Cs were found to be widely distributed in Fukushima and its adjacent prefectures in eastern Japan. However, the release of non-volatile actinides, in particular, Pu isotopes remains uncertain almost one year after the accident. Here we report the isotopic evidence for the release of Pu into the atmosphere and deposition on the ground in northwest and south of the Fukushima DNPP in the 20–30 km zones. The high activity ratio of 241Pu/239+240Pu (> 100) from the Fukushima DNPP accident highlights the need for long-term 241Pu dose assessment, and the ingrowth of 241Am. The results are important for the estimation of reactor damage and have significant implication in the strategy of decontamination. PMID:22403743

Managing the Nuclear Fuel Cycle: Policy Implications of Expanding Global Access to Nuclear Power

DTIC Science & Technology

2009-07-01

inalienable right and, by and large, neither have U.S. government officials. However, the case of Iran raises perhaps the most critical question in this...slight difference in atomic mass between 235U and 238U. The typical enrichment process requires about 10 lbs of uranium U3O8 to produce 1 lb of low...thermal neutrons but can induce fission in all actinides , including all plutonium isotopes. Therefore, nuclear fuel for a fast reactor must have a

Methods to Collect, Compile, and Analyze Observed Short-lived Fission Product Gamma Data

DOE Office of Scientific and Technical Information (OSTI.GOV)

Finn, Erin C.; Metz, Lori A.; Payne, Rosara F.

2011-09-29

A unique set of fission product gamma spectra was collected at short times (4 minutes to 1 week) on various fissionable materials. Gamma spectra were collected from the neutron-induced fission of uranium, neptunium, and plutonium isotopes at thermal, epithermal, fission spectrum, and 14-MeV neutron energies. This report describes the experimental methods used to produce and collect the gamma data, defines the experimental parameters for each method, and demonstrates the consistency of the measurements.

Hunting a Black Swan: Policy Options for America’s Police in Preventing Radiological/Nuclear Terrorism

DTIC Science & Technology

2012-09-01

patrol vehicles. The Department’s Counter-Terror Operations Unit serves as the program coordinator and as the archetypical NIMS Type I Team. The...is defined by Title I of the Atomic Energy Act of 1954 as plutonium, uranium-233, or uranium enriched in the isotopes uranium-233 or uranium...end of World War II. Radioactive Materials—materials that contain radioactive atoms . Radioactive atoms are unstable; that is, they have too much

Stable water isotope patterns in a climate change hotspot: the isotope hydrology framework of Corsica (western Mediterranean).

PubMed

van Geldern, Robert; Kuhlemann, Joachim; Schiebel, Ralf; Taubald, Heinrich; Barth, Johannes A C

2014-06-01

The Mediterranean is regarded as a region of intense climate change. To better understand future climate change, this area has been the target of several palaeoclimate studies which also studied stable isotope proxies that are directly linked to the stable isotope composition of water, such as tree rings, tooth enamel or speleothems. For such work, it is also essential to establish an isotope hydrology framework of the region of interest. Surface waters from streams and lakes as well as groundwater from springs on the island of Corsica were sampled between 2003 and 2009 for their oxygen and hydrogen isotope compositions. Isotope values from lake waters were enriched in heavier isotopes and define a local evaporation line (LEL). On the other hand, stream and spring waters reflect the isotope composition of local precipitation in the catchment. The intersection of the LEL and the linear fit of the spring and stream waters reflect the mean isotope composition of the annual precipitation (δP) with values of-8.6(± 0.2) ‰ for δ(18)O and-58(± 2) ‰ for δ(2)H. This value is also a good indicator of the average isotope composition of the local groundwater in the island. Surface water samples reflect the altitude isotope effect with a value of-0.17(± 0.02) ‰ per 100 m elevation for oxygen isotopes. At Vizzavona Pass in central Corsica, water samples from two catchments within a lateral distance of only a few hundred metres showed unexpected but systematic differences in their stable isotope composition. At this specific location, the direction of exposure seems to be an important factor. The differences were likely caused by isotopic enrichment during recharge in warm weather conditions in south-exposed valley flanks compared to the opposite, north-exposed valley flanks.

Hadean Oceanography: Experimental Constraints on the Development of the Terrestrial Hydrosphere and the Origin of Life on Earth

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ryerson, F J

The oxygen isotopic compositions of the world's oldest mineral grains, zircon, have recently been used to infer the compositions of the rocks from which they crystallized. The results appear to require a source that had once experienced isotopic fractionation between clay minerals and liquid water, thereby implying the presence of liquid water at the Earth's surface prior to 4.4 billion years ago, less than 2 million years after accretion. This observation has important implications for the development of the Earth's continental crust. The inferred composition of the zircon source rock is directly dependent upon the oxygen isotopic fractionation between zirconmore » and melt, and zircon and water. These fractionation factors have not been determined experimentally, however, constituting the weak link in this argument. A series of experiments to measure these fractionation factors has been conducted. The experiments consist of finely powdered quartz, a polished single crystal of zircon and isotopically-enriched or isotopically normal water to provide a range of isotopic compositions. The experiments will be run until quartz is in isotopic equilibrium with water. Zircon was expected to partially equilibrate producing an oxygen isotopic diffusion profile perpendicular to the surface. Ion probe spot analysis of quartz and depth profiling of zircon will determine the bulk and surface isotopic compositions of the phases, respectively. The well-known quartz-water isotopic fractionation factors can be used to calculate the oxygen isotopic composition of the fluid, and with the zircon surface composition, the zircon-water fractionation factor. Run at temperatures up to 1000 C for as long as 500 hours have not produced diffusion profiles longer than 50 nm. The steep isotopic gradient at the samples surface precludes use of the diffusion profile for estimation on the surface isotopic composition. The short profiles may be the result of surface dissolution, although such dissolution cannot be resolved in SEM images. The sluggish nature of diffusion in zircon may require that fractionation factors be determined by direct hydrothermal synthesis of zircon rather than by mineral-fluid exchange.« less

Iron and nickel isotope compositions of presolar silicon carbide grains from supernovae

NASA Astrophysics Data System (ADS)

Kodolányi, János; Stephan, Thomas; Trappitsch, Reto; Hoppe, Peter; Pignatari, Marco; Davis, Andrew M.; Pellin, Michael J.

2018-01-01

We report the carbon, silicon, iron, and nickel isotope compositions of twenty-five presolar SiC grains of mostly supernova (SN) origin. The iron and nickel isotope compositions were measured with the new Chicago Instrument for Laser Ionization, CHILI, which allows the analysis of all iron and nickel isotopes without the isobaric interferences that plagued previous measurements with the NanoSIMS. Despite terrestrial iron and nickel contamination, significant isotopic anomalies in 54Fe/56Fe, 57Fe/56Fe, 60Ni/58Ni, 61Ni/58Ni, 62Ni/58Ni, and 64Ni/58Ni were detected in nine SN grains (of type X). Combined multi-isotope data of three grains with the largest nickel isotope anomalies (>100‰ or <-100‰ in at least one isotope ratio, when expressed as deviation from the solar value) are compared with the predictions of two SN models, one with and one without hydrogen ingestion in the He shell prior to SN explosion. One grain's carbon-silicon-iron-nickel isotope composition is consistent with the prediction of the model without hydrogen ingestion, whereas the other two grains' isotope anomalies could not be reproduced using either SN models. The discrepancies between the measured isotope compositions and model predictions may indicate element fractionation in the SN ejecta prior to or during grain condensation, and reiterate the need for three-dimensional SN models.

Nuclear Forensics: A Methodology Applicable to Nuclear Security and to Non-Proliferation

NASA Astrophysics Data System (ADS)

Mayer, K.; Wallenius, M.; Lützenkirchen, K.; Galy, J.; Varga, Z.; Erdmann, N.; Buda, R.; Kratz, J.-V.; Trautmann, N.; Fifield, K.

2011-09-01

Nuclear Security aims at the prevention and detection of and response to, theft, sabotage, unauthorized access, illegal transfer or other malicious acts involving nuclear material. Nuclear Forensics is a key element of nuclear security. Nuclear Forensics is defined as a methodology that aims at re-establishing the history of nuclear material of unknown origin. It is based on indicators that arise from known relationships between material characteristics and process history. Thus, nuclear forensics analysis includes the characterization of the material and correlation with production history. To this end, we can make use of parameters such as the isotopic composition of the nuclear material and accompanying elements, chemical impurities, macroscopic appearance and microstructure of the material. In the present paper, we discuss the opportunities for attribution of nuclear material offered by nuclear forensics as well as its limitations. Particular attention will be given to the role of nuclear reactions. Such reactions include the radioactive decay of the nuclear material, but also reactions with neutrons. When uranium (of natural composition) is exposed to neutrons, plutonium is formed, as well as 236U. We will illustrate the methodology using the example of a piece of uranium metal that dates back to the German nuclear program in the 1940's. A combination of different analytical techniques and model calculations enables a nuclear forensics interpretation, thus correlating the material characteristics with the production history.

Reconstruction of the Nd isotope composition of seawater on epicontinental seas: Testing the potential of Fe-Mn oxyhydroxide coatings on foraminifera tests for deep-time investigations

NASA Astrophysics Data System (ADS)

Charbonnier, Guillaume; Pucéat, Emmanuelle; Bayon, Germain; Desmares, Delphine; Dera, Guillaume; Durlet, Christophe; Deconinck, Jean-François; Amédro, Francis; Gourlan, Alexandra T.; Pellenard, Pierre; Bomou, Brahimsamba

2012-12-01

The Fe-Mn oxide fraction leached from deep-sea sediments has been increasingly used to reconstruct the Nd isotope composition of deep water masses, that can be used to track changes in oceanic circulation with a high temporal resolution. Application of this archive to reconstruct the Nd isotope composition of bottom seawater in shallow shelf environments remained however to be tested. Yet as the Nd isotope composition of seawater on continental margins is particularly sensitive to changes in erosional inputs, establishment of neritic seawater Nd isotope evolution around areas of deep water formation would be useful to discriminate the influence of changes in oceanic circulation and in isotopic composition of erosional inputs on the Nd isotope record of deep waters. The purpose of this study is to test the potential of Fe-Mn coatings leached from foraminifera tests to reconstruct the Nd isotope composition of seawater in shelf environments for deep-time intervals. Albian to Turonian samples from two different outcrops have been recovered, from the Paris Basin (Wissant section, northern France) and from the Western Interior Seaway (Hot Spring, South Dakota, USA), that were deposited in epicontinental seas. Rare Earth Element (REE) spectra enriched in middle REEs in the foraminifera leach at Wissant highlight the presence of Fe-Mn oxides. The similarity of the Nd isotopic signal of the Fe-Mn oxide fraction leached from foraminifera tests with that of fish teeth suggests that Fe-Mn oxides coating foraminifera can be good archives of shelf bottom seawater Nd isotopic composition. Inferred bottom shelf water Nd isotope compositions at Wissant range from -8.5 to -9.7 ɛ-units, about 1.5-2 ɛ-units higher than that of the contemporaneous local detrital fraction. At Hot Spring, linear REE spectra characterizing foraminifera leach may point to an absence of authigenic marine Fe-Mn oxide formation in this area during the Late Cenomanian-Early Turonian, consistent with dysoxic to anoxic conditions at Hot Spring, contemporaneous to an Oceanic Anoxic Event. The similarity of the Nd isotopic signal of the carbonate matrix of foraminifera with that of fish teeth suggests that it records the Nd isotope composition of bottom shelf seawater as well. Inferred bottom shelf water Nd isotope compositions at Hot Spring are quite radiogenic, between -7 and -6 ɛ-units, about 2.5-4 ɛ-units higher than that of the contemporaneous local detrital fraction. In contrast, in both sections Fe-Mn oxides leached directly from the decarbonated sediment tend to yield a less radiogenic Nd isotopic composition, typically between 0.2 and 0.8 ɛ-units lower, that is intermediate between that of fish teeth and of the detrital fraction. This suggests the contribution of pre-formed continental Fe-Mn oxides to the Nd isotopic signal, along with authigenic marine oxides, or a detrital contamination during leaching.

Hydrogen and oxygen in brine shrimp chitin reflect environmental water and dietary isotopic composition

NASA Astrophysics Data System (ADS)

Nielson, Kristine E.; Bowen, Gabriel J.

2010-03-01

Hydrogen and oxygen isotope ratios of the common structural biopolymer chitin are a potential recorder of ecological and environmental information, but our understanding of the mechanisms of incorporation of H and O from environmental substrates into chitin is limited. We report the results of a set of experiments in which the isotopic compositions of environmental water and diet were varied independently in order to assess the contribution of these variables to the H and O isotopic composition of Artemia franciscana chitin. Hydrogen isotope ratios of chitin were strongly linearly correlated with both food and water, with approximately 26% of the hydrogen signal reflecting food and approximately 38% reflecting water. Oxygen isotopes were also strongly correlated with the isotopic composition of water and food, but whereas 69% of oxygen in chitin exchanged with environmental water, only 10% was derived from food. We propose that these observations reflect the position-specific, partial exchange of H and O atoms with brine shrimp body water during the processes of digestion and chitin biosynthesis. Comparison of culture experiments with a set of natural samples collected from the Great Salt Lake, UT in 2006 shows that, with some exceptions, oxygen isotope compositions of chitin track those of water, whereas hydrogen isotopes vary inversely with those of lake water. The different behavior of the two isotopic systems can be explained in terms of a dietary shift from allochthonous particulate matter with relatively higher δ 2H values in the early spring to autochthonous particulate matter with significantly lower δ 2H values in the late summer to autumn. These results suggest oxygen in chitin may be a valuable proxy for the oxygen isotopic composition of environmental water, whereas hydrogen isotope values from the same molecule may reveal ecological and biogeochemical changes within lakes.

Isotopologue Distributions of Peptide Product Ions by Tandem Mass Spectrometry: Quantitation of Low Levels of Deuterium Incorporation1

PubMed Central

Wang, Benlian; Sun, Gang; Anderson, David R.; Jia, Minghong; Previs, Stephen; Anderson, Vernon E.

2007-01-01

Protonated molecular peptide ions and their product ions generated by tandem mass spectrometry appear as isotopologue clusters due to the natural isotopic variations of carbon, hydrogen, nitrogen, oxygen and sulfur. Quantitation of the isotopic composition of peptides can be employed in experiments involving isotope effects, isotope exchange, isotopic labeling by chemical reactions, and studies of metabolism by stable isotope incorporation. Both ion trap and quadrupole-time of flight mass spectrometry are shown to be capable of determining the isotopic composition of peptide product ions obtained by tandem mass spectrometry with both precision and accuracy. Tandem mass spectra obtained in profile-mode of clusters of isotopologue ions are fit by non-linear least squares to a series of Gaussian peaks (described in the accompanying manuscript) which quantify the Mn/M0 values which define the isotopologue distribution (ID). To determine the isotopic composition of product ions from their ID, a new algorithm that predicts the Mn/M0 ratios is developed which obviates the need to determine the intensity of all of the ions of an ID. Consequently a precise and accurate determination of the isotopic composition a product ion may be obtained from only the initial values of the ID, however the entire isotopologue cluster must be isolated prior to fragmentation. Following optimization of the molecular ion isolation width, fragmentation energy and detector sensitivity, the presence of isotopic excess (2H, 13C, 15N, 18O) is readily determined within 1%. The ability to determine the isotopic composition of sequential product ions permits the isotopic composition of individual amino acid residues in the precursor ion to be determined. PMID:17559791

Nucleosynthetic Heterogeneity Controls Vanadium Isotope Variations in Bulk Chondrites

NASA Technical Reports Server (NTRS)

Nielsen, S. G.; Righter, K.; Wu, F.; Owens, J. D.; Prytulak, J.; Burton, K.; Parkinson, I.; Davis, D.

2018-01-01

The vanadium (V) isotope composition of early solar system materials have been hypothesized to be sensitive to high energy irradiation that originated from the young Sun. Vanadium has two isotopes with masses 50 and 51 that have (51)V/(50)V ratio of approximately 410. High energy irradiation produces (50)V from various target isotopes of Ti, Cr and Fe, which would result in light V isotope compositions (expressed as delta (51)V in per mille = 1000 x (((51)V/(50)V(sub sample)/(51)V/(50)V(sub AlfaAesar)) - 1)) relative to a presumably chondritic starting composition. Recently published V isotope data for calcium aluminium inclusions (CAIs) has revealed some very negative values relative to chondrites (by almost -4 per mille) that were indeed interpreted to reflect irradiation processes despite the fact that the studied CAIs all exhibited significant initial abundances of (10)Be, while only a few CAIs displayed light V isotope compositions. It is difficult to relate V isotope variations directly to a singular process because V only possesses two isotopes. Therefore, V isotope variations can principally be produced both mass dependent and independent processes. Mass dependent kinetic stable isotope fractionation is common in CAIs for refractory elements due to partial condensation/evaporation processes. The element strontium (Sr) has an almost identical condensation temperature to V and studies of stable Sr isotope compositions in CAIs reveal both heavy and light values relative to chondrites of several permil. These variations are similar in magnitude to those reported for V isotopes in CAIs, which suggests it is possible that some of the V isotope variation in CAIs could be due to kinetic stable isotope fractionation during condensation/evaporation processes.

The stable isotope composition of nitrogen and carbon and elemental contents in modern and fossil seabird guano from Northern Chile - Marine sources and diagenetic effects.

PubMed

Lucassen, Friedrich; Pritzkow, Wolfgang; Rosner, Martin; Sepúlveda, Fernando; Vásquez, Paulina; Wilke, Hans; Kasemann, Simone A

2017-01-01

Seabird excrements (guano) have been preserved in the arid climate of Northern Chile since at least the Pliocene. The deposits of marine organic material in coastal areas potentially open a window into the present and past composition of the coastal ocean and its food web. We use the stable isotope composition of nitrogen and carbon as well as element contents to compare the principal prey of the birds, the Peruvian anchovy, with the composition of modern guano. We also investigate the impact of diagenetic changes on the isotopic composition and elemental contents of the pure ornithogenic sediments, starting with modern stratified deposits and extending to fossil guano. Where possible, 14C systematics is used for age information. The nitrogen and carbon isotopic composition of the marine prey (Peruvian anchovy) of the birds is complex as it shows strong systematic variations with latitude. The detailed study of a modern profile that represents a few years of guano deposition up to present reveals systematic changes in nitrogen and carbon isotopic composition towards heavier values that increase with age, i.e. depth. Only the uppermost, youngest layers of modern guano show compositional affinity to the prey of the birds. In the profile, the simultaneous loss of nitrogen and carbon occurs by degassing, and non-volatile elements like phosphorous and calcium are passively enriched in the residual guano. Fossil guano deposits are very low in nitrogen and low in carbon contents, and show very heavy nitrogen isotopic compositions. One result of the study is that the use of guano for tracing nitrogen and carbon isotopic and elemental composition in the marine food web of the birds is restricted to fresh material. Despite systematic changes during diagenesis, there is little promise to retrieve reliable values of marine nitrogen and carbon signatures from older guano. However, the changes in isotopic composition from primary marine nitrogen isotopic signatures towards very heavy values generate a compositionally unique material. These compositions trace the presence of guano in natural ecosystems and its use as fertilizer in present and past agriculture.

The stable isotope composition of nitrogen and carbon and elemental contents in modern and fossil seabird guano from Northern Chile – Marine sources and diagenetic effects

PubMed Central

Pritzkow, Wolfgang; Rosner, Martin; Sepúlveda, Fernando; Vásquez, Paulina; Wilke, Hans; Kasemann, Simone A.

2017-01-01

Seabird excrements (guano) have been preserved in the arid climate of Northern Chile since at least the Pliocene. The deposits of marine organic material in coastal areas potentially open a window into the present and past composition of the coastal ocean and its food web. We use the stable isotope composition of nitrogen and carbon as well as element contents to compare the principal prey of the birds, the Peruvian anchovy, with the composition of modern guano. We also investigate the impact of diagenetic changes on the isotopic composition and elemental contents of the pure ornithogenic sediments, starting with modern stratified deposits and extending to fossil guano. Where possible, 14C systematics is used for age information. The nitrogen and carbon isotopic composition of the marine prey (Peruvian anchovy) of the birds is complex as it shows strong systematic variations with latitude. The detailed study of a modern profile that represents a few years of guano deposition up to present reveals systematic changes in nitrogen and carbon isotopic composition towards heavier values that increase with age, i.e. depth. Only the uppermost, youngest layers of modern guano show compositional affinity to the prey of the birds. In the profile, the simultaneous loss of nitrogen and carbon occurs by degassing, and non-volatile elements like phosphorous and calcium are passively enriched in the residual guano. Fossil guano deposits are very low in nitrogen and low in carbon contents, and show very heavy nitrogen isotopic compositions. One result of the study is that the use of guano for tracing nitrogen and carbon isotopic and elemental composition in the marine food web of the birds is restricted to fresh material. Despite systematic changes during diagenesis, there is little promise to retrieve reliable values of marine nitrogen and carbon signatures from older guano. However, the changes in isotopic composition from primary marine nitrogen isotopic signatures towards very heavy values generate a compositionally unique material. These compositions trace the presence of guano in natural ecosystems and its use as fertilizer in present and past agriculture. PMID:28594902

Seasonality of Leaf Carbon Isotopic Composition and Leaf Water Isotopic Enrichment in a Mixed Evergreen Forest in Southern California

NASA Astrophysics Data System (ADS)

Santiago, L. S.; Sickman, J. O.; Goulden, M.; DeVan, C.; Pasquini, S. C.; Pivovaroff, A. L.

2011-12-01

Leaf carbon isotopic composition and leaf water isotopic enrichment reflect physiological processes and are important for linking local and regional scale processes to global patterns. We investigated how seasonality affects the isotopic composition of bulk leaf carbon, leaf sugar carbon, and leaf water hydrogen under a Mediterranean climate. Leaf and stem samples were collected monthly from four tree species (Calocedrus decurrens, Pinus lambertiana, Pinus ponderosa, and Quercus chrysolepis) at the James San Jacinto Mountain Reserve in southern California. Mean monthly bulk leaf carbon isotopic composition varied from -34.5 % in P. ponderosa to -24.7 % in P. lambertiana and became more depleted in 13C from the spring to the summer. Mean monthly leaf sugar varied from -29.3 % in P. ponderosa to -21.8 % in P. lambertiana and was enriched in 13C during the winter, spring and autumn, but depleted during the mid-summer. Leaf water hydrogen isotopic composition was 28.4 to 68.8 % more enriched in deuterium than source water and this enrichment was greater as seasonal drought progressed. These data indicate that leaf carbon and leaf water hydrogen isotopic composition provide sensitive measures that connect plant physiological processes to short-term climatic variability.

Isotopic composition of atmospheric moisture from pan water evaporation measurements.

PubMed

Devi, Pooja; Jain, Ashok Kumar; Rao, M Someshwer; Kumar, Bhishm

2015-01-01

A continuous and reliable time series data of the stable isotopic composition of atmospheric moisture is an important requirement for the wider applicability of isotope mass balance methods in atmospheric and water balance studies. This requires routine sampling of atmospheric moisture by an appropriate technique and analysis of moisture for its isotopic composition. We have, therefore, used a much simpler method based on an isotope mass balance approach to derive the isotopic composition of atmospheric moisture using a class-A drying evaporation pan. We have carried out the study by collecting water samples from a class-A drying evaporation pan and also by collecting atmospheric moisture using the cryogenic trap method at the National Institute of Hydrology, Roorkee, India, during a pre-monsoon period. We compared the isotopic composition of atmospheric moisture obtained by using the class-A drying evaporation pan method with the cryogenic trap method. The results obtained from the evaporation pan water compare well with the cryogenic based method. Thus, the study establishes a cost-effective means of maintaining time series data of the isotopic composition of atmospheric moisture at meteorological observatories. The conclusions drawn in the present study are based on experiments conducted at Roorkee, India, and may be examined at other regions for its general applicability.

Stable Isotope Systematics in Grasshopper Assemblages Along an Elevation Gradient, Colorado

NASA Astrophysics Data System (ADS)

Kohn, M. J.; Evans, S.; Dean, J.; Nufio, C.

2012-12-01

Insects comprise over three quarters of all animal species, yet studies of body water isotopic composition are limited to only the cockroach, the hoverfly, and chironomid flies. These studies suggest that oxygen and hydrogen isotopic compositions in body water are primarily controlled by dietary water sources, with modification from respiratory and metabolic processes. In particular, outward diffusion of isotopically depleted water vapor through insect spiracles at low humidity enriches residual body water in 18O and 2H (D). Stable isotope compositions (δ18O and δD) also respond to gradients in elevation and humidity, but these influences remain poorly understood. In this study, we measured grasshopper body water and local vegetation isotopic compositions along an elevation gradient in Colorado to evaluate three hypotheses: 1) Insect body water isotopic composition is directly related to food source water composition 2) Water vapor transport alters body water isotopic compositions relative to original diet sources, and 3) Elevation gradients influence isotopic compositions in insect body water. Thirty-five species of grasshopper were collected from 14 locations in Colorado grasslands, ranging in elevation from 450 to 800 meters (n=131). Body water was distilled from previously frozen grasshopper specimens using a vacuum extraction line, furnaces (90 °C), and liquid nitrogen traps. Water samples were then analyzed for δ18O and δD on an LGR Liquid Water Isotope Analyzer, housed in the Department of Geosciences, Boise State University. Grasshopper body water isotopic compositions show wide variation, with values ranging between -76.64‰ to +42.82‰ in δD and -3.06‰ to +26.78‰ in δ18O. Precipitation δ18O values over the entire Earth excluding the poles vary by approximately 30‰, comparable to the total range measured in our single study area. Most grasshopper values deviate from the global meteoric water line relating δ18O and δD in precipitation, consistent with evaporative enrichment in food (plants) due to plant transpiration. However, grasshopper body water from any given location is further enriched in 18O and D relative to food. Isotopic values decrease slightly with increasing elevation, but some specific grasshopper species appear more sensitive to elevation. Overall, evaporative enrichment of 18O and D in this relatively dry environment appears the strongest factors influencing grasshopper compositions.

Process for making a ceramic composition for immobilization of actinides

DOEpatents

Ebbinghaus, Bartley B.; Van Konynenburg, Richard A.; Vance, Eric R.; Stewart, Martin W.; Walls, Philip A.; Brummond, William Allen; Armantrout, Guy A.; Herman, Connie Cicero; Hobson, Beverly F.; Herman, David Thomas; Curtis, Paul G.; Farmer, Joseph

2001-01-01

Disclosed is a process for making a ceramic composition for the immobilization of actinides, particularly uranium and plutonium. The ceramic is a titanate material comprising pyrochlore, brannerite and rutile. The process comprises oxidizing the actinides, milling the oxides to a powder, blending them with ceramic precursors, cold pressing the blend and sintering the pressed material.

Nitrogen Isotope Evidence for a Shift in Eastern Beringian Nitrogen Cycle after the Terminal Pleistocene

NASA Astrophysics Data System (ADS)

Tahmasebi, F.; Longstaffe, F. J.; Zazula, G.

2016-12-01

The loess deposits of eastern Beringia, a region in North America between 60° and 70°N latitude and bounded by Chukchi Sea to the west and the Mackenzie River to the east, are a magnificent repository of Late Pleistocene megafauna fossils. The stable carbon and nitrogen isotope compositions of these fossils are measured to determine the paleodiet of these animals, and hence the paleoenvironment of this ecosystem during the Quaternary. For this approach to be most successful, however, requires consideration of possible changes in nutrient cycling and hence the carbon and nitrogen isotopic compositions of vegetation in this ecosystem. To test for such a shift following the terminal Pleistocene, we analyzed the stable carbon and nitrogen isotope compositions of modern plants and bone collagen of Arctic ground squirrels from Yukon Territory, and fossil plants and bones recovered from Late Pleistocene fossil Arctic ground squirrel nests. The data for modern samples provided a measure of the isotopic fractionation between ground squirrel bone collagen and their diet. The over-wintering isotopic effect of decay on typical forage grasses was also measured to evaluate its role in determining fossil plant isotopic compositions. The grasses showed only a minor change ( 0-1 ‰) in carbon isotope composition, but a major change ( 2-10 ‰) in nitrogen isotope composition over the 317-day experiment. Based on the modern carbon isotope fractionation between ground squirrel bone collagen and their diet, the modern vegetation carbon isotopic baseline provides a suitable proxy for the Late Pleistocene of eastern Beringia, after accounting for the Suess effect. However, the predicted nitrogen isotope composition of vegetation comprising the diet of fossil ground squirrels remains 2.5 ‰ higher than modern grasslands in this area, even after accounting for possible N-15 enrichment during decay. This result suggests a change in N cycling in this region since the Late Pleistocene.

Thallium isotope composition of the upper continental crust and rivers - An investigation of the continental sources of dissolved marine thallium

USGS Publications Warehouse

Nielsen, S.G.; Rehkamper, M.; Porcelli, D.; Andersson, P.; Halliday, A.N.; Swarzenski, P.W.; Latkoczy, C.; Gunther, D.

2005-01-01

The thallium (Tl) concentrations and isotope compositions of various river and estuarine waters, suspended riverine particulates and loess have been determined. These data are used to evaluate whether weathering reactions are associated with significant Tl isotope fractionation and to estimate the average Tl isotope composition of the upper continental crust as well as the mean Tl concentration and isotope composition of river water. Such parameters provide key constraints on the dissolved Tl fluxes to the oceans from rivers and mineral aerosols. The Tl isotope data for loess and suspended riverine detritus are relatively uniform with a mean of ??205Tl = -2.0 ?? 0.3 (??205Tl represents the deviation of the 205Tl/203Tl isotope ratio of a sample from NIST SRM 997 Tl in parts per 104). For waters from four major and eight smaller rivers, the majority were found to have Tl concentrations between 1 and 7 ng/kg. Most have Tl isotope compositions very similar (within ??1.5 ??205Tl) to that deduced for the upper continental crust, which indicates that no significant Tl isotope fractionation occurs during weathering. Based on these results, it is estimated that rivers have a mean natural Tl concentration and isotope composition of 6 ?? 4 ng/kg and ??205Tl = -2.5 ?? 1.0, respectively. In the Amazon estuary, both additions and losses of Tl were observed, and these correlate with variations in Fe and Mn contents. The changes in Tl concentrations have much lower amplitudes, however, and are not associated with significant Tl isotope effects. In the Kalix estuary, the Tl concentrations and isotope compositions can be explained by two-component mixing between river water and a high-salinity end member that is enriched in Tl relative to seawater. These results indicate that Tl can display variable behavior in estuarine systems but large additions and losses of Tl were not observed in the present study. Copyright ?? 2005 Elsevier Ltd.

Deciphering the iron isotope message of the human body

NASA Astrophysics Data System (ADS)

Walczyk, Thomas; von Blanckenburg, Friedhelm

2005-04-01

Mass-dependent variations in isotopic composition are known since decades for the light elements such as hydrogen, carbon or oxygen. Multicollector-inductively coupled plasma mass spectrometry (MC-ICP-MS) and double-spike thermal ionization mass spectrometry (TIMS) permit us now to resolve small variations in isotopic composition even for the heavier elements such as iron. Recent studies on the iron isotopic composition of human blood and dietary iron sources have shown that lighter iron isotopes are enriched along the food chain and that each individual bears a certain iron isotopic signature in blood. To make use of this finding in biomedical research, underlying mechanisms of isotope fractionation by the human body need to be understood. In this paper available iron isotope data for biological samples are discussed within the context of isotope fractionation concepts and fundamental aspects of human iron metabolism. This includes evaluation of new data for body tissues which show that blood and muscle tissue have a similar iron isotopic composition while heavier iron isotopes are concentrated in the liver. This new observation is in agreement with our earlier hypothesis of a preferential absorption of lighter iron isotopes by the human body. Possible mechanisms for inducing an iron isotope effect at the cellular and molecular level during iron uptake are presented and the potential of iron isotope effects in human blood as a long-term measure of dietary iron absorption is discussed.

Tooth enamel maturation reequilibrates oxygen isotope compositions and supports simple sampling methods

NASA Astrophysics Data System (ADS)

Trayler, Robin B.; Kohn, Matthew J.

2017-02-01

Oxygen isotope and major element zoning patterns of several disparate ungulate teeth were collected to evaluate the timing and geometry of enamel formation, records of isotope zoning, and tooth enamel sampling strategies. Isotopic zoning in mammalian tooth enamel encodes a sub-annual time series of isotopic variation of an animal's body water composition, with a damping factor that depends on the specifics of how enamel mineralizes. Enamel formation comprises two stages: precipitation of appositional enamel with a high CO3:PO4 ratio, followed by precipitation of maturational enamel with a lower CO3:PO4. If appositional and maturational enamel both contribute to isotope compositions (but with different CO3:PO4), and if isotope compositions vary seasonally, paired δ18O values from CO3 and PO4 profiles should show a spatial separation. CO3 isotope patterns should be shifted earlier seasonally than PO4 isotope patterns. Such paired profiles for new and published data show no resolvable shifts, i.e. CO3 and PO4 δ18O profiles show coincident maxima and minima. This coincidence suggests that enamel maturation reequilibrates appositional isotope compositions. If enamel maturation establishes enamel isotope compositions, the geometry of maturation, not apposition, should be considered when devising sampling protocols. X-ray maps of Ca zoning show that the majority of enamel (inner and middle layers) mineralizes heavily at a high angle to the external tooth surface and the enamel-dentine junction over length scales of 2-4 mm, while the outer enamel surface mineralizes more slowly. These data suggest that isotopic sampling strategies should parallel maturational geometry and focus on interior enamel to improve data fidelity. The magnitude of isotopic damping is also smaller than implied in previous studies, so tooth enamel zoning more closely reflects original body water isotopic variations than previously assumed.

Lead isotope compositions of Late Cretaceous and early Tertiary igneous rocks and sulfide minerals in Arizona: Implications for the sources of plutons and metals in porphyry copper deposits

USGS Publications Warehouse

Bouse, R.M.; Ruiz, J.; Titley, S.R.; Tosdal, R.M.; Wooden, J.L.

1999-01-01

Porphyry copper deposits in Arizona are genetically associated with Late Cretaceous and early Tertiary igneous complexes that consist of older intermediate volcanic rocks and younger intermediate to felsic intrusions. The igneous complexes and their associated porphyry copper deposits were emplaced into an Early Proterozoic basement characterized by different rocks, geologic histories, and isotopic compositions. Lead isotope compositions of the Proterozoic basement rocks define, from northwest to southeast, the Mojave, central Arizona, and southeastern Arizona provinces. Porphyry copper deposits are present in each Pb isotope province. Lead isotope compositions of Late Cretaceous and early Tertiary plutons, together with those of sulfide minerals in porphyry copper deposits and of Proterozoic country rocks, place important constraints on genesis of the magmatic suites and the porphyry copper deposits themselves. The range of age-corrected Pb isotope compositions of plutons in 12 Late Cretaceous and early Tertiary igneous complexes is 206Pb/204Pb = 17.34 to 22.66, 207Pb/204Pb = 15.43 to 15.96, and 208Pb/204Pb = 37.19 to 40.33. These Pb isotope compositions and calculated model Th/U are similar to those of the Proterozoic rocks in which the plutons were emplaced, thereby indicating that Pb in the younger rocks and ore deposits was inherited from the basement rocks and their sources. No Pb isotope differences distinguish Late Cretaceous and early Tertiary igneous complexes that contain large economic porphyry copper deposits from less rich or smaller deposits that have not been considered economic for mining. Lead isotope compositions of Late Cretaceous and early Tertiary plutons and sulfide minerals from 30 metallic mineral districts, furthermore, require that the southeastern Arizona Pb province be divided into two subprovinces. The northern subprovince has generally lower 206Pb/204Pb and higher model Th/U, and the southern subprovince has higher 206Pb/204Pb and lower model Th/U. These Pb isotope differences are inferred to result from differences in their respective post-1.7 Ga magmatic histories. Throughout Arizona, Pb isotope compositions of Late Cretaceous and early Tertiary plutons and associated sulfide minerals are distinct from those of Jurassic plutons and also middle Tertiary igneous rocks and sulfide minerals. These differences most likely reflect changes in tectonic setting and magmatic sources. Within Late Cretaceous and early Tertiary igneous complexes that host economic porphyry copper deposits, there is commonly a decrease in Pb isotope composition from older to younger plutons. This decrease in Pb isotope values with time suggests an increasing involvement of crust with lower U/Pb than average crust in the source(s) of Late Cretaceous and early Tertiary magmas. Lead isotope compositions of the youngest porphyries in the igneous complexes are similar to those in most sulfide minerals within the associated porphyry copper deposit. This Pb isotope similarity argues for a genetic link between them. However, not all Pb in the sulfide minerals in porphyry copper deposits is magmatically derived. Some sulfide minerals, particularly those that are late stage, or distal to the main orebody, or in Proterozoic or Paleozoic rocks, have elevated Pb isotope compositions displaced toward the gross average Pb isotope composition of the local country rocks. The more radiogenic isotopic compositions argue for a contribution of Pb from those rocks at the site of ore deposition. Combining the Pb isotope data with available geochemical, isotopic, and petrologic data suggests derivation of the young porphyry copper-related plutons, most of their Pb, and other metals from a hybridized lower continental crustal source. Because of the likely involvement of subduction-related mantle-derived basaltic magma in the hybridized lower crustal source, an indiscernible mantle contribution is probable in the porphyry magmas. Clearly, in addition

Isotopic Compositions of the Elements, 2001

NASA Astrophysics Data System (ADS)

Böhlke, J. K.; de Laeter, J. R.; De Bièvre, P.; Hidaka, H.; Peiser, H. S.; Rosman, K. J. R.; Taylor, P. D. P.

2005-03-01

The Commission on Atomic Weights and Isotopic Abundances of the International Union of Pure and Applied Chemistry completed its last review of the isotopic compositions of the elements as determined by isotope-ratio mass spectrometry in 2001. That review involved a critical evaluation of the published literature, element by element, and forms the basis of the table of the isotopic compositions of the elements (TICE) presented here. For each element, TICE includes evaluated data from the "best measurement" of the isotope abundances in a single sample, along with a set of representative isotope abundances and uncertainties that accommodate known variations in normal terrestrial materials. The representative isotope abundances and uncertainties generally are consistent with the standard atomic weight of the element Ar(E) and its uncertainty U[Ar(E)] recommended by CAWIA in 2001.

[High-precision in situ analysis of the lead isotopic composition in copper using femtosecond laser ablation MC-ICP-MS and the application in ancient coins].

PubMed

Chen, Kai-Yun; Fan, Chao; Yuan, Hong-Lin; Bao, Zhi-An; Zong, Chun-Lei; Dai, Meng-Ning; Ling, Xue; Yang, Ying

2013-05-01

In the present study we set up a femtosecond laser ablation MC-ICP-MS method for lead isotopic analysis. Pb isotopic composition of fifteen copper (brass, bronze) standard samples from the National Institute of Standards Material were analyzed using the solution method (MC-ICP-MS) and laser method (fLA-MC-ICPMS) respectively, the results showed that the Pb isotopic composition in CuPb12 (GBW02137) is very homogeneous, and can be used as external reference material for Pb isotopic in situ analysis. On CuPb12 112 fLA-MC-ICPMS Pb isotope analysis, the weighted average values of the Pb isotopic ratio are in good agreement with the results analyzed by bulk solution method within 2sigma error, the internal precision RSEs of the 208 Pb/204 Pb ratio and 207 Pb/206 Pb ratio are less than 90 and 40 ppm respectively, and the external precision RSDs of them are less than 60 and 30 ppm respectively. Pb isotope of thirteen ancient bronze coins was analyzed via fLA-MC-ICPMS, the results showed that the Pb isotopic composition of ancient coins of different dynasties is significantly different, and not all the Pb isotopic compositions in the coins even from the same dynasty are in agreement with each other.

Nuclear Fuel Reprocessing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harold F. McFarlane; Terry Todd

2013-11-01

Reprocessing is essential to closing nuclear fuel cycle. Natural uranium contains only 0.7 percent 235U, the fissile (see glossary for technical terms) isotope that produces most of the fission energy in a nuclear power plant. Prior to being used in commercial nuclear fuel, uranium is typically enriched to 3–5% in 235U. If the enrichment process discards depleted uranium at 0.2 percent 235U, it takes more than seven tonnes of uranium feed to produce one tonne of 4%-enriched uranium. Nuclear fuel discharged at the end of its economic lifetime contains less one percent 235U, but still more than the natural ore.more » Less than one percent of the uranium that enters the fuel cycle is actually used in a single pass through the reactor. The other naturally occurring isotope, 238U, directly contributes in a minor way to power generation. However, its main role is to transmute into plutoniumby neutron capture and subsequent radioactive decay of unstable uraniumand neptuniumisotopes. 239Pu and 241Pu are fissile isotopes that produce more than 40% of the fission energy in commercially deployed reactors. It is recovery of the plutonium (and to a lesser extent the uranium) for use in recycled nuclear fuel that has been the primary focus of commercial reprocessing. Uraniumtargets irradiated in special purpose reactors are also reprocessed to obtain the fission product 99Mo, the parent isotope of technetium, which is widely used inmedical procedures. Among the fission products, recovery of such expensive metals as platinum and rhodium is technically achievable, but not economically viable in current market and regulatory conditions. During the past 60 years, many different techniques for reprocessing used nuclear fuel have been proposed and tested in the laboratory. However, commercial reprocessing has been implemented along a single line of aqueous solvent extraction technology called plutonium uranium reduction extraction process (PUREX). Similarly, hundreds of types of reactor fuels have been irradiated for different purposes, but the vast majority of commercial fuel is uranium oxide clad in zirconium alloy tubing. As a result, commercial reprocessing plants have relatively narrow technical requirements for used nuclear that is accepted for processing.« less

Statistical clumped isotope signatures

PubMed Central

Röckmann, T.; Popa, M. E.; Krol, M. C.; Hofmann, M. E. G.

2016-01-01

High precision measurements of molecules containing more than one heavy isotope may provide novel constraints on element cycles in nature. These so-called clumped isotope signatures are reported relative to the random (stochastic) distribution of heavy isotopes over all available isotopocules of a molecule, which is the conventional reference. When multiple indistinguishable atoms of the same element are present in a molecule, this reference is calculated from the bulk (≈average) isotopic composition of the involved atoms. We show here that this referencing convention leads to apparent negative clumped isotope anomalies (anti-clumping) when the indistinguishable atoms originate from isotopically different populations. Such statistical clumped isotope anomalies must occur in any system where two or more indistinguishable atoms of the same element, but with different isotopic composition, combine in a molecule. The size of the anti-clumping signal is closely related to the difference of the initial isotope ratios of the indistinguishable atoms that have combined. Therefore, a measured statistical clumped isotope anomaly, relative to an expected (e.g. thermodynamical) clumped isotope composition, may allow assessment of the heterogeneity of the isotopic pools of atoms that are the substrate for formation of molecules. PMID:27535168

The Manhattan Project; A very brief introduction to the physics of nuclear weapons

NASA Astrophysics Data System (ADS)

Reed, B. Cameron

2017-05-01

The development of nuclear weapons by the Manhattan Project during World War II was one of the most dramatic scientific/technological episodes in human history. This book, prepared by a recognized expert on the Manhattan Project, offers a concise survey of the essential physics concepts underlying fission weapons. The text describes the energetics and timescales of fast-neutron chain reactions, why only certain isotopes of uranium and plutonium are suitable for use in fission weapons, how critical mass and bomb yield can be estimated, how the efficiency of nuclear weapons can be enhanced, how the fissile forms of uranium and plutonium were obtained, some of the design details of the 'Little Boy' and 'Fat Man' bombs, and some of the thermal, shock, and radiation effects of nuclear weapons. Calculation exercises are provided, and a Bibliography lists authoritative print and online sources of information for readers who wish to pursue more detailed study of this fascinating topic.

Neutron Radiation Characteristics of Plutonium Dioxide Fuel

NASA Technical Reports Server (NTRS)

Taherzadeh, M.

1972-01-01

The major sources of neutrons from plutonium dioxide nuclear fuel are considered in detail. These sources include spontaneous fission of several of the Pu isotopes, reactions with low Z impurities in the fuel, and reactions with O-18. For spontaneous fission neutrons a value of (1.95 plus or minus 0.07) X 1,000 n/s/q PuO2 is obtained. The neutron yield from (alpha, neutron) reactions with oxygen is calculated by integrating the reaction rate equation over all alpha particle energies and all center-of-mass angles. The results indicate a neutron emission rate of (1.42 plus or minus 0.32) X 10,000 n/s/q PuO2. The neutron yield from (alpha, neutron) reactions with low Z impurities in the fuel is presented in tabular form for one part per million of each impurity. The total neutron flux emitted from a particular fuel geometry is estimated by adding the neutron yield due to the induced fission to the other neutron sources.

Interim Safe Storage of Plutonium Production Reactors at the US DOE Hanford Site - 13438

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schilperoort, Daryl L.; Faulk, Darrin

2013-07-01

Nine plutonium production reactors located on DOE's Hanford Site are being placed into an Interim Safe Storage (ISS) period that extends to 2068. The Environmental Impact Statement (EIS) for ISS [1] was completed in 1993 and proposed a 75-year storage period that began when the EIS was finalized. Remote electronic monitoring of the temperature and water level alarms inside the safe storage enclosure (SSE) with visual inspection inside the SSE every 5 years are the only planned operational activities during this ISS period. At the end of the ISS period, the reactor cores will be removed intact and buried inmore » a landfill on the Hanford Site. The ISS period allows for radioactive decay of isotopes, primarily Co-60 and Cs-137, to reduce the dose exposure during disposal of the reactor cores. Six of the nine reactors have been placed into ISS by having an SSE constructed around the reactor core. (authors)« less

Spatial patterns of throughfall isotopic composition at the event and seasonal timescales

Treesearch

Scott T. Allen; Richard F. Keim; Jeffrey J. McDonnell

2015-01-01

Spatial variability of throughfall isotopic composition in forests is indicative of complex processes occurring in the canopy and remains insufficiently understood to properly characterize precipitation inputs to the catchment water balance. Here we investigate variability of throughfall isotopic composition with the objectives: (1) to quantify the spatial variability...

The Effects of Core Composition on Iron Isotope Fractionation During Planetary Differentiation

NASA Astrophysics Data System (ADS)

Elardo, S. M.; Shahar, A.; Caracas, R.; Mock, T. D.; Sio, C. K. I.

2018-05-01

High pressure and temperature isotope exchange experiments and density functional theory calculations show how the composition of planetary cores affects the fractionation of iron isotopes during planetary differentiation.

Study on Utilization of Super Grade Plutonium in Molten Salt Reactor FUJI-U3 using CITATION Code

NASA Astrophysics Data System (ADS)

Wulandari, Cici; Waris, Abdul; Pramuditya, Syeilendra; Asril, Pramutadi AM; Novitrian

2017-07-01

FUJI-U3 type of Molten Salt Reactor (MSR) has a unique design since it consists of three core regions in order to avoid the replacement of graphite as moderator. MSR uses floride as a nuclear fuel salt with the most popular chemical composition is LiF-BeF2-ThF4-233UF4. ThF4 and 233UF4 are the fertile and fissile materials, respectively. On the other hand, LiF and BeF2 working as both fuel and heat transfer medium. In this study, the super grade plutonium will be utilized as substitution of 233U since plutonium is easier to be obtained compared to 233U as main fuel. Neutronics calculation was performed by using PIJ and CITATION modules of SRAC 2002 code with JENDL 3.2 as nuclear data library.

Effect of cooling rate on achieving thermodynamic equilibrium in uranium-plutonium mixed oxides

NASA Astrophysics Data System (ADS)

Vauchy, Romain; Belin, Renaud C.; Robisson, Anne-Charlotte; Hodaj, Fiqiri

2016-02-01

In situ X-ray diffraction was used to study the structural changes occurring in uranium-plutonium mixed oxides U1-yPuyO2-x with y = 0.15; 0.28 and 0.45 during cooling from 1773 K to room-temperature under He + 5% H2 atmosphere. We compare the fastest and slowest cooling rates allowed by our apparatus i.e. 2 K s-1 and 0.005 K s-1, respectively. The promptly cooled samples evidenced a phase separation whereas samples cooled slowly did not due to their complete oxidation in contact with the atmosphere during cooling. Besides the composition of the annealing gas mixture, the cooling rate plays a major role on the control of the Oxygen/Metal ratio (O/M) and then on the crystallographic properties of the U1-yPuyO2-x uranium-plutonium mixed oxides.

Inert matrix fuel in dispersion type fuel elements

NASA Astrophysics Data System (ADS)

Savchenko, A. M.; Vatulin, A. V.; Morozov, A. V.; Sirotin, V. L.; Dobrikova, I. V.; Kulakov, G. V.; Ershov, S. A.; Kostomarov, V. P.; Stelyuk, Y. I.

2006-06-01

The advantages of using inert matrix fuel (IMF) as a dispersion fuel in an aluminium alloy matrix are considered, in particular, low temperatures in the fuel centre, achievable high burn-ups, serviceability in transients and an environmentally friendly process of fuel rod fabrication. Two main versions of IMF are under development at A.A. Bochvar Institute, i.e. heterogeneous or isolated distribution of plutonium. The out-of-pile results on IMF loaded with uranium dioxide as plutonium simulator are presented. Fuel elements with uranium dioxide composition fabricated at A.A. Bochvar Institute are currently under MIR tests (RIAR, Dimitrovgrad). The fuel elements reached a burn-up of 88 MW d kg-1 (equivalent to the burn up of the standard uranium dioxide pelletized fuel) without loss of leak-tightness of the cladding. The feasibility of fabricating IMF of these particular types with plutonium dioxide is considered with a view to in-pile irradiation.

Weathering and vegetation controls on nickel isotope fractionation in surface ultramafic environments (Albania)

NASA Astrophysics Data System (ADS)

Estrade, Nicolas; Cloquet, Christophe; Echevarria, Guillaume; Sterckeman, Thibault; Deng, Tenghaobo; Tang, YeTao; Morel, Jean-Louis

2015-08-01

The dissolved nickel (Ni) isotopic composition of rivers and oceans presents an apparent paradox. Even though rivers represent a major source of Ni in the oceans, seawater is more enriched in the heavier isotopes than river-water. Additional sources or processes must therefore be invoked to account for the isotopic budget of dissolved Ni in seawater. Weathering of continental rocks is thought to play a major role in determining the magnitude and sign of isotopic fractionation of metals between a rock and the dissolved product. We present a study of Ni isotopes in the rock-soil-plant systems of several ultramafic environments. The results reveal key insights into the magnitude and the control of isotopic fractionation during the weathering of continental ultramafic rocks. This study introduces new constraints on the influence of vegetation during the weathering process, which should be taken into account in interpretations of the variability of Ni isotopes in rivers. The study area is located in a temperate climate zone within the ophiolitic belt area of Albania. The serpentinized peridotites sampled present a narrow range of heavy Ni isotopic compositions (δ60Ni = 0.25 ± 0.16 ‰, 2SD n = 2). At two locations, horizons within two soil profiles affected by different degrees of weathering all presented light isotopic compositions compared to the parent rock (Δ60Nisoil-rock up to - 0.63 ‰). This suggests that the soil pool takes up the light isotopes, while the heavier isotopes remain in the dissolved phase. By combining elemental and mineralogical analyses with the isotope compositions determined for the soils, the extent of fractionation was found to be controlled by the secondary minerals formed in the soil. The types of vegetation growing on ultramafic-derived soils are highly adapted and include both Ni-hyperaccumulating species, which can accumulate several percent per weight of Ni, and non-accumulating species. Whole-plant isotopic compositions were found to be isotopically heavier than the soil (Δ60Niwhole plant-soil up to 0.40‰). Fractions of Ni extracted by DTPA (diethylenetriaminepentaacetic acid) presented isotopically heavy compositions compared to the soil (Δ60NiDTPA-soil up to 0.89‰), supporting the hypothesis that the dissolved Ni fraction controlled by weathering has a heavy isotope signature. The non-hyperaccumulators (n = 2) were inclined to take up and translocate light Ni isotopes with a large degree of fractionation (Δ60Nileaves-roots up to - 0.60 ‰). For Ni-hyperaccumulators (n = 7), significant isotopic fractionation was observed in the plants in their early growth stages, while no fractionation occurred during later growth stages, when plants are fully loaded with Ni. This suggests that (i) the high-efficiency translocation process involved in hyperaccumulators does not fractionate Ni isotopes, and (ii) the root uptake process mainly controls the isotopic composition of the plant. In ultramafic contexts, vegetation composed of hyperaccumulators can significantly influence isotopic compositions through its remobilization in the upper soil horizon, thereby influencing the isotopic balance of Ni exported to rivers.

Influences on the stable oxygen and carbon isotopes in gerbillid rodent teeth in semi-arid and arid environments: Implications for past climate and environmental reconstruction

NASA Astrophysics Data System (ADS)

Jeffrey, Amy; Denys, Christiane; Stoetzel, Emmanuelle; Lee-Thorp, Julia A.

2015-10-01

The stable isotope composition of small mammal tissues has the potential to provide detailed information about terrestrial palaeoclimate and environments, because their remains are abundant in palaeontological and archaeological sites, and they have restricted home ranges. Applications to the Quaternary record, however, have been sparse and limited by an acute lack of understanding of small mammal isotope ecology, particularly in arid and semi-arid environments. Here we document the oxygen and carbon isotope composition of Gerbillinae (gerbil) tooth apatite across a rainfall gradient in northwestern Africa, in order to test the relative influences of the 18O/16O in precipitation or moisture availability on gerbil teeth values, the sensitivity of tooth apatite 13C/12C to plant responses to moisture availability, and the influence of developmental period on the isotopic composition of gerbil molars and incisors. The results show that the isotopic composition of molars and incisors from the same individuals differs consistent with the different temporal periods reflected by the teeth; molar teeth are permanently rooted and form around the time of birth, whereas incisors grow continuously. The results indicate that tooth choice is an important consideration for applications as proxy Quaternary records, but also highlights a new potential means to distinguish seasonal contexts. The oxygen isotope composition of gerbil tooth apatite is strongly correlated with mean annual precipitation (MAP) below 600 mm, but above 600 mm the teeth reflect the oxygen isotope composition of local meteoric water instead. Predictably, the carbon isotope composition of the gerbil teeth reflected C3 and C4 dietary inputs, however arid and mesic sites could not be distinguished because of the high variability displayed in the carbon isotope composition of the teeth due to the microhabitat and short temporal period reflected by the gerbil. We show that the oxygen isotope composition of small mammal teeth strongly reflects moisture availability in semi-arid and arid environments and would provide an excellent record of palaeo-aridity in a terrestrial setting. The results illustrate that an understanding of an animal's physiology is essential for interpreting the animal's isotopic responses to external contexts, especially in arid zones.

Stable lead isotopic analyses of historic and contemporary lead contamination of San Francisco Bay estuary

USGS Publications Warehouse

Ritson, P.I.; Bouse, R.M.; Flegal, A.R.; Luoma, S.N.

1999-01-01

Variations in stable lead isotopic composition (240Pb, 206Pb, 207Pb, 208Pb) in three sediment cores from the San Francisco Bay estuary document temporal changes in sources of lead during the past two centuries. Sediment, with lead from natural geologic sources, and relatively homogeneous lead isotopic compositions are overlain by sediments whose isotopic compositions indicate change in the sources of lead associated with anthropogenic modification of the estuary. The first perturbations of lead isotopic composition in the cores occur in the late 1800s concordant with the beginning of industrialization around the estuary. Large isotopic shifts, toward lower 206Pb/207Pb, occur after the turn of the century in both Richardson and San Pablo Bays. A similar relationship among lead isotopic compositions and lead concentrations in both Bays suggest contamination from the same source (a lead smelter). The uppermost sediments (post 1980) of all cores also have a relatively homogenous lead isotopic composition distinct from pre-anthropogenic and recent aerosol signatures. Lead isotopic compositions of leachates from fourteen surface sediments and five marsh samples from the estuary were also analyzed. These analyses suggest that the lead isotopic signature identified in the upper horizons of the cores is spatially homogeneous among recently deposited sediments throughout the estuary. Current aerosol lead isotopic compositions [Smith, D.R., Niemeyer, S., Flegal, A.R., 1992. Lead sources to California sea otters: industrial inputs circumvent natural lead biodepletion mechanisms. Environmental Research 57, 163-175] are distinct from the isotopic compositions of the surface sediments, suggesting that the major source of lead is cycling of historically contaminated sediments back through the water column. Both the upper core sediments and surface sediments apparently derive their lead predominantly from sources internal to the estuary. These results support the idea that geochemical cycling of lead between sediments and water accounts for persistently elevated lead concentrations in the water column despite 10-fold reduction of external source inputs to San Francisco Bay [Flegal, A.R., Rivera-Duarte, I., Ritson, P.I., Scelfo, G., Smith, G.J., Gordon, M., Sanudo-Wilhelmy, S.A., 1996. Metal contamination in San Francisco Waters: historic perturbations, contemporary concentrations, and future considerations in San Francisco Bay. In: Hollobaugh, J.T. (Ed.), The Ecosystem. AAAS, pp. 173-188].

Test results of a new detector system for gamma ray isotopic measurements

DOE Office of Scientific and Technical Information (OSTI.GOV)

Malcom, J.E.; Bonner, C.A.; Hurd, J.R.

1993-08-01

A new type of gamma-ray detector system for isotopic measurements has been developed. This new system, a ``Duo detector`` array, consists of two intrinsic germanium detectors, a planar followed by a coaxial mounted on the same axis within a single cryostat assembly. This configuration allows the isotopic analysis system to take advantage of spectral data results that are collected simultaneously from different gamma-ray energy regimes. Princeton Gamma Tech (PGT) produced several prototypes of this Duo detector array which were then tested by Rocky Flats personnel until the design was optimized. An application for this detector design is in automated, roboticizedmore » NDA systems such as those being developed at the Los Alamos TA-55 Plutonium Facility. The Duo detector design reduces the space necessary for the isotopic instrument by a factor of two (only one liquid nitrogen dewar is needed), and also reduces the complexity of the mechanical systems and controlling software. Data will be presented on measurements of nuclear material with a Duo detector for a wide variety of matrices. Results indicate that the maximum count rate can be increased up to 100,000 counts per second yet maintaining excellent resolution and energy rate product.« less

Isotopic compositions of the elements, 2001

USGS Publications Warehouse

Böhlke, J.K.; De Laeter, J. R.; De Bievre, P.; Hidaka, H.; Peiser, H.S.; Rosman, K.J.R.; Taylor, P.D.P.

2005-01-01

The Commission on Atomic Weights and Isotopic Abundances of the International Union of Pure and Applied Chemistry completed its last review of the isotopic compositions of the elements as determined by isotope-ratio mass spectrometry in 2001. That review involved a critical evaluation of the published literature, element by element, and forms the basis of the table of the isotopic compositions of the elements (TICE) presented here. For each element, TICE includes evaluated data from the “best measurement” of the isotope abundances in a single sample, along with a set of representative isotope abundances and uncertainties that accommodate known variations in normal terrestrial materials. The representative isotope abundances and uncertainties generally are consistent with the standard atomic weight of the element Ar(E)">Ar(E)Ar(E) and its uncertainty U[Ar(E)]">U[Ar(E)]U[Ar(E)] recommended by CAWIA in 2001.

Calcium Isotopic Compositions of Forearc Sediments from DSDP Site 144

NASA Astrophysics Data System (ADS)

Zhang, Z.; Zhu, H.; Nan, X.; Li, X.; Huang, F.

2016-12-01

It is important to investigate calcium isotopic compositions of reservoirs of the Earth for better application of Ca isotopes into studies of a variety of geochemical problems. Because Ca isotopic compositions for igneous rocks and carbonates are increasingly reported, this maybe bring new requirements on carefully understanding the isotopic compositions of subducted marine sediments. Marine sediments mainly contains carbonates and clays, controlling the compositions of slab-derived materials which are added to the mantle wedge. Obviously, it could have different elemental and calcium isotopic compositions with marine carbonate. Thus, it could also put biases on calcium isotopic signatures of basalts resulted from recycling oceanic carbonate into the mantle. Here, we report calcium isotopic compositions of 17 sediment samples from Deep Sea Drilling Project (DSDP) site 144 (09°27.23' N, 54°20.52' W) which is located about 400 km north of Surinam on the northern flank of the Demerara Rise with a water depth of 2957 meters. These samples have CaO contents ranging from 14.56 wt.% to 41.46 wt.% with an average of 29.61 ± 18.21 (2SD), δ44/40Ca ranges from 0.19 to 0.58 (relative to SRM915a) with an average of 0.40 ± 0.22 (2SD). These carbonate-rich sediments can be used to represent an endmember with high CaO content and low δ44/40Ca, which could modify chemical composition of the upper mantle and subduction zone lavas if they are recycled to the convective mantle during subduction. The positive linear correlation between CaO and δ44/40Ca in the sediments cannot be explained by a simple mixing between marine carbonate and clay. Instead, δ44/40Ca of these samples roughly increase from the Upper Cretaceous to the Early Oligocene, which might reflect the evolution of calcium isotopic compositions of seawater through time.

Oxygen Isotopic Analyses of Water Extracted from the Martian Meteorite NWA 7034

NASA Astrophysics Data System (ADS)

Nunn, M.; Agee, C. B.; Thiemens, M. H.

2012-12-01

Introduction: The NWA 7034 meteorite has been identified as Martian, but it is distinct from the Shergottite-Nakhlite-Chassignite (SNC) grouping of meteorites in its petrology (it is the only known Martian basaltic breccia) and bulk silicate oxygen isotopic composition (Δ17O = 0.56 ± 0.06 ‰, where Δ17O = δ17O - 0.528 x δ18O, compared to the average SNC Δ17O ≈ 0.3 ‰) [e.g., 1-2]. We report here measurements of the oxygen isotopic composition of water extracted from NWA 7034 by stepwise heating. Methods: A piece (~1.2g) of NWA 7034 was pumped to vacuum until outgassing had stopped before heating to 50, 150, 320, 500, and 1000°C. The sample was maintained at each temperature step for at least one hour while collecting evolved volatiles in a liquid nitrogen cold trap. Water was selectively converted to molecular oxygen, the oxygen isotopic composition of which was then measured on a double collecting isotope ratio mass spectrometer. Results: Our stepwise heating experiments indicate NWA 7034 contains 3330ppm water, and this water has an average oxygen isotopic composition of Δ17O = 0.330 ± 0.011‰. The oxygen isotopic composition of water in NWA 7034 is unlike that of the silicates from which it is extracted (Δ17O = 0.56 ± 0.06 ‰) but is comparable to the average SNC silicate composition (Δ17O ≈ 0.3 ‰). However, there is no consensus on the oxygen isotopic composition of water in SNCs because aliquots of water extracted from different samples (separate pieces of a single meteorite or from different meteorites) have different oxygen isotopic compositions [3]. Furthermore, carbonates and sulfates extracted from SNCs also possess distinct oxygen isotopic compositions [4]. The variation in oxygen isotopic composition among these phases most likely results from the existence of isotopically distinct oxygen reservoirs on Mars that were not equilibrated. On Earth, interaction of ozone (O3) and carbon dioxide (CO2) leads to a mass independent oxygen isotopic composition of atmospheric CO2 [5]. This anomaly is transferred by exchange from CO2 to water and subsequently to secondary minerals. The much larger CO2 to water ratio on Mars could allow this process to introduce a measurable oxygen isotopic anomaly to sulfates, carbonates, and water. The magnitude and variability of this anomaly would depend on the formation mechanism of the species (particularly the source of oxygen), as is consistent with measurements to date of phases in SNCs. References: [1] Franchi, I.A., et al. (1999) MAPS 34, 657-661. [2] Rumble, D. and Irving, A.J. (2009) LPSC XXXX, #2293 [3] Karlsson, H.R., et al. (1992) Science 255, 1409-1411. [4] Farquhar, J. and Thiemens, M.H. (2000) J. Geophys. Res. 105, 11991-11997. [5] Yung, Y.L., et al. (1991) Geophys. Res. Lett. 18, 13-16.

Radioactivity levels in major French rivers: summary of monitoring chronicles acquired over the past thirty years and current status.

PubMed

Eyrolle, Frédérique; Claval, David; Gontier, Gilles; Antonelli, Christelle

2008-07-01

Since the beginning of the 1990 s, liquid releases of gamma-emitting radionuclides from French nuclear facilities have generally fallen by almost 85%. Almost 65% of gamma-emitting liquid effluents released into freshwater rivers concerned the River Rhône (Southeast France), with around 85% of this originating from the Marcoule spent fuel reprocessing plant. Upstream of French nuclear plants, artificial radionuclides still detected by gamma spectrometry in 2006, include (137)Cs, (131)I as well as (60)Co, (58)Co and (54)Mn in the case of the Rhine (Switzerland nuclear industries). In the wake of the fallout from the Chernobyl accident, (103)Ru, (106)Rh-Ru, (110 m)Ag, (141)Ce and (129)Te were detected in rivers in the east of France. Some of these radionuclides were found in aquatic plants until 1989. In eastern France, (137)Cs activity in river sediments and mosses is still today two to three times greater than that observed in similar environments in western France. No (134)Cs has been detected upstream of nuclear plants in French rivers since 2001. Downstream of nuclear plants, the gamma emitters still detected regularly in rivers in 2006 are (137)Cs, (134)Cs, (60)Co, (58)Co, (110 m)Ag, (54)Mn, (131)I, together with (241)Am downstream of the Marcoule spent fuel reprocessing plant. Alpha and beta emitters such as plutonium isotopes and (90)Sr first entered freshwaters at the early 1950s due to the leaching of soils contaminated by atmospheric fallout from nuclear testing. These elements were also introduced, in the case of the Rhône River, via effluent from the Marcoule reprocessing plant. Until the mid 1990 s, plutonium isotope levels observed in the lower reaches of the Rhône were 10 to 1000 times higher than those observed in other French freshwaters. Data gathered over a period of almost thirty years of radioecological studies reveal that the only radionuclides detected in fish muscles are (137)Cs, (90)Sr, plutonium isotopes and (241)Am. At the scale of the French territory, there is no significant difference since the mid 1990 s between (137)Cs activity observed downstream of nuclear facilities and that observed upstream, whether in sediments, mosses and fish. Finally, this study highlights that the natural radioactivity of surface freshwaters are around 25 times greater than artificial radioactivity from gamma emitters. However, non gamma emitters released by nuclear industries, such as (3)H, may lead to artificial activity levels 2 to 20 times higher than natural levels.

Isotopic Resonance Hypothesis: Experimental Verification by Escherichia coli Growth Measurements

NASA Astrophysics Data System (ADS)

Xie, Xueshu; Zubarev, Roman A.

2015-03-01

Isotopic composition of reactants affects the rates of chemical and biochemical reactions. As a rule, enrichment of heavy stable isotopes leads to progressively slower reactions. But the recent isotopic resonance hypothesis suggests that the dependence of the reaction rate upon the enrichment degree is not monotonous. Instead, at some ``resonance'' isotopic compositions, the kinetics increases, while at ``off-resonance'' compositions the same reactions progress slower. To test the predictions of this hypothesis for the elements C, H, N and O, we designed a precise (standard error +/-0.05%) experiment that measures the parameters of bacterial growth in minimal media with varying isotopic composition. A number of predicted resonance conditions were tested, with significant enhancements in kinetics discovered at these conditions. The combined statistics extremely strongly supports the validity of the isotopic resonance phenomenon (p << 10-15). This phenomenon has numerous implications for the origin of life studies and astrobiology, and possible applications in agriculture, biotechnology, medicine, chemistry and other areas.

[Sources of Methane in the Boreal Region

NASA Technical Reports Server (NTRS)

1998-01-01

In determining the global methane budget the sources of methane must be balanced with the sinks and atmospheric inventory. The approximate contribution of the different methane sources to the budget has been establish showing the major terrestrial inputs as rice, wetlands, bogs, fens, and tundra. Measurements and modeling of production in these sources suggest that temperature, water table height and saturation along with substratum composition are important in controlling methane production and emission. The isotopic budget of 13 C and D/H in methane can be used as a tool to clarify the global budget. This approach has achieved success at constraining the inputs. Studies using the isotopic approach place constraints on global methane production from different sources. Also, the relation between the two biogenic production pathways, acetate fermentation and CO2 reduction, and the effect of substratum composition can be made using isotope measurements shows the relation between the different biogenic, thermogenic and anthropogenic sources of methane as a function of the carbon and hydrogen isotope values for each source and the atmosphere, tropospheric composition. Methane emissions from ponds and fens are a significant source in the methane budget of the boreal region. An initial study in 1993 and 1994 on the isotopic composition of this methane source and the isotopic composition in relation to oxidation of methane at the sediment surface of the ponds or fen was conducted as part of our BOREAS project. The isotopic composition of methane emitted by saturated anoxic sediment is dependent on the sediment composition and geochemistry, but will be influenced by in situ oxidation, in part, a function of rooted plant activity. The influence of oxidation mediated by rooted plant activities on the isotopic composition of methane is not well known and will depend on the plant type, sediment temperature, and numerous other variables. Information on this isotopic composition is important in both understanding the bio-geochemistry of the system and also in determining the regional and global inputs for the methane isotope budget. In determining the destruction of methane for balancing the atmospheric methane budget soil oxidation must be considered.

Iron isotopic composition of blood serum in anemia of chronic kidney disease.

PubMed

Anoshkina, Yulia; Costas-Rodríguez, Marta; Speeckaert, Marijn; Van Biesen, Wim; Delanghe, Joris; Vanhaecke, Frank

2017-05-24

Chronic kidney disease (CKD) is a general term for disorders that affect the structure and function of the kidneys. Iron deficiency (ID) and anemia occur in the vast majority of CKD patients, most of whom are elderly. However, establishing the cause of anemia in CKD, and therefore making an informed decision concerning the corresponding therapeutic treatment, is still a challenge. High-precision Fe isotopic analysis of blood serum samples of CKD patients with and without ID/anemia was performed via multi-collector inductively coupled plasma-mass spectrometry (MC-ICP-MS) for such a purpose. Patients with CKD and/or iron disorders showed a heavier serum Fe isotopic composition than controls. Many clinical parameters used for the diagnosis and follow-up of anemia correlated significantly with the serum Fe isotopic composition. In contrast, no relation was observed between the serum Fe isotopic composition and the estimated glomerular filtration rate as a measure of kidney function. Among the CKD patients, the serum Fe isotopic composition was substantially heavier in the occurrence of ID anemia, while erythropoietin-related anemia did not exert this effect. The Fe isotopic composition can thus be useful for distinguishing these different types of anemias in CKD patients, i.e. ID anemia vs. erythropoietin-related anemia.

Xenon isotopic composition of the Mid Ocean Ridge Basalt (MORB) source

NASA Astrophysics Data System (ADS)

Peto, M. K.; Mukhopadhyay, S.

2012-12-01

Although convection models do not preclude preservation of smaller mantle regions with more pristine composition throughout Earth's history, it has been widely assumed that the moon forming giant impact likely homogenizes the whole mantle following a magma ocean that extended all the way to the bottom of the mantle. Recent findings of tungsten and xenon heterogeneities in the mantle [1,2,3,4], however, imply that i) the moon forming giant impact may not have homogenized the whole mantle and ii) plate tectonics was inefficient in erasing early formed compositional differences, particularly for the xenon isotopes. Therefore, the xenon isotope composition in the present day mantle still preserves a memory of early Earth processes. However, determination of the xenon isotopic composition of the mantle source is still scarce, since the mantle composition is overprinted by post-eruptive atmospheric contamination in basalts erupted at ocean islands and mid ocean ridges. The xenon composition of the depleted upper mantle has been defined by the gas rich sample, 2πD43 (also known as "popping rock"), from the North Atlantic (13° 469`N). However, the composition of a single sample is not likely to define the composition of the upper mantle, especially since popping rock has an "enriched" trace element composition. We will present Ne, Ar and Xe isotope data on MORB glass samples with "normal" helium isotope composition (8±1 Ra) from the Southeast Indian Ridge, the South Atlantic Ridge, the Sojourn Ridge, the Juan de Fuca, the East Pacific Rise, and the Gakkel Ridge. Following the approach of [1], we correct for syn- and post-eruptive atmosphere contamination, and determine the variation of Ar and Xe isotope composition of the "normal" MORB source. We investigate the effect of atmospheric recycling in the variation of MORB mantle 40Ar/36Ar and 129Xe/130Xe ratios, and attempt to constrain the average upper mantle argon and xenon isotopic compositions. [1] Mukhopadhyay, Nature 2012; [2] Tucker et al., EPSL (in review); [3] Moreira et al., Nature 1998 [4] Touboul et al., Science 2012.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Scott, Bobby R.; Tokarskaya, Zoya B.; Zhuntova, Galina V.

This report summarizes 4 years of research achievements in this Office of Science (BER), U.S. Department of Energy (DOE) project. The research described was conducted by scientists and supporting staff at Lovelace Respiratory Research Institute (LRRI)/Lovelace Biomedical and Environmental Research Institute (LBERI) and the Southern Urals Biophysics Institute (SUBI). All project objectives and goals were achieved. A major focus was on obtaining improved cancer risk estimates for exposure via inhalation to plutonium (Pu) isotopes in the workplace (DOE radiation workers) and environment (public exposures to Pu-contaminated soil). A major finding was that low doses and dose rates of gamma raysmore » can significantly suppress cancer induction by alpha radiation from inhaled Pu isotopes. The suppression relates to stimulation of the body's natural defenses, including immunity against cancer cells and selective apoptosis which removes precancerous and other aberrant cells.« less

POWER REACTOR

DOEpatents

Zinn, W.H.

1958-07-01

A fast nuclear reactor system ls described for producing power and radioactive isotopes. The reactor core is of the heterogeneous, fluid sealed type comprised of vertically arranged elongated tubular fuel elements having vertical coolant passages. The active portion is surrounded by a neutron reflector and a shield. The system includes pumps and heat exchangers for the primary and secondary coolant circuits. The core, primary coolant pump and primary heat exchanger are disposed within an irapenforate tank which is filled with the primary coolant, in this case a liquid metal such as Na or NaK, to completely submerge these elements. The tank is completely surrounded by a thick walled concrete shield. This reactor system utilizes enriched uranium or plutonium as the fissionable material, uranium or thorium as a diluent and thorium or uranium containing less than 0 7% of the U/sup 235/ isotope as a fertile material.

Modelling and intepreting the isotopic composition of water vapour in convective updrafts

NASA Astrophysics Data System (ADS)

Bolot, M.; Legras, B.; Moyer, E. J.

2012-08-01

The isotopic compositions of water vapour and its condensates have long been used as tracers of the global hydrological cycle, but may also be useful for understanding processes within individual convective clouds. We review here the representation of processes that alter water isotopic compositions during processing of air in convective updrafts and present a unified model for water vapour isotopic evolution within undiluted deep convective cores, with a special focus on the out-of-equilibrium conditions of mixed phase zones where metastable liquid water and ice coexist. We use our model to show that a combination of water isotopologue measurements can constrain critical convective parameters including degree of supersaturation, supercooled water content and glaciation temperature. Important isotopic processes in updrafts include kinetic effects that are a consequence of diffusive growth or decay of cloud particles within a supersaturated or subsaturated environment; isotopic re-equilibration between vapour and supercooled droplets, which buffers isotopic distillation; and differing mechanisms of glaciation (droplet freezing vs. the Wegener-Bergeron-Findeisen process). As all of these processes are related to updraft strength, droplet size distribution and the retention of supercooled water, isotopic measurements can serve as a probe of in-cloud conditions of importance to convective processes. We study the sensitivity of the profile of water vapour isotopic composition to differing model assumptions and show how measurements of isotopic composition at cloud base and cloud top alone may be sufficient to retrieve key cloud parameters.

Modelling and interpreting the isotopic composition of water vapour in convective updrafts

NASA Astrophysics Data System (ADS)

Bolot, M.; Legras, B.; Moyer, E. J.

2013-08-01

The isotopic compositions of water vapour and its condensates have long been used as tracers of the global hydrological cycle, but may also be useful for understanding processes within individual convective clouds. We review here the representation of processes that alter water isotopic compositions during processing of air in convective updrafts and present a unified model for water vapour isotopic evolution within undiluted deep convective cores, with a special focus on the out-of-equilibrium conditions of mixed-phase zones where metastable liquid water and ice coexist. We use our model to show that a combination of water isotopologue measurements can constrain critical convective parameters, including degree of supersaturation, supercooled water content and glaciation temperature. Important isotopic processes in updrafts include kinetic effects that are a consequence of diffusive growth or decay of cloud particles within a supersaturated or subsaturated environment; isotopic re-equilibration between vapour and supercooled droplets, which buffers isotopic distillation; and differing mechanisms of glaciation (droplet freezing vs. the Wegener-Bergeron-Findeisen process). As all of these processes are related to updraft strength, particle size distribution and the retention of supercooled water, isotopic measurements can serve as a probe of in-cloud conditions of importance to convective processes. We study the sensitivity of the profile of water vapour isotopic composition to differing model assumptions and show how measurements of isotopic composition at cloud base and cloud top alone may be sufficient to retrieve key cloud parameters.

Isotope effects on the optical spectra of semiconductors

NASA Astrophysics Data System (ADS)

Cardona, Manuel; Thewalt, M. L. W.

2005-10-01

Since the end of the cold war, macroscopic amounts of separated stable isotopes of most elements have been available “off the shelf” at affordable prices. Using these materials, single crystals of many semiconductors have been grown and the dependence of their physical properties on isotopic composition has been investigated. The most conspicuous effects observed have to do with the dependence of phonon frequencies and linewidths on isotopic composition. These affect the electronic properties of solids through the mechanism of electron-phonon interaction, in particular, in the corresponding optical excitation spectra and energy gaps. This review contains a brief introduction to the history, availability, and characterization of stable isotopes, including their many applications in science and technology. It is followed by a concise discussion of the effects of isotopic composition on the vibrational spectra, including the influence of average isotopic masses and isotopic disorder on the phonons. The final sections deal with the effects of electron-phonon interaction on energy gaps, the concomitant effects on the luminescence spectra of free and bound excitons, with particular emphasis on silicon, and the effects of isotopic composition of the host material on the optical transitions between the bound states of hydrogenic impurities.

Determination of lithium isotopes at natural abundance levels by atomic absorption spectrometry

USGS Publications Warehouse

Meier, A.L.

1982-01-01

The relationships of the absorption of 6Li and 7Li hollow cathode lamp emissions are used to determine lithium isotopic composition in the natural abundance range of geologic materials. Absorption was found to have a nonlinear dependence upon total lithium concentration and isotopic composition. A method using nonlinear equations to describe the relationship of the absorption of 6Li and 7Li lamp radiation is proposed as a means of calculating isotopic composition that is independent of total lithium concentration.

Latitudinal change in precipitation and water vapor isotopes over Southern ocean

NASA Astrophysics Data System (ADS)

Rahul, P.

2015-12-01

The evaporation process over ocean is primary source of water vapor in the hydrological cycle. The Global Network of Isotopes in Precipitation (GNIP) dataset of rainwater and water vapor isotopes are predominantly based on continental observations, with very limited observation available from the oceanic area. Stable isotope ratios in precipitation provide valuable means to understand the process of evaporation and transport of water vapor. This is further extended in the study of past changes in climate from the isotopic composition of ice core. In this study we present latitudinal variability of water vapor and rainwater isotopic composition and compared it with factors like physical condition of sea surface water from near equator (1°S) to the polar front (56°S) during the summer time expedition of the year 2013. The water vapor and rainwater isotopes showed a sharp depletion in isotopes while progressively move southward from the tropical regions (i.e. >30°S), which follows the pattern recorded in the surface ocean water isotopic composition. From the tropics to the southern latitudes, the water vapor d18O varied between -11.8‰ to -14.7‰ while dD variation ranges between -77.7‰ to -122.2‰. Using the data we estimated the expected water vapor isotopic composition under kinetic as well as equilibrium process. Our observation suggests that the water vapor isotopic compositions are in equilibrium with the sea water in majority of cases. At one point of observation, where trajectory of air parcel originated from the continental region, we observed a large deviation from the existing trend of latitudinal variability. The deduced rainwater composition adopting equilibrium model showed a consistent pattern with observed values at the tropical region, while role of kinetic process become dominant on progressive shift towards the southern latitudes. We will draw comparison of our observation with other data available in the literature together with isotope model data during the presentation.

Stable Isotope Anatomy of Tropical Cyclone Ita, North-Eastern Australia, April 2014

PubMed Central

Munksgaard, Niels C.; Zwart, Costijn; Kurita, Naoyuki; Bass, Adrian; Nott, Jon; Bird, Michael I.

2015-01-01

The isotope signatures registered in speleothems during tropical cyclones (TC) provides information about the frequency and intensity of past TCs but the precise relationship between isotopic composition and the meteorology of TCs remain uncertain. Here we present continuous δ18O and δ2H data in rainfall and water vapour, as well as in discrete rainfall samples, during the passage of TC Ita and relate the evolution in isotopic compositions to local and synoptic scale meteorological observations. High-resolution data revealed a close relationship between isotopic compositions and cyclonic features such as spiral rainbands, periods of stratiform rainfall and the arrival of subtropical and tropical air masses with changing oceanic and continental moisture sources. The isotopic compositions in discrete rainfall samples were remarkably constant along the ~450 km overland path of the cyclone when taking into account the direction and distance to the eye of the cyclone at each sampling time. Near simultaneous variations in δ18O and δ2H values in rainfall and vapour and a near-equilibrium rainfall-vapour isotope fractionation indicates strong isotopic exchange between rainfall and surface inflow of vapour during the approach of the cyclone. In contrast, after the passage of spiral rainbands close to the eye of the cyclone, different moisture sources for rainfall and vapour are reflected in diverging d-excess values. High-resolution isotope studies of modern TCs refine the interpretation of stable isotope signatures found in speleothems and other paleo archives and should aim to further investigate the influence of cyclone intensity and longevity on the isotopic composition of associated rainfall. PMID:25742628

Elemental and iron isotopic composition of aerosols collected in a parking structure.

PubMed

Majestic, Brian J; Anbar, Ariel D; Herckes, Pierre

2009-09-01

The trace metal contents and iron isotope composition of size-resolved aerosols were determined in a parking structure in Tempe, AZ, USA. Particulate matter (PM)<2.5 microm in diameter (the fine fraction) and PM>2.5 microm were collected. Several air toxics (e.g., arsenic, cadmium, and antimony) were enriched above the crustal average, implicating automobiles as an important source. Extremely high levels of fine copper (up to 1000 ng m(-3)) were also observed in the parking garage, likely from brake wear. The iron isotope composition of the aerosols were found to be +0.15+/-0.03 per thousand and +0.18+/-0.03 per thousand for the PM<2.5 microm and PM>2.5 microm fractions, respectively. The similarity of isotope composition indicates a common source for each size fraction. To better understand the source of iron in the parking garage, the elemental composition in four brake pads (two semi-metallic and two ceramic), two tire tread samples, and two waste oil samples were determined. Striking differences in the metallic and ceramic brake pads were observed. The ceramic brake pads contained 10-20% copper by mass, while the metallic brake pads contained about 70% iron, with very little copper. Both waste oil samples contained significant amounts of calcium, phosphorous, and zinc, consistent with the composition of some engine oil additives. Differences in iron isotope composition were observed between the source materials; most notably between the tire tread (average=+0.02 per thousand) and the ceramic brake linings (average=+0.65 per thousand). Differences in isotopic composition were also observed between the metallic (average=+0.18 per thousand) and ceramic brake pads, implying that iron isotope composition may be used to resolve these sources. The iron isotope composition of the metallic brake pads was found to be identical to the aerosols, implying that brake dust is the dominant source of iron in a parking garage.

Intramolecular Isotopic Studies: Chemical Enhancements and Alternatives

NASA Astrophysics Data System (ADS)

Hayes, J. M.

2016-12-01

As mass spectroscopic and NMR-based methods now appropriately flourish, chemical techniques should not be forgotten. First, the methods developed by pioneering intramolecular analysts can be reapplied to new samples. Second, they can be extended. The synthesis of intramolecular isotopic standards is particularly important and straightforward. It requires only that a chemical reaction has no secondary products. An example is provided by the addition of carbon dioxide to a Grignard reagent. The reaction proceeds with an isotope effect. The isotopic composition of the carboxyl group in the acid which is produced is thus not equal to that of the starting carbon dioxide but the unconsumed CO2 can be recovered and analyzed. A simple titration can show that all the rest of the CO2 is in the product acid. The isotopic composition of the carboxyl group can then be calculated by difference. The product is an intramolecular isotopic standard, an organic molecule in which the isotopic composition of a specific carbon position is known accurately. Both analysts and reviewers can thus gain invaluable confidence in the accuracy of instrumental results. A second example: the haloform reaction quantitatively degrades methyl ketones, producing a carboxylic acid which can be decarboxylated to determine the isotopic composition of the parent carbonyl and a haloform (CHI3, for example) that can be combusted to determine the isotopic composition of the methyl group. Ketones thus analyzed can be combined with Grignard reagents to yield carbon skeletons in which the isotopic compositions of internal and terminal -CH2- and -CH3 groups are known accurately. In general, analysts accustomed to demanding quantitative reactions should remember the power of mass balances and recognize that many organic-chemical reactions, while not quantitative, lack side products and can be driven to the total consumption of at least one reactant.

Testing the chondrule-rich accretion model for planetary embryos using calcium isotopes

NASA Astrophysics Data System (ADS)

Amsellem, Elsa; Moynier, Frédéric; Pringle, Emily A.; Bouvier, Audrey; Chen, Heng; Day, James M. D.

2017-07-01

Understanding the composition of raw materials that formed the Earth is a crucial step towards understanding the formation of terrestrial planets and their bulk composition. Calcium is the fifth most abundant element in terrestrial planets and, therefore, is a key element with which to trace planetary composition. However, in order to use Ca isotopes as a tracer of Earth's accretion history, it is first necessary to understand the isotopic behavior of Ca during the earliest stages of planetary formation. Chondrites are some of the oldest materials of the Solar System, and the study of their isotopic composition enables understanding of how and in what conditions the Solar System formed. Here we present Ca isotope data for a suite of bulk chondrites as well as Allende (CV) chondrules. We show that most groups of carbonaceous chondrites (CV, CI, CR and CM) are significantly enriched in the lighter Ca isotopes (δ 44 / 40 Ca = + 0.1 to + 0.93 ‰) compared with bulk silicate Earth (δ 44 / 40 Ca = + 1.05 ± 0.04 ‰, Huang et al., 2010) or Mars, while enstatite chondrites are indistinguishable from Earth in Ca isotope composition (δ 44 / 40 Ca = + 0.91 to + 1.06 ‰). Chondrules from Allende are enriched in the heavier isotopes of Ca compared to the bulk and the matrix of the meteorite (δ 44 / 40 Ca = + 1.00 to + 1.21 ‰). This implies that Earth and Mars have Ca isotope compositions that are distinct from most carbonaceous chondrites but that may be like chondrules. This Ca isotopic similarity between Earth, Mars, and chondrules is permissive of recent dynamical models of planetary formation that propose a chondrule-rich accretion model for planetary embryos.

Plutonium immobilization in glass and ceramics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Knecht, D.A.; Murphy, W.M.

1996-05-01

The Materials Research Society Nineteenth Annual Symposium on the Scientific Basis for Nuclear Waste Management was held in Boston on November 27 to December 1, 1995. Over 150 papers were presented at the Symposium dealing with all aspects of nuclear waste management and disposal. Fourteen oral sessions and on poster session included a Plenary session on surplus plutonium dispositioning and waste forms. The proceedings, to be published in April, 1996, will provide a highly respected, referred compilation of the state of scientific development in the field of nuclear waste management. This paper provides a brief overview of the selected Symposiummore » papers that are applicable to plutonium immobilization and plutonium waste form performance. Waste forms that were described at the Symposium cover most of the candidate Pu immobilization options under consideration, including borosilicate glass with a melting temperature of 1150 {degrees}C, a higher temperature (1450 {degrees}C) lanthanide glass, single phase ceramics, multi-phase ceramics, and multi-phase crystal-glass composites (glass-ceramics or slags). These Symposium papers selected for this overview provide the current status of the technology in these areas and give references to the relevant literature.« less

Non-destructive measurement of carbonic anhydrase activity and the oxygen isotope composition of soil water

NASA Astrophysics Data System (ADS)

Jones, Sam; Sauze, Joana; Ogée, Jérôme; Wohl, Steven; Bosc, Alexandre; Wingate, Lisa

2016-04-01

Carbonic anhydrases are a group of metalloenzymes that catalyse the hydration of aqueous carbon dioxide (CO2). The expression of carbonic anhydrase by bacteria, archaea and eukarya has been linked to a variety of important biological processes including pH regulation, substrate supply and biomineralisation. As oxygen isotopes are exchanged between CO2 and water during hydration, the presence of carbonic anhydrase in plants and soil organisms also influences the oxygen isotope budget of atmospheric CO2. Leaf and soil water pools have distinct oxygen isotope compositions, owing to differences in pool sizes and evaporation rates, which are imparted on CO2during hydration. These differences in the isotopic signature of CO2 interacting with leaves and soil can be used to partition the contribution of photosynthesis and soil respiration to net terrestrial CO2 exchange. However, this relies on our knowledge of soil carbonic anhydrase activity and currently, the prevalence and function of these enzymes in soils is poorly understood. Isotopic approaches used to estimate soil carbonic anhydrase activity typically involve the inversion of models describing the oxygen isotope composition of CO2 fluxes to solve for the apparent, potentially catalysed, rate of oxygen exchange during hydration. This requires information about the composition of CO2 in isotopic equilibrium with soil water obtained from destructive, depth-resolved soil water sampling. This can represent a significant challenge in data collection given the considerable potential for spatial and temporal variability in the isotopic composition of soil water and limited a priori information with respect to the appropriate sampling resolution and depth. We investigated whether we could circumvent this requirement by constraining carbonic anhydrase activity and the composition of soil water in isotopic equilibrium with CO2 by solving simultaneously the mass balance for two soil CO2 steady states differing only in the oxygen isotope composition of ambient CO2. This non-destructive approach was tested through laboratory incubations of air-dried soils that were re-wetted with water of known isotopic composition. Performance was assessed by comparing estimates of the soil water oxygen isotope composition derived from open chamber flux measurements with those measured in the irrigation water and soil water extracted following incubations. The influence of soil pH and bovine carbonic anhydrase additions on these estimates was also investigated. Coherent values were found between the soil water composition estimates obtained from the dual steady state approach and those measured for irrigation waters. Estimates of carbonic anhydrase activity made using this approach also reflected well artificial increases to the concentration of carbonic anhydrase and indicated that this activity was sensitive to soil pH.

Multiple stable isotope fronts during non-isothermal fluid flow

NASA Astrophysics Data System (ADS)

Fekete, Szandra; Weis, Philipp; Scott, Samuel; Driesner, Thomas

2018-02-01

Stable isotope signatures of oxygen, hydrogen and other elements in minerals from hydrothermal veins and metasomatized host rocks are widely used to investigate fluid sources and paths. Previous theoretical studies mostly focused on analyzing stable isotope fronts developing during single-phase, isothermal fluid flow. In this study, numerical simulations were performed to assess how temperature changes, transport phenomena, kinetic vs. equilibrium isotope exchange, and isotopic source signals determine mineral oxygen isotopic compositions during fluid-rock interaction. The simulations focus on one-dimensional scenarios, with non-isothermal single- and two-phase fluid flow, and include the effects of quartz precipitation and dissolution. If isotope exchange between fluid and mineral is fast, a previously unrecognized, significant enrichment in heavy oxygen isotopes of fluids and minerals occurs at the thermal front. The maximum enrichment depends on the initial isotopic composition of fluid and mineral, the fluid-rock ratio and the maximum change in temperature, but is independent of the isotopic composition of the incoming fluid. This thermally induced isotope front propagates faster than the signal related to the initial isotopic composition of the incoming fluid, which forms a trailing front behind the zone of transient heavy oxygen isotope enrichment. Temperature-dependent kinetic rates of isotope exchange between fluid and rock strongly influence the degree of enrichment at the thermal front. In systems where initial isotope values of fluids and rocks are far from equilibrium and isotope fractionation is controlled by kinetics, the temperature increase accelerates the approach of the fluid to equilibrium conditions with the host rock. Consequently, the increase at the thermal front can be less dominant and can even generate fluid values below the initial isotopic composition of the input fluid. As kinetics limit the degree of isotope exchange, a third front may develop in kinetically limited systems, which propagates with the advection speed of the incoming fluid and is, therefore, traveling fastest. The results show that oxygen isotope signatures at thermal fronts recorded in rocks and veins that experienced isotope exchange with fluids can easily be misinterpreted, namely if bulk analytical techniques are applied. However, stable isotope microanalysis on precipitated minerals may - if later isotope exchange is kinetically limited - provide a valuable archive of the transient thermal and hydrological evolution of a system.

Using multiple isotopes to understand the source of ingredients used in golden beverages

NASA Astrophysics Data System (ADS)

Wynn, J. G.

2011-12-01

Traditionally, beer contains 4 simple ingredients: water, barley, hops and yeast. Each of these ingredients used in the brewing process contributes some combination of a number of "traditional" stable isotopes (i.e., isotopes of H, C, O, N and S) to the final product. As an educational exercise in an "Analytical Techniques in Geology" course, a group of students analyzed the isotopic composition of the gas, liquid and solid phases of a variety of beer samples collected from throughout the world (including other beverages). The hydrogen and oxygen isotopic composition of the water followed closely the isotopic composition of local meteoric water at the source of the brewery, although there is a systematic offset from the global meteoric water line that may be due to the effects of CO2-H2O equilibration. The carbon isotopic composition of the CO2 reflected that of the solid residue (the source of carbon used as a fermentation substrate), but may potentially be modified by addition of gas-phase CO2 from an inorganic source. The carbon isotopic composition of the solid residue similarly tracks that of the fermentation substrate, and may indicate some alcohol fermented from added sugars in some cases. The nitrogen isotopic composition of the solid residue was relatively constant, and may track the source of nitrogen in the barley, hops and yeast. Each of the analytical methods used is a relatively standard technique used in geological applications, making this a "fun" exercise for those involved, and gives the students hands-on experience with a variety of analytes from a non-traditional sample material.

The ruthenium isotopic composition of the oceanic mantle

NASA Astrophysics Data System (ADS)

Bermingham, K. R.; Walker, R. J.

2017-09-01

The approximately chondritic relative, and comparatively high absolute mantle abundances of the highly siderophile elements (HSE), suggest that their concentrations in the bulk silicate Earth were primarily established during a final ∼0.5 to 1% of ;late accretion; to the mantle, following the cessation of core segregation. Consequently, the isotopic composition of the HSE Ru in the mantle reflects an amalgamation of the isotopic compositions of late accretionary contributions to the silicate portion of the Earth. Among cosmochemical materials, Ru is characterized by considerable mass-independent isotopic variability, making it a powerful genetic tracer of Earth's late accretionary building blocks. To define the Ru isotopic composition of the oceanic mantle, the largest portion of the accessible mantle, we report Ru isotopic data for materials from one Archean and seven Phanerozoic oceanic mantle domains. A sample from a continental lithospheric mantle domain is also examined. All samples have identical Ru isotopic compositions, within analytical uncertainties, indicating that Ru isotopes are well mixed in the oceanic mantle, defining a μ100Ru value of 1.2 ± 7.2 (2SD). The only known meteorites with the same Ru isotopic composition are enstatite chondrites and, when corrected for the effects of cosmic ray exposure, members of the Main Group and sLL subgroup of the IAB iron meteorite complex which have a collective CRE corrected μ100Ru value of 0.9 ± 3.0. This suggests that materials from the region(s) of the solar nebula sampled by these meteorites likely contributed the dominant portion of late accreted materials to Earth's mantle.

The influence of diet on the δ 13C of shell carbon in the pulmonate snail Helix aspersa

NASA Astrophysics Data System (ADS)

Stott, Lowell D.

2002-02-01

The influence of diet and atmospheric CO 2 on the carbon isotope composition of shell aragonite and shell-bound organic carbon in the pulmonate snail Helix aspersa raised in the laboratory was investigated. Three separate groups of snails were raised on romaine lettuce (C3 plant, δ 13C=-25.8‰), corn (C4 plant, δ 13C=-10.5‰), and sour orange ( 12C-enriched C3 plant, δ 13C=-39.1‰). The isotopic composition of body tissues closely tracked the isotopic composition of the snail diet as demonstrated previously. However, the isotopic composition of the acid insoluble organic matrix extracted from the aragonite shells does not track diet in all groups. In snails that were fed corn the isotopic composition of the organic matrix was more negative than the body by as much as 5‰ whereas the matrix was approximately 1‰ heavier than the body tissues in snails fed a diet of C3 plant material. These results indicate that isotopic composition of the organic matrix carbon cannot be used as an isotopic substrate for paleodietary reconstructions without first determining the source of the carbon and any associated fractionations. The isotopic composition of the shell aragonite is offset from the body tissues by 12.3‰ in each of the culture groups. This offset was not influenced by the consumption of carbonate and is not attributable to the diffusion of atmospheric CO 2 into the hemolymph. The carbon isotopic composition of shell aragonite is best explained in terms of equilibrium fractionations associated with exchange between metabolic CO 2 and HCO 3 in the hemolymph and the fractionation associated with carbonate precipitation. These results differ from previous studies, based primarily on samples collected in the field, that have suggested atmospheric carbon dioxide contributes significantly to the shell δ 13C. The culture results indicate that the δ 13C of aragonite is a good recorder of the isotopic composition of the snail body tissue, and therefore a better recorder of diet than is the insoluble shell organic carbon. Because the systematic fractionation of carbon isotopes within the snail is temperature dependent, the δ 13C of the shell could provide an independent technique for estimating paleotemperature changes.

Strontium and neodymium isotopes in hot springs on the East Pacific Rise and Guaymas Basin

NASA Technical Reports Server (NTRS)

Piepgras, D. J.; Wasserburg, G. J.

1985-01-01

Solutions collected from 21 deg N, East Pacific Rise (Epr) and Guaymas Basin, Gulf of California, are analyzed for Nd isotopic composition and Sm and Nd concentrations. The results indicate extensive but not complete isotopic exchange with Sr in the depleted oceanic crust and that Sr concentrations in these solutions are buffered. In contrast, the Nd data exhibit a wide range in isotopic composition and concentration between vents. Many samples show substantial contributions from MORB, but all have isotopic compositions below MORB, in spite of enrichments in Nd up to 100 times seawater. It is shown that the fluids must exchange Nd with a sedimentary reservoir having an isotopic composition less than Pacific seawater. Low-temperature reactions with metalliferous sediments on the flanks of the EPR may provide such a source. Using a simple box method, estimates of the hydrothermal fluxes of Nd are compared to fluxes which are necessary to maintain a radiogenic isotopic composition of about -3 in the Pacific against the influx of Antarctic waters. It is concluded that erosion from island arcs is the main source of radiogenic Nd in the Pacific.

Measurement of natural carbon isotopic composition of acetone in human urine.

PubMed

Yamada, Keita; Ohishi, Kazuki; Gilbert, Alexis; Akasaka, Mai; Yoshida, Naohiro; Yoshimura, Ryoko

2016-02-01

The natural carbon isotopic composition of acetone in urine was measured in healthy subjects using gas chromatography-combustion-isotope ratio mass spectrometry combined with headspace solid-phase microextraction (HS-SPME-GC-C-IRMS). Before applying the technique to a urine sample, we optimized the measurement conditions of HS-SPME-GC-C-IRMS using aqueous solutions of commercial acetone reagents. The optimization enabled us to determine the carbon isotopic compositions within ±0.2 ‰ of precision and ±0.3‰ of error using 0.05 or 0.2 mL of aqueous solutions with acetone concentrations of 0.3-121 mg/L. For several days, we monitored the carbon isotopic compositions and concentrations of acetone in urine from three subjects who lived a daily life with no restrictions. We also monitored one subject for 3 days including a fasting period of 24 h. These results suggest that changes in the availability of glucose in the liver are reflected in changes in the carbon isotopic compositions of urine acetone. Results demonstrate that carbon isotopic measurement of metabolites in human biological samples at natural abundance levels has great potential as a tool for detecting metabolic changes caused by changes in physiological states and disease.

Sr isotopic tracer study of the Samail ophiolite, Oman.

USGS Publications Warehouse

Lanphere, M.A.; Coleman, R.G.; Hopson, C.A.

1981-01-01

Rb and Sr concentrations and Sr-isotopic compositions were measured in 41 whole-rock samples and 12 mineral separates from units of the Samail ophiolite, including peridotite, gabbro, plagiogranite, diabase dykes, and gabbro and websterite dykes within the metamorphic peridotite. Ten samples of cumulate gabbro from the Wadir Kadir section and nine samples from the Wadi Khafifah section have 87Sr/86Sr ratios of 0.70314 + or - 0.00030 and 0.70306 + or - 0.00034, respectively. The dispersion in Sr- isotopic composition may reflect real heterogeneities in the magma source region. The average Sr-isotopic composition of cumulate gabbro falls in the range of isotopic compositions of modern MORB. The 87Sr/86Sr ratios of noncumulate gabbro, plagiogranite, and diabase dykes range 0.7034-0.7047, 0.7038-0.7046 and 0.7037- 0.7061, respectively. These higher 87Sr/86Sr ratios are due to alteration of initial magmatic compositions by hydrothermal exchange with sea-water. Mineral separates from dykes that cut harzburgite tectonite have Sr-isotopic compositions which agree with that of cumulate gabbro. These data indicate that the cumulate gabbro and the different dykes were derived from partial melting of source regions that had similar long-term histories and chemical compositions.-T.R.

Rare earth element transport in the western North Atlantic inferred from Nd isotopic observations

NASA Technical Reports Server (NTRS)

Piepgras, D. J.; Wasserburg, G. J.

1987-01-01

The relationship between the Nd isotopic composition in the Atlantic waters and the origin and circulation of the water masses was investigated. Samples were collected in the western North Atlantic between 7 and 54 deg N. The isotopic composition (Nd-143/Nd-144 ratios) showed extensive vertical structure at all locations. In regions where a thermocline was well-developed, large isotopic shifts were observed across the base of the thermocline, while regions without a thermocline were characterized by much more gradual shifts in isotopic composition with depth. The data reveal an excellent correlation between the Nd isotopic distribution in the western North Atlantic water column and the distribution of water masses identified from temperature and salinity measurements.

Sm-Nd in marine carbonates and phosphates - Implications for Nd isotopes in seawater and crustal ages

NASA Technical Reports Server (NTRS)

Shaw, H. F.; Wasserburg, G. J.

1985-01-01

The possibility of establishing a record of variations in the isotopic composition of Nd in seawater over geologic time is explored. To construct such a record, a phase must be identified which incorporated Nd with the same isotopic composition as seawater at the time of its formation, preserves that composition, and which is relatively common in sediments. To evaluate the suitability of carbonates and phosphates, the Rb, Sr, Sm, and Nd concentrations and the Nd and Sr isotopic composition of a variety of modern and ancient marine calcite, aragonite, and apatite samples have been measured and the results are presented and discussed.

Fingerprints of carbon, nitrogen, and silicon isotopes in small interstellar SiC grains from the Murchison meteorite

NASA Technical Reports Server (NTRS)

Hoppe, Peter; Geiss, Johannes; Buehler, Fritz; Neuenschwander, Juerg; Amari, Sachiko; Lewis, Roy S.

1993-01-01

We report ion microprobe determinations of the carbon, nitrogen, and silicon isotopic compositions of small SiC grains from the Murchison CM2 chondrite. Analyses were made on samples containing variable numbers of grains and on 14 individual grains. In some cases the multiple-grain sample compositions were probably dominated by only one or two grains. Total ranges observed are given. Only a few grains show values near the range limits. Both the total ranges of carbon and nitrogen isotopic compositions, and even the narrower ranges typical for the majority of the grains, are similar to those observed for larger SiC grains. Two rare components appear to be present in the smaller-size fraction, one characterized by C-12/C-13 about 12-16 and the other by very heavy nitrogen. The carbon and nitrogen isotopic compositions qualitatively may reflect hydrostatic H-burning via the CNO cycle and He-burning in red giants, as well as explosive H-burning in novae. The silicon isotopic compositions of most grains qualitatively show what is the signature of He-burning. The silicon isotopic composition of one grain, however, suggests a different process.

Characterization of the Old Hydrofracture Facility (OHF) waste tanks located at ORNL

DOE Office of Scientific and Technical Information (OSTI.GOV)

Keller, J.M.; Giaquinto, J.M.; Meeks, A.M.

1997-04-01

The Old Hydrofracture Facility (OHF) is located in Melton Valley within Waste Area Grouping (WAG) 5 and includes five underground storage tanks (T1, T2, T3, T4, and T9) ranging from 13,000 to 25,000 gal. capacity. During the period of 1996--97 there was a major effort to re-sample and characterize the contents of these inactive waste tanks. The characterization data summarized in this report was needed to address waste processing options, examine concerns dealing with the performance assessment (PA) data for the Waste Isolation Pilot Plant (WIPP), evaluate the waste characteristics with respect to the waste acceptance criteria (WAC) for WIPPmore » and Nevada Test Site (NTS), address criticality concerns, and to provide the data needed to meet DOT requirements for transporting the waste. This report discusses the analytical characterization data collected on both the supernatant and sludge samples taken from three different locations in each of the OHF tanks. The isotopic data presented in this report supports the position that fissile isotopes of uranium ({sup 233}U and {sup 235}U) do not satisfy the denature ratios required by the administrative controls stated in the ORNL LLLW waste acceptance criteria (WAC). The fissile isotope of plutonium ({sup 239}Pu and {sup 241}Pu) are diluted with thorium far above the WAC requirements. In general, the OHF sludge was found to be hazardous (RCRA) based on total metal content and the transuranic alpha activity was well above the 100 nCi/g limit for TRU waste. The characteristics of the OHF sludge relative to the WIPP WAC limits for fissile gram equivalent, plutonium equivalent activity, and thermal power from decay heat were estimated from the data in this report and found to be far below the upper boundary for any of the remote-handled transuranic waste (RH-TRU) requirements for disposal of the waste in WIPP.« less

Common Occurrence of Explosive Hydrogen Burning in Type II Supernovae

NASA Astrophysics Data System (ADS)

Liu, Nan; Stephan, Thomas; Boehnke, Patrick; Nittler, Larry R.; Meyer, Bradley S.; O’D. Alexander, Conel M.; Davis, Andrew M.; Trappitsch, Reto; Pellin, Michael J.

2018-03-01

We report Mo isotopic data for 16 15N-rich presolar SiC grains of type AB (14N/15N < solar, AB1) and their correlated Sr and Ba isotope ratios when available. Of the 16 AB1 grains, 8 show s-process Mo isotopic compositions, together with s-process Ba and/or Sr isotopic compositions. We found that a higher percentage of AB1 grains show anomalous isotopic compositions than that of AB2 grains (14N/15N > solar), thus providing further support to the division of the two AB subgroups recently proposed by Liu et al., who showed that AB1 grains most likely originated from Type II supernovae (SNe) with explosive H burning. Comparison of the Sr, Mo, and Ba isotopic compositions of the AB1 grains with SN model predictions indicates that the s-process isotopic compositions of AB1 grains resulted from neutron-capture processes occurring during the progenitor massive stars’ pre-SN evolution rather than from an explosive neutron-capture process. In addition, the observations of (1) explosive H burning occurring in the C-rich regions of the progenitor SNe of X grains as suggested by the isotopic compositions of X grains, and (2) explosive H burning occurring both at the bottom of the He/C zone and at the top of the He/N zone as suggested by model simulations, imply that explosive H burning is a common phenomenon in outer SN zones.

Common Occurrence of Explosive Hydrogen Burning in Type II Supernovae

DOE PAGES

Liu, Nan; Stephan, Thomas; Boehnke, Patrick; ...

2018-03-16

In this paper, we report Mo isotopic data for 16 15N-rich presolar SiC grains of type AB ( 14N/ 15N < solar, AB1) and their correlated Sr and Ba isotope ratios when available. Of the 16 AB1 grains, 8 show s-process Mo isotopic compositions, together with s-process Ba and/or Sr isotopic compositions. We found that a higher percentage of AB1 grains show anomalous isotopic compositions than that of AB2 grains ( 14N/ 15N > solar), thus providing further support to the division of the two AB subgroups recently proposed by Liu et al., who showed that AB1 grains most likelymore » originated from Type II supernovae (SNe) with explosive H burning. Comparison of the Sr, Mo, and Ba isotopic compositions of the AB1 grains with SN model predictions indicates that the s-process isotopic compositions of AB1 grains resulted from neutron-capture processes occurring during the progenitor massive stars' pre-SN evolution rather than from an explosive neutron-capture process. Finally, in addition, the observations of (1) explosive H burning occurring in the C-rich regions of the progenitor SNe of X grains as suggested by the isotopic compositions of X grains, and (2) explosive H burning occurring both at the bottom of the He/C zone and at the top of the He/N zone as suggested by model simulations, imply that explosive H burning is a common phenomenon in outer SN zones.« less

Common Occurrence of Explosive Hydrogen Burning in Type II Supernovae

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Nan; Stephan, Thomas; Boehnke, Patrick

In this paper, we report Mo isotopic data for 16 15N-rich presolar SiC grains of type AB ( 14N/ 15N < solar, AB1) and their correlated Sr and Ba isotope ratios when available. Of the 16 AB1 grains, 8 show s-process Mo isotopic compositions, together with s-process Ba and/or Sr isotopic compositions. We found that a higher percentage of AB1 grains show anomalous isotopic compositions than that of AB2 grains ( 14N/ 15N > solar), thus providing further support to the division of the two AB subgroups recently proposed by Liu et al., who showed that AB1 grains most likelymore » originated from Type II supernovae (SNe) with explosive H burning. Comparison of the Sr, Mo, and Ba isotopic compositions of the AB1 grains with SN model predictions indicates that the s-process isotopic compositions of AB1 grains resulted from neutron-capture processes occurring during the progenitor massive stars' pre-SN evolution rather than from an explosive neutron-capture process. Finally, in addition, the observations of (1) explosive H burning occurring in the C-rich regions of the progenitor SNe of X grains as suggested by the isotopic compositions of X grains, and (2) explosive H burning occurring both at the bottom of the He/C zone and at the top of the He/N zone as suggested by model simulations, imply that explosive H burning is a common phenomenon in outer SN zones.« less

Carbon, nitrogen, magnesium, silicon, and titanium isotopic compositions of single interstellar silicon carbide grains from the Murchison carbonaceous chondrite

NASA Technical Reports Server (NTRS)

Hoppe, Peter; Amari, Sachiko; Zinner, Ernst; Ireland, Trevor; Lewis, Roy S.

1994-01-01

Seven hundred and twenty SiC grains from the Murchison CM2 chondrite, ranging in size from 1 to 10 micrometers, were analyzed by ion microprobe mass spectrometry for their C-isotopic compositions. Subsets of the grains were also analyzed for N (450 grains), Si (183 grains), Mg (179 grains), and Ti (28 grains) isotopes. These results are compared with previous measurements on 41 larger SiC grains (up to 15 x 26 micrometers) from a different sample of Murchison analyzed by Virag et al. (1992) and Ireland, Zinner, & Amari (1991a). All grains of the present study are isotopically anomalous with C-12/C-13 ratios ranging from 0.022 to 28.4 x solar, N-14/N-15 ratios from 0.046 to 30 x solar, Si-29/Si-28 from 0.54 to 1.20 x solar, Si-30/Si-28 from 0.42 to 1.14 x solar, Ti-49/Ti-48 from 0.96 to 1.95 x solar, and Ti-50/Ti-48 from 0.94 to 1.39 x solar. Many grains have large Mg-26 excesses from the decay of Al-26 with inferred Al-26/Al-27 ratios ranging up to 0.61, or 12,200 x the ratio of 5 x 10(exp -5) inferred for the early solar system. Several groups can be distinguished among the SiC grains. Most of the grains have C-13 and N-14 excesses, and their Si isotopic compositions (mostly excesses in Si-29 and Si-30) plot close to a slope 1.34 line on a Delta Si-29/Si-28 versus Delta Si-30/Si-28 three-isotope plot. Grains with small C-12/C-13 ratios (less than 10) tend to have smaller or no N-14 excesses and high Al-26/Al-27 ratios (up to 0.01). Grains with C-12/C-13 greater than 150 fall into two groups: grains X have N-15 excesses and Si-29 and Si-30 deficits and the highest (0.1 to 0.6) Al-26/Al-27 ratios; grains Y have N-14 excesses and plot on a slope 0.35 line on a Si three-isotope plot. In addition, large SiC grains of the Virag et al. (1992) study fall into three-distinct clusters according to their C-, Si-, and Ti-isotopic compositions. The isotopic diversity of the grains and the clustering of their isotopic compositions imply distinct and multiple stellar sources. The C- and N-isotopic compositions of most grains are consistent with H-burning in the CNO cycle. These and s-process Kr, Xe, Ba, and Nd suggest asymptotic giant branch (AGB) or Wolf-Rayet stars as likely sources for the grains, but existing models of nucleosynthesis in these stellar sites fail to account in detail for all the observed isotopic compositions. Special problems are posed by grains with C-12/C-13 less than 10 and almost normal and heavy N-isotopic compositions. Also the Si- and Ti-isotopic compositions, with excesses in Si-29 and Si-30 relative to Si-28 and excesses in all Ti isotopes relative to Ti-48, do not precisely conform with the compositions predicted for slow neutron capture. Additional theoretical efforts are needed to achieve an understanding of the isotopic composition of the SiC grains and their stellar sources.

Rb-Sr and Sm-Nd Ages of Zagami DML and SR Isotopic Heterogeneity in Zagami

NASA Technical Reports Server (NTRS)

Nyquist, L.aurenceE.; Shih, C.-Y.; Reese, Y. D.

2010-01-01

Zagami contains lithologic heterogeneity suggesting that it did not form in a homogeneous, thick lava flow [1]. We have previously investigated the Sr and Nd isotopic systematics of Coarse-Grained (CG) and Fine-Grained (FG) lithologies described by [2]. Both appear to belong to Normal Zagami (NZ) [1,3], but their initial Sr-isotopic compositions differ [4,5]. Here we report new analyses of the Dark Mottled Lithology (DML, [3]) that show its age and initial Sr and Nd isotopic compositions to be identical within error limits with those of CG, but Sr initial isotopic compositions differ from those of FG.

Behaviour of Structural Carbonate Stable Carbon and Oxygen Isotope Compositions in Bioapatite During Burning of Bone

NASA Astrophysics Data System (ADS)

Munro, L. E.; Longstaffe, F. J.; White, C. D.

2003-12-01

Bioapatite, the principal inorganic phase comprising bone, commonly contains a small fraction of carbonate, which has been substituted into the phosphate structure during bone formation. The isotopic compositions of both the phosphate oxygen and the structural carbonate oxygen are now commonly used in palaeoclimatological and bioarchaeological investigations. The potential for post-mortem alteration of these isotopic compositions, therefore, is of interest, with the behaviour of structural carbonate being of most concern. In bioarchaeological studies, alteration of bone isotopic compositions has the potential to occur not only during low-temperature processes associated with burial but also during food preparation involving heating (burning, boiling). Here, we examine the stable isotopic behaviour of structural carbonate oxygen and carbon, and coexisting phosphate oxygen during the burning of bone. Freshly deceased (6<8 months) white-tailed deer leg bones (Odocoileus virginianus) were collected from Pinery Provincial Park, Ontario, Canada. Each long bone was sectioned and incrementally heated from 25 to 900° C, in 25° intervals. The samples were then ground to a standardized grain-size (45<63μ m), and changes in bioapatite crystallinity (CI) were determined using powder X-ray diffraction (pXRD), and Fourier transform infra-red spectroscopy (FTIR). Combined differential thermal and thermogravimetric analyses (DTA/TG) were used to evaluate weight loss and associated reactions during heating. Stable carbon isotope compositions of the bioapatite remain relatively constant (+/-1‰ ) during heating to 650° C. A 4‰ increase in stable carbon isotopic composition then occurs between 650-750° C, accompanied by an increase in CI, followed by a 10‰ decline at temperatures above 800° C, as carbonate carbon is lost. Carbonate and phosphate oxygen isotopic compositions are correlated over the entire heating range, with carbonate being enriched relative to phosphate by about 8-10‰ below 500° C, 5-6‰ between 500-700° C, and 8-10‰ above 700° C. CI and oxygen isotopic compositions of carbonate and phosphate are not well correlated. Only modest CI changes are recorded from 25-675° C, compared with much larger changes in oxygen isotopic composition, especially above 300° C. On average, original isotopic compositions are largely preserved for both phosphate (+/-1‰ ) and carbonate (+/-2‰ ) oxygen at <300° C. At higher temperatures, however, both phosphate and carbonate oxygen in the bioapatite are systematically depleted of oxygen-18 relative to original values.

Oxygen isotope analysis of fossil organic matter by secondary ion mass spectrometry

NASA Astrophysics Data System (ADS)

Tartèse, Romain; Chaussidon, Marc; Gurenko, Andrey; Delarue, Frédéric; Robert, François

2016-06-01

We have developed an analytical procedure for the measurement of oxygen isotope composition of fossil organic matter by secondary ion mass spectrometry (SIMS) at the sub-per mill level, with a spatial resolution of 20-30 μm. The oxygen isotope composition of coal and kerogen samples determined by SIMS are on average consistent with the bulk oxygen isotope compositions determined by temperature conversion elemental analysis - isotope ratio mass spectrometry (TC/EA-IRMS), but display large spreads of δ18O of ∼5-10‰, attributed to mixing of remnants of organic compounds with distinct δ18O signatures. Most of the δ18O values obtained on two kerogen residues extracted from the Eocene Clarno and Early Devonian Rhynie continental chert samples and on two immature coal samples range between ∼10‰ and ∼25‰. Based on the average δ18O values of these samples, and on the O isotope composition of water processed by plants that now constitute the Eocene Clarno kerogen, we estimated δ18Owater values ranging between around -11‰ and -1‰, which overall correspond well within the range of O isotope compositions for present-day continental waters. SIMS analyses of cyanobacteria-derived organic matter from the Silurian Zdanow chert sample yielded δ18O values in the range 12-20‰. Based on the O isotope composition measured on recent cyanobacteria from the hypersaline Lake Natron (Tanzania), and on the O isotope composition of the lake waters in which they lived, we propose that δ18O values of cyanobacteria remnants are enriched by about ∼18 ± 2‰ to 22 ± 2‰ relative to coeval waters. This relationship suggests that deep ocean waters in which the Zdanow cyanobacteria lived during Early Silurian times were characterised by δ18O values of around -5 ± 4‰. This study, establishing the feasibility of micro-analysis of Phanerozoic fossil organic matter samples by SIMS, opens the way for future investigations of kerogens preserved in Archean cherts and of the O isotopic composition of ocean water at that period in time.

Cleaning up the Legacy of the Cold War: Plutonium Oxides and the Role of Synchrotron Radiation Research

DOE Office of Scientific and Technical Information (OSTI.GOV)

Clark, David Lewis

2015-01-21

The deceptively simple binary formula of AnO 2 belies an incredibly complex structural nature, and propensity to form mixed-valent, nonstoichiometric phases of composition AnO 2±x. For plutonium, the very formation of PuO 2+x has challenged a long-established dogma, and raised fundamental questions for long-term storage and environmental migration. This presentation covers two aspects of Los Alamos synchrotron radiation studies of plutonium oxides: (1) the structural chemistry of laboratory-prepared AnO 2+x systems (An = U, Pu; 0 ≤ x ≤ 0.25) determined through a combination of x-ray absorption fine structure spectroscopy (XAFS) and x-ray scattering of laboratory prepared samples; and (2)more » the application of synchrotron radiation towards the decontamination and decommissioning of the Rocky Flats Environmental Technology Site. Making the case for particle transport mechanisms as the basis of plutonium and americium mobility, rather than aqueous sorption-desorption processes, established a successful scientific basis for the dominance of physical transport processes by wind and water. The scientific basis was successful because it was in agreement with general theory on insolubility of PuO 2 in oxidation state IV, results of ultrafiltration analyses of field water/sediment samples, XAFS analyses of soil, sediment, and concrete samples, and was also in general agreement with on-site monitoring data. This understanding allowed Site contractors to rapidly move to application of soil erosion and sediment transport models as the means of predicting plutonium and americium transport, which led to design and application of site-wide soil erosion control technology to help control downstream concentrations of plutonium and americium in streamflow.« less

Rainfall Type as a Dominant Control of the Isotopic Composition of Precipitation in the South Central United States

NASA Astrophysics Data System (ADS)

Sun, C.; Shanahan, T. M.; Partin, J. W.

2017-12-01

The processes that control the isotopic composition of precipitation in the mid-latitudes are understudied compared to the high and low latitudes, but are critical for interpreting paleo records using isotope proxies. To better understand these processes, we investigated changes of isotopic composition of rainwater in Central Texas using 20 months of event-based rainwater collection. We find that in both the event-based data and the monthly data from the Waco GNIP station, the dominant control on the isotopic composition of precipitation is the proportion that is derived from convective systems. This finding is consistent with previously reported data largely from tropical localities (Aggarwal et al., 2016), where large organized convective systems lead to high rainfall amounts and isotopically depleted precipitation. Although there are seasonal differences in the dominant rainfall types over the South Central US, with winter precipitation almost entirely stratiform, seasonality plays very little role in the net isotopic composition of precipitation because the total contribution during winter is small compared with spring, summer and fall. We also find that changes of source have little effect on the isotopic composition of rainfall, as the majority of the moisture is derived from the Gulf of Mexico with little influence of reevaporation or mixing. The majority of the warm season precipitation in the South Central US occurs in association with mesoscale convective systems (MCSs) and the development of these systems plays a critical role in the overall isotopic signature of precipitation. MCSs are characterized by a combination of intense, organized convection at their leading edges and trailing stratiform precipitation. Larger MCSs tend to contain higher proportions of stratiform rainfall and as a result, have isotopically depleted values. Proxy records from this region displaying more negative isotope values in the past should therefore be interpreted with caution as they could reflect either increases in cool versus warm season precipitation or changes in the intensity of warm season MCSs.

Silicon Isotopic Fractionation of CAI-like Vacuum Evaporation Residues

DOE Office of Scientific and Technical Information (OSTI.GOV)

Knight, K; Kita, N; Mendybaev, R

2009-06-18

Calcium-, aluminum-rich inclusions (CAIs) are often enriched in the heavy isotopes of magnesium and silicon relative to bulk solar system materials. It is likely that these isotopic enrichments resulted from evaporative mass loss of magnesium and silicon from early solar system condensates while they were molten during one or more high-temperature reheating events. Quantitative interpretation of these enrichments requires laboratory determinations of the evaporation kinetics and associated isotopic fractionation effects for these elements. The experimental data for the kinetics of evaporation of magnesium and silicon and the evaporative isotopic fractionation of magnesium is reasonably complete for Type B CAI liquidsmore » (Richter et al., 2002, 2007a). However, the isotopic fractionation factor for silicon evaporating from such liquids has not been as extensively studied. Here we report new ion microprobe silicon isotopic measurements of residual glass from partial evaporation of Type B CAI liquids into vacuum. The silicon isotopic fractionation is reported as a kinetic fractionation factor, {alpha}{sub Si}, corresponding to the ratio of the silicon isotopic composition of the evaporation flux to that of the residual silicate liquid. For CAI-like melts, we find that {alpha}{sub Si} = 0.98985 {+-} 0.00044 (2{sigma}) for {sup 29}Si/{sup 28}Si with no resolvable variation with temperature over the temperature range of the experiments, 1600-1900 C. This value is different from what has been reported for evaporation of liquid Mg{sub 2}SiO{sub 4} (Davis et al., 1990) and of a melt with CI chondritic proportions of the major elements (Wang et al., 2001). There appears to be some compositional control on {alpha}{sub Si}, whereas no compositional effects have been reported for {alpha}{sub Mg}. We use the values of {alpha}Si and {alpha}Mg, to calculate the chemical compositions of the unevaporated precursors of a number of isotopically fractionated CAIs from CV chondrites whose chemical compositions and magnesium and silicon isotopic compositions have been previously measured.« less

Re-assessing the Molybdenum Isotope Composition of Pre-GOE Seawater: Evidence for Dynamic Ocean Redox

NASA Astrophysics Data System (ADS)

Ostrander, C. M.; Kendall, B.; Roy, M.; Romaniello, S. J.; Nunn, S. J.; Gordon, G. W.; Olson, S. L.; Lyons, T. W.; Zheng, W.; Anbar, A. D.

2016-12-01

Molybdenum (Mo) isotope compositions of Archean shales can provide important insights into ocean and atmosphere redox dynamics prior to the Great Oxidation Event (GOE). Unfortunately, the relatively limited Mo isotope database and small number of sample sets for Archean shales do not allow for in-depth reconstructions and specifically make it difficult to differentiate global from local effects. To accurately estimate the Mo isotope composition of Archean seawater and better investigate the systematics of local and global redox, more complete sample sets are needed. We carried out a Mo isotope analysis of the euxinic 2.65 Ga Roy Hill Shale sampled in two stratigraphically correlated cores, and revisited the well-studied euxinic 2.5 Ga Mt. McRae Shale in higher resolution. Our data show contrasting Mo isotope values in the 2.65 Ga Roy Hill Shale between near- and offshore depositional environments, with systematically heavier isotope values in the near-shore environment. High-resolution analysis of the Mt. McRae Shale yields oscillating Mo concentrations and isotope values at the cm- to dm-scale during the well-characterized "whiff of O2" interval, with the heaviest isotope values measured during euxinic deposition. Variations in the measured isotope values within each section are primarily associated with redox changes in the local depositional environment and amount of detrital content. Both non-quantitative removal of Mo associated with incorporation into non-euxinic sediments and large detrital Mo contributions shift some measured isotopic compositions toward lighter values. This is readily apparent in the near-shore Roy Hill Shale section and the Mt. McRae Shale, but may not fully explain variations observed in the offshore Roy Hill Shale deposit. Here, euxinic deposition is not accompanied by Mo enrichments or isotopic compositions as heavy as the near-shore equivalent, even after detrital correction. This disparity between the near- and offshore environment could signify spatial variation in the Mo isotope composition of 2.65 Ga seawater and highlights the need for multi-site and high-resolution studies in order to best assess paleoenvironmental conditions.

Cryogenic Calcite: A Morphologic and Isotopic Analog to the ALH84001 Carbonates

NASA Technical Reports Server (NTRS)

Niles, P. B.; Leshin, L. A.; Socki, R. A.; Guan, Y.; Ming, D. W.; Gibson, E. K.

2004-01-01

Martian meteorite ALH84001 carbonates preserve large and variable microscale isotopic compositions, which in some way reflect their formation environment. These measurements show large variations (>20%) in the carbon and oxygen isotopic compositions of the carbonates on a 10-20 micron scale that are correlated with chemical composition. However, the utilization of these data sets for interpreting the formation conditions of the carbonates is complex due to lack of suitable terrestrial analogs and the difficulty of modeling under non-equilibrium conditions. Thus, the mechanisms and processes are largely unknown that create and preserve large microscale isotopic variations in carbonate minerals. Experimental tests of the possible environments and mechanisms that lead to large microscale isotopic variations can help address these concerns. One possible mechanism for creating large carbon isotopic variations in carbonates involves the freezing of water. Carbonates precipitate during extensive CO2 degassing that occurs during the freezing process as the fluid s decreasing volume drives CO2 out. This rapid CO2 degassing results in a kinetic isotopic fractionation where the CO2 gas has a much lighter isotopic composition causing an enrichment of 13C in the remaining dissolved bicarbonate. This study seeks to determine the suitability of cryogenically formed carbonates as analogs to ALH84001 carbonates. Specifically, our objective is to determine how accurately models using equilibrium fractionation factors approximate the isotopic compositions of cryogenically precipitated carbonates. This includes determining the accuracy of applying equilibrium fractionation factors during a kinetic process, and determining how isotopic variations in the fluid are preserved in microscale variations in the precipitated carbonates.

Stable isotope study of a new chondrichthyan fauna (Kimmeridgian, Porrentruy, Swiss Jura): an unusual freshwater-influenced isotopic composition for the hybodont shark Asteracanthus

NASA Astrophysics Data System (ADS)

Leuzinger, L.; Kocsis, L.; Billon-Bruyat, J.-P.; Spezzaferri, S.; Vennemann, T.

2015-12-01

Chondrichthyan teeth (sharks, rays, and chimaeras) are mineralized in isotopic equilibrium with the surrounding water, and parameters such as water temperature and salinity can be inferred from the oxygen isotopic composition (δ18Op) of their bioapatite. We analysed a new chondrichthyan assemblage, as well as teeth from bony fish (Pycnodontiformes). All specimens are from Kimmeridgian coastal marine deposits of the Swiss Jura (vicinity of Porrentruy, Ajoie district, NW Switzerland). While the overall faunal composition and the isotopic composition of bony fish are generally consistent with marine conditions, unusually low δ18Op values were measured for the hybodont shark Asteracanthus. These values are also lower compared to previously published data from older European Jurassic localities. Additional analyses on material from Solothurn (Kimmeridgian, NW Switzerland) also have comparable, low-18O isotopic compositions for Asteracanthus. The data are hence interpreted to represent a so far unique, freshwater-influenced isotopic composition for this shark that is classically considered a marine genus. While reproduction in freshwater or brackish realms is established for other hybodonts, a similar behaviour for Asteracanthus is proposed here. Regular excursions into lower salinity waters can be linked to the age of the deposits and correspond to an ecological adaptation, most likely driven by the Kimmeridgian transgression and by the competition of the hybodont shark Asteracanthus with the rapidly diversifying neoselachians (modern sharks).

Stable isotope study of a new chondrichthyan fauna (Kimmeridgian, Porrentruy, Swiss Jura): an unusual freshwater-influenced isotopic composition for the hybodont shark Asteracanthus

NASA Astrophysics Data System (ADS)

Leuzinger, L.; Kocsis, L.; Billon-Bruyat, J.-P.; Spezzaferri, S.; Vennemann, T.

2015-08-01

Chondrichthyan teeth (sharks, rays and chimaeras) are mineralised in isotopic equilibrium with the surrounding water, and parameters such as water temperature and salinity can be inferred from the oxygen isotopic composition (δ18Op) of their bioapatite. We analysed a new chondrichthyan assemblage, as well as teeth from bony fish (Pycnodontiformes). All specimens are from Kimmeridgian coastal marine deposits of the Swiss Jura (vicinity of Porrentruy, Ajoie district, NW Switzerland). While the overall faunal composition and the isotopic composition of bony fish are consistent with marine conditions, unusually low δ18Op values were measured for the hybodont shark Asteracanthus. These values are also lower compared to previously published data from older European Jurassic localities. Additional analyses on material from Solothurn (Kimmeridgian, NW Switzerland) also have comparable, low-18O isotopic compositions for Asteracanthus. The data are hence interpreted to represent a so far unique, freshwater-influenced isotopic composition for this shark that is classically considered as a marine genus. While reproduction in freshwater or brackish realms is established for other hybodonts, a similar behaviour for Asteracanthus is proposed here. Regular excursions into lower salinity waters can be linked to the age of the deposits and correspond to an ecological adaptation, most likely driven by the Kimmeridgian transgression and by the competition of the primitive shark Asteracanthus with the rapidly diversifying neoselachians (modern sharks).

The earliest Lunar Magma Ocean differentiation recorded in Fe isotopes

NASA Astrophysics Data System (ADS)

Wang, Kun; Jacobsen, Stein B.; Sedaghatpour, Fatemeh; Chen, Heng; Korotev, Randy L.

2015-11-01

Recent high-precision isotopic measurements show that the isotopic similarity of Earth and Moon is unique among all known planetary bodies in our Solar System. These observations provide fundamental constraints on the origin of Earth-Moon system, likely a catastrophic Giant Impact event. However, in contrast to the isotopic composition of many elements (e.g., O, Mg, Si, K, Ti, Cr, and W), the Fe isotopic compositions of all lunar samples are significantly different from those of the bulk silicate Earth. Such a global Fe isotopic difference between the Moon and Earth provides an important constraint on the lunar formation - such as the amount of Fe evaporation as a result of a Giant Impact origin of the Moon. Here, we show through high-precision Fe isotopic measurements of one of the oldest lunar rocks (4.51 ± 0.10 Gyr dunite 72 415), compared with Fe isotope results of other lunar samples from the Apollo program, and lunar meteorites, that the lunar dunite is enriched in light Fe isotopes, complementing the heavy Fe isotope enrichment in other lunar samples. Thus, the earliest olivine accumulation in the Lunar Magma Ocean may have been enriched in light Fe isotopes. This new observation allows the Fe isotopic composition of the bulk silicate Moon to be identical to that of the bulk silicate Earth, by balancing light Fe in the deep Moon with heavy Fe in the shallow Moon rather than the Moon having a heavier Fe isotope composition than Earth as a result of Giant Impact vaporization.

The role of stable isotopes in understanding rainfall interception processes: a review

EPA Science Inventory

The isotopic composition of water transmitted by the canopy as throughfall or stemflow reflects important hydrologic processes occurring in the canopy. A synthesis of the literature shows that complex spatiotemporal variations of isotopic composition are created by canopy interce...

Metal stable isotopes in weathering and hydrology: Chapter 10

USGS Publications Warehouse

Bullen, Thomas D.; Holland, Heinrich; Turekian, K.

2014-01-01

This chapter highlights some of the major developments in the understanding of the causes of metal stable isotope compositional variability in and isotope fractionation between natural materials and provides numerous examples of how that understanding is providing new insights into weathering and hydrology. At this stage, our knowledge of causes of stable isotope compositional variability among natural materials is greatest for the metals lithium, magnesium, calcium, and iron, the isotopes of which have already provided important information on weathering and hydrological processes. Stable isotope compositional variability for other metals such as strontium, copper, zinc, chromium, barium, molybdenum, mercury, cadmium, and nickel has been demonstrated but is only beginning to be applied to questions related to weathering and hydrology, and several research groups are currently exploring the potential. And then there are other metals such as titanium, vanadium, rhenium, and tungsten that have yet to be explored for variability of stable isotope composition in natural materials, but which may hold untold surprises in their utility. This impressive list of metals having either demonstrated or potential stable isotope signals that could be used to address important unsolved questions related to weathering and hydrology, constitutes a powerful toolbox that will be increasingly utilized in the coming decades.

Quality assurance and quality control in light stable isotope laboratories: A case study of Rio Grande, Texas, water samples

USGS Publications Warehouse

Coplen, T.B.; Qi, H.

2009-01-01

New isotope laboratories can achieve the goal of reporting the same isotopic composition within analytical uncertainty for the same material analysed decades apart by (1) writing their own acceptance testing procedures and putting them into their mass spectrometric or laser-based isotope-ratio equipment procurement contract, (2) requiring a manufacturer to demonstrate acceptable performance using all sample ports provided with the instrumentation, (3) for each medium to be analysed, prepare two local reference materials substantially different in isotopic composition to encompass the range in isotopic composition expected in the laboratory and calibrated them with isotopic reference materials available from the International Atomic Energy Agency (IAEA) or the US National Institute of Standards and Technology (NIST), (4) using the optimum storage containers (for water samples, sealing in glass ampoules that are sterilised after sealing is satisfactory), (5) interspersing among sample unknowns local laboratory isotopic reference materials daily (internationally distributed isotopic reference materials can be ordered at three-year intervals, and can be used for elemental analyser analyses and other analyses that consume less than 1 mg of material) - this process applies to H, C, N, O, and S isotope ratios, (6) calculating isotopic compositions of unknowns by normalising isotopic data to that of local reference materials, which have been calibrated to internationally distributed isotopic reference materials, (7) reporting results on scales normalised to internationally distributed isotopic reference materials (where they are available) and providing to sample submitters the isotopic compositions of internationally distributed isotopic reference materials of the same substance had they been analysed with unknowns, (8) providing an audit trail in the laboratory for analytical results - this trail commonly will be in electronic format and might include a laboratory information management system, (9) making at regular intervals a complete backup of laboratory analytical data (both of samples logged into the laboratory and of mass spectrometric analyses), being sure to store one copy of this backup offsite, and (10) participating in interlaboratory comparison exercises sponsored by the IAEA and other agencies at regular intervals. ?? Taylor & Francis.

Using Redwood Tree Ring Chronologies to Obtain the Long-View on California's Coastal Climate

NASA Astrophysics Data System (ADS)

Dawson, T. E.; Roden, J. S.; Voelker, S. L.; Johnstone, J. A.; Ambrose, A.

2014-12-01

Coast redwood (Sequoia sempervirens) occupies a long and narrow range at the land-sea interface from the southern Big Bur region to the California-Oregon boarder. Since mature trees can live in excess of 2000 years, using the interannual variability in the oxygen and carbon stable isotope composition of tree rings obtained from trees growing in different parts of the redwood range holds the potential for obtaining a long-term record of California's coastal climate, including the history of temperatures, low cloud / fog, rainfall and associated climatic drivers of their variation. We analyzed the oxygen and carbon stable isotope composition of tree ring cellulose from both tree cores and whole cross-sectional slabs and compared these data to several regional climate indicies and to published growth chronologies to obtain the long-view on California's coastal climate. Several highlights will be presented and discussed. These include: (1) redwoods faithfully record water sources they use in the oxygen stable isotope composition of their tree ring cellulose; (2) these is both strong watershed- and regional-scale coherence; (3) redwood tree ring carbon isotope composition shows its strongest correlations to tree water status, stand-scale humidity, and at the regional scale to what we term "summer precipitation" anomalies (lack of rain with presence of fog); also (4) that carbon stable isotope composition is very sensitive to within tree and stand microclimate while oxygen stable isotope composition seems to be sensitive to topographic site factors like slope position and proximity to riparian / gully habitats; (5) multivariate climatic analyses reveal that summertime drought recorded in the isotope excursions are most strongly linked to atmospheric circulation anomalies; and (6) that redwood tree rings and their isotope composition provide great potential for reconstructing high-resolution paleo-climate along the California coast.

Rapid fusion method for the determination of refractory thorium and uranium isotopes in soil samples

DOE PAGES

Maxwell, Sherrod L.; Hutchison, Jay B.; McAlister, Daniel R.

2015-02-14

Recently, approximately 80% of participating laboratories failed to accurately determine uranium isotopes in soil samples in the U.S Department of Energy Mixed Analyte Performance Evaluation Program (MAPEP) Session 30, due to incomplete dissolution of refractory particles in the samples. Failing laboratories employed acid dissolution methods, including hydrofluoric acid, to recover uranium from the soil matrix. The failures illustrate the importance of rugged soil dissolution methods for the accurate measurement of analytes in the sample matrix. A new rapid fusion method has been developed by the Savannah River National Laboratory (SRNL) to prepare 1-2 g soil sample aliquots very quickly, withmore » total dissolution of refractory particles. Soil samples are fused with sodium hydroxide at 600 ºC in zirconium crucibles to enable complete dissolution of the sample. Uranium and thorium are separated on stacked TEVA and TRU extraction chromatographic resin cartridges, prior to isotopic measurements by alpha spectrometry on cerium fluoride microprecipitation sources. Plutonium can also be separated and measured using this method. Batches of 12 samples can be prepared for measurement in <5 hours.« less

Sources of Radioactive Isotopes for Dirty Bombs

NASA Astrophysics Data System (ADS)

Lubenau, Joel

2004-05-01

From the security perspective, radioisotopes and radioactive sources are not created equal. Of the many radioisotopes used in industrial applications, medical treatments, and scientific research, only eight, when present in relatively large amounts in radioactive sources, pose high security risks primarily because of their prevalence and physical properties. These isotopes are americium-241, californium-252, cesium-137, cobalt-60, iridium-192, radium-226, plutonium-238, and strontium-90. Except for the naturally occurring radium-226, nuclear reactors produce the other seven in bulk commercial quantities. Half of these isotopes emit alpha radiation and would, thus, primarily pose internal threats to health; the others are mainly high-energy gamma emitters and would present both external and internal health hazards. Therefore, the response to a "dirty bomb" event depends on what type of radioisotope is chosen and how it is employed. While only a handful of major corporations produce the reactor-generated radioisotopes, they market these materials to thousands of smaller companies and users throughout the world. Improving the security of the high-risk radioactive sources will require, among other efforts, cooperation among source suppliers and regulatory agencies.

Titanium stable isotope investigation of magmatic processes on the Earth and Moon

NASA Astrophysics Data System (ADS)

Millet, Marc-Alban; Dauphas, Nicolas; Greber, Nicolas D.; Burton, Kevin W.; Dale, Chris W.; Debret, Baptiste; Macpherson, Colin G.; Nowell, Geoffrey M.; Williams, Helen M.

2016-09-01

We present titanium stable isotope measurements of terrestrial magmatic samples and lunar mare basalts with the aims of constraining the composition of the lunar and terrestrial mantles and evaluating the potential of Ti stable isotopes for understanding magmatic processes. Relative to the OL-Ti isotope standard, the δ49Ti values of terrestrial samples vary from -0.05 to +0.55‰, whereas those of lunar mare basalts vary from -0.01 to +0.03‰ (the precisions of the double spike Ti isotope measurements are ca. ±0.02‰ at 95% confidence). The Ti stable isotope compositions of differentiated terrestrial magmas define a well-defined positive correlation with SiO2 content, which appears to result from the fractional crystallisation of Ti-bearing oxides with an inferred isotope fractionation factor of ΔTi49oxide-melt = - 0.23 ‰ ×106 /T2. Primitive terrestrial basalts show no resolvable Ti isotope variations and display similar values to mantle-derived samples (peridotite and serpentinites), indicating that partial melting does not fractionate Ti stable isotopes and that the Earth's mantle has a homogeneous δ49Ti composition of +0.005 ± 0.005 (95% c.i., n = 29). Eclogites also display similar Ti stable isotope compositions, suggesting that Ti is immobile during dehydration of subducted oceanic lithosphere. Lunar basalts have variable δ49Ti values; low-Ti mare basalts have δ49Ti values similar to that of the bulk silicate Earth (BSE) while high-Ti lunar basalts display small enrichment in the heavy Ti isotopes. This is best interpreted in terms of source heterogeneity resulting from Ti stable isotope fractionation associated with ilmenite-melt equilibrium during the generation of the mantle source of high-Ti lunar mare basalts. The similarity in δ49Ti between terrestrial samples and low-Ti lunar basalts provides strong evidence that the Earth and Moon have identical stable Ti isotope compositions.

The post-Paleozoic chronology and mechanism of 13C depletion in primary marine organic matter

NASA Technical Reports Server (NTRS)

Popp, B. N.; Takigiku, R.; Hayes, J. M.; Louda, J. W.; Baker, E. W.

1989-01-01

Carbon-isotopic compositions of geoporphyrins have been measured from marine sediments of Mesozoic and Cenozoic age in order to elucidate the timing and extent of depletion of 13C in marine primary producers. These results indicate that the difference in isotopic composition of coeval marine carbonates and marine primary photosynthate was approximately 5 to 7 permil greater during the Mesozoic and early Cenozoic than at present. In contrast to the isotopic record of marine primary producers, isotopic compositions of terrestrial organic materials have remained approximately constant for this same interval of time. This difference in the isotopic records of marine and terrestrial organic matter is considered in terms of the mechanisms controlling the isotopic fractionation associated with photosynthetic fixation of carbon. We show that the decreased isotopic fractionation between marine carbonates and organic matter from the Early to mid-Cenozoic may record variations in the abundance of atmospheric CO2.

Zirconium isotope constraints on the composition of Theia and current Moon-forming theories

NASA Astrophysics Data System (ADS)

Akram, W.; Schönbächler, M.

2016-09-01

The giant impact theory is the most widely recognized formation scenario of the Earth's Moon. Giant impact models based on dynamical simulations predict that the Moon acquired a significant amount of impactor (Theia) material, which is challenging to reconcile with geochemical data for O, Si, Cr, Ti and W isotopes in the Earth and Moon. Three new giant impact scenarios have been proposed to account for this discrepancy - hit-and-run impact, impact with a fast-spinning protoEarth and massive impactors - each one reducing the proportion of the impactor in the Moon compared to the original canonical giant impact model. The validity of each theory and their different dynamical varieties are evaluated here using an integrated approach that considers new high-precision Zr isotope measurements of lunar rocks, and quantitative geochemical modelling of the isotopic composition of the impactor Theia. All analysed lunar samples (whole-rock, ilmenite and pyroxene separates) display identical Zr isotope compositions to that of the Earth within the uncertainty of 13 ppm for 96Zr/90Zr (2σ weighted average). This 13 ppm upper limit is used to infer the most extreme isotopic composition that Theia could have possessed, relative to the Earth, for each of the proposed giant impact theories. The calculated Theian composition is compared with the Zr isotope compositions of different solar system materials in order to constrain the source region of the impactor. As a first order approximation, we show that all considered models (including the canonical) are plausible, alleviating the initial requirement for the new giant impact models. Albeit, the canonical and hit-and-run models are the most restrictive, suggesting that the impactor originated from a region close to the Earth. The fast-spinning protoEarth and massive impactor models are more relaxed and increase the allowed impactor distance from the Earth. Similar calculations carried out for O, Cr, Ti and Si isotope data support these conclusions but exclude a CI- and enstatite chondrite-like composition for Theia. Thus, the impactor Theia most likely had a Zr isotope composition close to that of the Earth, and this suggests that a large part of the inner solar system (or accretion region of the Earth, Theia and enstatite chondrites) had a uniform Zr isotope composition.

Isotopic compositions of cometary matter returned by Stardust.

PubMed

McKeegan, Kevin D; Aléon, Jerome; Bradley, John; Brownlee, Donald; Busemann, Henner; Butterworth, Anna; Chaussidon, Marc; Fallon, Stewart; Floss, Christine; Gilmour, Jamie; Gounelle, Matthieu; Graham, Giles; Guan, Yunbin; Heck, Philipp R; Hoppe, Peter; Hutcheon, Ian D; Huth, Joachim; Ishii, Hope; Ito, Motoo; Jacobsen, Stein B; Kearsley, Anton; Leshin, Laurie A; Liu, Ming-Chang; Lyon, Ian; Marhas, Kuljeet; Marty, Bernard; Matrajt, Graciela; Meibom, Anders; Messenger, Scott; Mostefaoui, Smail; Mukhopadhyay, Sujoy; Nakamura-Messenger, Keiko; Nittler, Larry; Palma, Russ; Pepin, Robert O; Papanastassiou, Dimitri A; Robert, François; Schlutter, Dennis; Snead, Christopher J; Stadermann, Frank J; Stroud, Rhonda; Tsou, Peter; Westphal, Andrew; Young, Edward D; Ziegler, Karen; Zimmermann, Laurent; Zinner, Ernst

2006-12-15

Hydrogen, carbon, nitrogen, and oxygen isotopic compositions are heterogeneous among comet 81P/Wild 2 particle fragments; however, extreme isotopic anomalies are rare, indicating that the comet is not a pristine aggregate of presolar materials. Nonterrestrial nitrogen and neon isotope ratios suggest that indigenous organic matter and highly volatile materials were successfully collected. Except for a single (17)O-enriched circumstellar stardust grain, silicate and oxide minerals have oxygen isotopic compositions consistent with solar system origin. One refractory grain is (16)O-enriched, like refractory inclusions in meteorites, suggesting that Wild 2 contains material formed at high temperature in the inner solar system and transported to the Kuiper belt before comet accretion.

Isotopic Analysis and Evolved Gases

NASA Technical Reports Server (NTRS)

Swindle, Timothy D.; Boynton, William V.; Chutjian, Ara; Hoffman, John H.; Jordan, Jim L.; Kargel, Jeffrey S.; McEntire, Richard W.; Nyquist, Larry

1996-01-01

Precise measurements of the chemical, elemental, and isotopic composition of planetary surface material and gases, and observed variations in these compositions, can contribute significantly to our knowledge of the source(s), ages, and evolution of solar system materials. The analyses discussed in this paper are mostly made by mass spectrometers or some other type of mass analyzer, and address three broad areas of interest: (1) atmospheric composition - isotopic, elemental, and molecular, (2) gases evolved from solids, and (3) solids. Current isotopic data on nine elements, mostly from in situ analysis, but also from meteorites and telescopic observations are summarized. Potential instruments for isotopic analysis of lunar, Martian, Venusian, Mercury, and Pluto surfaces, along with asteroid, cometary and icy satellites, surfaces are discussed.

Approaches to Plant Hydrogen and Oxygen Isoscapes Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

West, Jason B.; Kreuzer-Martin, Helen W.; Ehleringer, James

2009-12-01

Plant hydrogen and oxygen isoscapes have been utilized to address important and somewhat disparate research goals. The isotopic composition of leaf water affects the isotopic composition of atmospheric CO2 and O2 and is a logical starting point for understanding the isotopic composition of plant organic compounds since photosynthesis occurs in the leaf water environment. Leaf water isoscapes have been produced largely as part of efforts to understand atmospheric gas isotopic composition. The isotopic composition of plant organic matter has also been targeted for its potential to serve as a proxy for past environmental conditions. Spatially distributed sampling and modeling ofmore » modern plant H & O isoscapes can improve our understanding of the controls of the isotope ratios of compounds such as cellulose or n-alkanes from plants and therefore their utility for paleoreconstructions. Spatially varying plant hydrogen and oxygen isotopes have promise for yielding geographic origin information for a variety of plant products, including objects of criminal forensic interest or food products. The future has rich opportunities for the continued development of mechanistic models, methodologies for the generation of hydrogen and oxygen isoscapes, and cross-disciplinary interactions as these tools for understanding are developed, shared, and utilized to answer large-scale questions.« less

The evolution of 13C and 18O isotope composition of DIC in a calcite depositing film of water with isotope exchange between the DIC and a CO2 containing atmosphere, and simultaneous evaporation of the water. Implication to climate proxies from stalagmites: A theoretical model

NASA Astrophysics Data System (ADS)

Dreybrodt, Wolfgang; Romanov, Douchko

2016-12-01

The most widely applied climate proxies in speleothems are the isotope compositions of carbon and oxygen expressed by δ13C and δ18O values. However, mechanisms, which are not related to climate changes, overlay the climate signal. One is the temporal increase of both, δ13C and δ18O values by kinetic processes during precipitation of calcite. Isotope exchange between DIC in the water and the CO2 in the surrounding cave atmosphere can also change isotope composition. Here we present a theoretical model of the temporal isotope evolution of DIC in a thin water layer during precipitation of calcite and simultaneous isotope exchange with the cave atmosphere, and simultaneous evaporation of water. The exchange of oxygen isotopes in the DIC with those in the water is also considered.

Vaporization chemistry of hypo-stoichiometric (U,Pu)O 2

NASA Astrophysics Data System (ADS)

Viswanathan, R.; Krishnaiah, M. V.

2001-04-01

Calculations were performed on hypo-stoichiometric uranium plutonium di-oxide to examine its vaporization behavior as a function of O/ M ( M= U+ Pu) ratio and plutonium content. The phase U (1- y) Pu yO z was treated as an ideal solid solution of (1- y)UO 2+ yPuO (2- x) such that x=(2- z)/ y. Oxygen potentials for different desired values of y, z, and temperature were used as the primary input to calculate the corresponding partial pressures of various O-, U-, and Pu-bearing gaseous species. Relevant thermodynamic data for the solid phases UO 2 and PuO (2- x) , and the gaseous species were taken from the literature. Total vapor pressure varies with O/M and goes through a minimum. This minimum does not indicate a congruently vaporizing composition. Vaporization behavior of this system can at best be quasi-congruent. Two quasi-congruently vaporizing compositions (QCVCs) exist, representing the equalities (O/M) vapor=(O/M) mixed-oxide and (U/Pu) vapor=(U/Pu) mixed-oxide, respectively. The (O/M) corresponding to QCVC1 is lower than that corresponding to QCVC2, but very close to the value where vapor pressure minimum occurs. The O/M values of both QCVCs increase with decrease in plutonium content. The vaporization chemistry of this system, on continuous vaporization under dynamic condition, is discussed.

Heterogeneity of the Caribbean plateau mantle source: Sr, O and He isotopic compositions of olivine and clinopyroxene from Gorgona Island

NASA Astrophysics Data System (ADS)

Révillon, S.; Chauvel, C.; Arndt, N. T.; Pik, R.; Martineau, F.; Fourcade, S.; Marty, B.

2002-12-01

The composition of the mantle plumes that created large oceanic plateaus such as Ontong Java or the Caribbean is still poorly known. Geochemical and isotopic studies on accreted portions of the Caribbean plateau have shown that the plume source was heterogeneous and contained isotopically depleted and relatively enriched portions. A distinctive feature of samples from the Caribbean plateau is their unusual Sr isotopic compositions, which, at a given Nd isotopic ratio, are far higher than in samples from other oceanic plateaus. Sr, O and He isotopic compositions of whole rocks and magmatic minerals (clinopyroxene or olivine) separated from komatiites, gabbros and peridotites from Gorgona Island in Colombia were determined to investigate the origin of these anomalously radiogenic compositions. Sequentially leached clinopyroxenes have Sr isotopic compositions in the range 87Sr/ 86Sr=0.70271-0.70352, systematically lower than those of leached and unleached whole rocks. Oxygen isotopic ratios of clinopyroxene vary within the range δ 18O=5.18-5.35‰, similar to that recorded in oceanic island basalts. He isotopic ratios are high ( R/ Ra=8-19). The lower 87Sr/ 86Sr ratios of most of the clinopyroxenes shift the field of the Caribbean plateau in Nd-Sr isotope diagrams toward more 'normal' values, i.e. a position closer to the field defined by mid-ocean ridge basalts and oceanic-island basalts. Three clinopyroxenes have slightly higher 87Sr/ 86Sr ratios that cannot be explained by an assimilation model. The high 87Sr/ 86Sr and variations of 143Nd/ 144Nd are interpreted as a source characteristic. Trace-element ratios, however, are controlled mainly by fractionation during partial melting. We combine these isotopic data in a heterogeneous plume source model that accounts for the diversity of isotopic signatures recorded on Gorgona Island and throughout the Caribbean plateau. The heterogeneities are related to old recycled oceanic lithosphere in the plume source; the high 3He/ 4He ratios may indicate that the source material once resided in the lower mantle.

Nd Isotope and U-Th-Pb Age Mapping of Single Monazite Grains by Laser Ablation Split Stream Analysis

NASA Astrophysics Data System (ADS)

Fisher, C. M.; Hanchar, J. M.; Miller, C. F.; Phillips, S.; Vervoort, J. D.; Martin, W.

2015-12-01

Monazite is a common accessory mineral that occurs in medium to high grade metamorphic and Ca-poor felsic igneous rocks, and often controls the LREE budget (including Sm and Nd) of the host rock in which it crystallizes. Moreover, it contains appreciable U and Th, making it an ideal mineral for determining U-Th-Pb ages and Sm-Nd isotopic compositions, both of which are readily determined using in situ techniques with very high spatial resolution like LA-MC-ICPMS. Here, we present the results of laser ablation split stream analyses (LASS), which allows for simultaneous determination of the age and initial Nd isotopic composition in a single analysis. Analyses were done using a 20mm laser spot that allowed for detailed Nd isotope mapping of monazite grains (~30 analyses per ~250mm sized grain). Combined with LREE ratios (e.g., Sm/Nd, Ce/Gd, and Eu anomalies) these results yield important petrogenetic constraints on the evolution of peraluminous granites from the Old Woman-Piute batholith in southeastern California. Our findings also allow an improved understanding of the causes of isotope heterogeneity in granitic rocks. U-Th-Pb age mapping across the crystals reveals a single Cretaceous age for all grains with precision and accuracy typical of laser ablation analyses (~2%). In contrast, the concurrent Nd isotope mapping yields homogeneous initial Nd isotope compositions for some grains and large initial intra-grain variations of up to 8 epsilon units in others. The grains that yield homogeneous Nd isotope compositions have REE ratios suggesting that they crystallized in a fractionally crystallizing magma. Conversely, other grains, which also record fractional crystallization of both feldspar and LREE rich minerals, demonstrate a change in the Nd isotope composition of the magma during crystallization of monazite. Comparison of inter- and intra-grain Nd isotope compositions reveals further details on the potential mechanisms responsible for isotope heterogeneity present in single rock samples. This method highlights the potential of single grain isotope mapping of LREE phases such as monazite, allanite, and titanite for understanding both igneous and metamorphic petrogenesis.

Isotopic inferences of ancient biochemistries - Carbon, sulfur, hydrogen, and nitrogen

NASA Technical Reports Server (NTRS)

Schidlowski, M.; Hayes, J. M.; Kaplan, I. R.

1983-01-01

In processes of biological incorporation and subsequent biochemical processing sizable isotope effects occur as a result of both thermodynamic and kinetic fractionations which take place during metabolic and biosynthetic reactions. In this chapter a review is provided of earlier work and recent studies on isotope fractionations in the biogeochemical cycles of carbon, sulfur, hydrogen, and nitrogen. Attention is given to the biochemistry of carbon isotope fractionation, carbon isotope fractionation in extant plants and microorganisms, isotope fractionation in the terrestrial carbon cycle, the effects of diagenesis and metamorphism on the isotopic composition of sedimentary carbon, the isotopic composition of sedimentary carbon through time, implications of the sedimentary carbon isotope record, the biochemistry of sulfur isotope fractionation, pathways of the biogeochemical cycle of nitrogen, and the D/H ratio in naturally occurring materials.

Isotopic compositions of the elements 2013 (IUPAC Technical Report)

USGS Publications Warehouse

Meija, Juris; Coplen, Tyler B.; Berglund, Michael; Brand, Willi A.; De Bièvre, Paul; Gröning, Manfred; Holden, Norman E.; Irrgeher, Johanna; Loss, Robert D.; Walczyk, Thomas; Prohaska, Thomas

2016-01-01

The Commission on Isotopic Abundances and Atomic Weights (ciaaw.org) of the International Union of Pure and Applied Chemistry (iupac.org) has revised the Table of Isotopic Compositions of the Elements (TICE). The update involved a critical evaluation of the recent published literature. The new TICE 2013 includes evaluated data from the “best measurement” of the isotopic abundances in a single sample, along with a set of representative isotopic abundances and uncertainties that accommodate known variations in normal terrestrial materials.

Airborne Plutonium and non-natural Uranium from the Fukushima DNPP found at 120 km distance a few days after reactor hydrogen explosions.

PubMed

Shinonaga, Taeko; Steier, Peter; Lagos, Markus; Ohkura, Takehisa

2014-04-01

Plutonium (Pu) and non-natural uranium (U) originating from the Fukushima Daiichi Nuclear Power Plant (FDNPP) were identified in the atmosphere at 120 km distance from the FDNPP analyzing the ratio of number of atoms, following written as n(isotope)/n(isotope), of Pu and U. The n((240)Pu)/n((239)Pu), n((241)Pu)/n((239)Pu), n((234)U)/n((238)U), n((235)U)/n((238)U) and n((236)U)/n((238)U) in aerosol samples collected before and after the FDNPP incident were analyzed by accelerator mass spectrometry (AMS) and inductively coupled plasma mass spectrometry (ICPMS). The activity concentrations of (137)Cs and (134)Cs in the same samples were also analyzed by gamma spectrometry before the destructive analysis. Comparing the time series of analytical data on Pu and U obtained in this study with previously reported data on Pu, U, and radioactive Cs, we concluded that Pu and non-natural U from the FDNPP were transported in the atmosphere directly over a 120 km distance by aerosol and wind within a few days after the reactor hydrogen explosions. Effective dose of Pu were calculated using the data of Pu: (130 ± 21) nBq/m(3), obtained in this study. We found that the airborne Pu contributes only negligibly to the total dose at the time of the incident. However the analytical results show that the amount of Pu and non-natural U certainly increased in the environment after the incident.

Relationship between the trajectory of mid-latitude cyclones in the eastern Pacific Ocean and the isotopic composition of snowfall in the Sierra Nevada, California

NASA Astrophysics Data System (ADS)

Vasquez, K. T.; Sickman, J. O.; Heard, A.; Lucero, D.

2013-12-01

Diatoms, preserved in lake sediments, provide a potential archive of snowfall variability in the Sierra Nevada through their sensitivity to changes in water chemistry (a proxy for runoff volume) and by recording the isotopic composition of snow-melt (potentially a proxy for sources of atmospheric moisture). In the Sierra Nevada, we hypothesize that the oxygen isotopic composition of diatom silica is principally controlled by snow and that the isotopic composition of snow varies as a function of the tracks of mid-latitude cyclonic storms in the eastern Pacific Ocean. Snow samples from discrete storms were collected from December 2012 to March 2013 at 2042 meters a.s.l. in Sequoia National Park. The δ18O and δ2H values of the snow samples were measured using a temperature-conversion elemental analyzer coupled to a Delta V isotope ratio mass spectrometer. The isotopic measurements were then coupled to 3, 5 and 7-day air mass back trajectories using the NOAA HYSPLIT model. The measured δ18O values ranged from -17.6 to -7.8 per mil and the δ2H ranged from -119.8 to -73.3 per mil. Both δ18O and δ2H were inversely related to the latitude of the storm origin (R^2 values of 0.67 and 0.57, respectively). Winter storms from the Gulf of Alaska were the most isotopically depleted while storms originating in the subtropical/tropical Pacific were the most isotopically enriched, reflecting the overall latitudinal pattern of ocean-water isotope composition in the Pacific Ocean. Our results suggest that the isotopic composition of Sierra Nevada snowfall is influenced by storm track trajectory and this relationship could be useful in interpreting the climatic significance of δ18O of diatom silica preserved in lake cores.

Overview and Brief History of the Boron Isotope Proxy for Past Seawater pH

NASA Astrophysics Data System (ADS)

Hoenisch, B.; Hemming, G.

2007-05-01

In 1992 Hemming and Hanson (GCA, vol. 56, p. 537-543) showed that a variety of modern marine carbonates revealed a boron isotopic composition close to the isotopic composition of dissolved borate at modern seawater pH, suggesting this was the boron species preferentially adsorbed and incorporated into marine carbonates. With a constant offset between the trigonal and tetrahedrally coordinated boron species and a pH-dependent variation in their fractions, it appeared that this system would be sensitive to pH changes in the natural range of seawater. Accordingly, it was suggested that the boron isotope composition of marine carbonates is a proxy for past seawater pH. Subsequent culture studies with living planktic foraminifers and corals, as well as synthetic precipitation experiments confirmed that the boron isotopic composition follows the isotopic composition of borate across a wide range of seawater pH. In order to use the proxy with confidence, however, all other controls apart from pH need to be thoroughly understood. Recent laboratory and sediment experiments have demonstrated that vital effects and partial shell dissolution have the potential to modify the primary seawater pH signal recorded in the boron isotopic composition of planktic foraminifers. However it has also been shown that careful sample selection allows for avoiding these potential complications. A record of reconstructed surface seawater pH and estimated aqueous PCO2 shows a remarkable match between boron isotope based atmospheric pCO2 estimates and the Vostok ice core CO2 record. This convincingly demonstrates that boron isotopes in planktic foraminifers allow quantitative estimates of atmospheric pCO2 in the past, and confirms that glacial surface ocean pH was ~0.2 units higher compared to interglacial periods. We are going to review and discuss the achievements generated in Gil Hanson's lab over the past 15 years in the light of recent empirical measurements of the boron isotope fractionation between boric acid and borate in seawater.

Calibrating NIST SRM 683 as A New International Reference Standard for Zn Isotopes

NASA Astrophysics Data System (ADS)

Yang, Y.; Zhang, X.; Yu, H.; Huang, F.

2017-12-01

Zinc isotopes have been widely applied in the cosmochemical, geochemical, and environmental studies (Moynier et al. 2017). Obtaining precise Zn isotopic data for inter-laboratory comparison is a prerequisite to these applications. Currently, the JMC3-0749L is the primary reference standard for Zn isotopes (Albarède 2004), but it is not commercially available now. Thus, it is necessary to calibrate a new international primary reference standard for Zn isotopic analysis. Chen et al. (2016) showed that NIST SRM 683 (a pure Zn metal nugget of 140 grams) has a δ66ZnJMC of 0.12‰, which is falling within the range of natural Zn isotopic compositions, and it may a good candidate for the next generation of international reference standard (Chen et al. 2016). In order to further examine whether NIST SRM 683 has a homogeneous Zn isotopic composition, we measured more NIST SRM 683 by double-spike methods using MC-ICPMS (Conway et al. 2013). The metal nuggets of NIST SRM 683 were intensively sampled by micro-drilling. Zinc isotope analyses for two nuggets show that they have δ66Zn of 0.14 ± 0.02‰ (2SD, N = 32) and 0.13 ± 0.02‰ (2SD, N = 33), respectively. These values are similar to those of two Zn metal nuggets (0.11 ± 0.02‰ vs. 0.12 ± 0.02‰) reported previously by Chen et al. (2016). We fully dissolved one nugget, producing pure Zn solution with identical Zn isotopic composition with the drilling samples. All results strongly support that NIST SRM 683 is homogeneous in Zn isotopic compositions which could be an ideal candidate for the next reference for Zn isotopes. Tests on more metal nuggets will be performed in a few months for further confirming the Zn isotope compositions and homogeneity. Reference: Albarède et al., 2004. 'The stable isotope geochemistry of copper and zinc', Reviews in Mineralogy and Geochemistry, 55: 409-27. Chen et al., 2016. 'Zinc Isotopic Compositions of NIST SRM 683 and Whole-Rock Reference Materials', Geostandards and Geoanalytical Research, 40: 417-32. Conway et al., 2013. 'A new method for precise determination of iron, zinc and cadmium stable isotope ratios in seawater by double-spike mass spectrometry', Analytica chimica acta, 793: 44-52. Moynier et al., 2017. 'The isotope geochemistry of zinc and copper', Reviews in Mineralogy and Geochemistry, 82: 543-600.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Conroy, Jessica L; Cobb, Kim M; Noone, David

The objective of this field campaign was to investigate climatic controls on the stable isotopic composition of water vapor, precipitation, and seawater in the western tropical Pacific. Simultaneous measurements of the stable isotopic composition of vapor and precipitation from April 28 to May 8, 2013, at the Manus Tropical Western Pacific Atmospheric Radiation Measurement site, provided several key insights into the nature of the climate signal archived in precipitation and vapor isotope ratios. We observed a large shift from lower to higher isotopic values in vapor and precipitation because of the passage of a mesoscale convective system west of themore » site and a transition from a regional stormy period into a more quiescent period. During the quiescent period, the stable isotopic composition of vapor and precipitation indicated the predominance of oceanic evaporation in determining the isotopic composition of boundary-layer vapor and local precipitation. There was not a consistent relationship between intra-event precipitation amount at the site and the stable isotopic composition of precipitation, thus challenging simplified assumptions about the isotopic “amount effect” in the tropics on the time scale of individual storms. However, some storms did show an amount effect, and deuterium excess values in precipitation had a significant relationship with several meteorological variables, including precipitation, temperature, relative humidity, and cloud base height across all measured storms. The direction of these relationships points to condensation controls on precipitation deuterium excess values on intra-event time scales. The relationship between simultaneous measurements of vapor and precipitation isotope ratios during precipitation events indicates the ratio of precipitation-to-vapor isotope ratios can diagnose precipitation originating from a vapor source unique from boundary-layer vapor and rain re-evaporation.« less

Origin of heavy Fe isotope compositions in high-silica igneous rocks: A rhyolite perspective

NASA Astrophysics Data System (ADS)

Du, De-Hong; Wang, Xiao-Lei; Yang, Tao; Chen, Xin; Li, Jun-Yong; Li, Weiqiang

2017-12-01

The origin of heavy Fe isotope compositions in high-silica (>70 wt% SiO2) igneous rocks remains a highly controversial topic. Considering that fluid exsolution in eruptive rocks is more straight-forward to constrain than in plutonic rocks, this study addresses the problem of Fe isotope fractionation in high-silica igneous rocks by measuring Fe isotope compositions of representative rhyolitic samples from the Neoproterozoic volcanic-sedimentary basins in southern China and the Triassic Tu Le Basin in northern Vietnam. The samples show remarkably varied δ56FeIRMM014 values ranging from 0.05 ± 0.05‰ to 0.55 ± 0.05‰, which is among the highest values reported from felsic rocks. The extensional tectonic setting and short melt residence time in magma chambers for the studied rhyolites rule out Soret diffusion and thermal migration processes as causes of the high δ56Fe values. Effects of volcanic degassing and fluid exsolution on bulk rock δ56Fe values for the rhyolites are also assessed using bulk rock geochemical indicators and Rayleigh fractionation models, and these processes are found to be insufficient to produce resolvable changes in Fe isotope compositions of the residual melt. The most probable mechanism accounting for heavy Fe isotope compositions in the high-silica rhyolites is narrowed down to fractional crystallization processes in the magma before rhyolite eruption. Removal of isotopically light Fe-bearing minerals (i.e. ulvöspinel-rich titanomagnetite, ilmenite and biotite) is proposed as the main cause of Fe isotope variation in silicic melts during magmatic evolution. This study implies that crystal fractionation is the dominant mechanism that controls Fe isotope fractionation in eruptive rocks and Fe isotopes could be used to study magmatic differentiation of high-silica magmas.

High-precision 87Sr/86Sr analyses in wines and their use as a geological fingerprint for tracing geographic provenance.

PubMed

Marchionni, Sara; Braschi, Eleonora; Tommasini, Simone; Bollati, Andrea; Cifelli, Francesca; Mulinacci, Nadia; Mattei, Massimo; Conticelli, Sandro

2013-07-17

The radiogenic isotopic compositions of inorganic heavy elements such as Sr, Nd, and Pb of the food chain may constitute a reliable geographic fingerprint, their isotopic ratios being inherited by the geological substratum of the territory of production. The Sr isotope composition of geomaterials (i.e., rocks and soils) is largely variable, and it depends upon the age of the rocks and their nature (e.g., genesis, composition). In this study we developed a high-precision analytical procedure for determining Sr isotopes in wines at comparable uncertainty levels of geological data. With the aim of verifying the possibility of using Sr isotope in wine as a reliable tracer for geographic provenance, we performed Sr isotope analyses of 45 bottled wines from four different geographical localities of the Italian peninsula. Their Sr isotope composition has been compared with that of rocks from the substrata (i.e., rocks) of their vineyards. In addition wines from the same winemaker but different vintage years have been analyzed to verify the constancy with time of the (87)Sr/(86)Sr. Sr isotope compositions have been determined by solid source thermal ionization mass spectrometry following purification of Sr in a clean laboratory. (87)Sr/(86)Sr of the analyzed wines is correlated with the isotopic values of the geological substratum of the vineyards, showing little or no variation within the same vineyard and among different vintages. Large (87)Sr/(86)Sr variation is observed among wines from the different geographical areas, reinforcing the link with the geological substratum of the production territory. This makes Sr isotopes a robust geochemical tool for tracing the geographic authenticity and provenance of wine.

Laboratory-based characterization of plutonium in soil particles using micro-XRF and 3D confocal XRF

DOE PAGES

McIntosh, Kathryn Gallagher; Cordes, Nikolaus Lynn; Patterson, Brian M.; ...

2015-03-29

The investigation of plutonium (Pu) in a soil matrix is of interest in safeguards, nuclear forensics, and environmental remediation activities. The elemental composition of two plutonium contaminated soil particles was characterized nondestructively using a pair of micro X-ray fluorescence spectrometry (micro-XRF) techniques including high resolution X-ray (hiRX) and 3D confocal XRF. The three dimensional elemental imaging capability of confocal XRF permitted the identification two distinct Pu particles within the samples: one external to the Ferich soil matrix and another co-located with Cu within the soil matrix. The size and morphology of the particles was assessed with X-ray transmission microscopy andmore » micro X-ray computed tomography (micro-CT) providing complementary morphological information. Limits of detection for a 30 μm Pu particle are <10 ng for each of the XRF techniques. Ultimately, this study highlights the capability for lab-based, nondestructive, spatially resolved characterization of heterogeneous matrices on the micrometer scale with nanogram sensitivity.« less

Effect Of Substrates On The Fractionation Of Hydrogen Isotopes During Lipid-Biosynthesis By Haloarcula marismortui

NASA Astrophysics Data System (ADS)

Dirghangi, S. S.; Pagani, M.

2010-12-01

Lipids form an important class of proxies for paleoclimatological research, and hydrogen isotope ratios of lipids are being increasingly used for understanding changes in the hydrological system. Proper understanding of hydrogen isotope fractionation during lipid biosynthesis is therefore important and attention has been directed toward understanding the magnitude of hydrogen isotope fractionation that occurs during lipid biosynthesis in various organisms. Hydrogen isotope ratios of lipids depend on the hydrogen isotopic composition of the ambient water, hydrogen isotopic composition of NADPH used during biosynthesis, growth conditions, pathways of lipid biosynthesis, and substrates in the case of heterotrophic organisms. Recently it has been observed that NADPH contributes a significant part of the hydrogen in fatty acids synthesized by bacteria during heterotrophic growth (Zhang et al, 2009). As NADPH is formed by reduction of NADP+ during metabolism of substrates, different metabolic pathways form NADPH with different D/H ratios, which in turn results in variation in D/H ratios of lipids (Zhang et al, 2009). Therefore, substrates play a significant role in hydrogen isotopic compositions of lipids. For this study, we are investigating the effects of substrates on hydrogen isotope fractionation during biosynthesis of isoprenoidal lipids by heterotrophically growing halophilic archaea. Haloarcula marismortui is a halophilic archaea which synthesizes Archaeol (a diether lipid) and other isoprenoidal lipids. We have grown Haloarcula marismortui in pure cultures on three different substrates and are in the process of evaluating isotopic variability of Archaeol and other lipids associated with substrate and the D/H composition of ambient water. Our results will be helpful for a better understanding of hydrogen isotope fractionations during lipid synthesis by archaea. Also, halophilic archaea are the only source of archaeol in hypersaline environments. Therefore, our results will also indicate whether archaeol can be used as a proxy of ambient water hydrogen isotopic compositions in hypersaline environments.

A carbon isotope mass balance for an anoxic marine sediment: Isotopic signatures of diagenesis

NASA Technical Reports Server (NTRS)

Boehme, Susan E.

1993-01-01

A carbon isotope mass balance was determined for the sediments of Cape Lookout Bight, NC to constrain the carbon budgets published previously. The diffusive, ebullitive and burial fluxes of sigma CO2 and CH4, as well as the carbon isotope signatures of these fluxes, were measured. The flux-weighted isotopic signature of the remineralized carbon (-18.9 plus or minus 2.7 per mil) agreed with the isotopic composition of the remineralized organic carbon determined from the particulate organic carbon (POC) delta(C-13) profiles (-19.2 plus or minus 0.2), verifying the flux and isotopic signature estimates. The measured delta(C-13) values of the sigma CO2 and CH4 diffusive fluxes were significantly different from those calculated from porewater gradients. The differences appear to be influenced by methane oxidation at the sediment-water interface, although other potential processes cannot be excluded. The isotope mass balance provides important information concerning the locations of potential diagenetic isotope effects. Specifically, the absence of downcore change in the delta(C-13) value of the POC fraction and the identical isotopic composition of the POC and the products of remineralization indicate that no isotopic fractionation is expressed during the initial breakdown of the POC, despite its isotopically heterogeneous composition.

Spacecraft measurements of the elemental and isotopic composition of solar energetic particles

NASA Technical Reports Server (NTRS)

Mewaldt, R. A.

1980-01-01

Within the past few years, instruments flown on satellites and space probes have made significant progress in measuring the elemental and isotopic composition of energetic heavy nuclei accelerated in solar flares. These new observations are discussed, focusing on: (1) the energy dependence of the elemental composition at energies not greater than 1 MeV/nucleon; (2) flare to flare variations in the composition; and (3) comparisons of the average solar particle abundances (Z not less than 2 and not greater than 28) with other measures of the solar composition, including photospheric, coronal, and solar wind observations. These comparisons have led to the suggestion that solar flares sample the composition of the corona. Isotopic measurements of heavy solar flare nuclei have recently added a new dimension to these studies. In particular, the isotopic composition of solar flare neon has been found to be significantly different from that measured in the solar wind, but consistent with the meteoritic component neon-A.

IER 203 CED-2 Report: LLNL Final Design for BERP Ball With a Composite Reflector of Thin Polyethylene Backed by Nickel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Percher, C. M.; Heinrichs, D. P.; Kim, S. K.

2016-07-18

This report documents the results of final design (CED-2) for IER 203, BERP Ball Composite Reflection, and focuses on critical configurations with a 4.5 kg α-phase plutonium sphere reflected by a combination of thin high-density polyethylene (HDPE) backed by a thick nickel reflector. The Lawrence Livermore National Laboratory’s (LLNL’s) Nuclear Criticality Safety Division, in support of fissile material operations, calculated surprisingly reactive configurations when a fissile core was surrounded by a thin, moderating reflector backed by a thick metal reflector. These composite reflector configurations were much more reactive than either of the single reflector materials separately. The calculated findings havemore » resulted in a stricter-than-anticipated criticality control set, impacting programmatic work. IER 203 was requested in response to these seemingly anomalous calculations to see if the composite reflection effect could be shown experimentally. This report focuses on the Beryllium Reflected Plutonium (BERP) ball as a fissile material core reflected by polyethylene and nickel. A total of four critical configurations were designed as part of CED-2. Fabrication costs are estimated to be $98,500, largely due to the cost of the large nickel reflectors. The IER 203 experiments could reasonably be expected to begin in early FY2017.« less

Individual Radiological Protection Monitoring of Utrok Atoll Residents Based on Whole Body Counting of Cesium-137 (137Cs) and Plutonium Bioassay

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hamilton, T; Kehl, S; Brown, T

2007-06-08

This report contains individual radiological protection surveillance data developed during 2006 for adult members of a select group of families living on Utrok Atoll. These Group I volunteers all underwent a whole-body count to determine levels of internally deposited cesium-137 ({sup 137}Cs) and supplied a bioassay sample for analysis of plutonium isotopes. Measurement data were obtained and the results compared with an equivalent set of measurement data for {sup 137}Cs and plutonium isotopes from a second group of adult volunteers (Group II) who were long-term residents of Utrok Atoll. For the purposes of this comparison, Group II volunteers were consideredmore » representative of the general population on Utrok Atoll. The general aim of the study was to determine residual systemic burdens of fallout radionuclides in each volunteer group, develop data in response to addressing some specific concerns about the preferential uptake and potential health consequences of residual fallout radionuclides in Group I volunteers, and generally provide some perspective on the significance of radiation doses delivered to volunteers (and the general Utrok Atoll resident population) in terms of radiological protection standards and health risks. Based on dose estimates from measurements of internally deposited {sup 137}Cs and plutonium isotopes, the data and information developed in this report clearly show that neither volunteer group has acquired levels of internally deposited fallout radionuclides specific to nuclear weapons testing in the Marshall Islands that are likely to have any consequence on human health. Moreover, the dose estimates are well below radiological protection standards as prescribed by U.S. regulators and international agencies, and are very small when compared to doses from natural sources of radiation in the Marshall Islands and the threshold where radiation health effects could be either medically diagnosed in an individual or epidemiologically discerned in a group of people. In general, the results from the whole-body counting measurements of 137Cs are consistent with our knowledge that a key pathway for exposure to residual fallout contamination on Utrok Atoll is low-level chronic uptake of {sup 137}Cs from the consumption of locally grown produce (Robison et al., 1999). The error-weighted, average body burden of {sup 137}Cs measured in Group I and Group II volunteers was 0.31 kBq and 0.62 kBq, respectively. The associated average, annual committed effective dose equivalent (CEDE) delivered to Group I and Group II volunteers from {sup 137}Cs during the year of measurement was 2.1 and 4.0 mrem. For comparative purposes, the annual dose limit for members of the public as recommended by the National Council on Radiation Protection and Measurements (NCRP) and the International Commission on Radiological Protection (ICRP) is 100 mrem. Consequently, specific concerns about elevated levels of {sup 137}Cs uptake and higher risks from radiation exposure to Group I volunteers would be considered unfounded. Moreover, the urinary excretion of plutonium-239 ({sup 239}Pu) from Group I and Group II volunteers is statistically indistinguishable. In this case, the error-weighted, average urinary excretion of {sup 239}Pu from Group I volunteers of 0.10 {mu}Bq per 24-h void with a range between -0.01 and 0.23 {mu}Bq per 24-h void compares with an error-weighted average from Group II volunteers of 0.11 {mu}Bq per 24-h void with a range between -0.20 and 0.47 {mu}Bq per 24-h void. The range in urinary excretion of {sup 239}Pu from Utrok Atoll residents is very similar to that observed for other population groups in the Marshall Islands (Bogen et al., 2006; Hamilton et al., 2006a; 2006b; 2006c, 2007a; 2007b; 2007c) and is generally considered representative of worldwide background.« less

Origin of petroporphyrins. 2. Evidence from stable carbon isotopes

NASA Technical Reports Server (NTRS)

Boreham, C. J.; Fookes, C. J.; Popp, B. N.; Hayes, J. M.

1990-01-01

Compared with the carbon-13 isotopic composition of the ubiquitous C32DPEP (DPEP, deoxophylloerythroetioporphyrin) the heavy but equivalent carbon-13 isotopic composition for the porphyrin structures 15(2)-methyl-15,17-ethano-17-nor-H-C30DPEP and 15,17-butano-, 13,15-ethano-13(2),17-propano-, and 13(1)-methyl-13,15-ethano-13(2),17-propanoporphyrin suggests a common precursor, presumably chlorophyll c, for these petroporphyrins isolated from the marine Julia Creek oil shale and the lacustrine Condor oil shale. Similarly, the heavy but variable carbon-13 isotopic composition of 7-nor-H-C31DPEP compared with C32DPEP is consistent with an origin from both chlorophyll b and chlorophyll c3. The equivalent carbon-13 isotopic composition for 13(2)-methyl-C33DPEP compared with C32DPEP suggests a common origin resulting from a weighted average of chlorophyll inputs.

New technique for study on isotopic fractionation between sea water and foraminiferal growing processes

NASA Astrophysics Data System (ADS)

Cang, Shuxi; Shackleton, N. J.

1990-12-01

The stable isotopic δ18O and δ13C composition of foraminiferal shell calcite varies as a function of many factors including temperature and salinity. In order to understand and interpret the variations in the isotopic composition of foraminiferal shell calcite, research has been recently focused on the role of the “vital effects”. Our examination of the lamella structure of several recent planktonic foraminifera indicates that the secretion of sequential lamellae results in multiple lamillae on earlier chambers and a single lamella on the final chamber. We used a very simple procedure to separate the individual whole test of foraminifera into several chambers and measured the isotopic composition of each growth stage chamber. The results indicate that the stable isotopic composition (carbon and oxygen), particularly that of the last two chambers, of the foraminiferal test varies as a function of the individual growing process.

Hafnium isotope stratigraphy of ferromanganese crusts

PubMed

Lee; Halliday; Hein; Burton; Christensen; Gunther

1999-08-13

A Cenozoic record of hafnium isotopic compositions of central Pacific deep water has been obtained from two ferromanganese crusts. The crusts are separated by more than 3000 kilometers but display similar secular variations. Significant fluctuations in hafnium isotopic composition occurred in the Eocene and Oligocene, possibly related to direct advection from the Indian and Atlantic oceans. Hafnium isotopic compositions have remained approximately uniform for the past 20 million years, probably reflecting increased isolation of the central Pacific. The mechanisms responsible for the increase in (87)Sr/(86)Sr in seawater through the Cenozoic apparently had no effect on central Pacific deep-water hafnium.

A Sr and Mg isotopic study of soil and stream waters along an erosional gradient, Sierra Nevada, California

NASA Astrophysics Data System (ADS)

Rosen, V. B.; Maher, K.; Kouba, C. M.; Weinman, B. A.; Yoo, K.; Mudd, S. M.

2012-12-01

Since chemical weathering rates are proposed to regulate atmospheric CO2 concentrations and by extension global temperature over geologic timescales, understanding the relationship between chemical weathering rates and physical erosion is crucial to accurately interpreting Earth's climate history. The rate of supply of fresh minerals to the weathering zone is known to be an important control on chemical weathering rates. However, the consequences of physical erosion on the isotopic composition of weathering-derived solutes are more difficult to assess. This study capitalizes on a series of granitic hillslope transects with different erosion rates but similar climate, vegetation, and bedrock, in order to assess the consequences of erosion on the Sr and Mg isotopic composition of solutes. Reactive transport model simulations of varying complexity have been used to complement the field measurements and to analyze the sensitivity of fluid isotopic compositions to changes in key parameters such as erosion rate, flow rate, and biological cycling. The three hillslopes in the Feather River Basin, California reflect different degrees of channel erosion at their bases—BRC is a hillslope with active channel incision (60% average slope, below the knickpoint), FTA is a hillslope reflecting the transition between the relict and modern-day incising areas (50% average slope, at the knickpoint), and POMD is a 30% average hillslope in the relict landscape above the knickpoint. We measured the major element compositions, as well as the Sr and Mg isotopic compositions of soil water leaches (deionized water leaches), lysimeters, stream waters, and groundwaters by multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). The 87Sr/86Sr values of soil and stream waters show minimal variation (0.7042 to 0.7046) as a function of soil depth, erosion rate, or sampling season despite abundant radiogenic biotite in the profiles. These results agree with the reactive transport model predictions at high erosion rates, and suggest that soil residence times and isotopic equilibrium times are too short for biotite weathering to influence the solute isotopic composition. In contrast, model results for δ26Mg of the soil waters and minerals suggest that the Mg isotopic composition of the solute changes as a function of erosion rate because of shorter isotopic equilibrium length scales at higher erosion rates. The isotopic reactive transport modeling, combined with hillslope depth profiles and stream water analyses, provides a useful approach for linking the isotopic composition of solutes to erosion rates. This study may provide insights into past and present riverine isotopic compositions, and contribute to our understanding of how surface processes have influenced past atmospheric conditions.

Importance of depth and intensity of convection on the isotopic composition of water vapor as seen from IASI and TES δD observations

NASA Astrophysics Data System (ADS)

Lacour, Jean-Lionel; Risi, Camille; Worden, John; Clerbaux, Cathy; Coheur, Pierre-François

2018-01-01

We use tropical observations of the water vapor isotopic composition, derived from IASI and TES spaceborne measurements, to show that the isotopic composition of water vapor in the free troposphere is sensitive to both the depth and the intensity of convection. We find that for any given precipitation intensity, vapor associated with deep convection is isotopically depleted relative to vapor associated with shallow convection. The intensity of precipitation also plays a role as for any given depth of convection, the relative enrichment of water vapor decreases as the intensity of precipitation increases. Shallow convection, via the uplifting of enriched boundary layer air into the free troposphere and the convective detrainment, enriches the free troposphere. In contrast, deep convection is associated with processes that deplete the water vapor in the free troposphere, such as rain re-evaporation. The results of this study allow for a better identification of the parameters controlling the isotopic composition of the free troposphere and indicate that the isotopic composition of water vapor can be used to evaluate the relative contributions of shallow and deep convection in global models.

Magnesium isotope evidence that accretional vapour loss shapes planetary compositions

PubMed Central

Hin, Remco C.; Coath, Christopher D.; Carter, Philip J.; Nimmo, Francis; Lai, Yi-Jen; Pogge von Strandmann, Philip A.E.; Willbold, Matthias; Leinhardt, Zoë M.; Walter, Michael J.; Elliott, Tim

2017-01-01

It has long been recognised that Earth and other differentiated planetary bodies are chemically fractionated compared to primitive, chondritic meteorites and by inference the primordial disk from which they formed. An important question has been whether the notable volatile depletions of planetary bodies are a consequence of accretion1, or inherited from prior nebular fractionation2. The isotopic compositions of the main constituents of planetary bodies can contribute to this debate3–6. Using a new analytical approach to address key issues of accuracy inherent in conventional methods, we show that all differentiated bodies have isotopically heavier magnesium compositions than chondritic meteorites. We argue that possible magnesium isotope fractionation during condensation of the solar nebula, core formation and silicate differentiation cannot explain these observations. However, isotopic fractionation between liquid and vapour followed by vapour escape during accretionary growth of planetesimals generates appropriate residual compositions. Our modelling implies that the isotopic compositions of Mg, Si and Fe and the relative abundances of the major elements of Earth, and other planetary bodies, are a natural consequence of substantial (~40% by mass) vapour loss from growing planetesimals by this mechanism. PMID:28959965

A rapid method for estimation of Pu-isotopes in urine samples using high volume centrifuge.

PubMed

Kumar, Ranjeet; Rao, D D; Dubla, Rupali; Yadav, J R

2017-07-01

The conventional radio-analytical technique used for estimation of Pu-isotopes in urine samples involves anion exchange/TEVA column separation followed by alpha spectrometry. This sequence of analysis consumes nearly 3-4 days for completion. Many a times excreta analysis results are required urgently, particularly under repeat and incidental/emergency situations. Therefore, there is need to reduce the analysis time for the estimation of Pu-isotopes in bioassay samples. This paper gives the details of standardization of a rapid method for estimation of Pu-isotopes in urine samples using multi-purpose centrifuge, TEVA resin followed by alpha spectrometry. The rapid method involves oxidation of urine samples, co-precipitation of plutonium along with calcium phosphate followed by sample preparation using high volume centrifuge and separation of Pu using TEVA resin. Pu-fraction was electrodeposited and activity estimated using 236 Pu tracer recovery by alpha spectrometry. Ten routine urine samples of radiation workers were analyzed and consistent radiochemical tracer recovery was obtained in the range 47-88% with a mean and standard deviation of 64.4% and 11.3% respectively. With this newly standardized technique, the whole analytical procedure is completed within 9h (one working day hour). Copyright © 2017 Elsevier Ltd. All rights reserved.

Spatial patterns of throughfall isotopic composition at the event and seasonal timescales

NASA Astrophysics Data System (ADS)

Allen, Scott T.; Keim, Richard F.; McDonnell, Jeffrey J.

2015-03-01

Spatial variability of throughfall isotopic composition in forests is indicative of complex processes occurring in the canopy and remains insufficiently understood to properly characterize precipitation inputs to the catchment water balance. Here we investigate variability of throughfall isotopic composition with the objectives: (1) to quantify the spatial variability in event-scale samples, (2) to determine if there are persistent controls over the variability and how these affect variability of seasonally accumulated throughfall, and (3) to analyze the distribution of measured throughfall isotopic composition associated with varying sampling regimes. We measured throughfall over two, three-month periods in western Oregon, USA under a Douglas-fir canopy. The mean spatial range of δ18O for each event was 1.6‰ and 1.2‰ through Fall 2009 (11 events) and Spring 2010 (7 events), respectively. However, the spatial pattern of isotopic composition was not temporally stable causing season-total throughfall to be less variable than event throughfall (1.0‰; range of cumulative δ18O for Fall 2009). Isotopic composition was not spatially autocorrelated and not explained by location relative to tree stems. Sampling error analysis for both field measurements and Monte-Carlo simulated datasets representing different sampling schemes revealed the standard deviation of differences from the true mean as high as 0.45‰ (δ18O) and 1.29‰ (d-excess). The magnitude of this isotopic variation suggests that small sample sizes are a source of substantial experimental error.

What controls silicon isotope fractionation during dissolution of diatom opal?

NASA Astrophysics Data System (ADS)

Wetzel, F.; de Souza, G. F.; Reynolds, B. C.

2014-04-01

The silicon isotope composition of opal frustules from photosynthesising diatoms is a promising tool for studying past changes in the marine silicon cycle, and indirectly that of carbon. Dissolution of this opal may be accompanied by silicon isotope fractionation that could disturb the pristine silicon isotope composition of diatom opal acquired in the surface ocean. It has previously been shown that dissolution of fresh and sediment trap diatom opal in seawater does fractionate silicon isotopes. However, as the mechanism of silicon isotope fractionation remained elusive, it is uncertain whether opal dissolution in general is associated with silicon isotope fractionation considering that opal chemistry and surface properties are spatially and temporally (i.e. opal of different age) diverse. In this study we dissolved sediment core diatom opal in 5 mM NaOH and found that this process is not associated with significant silicon isotope fractionation. Since no variability of the isotope effect was observed over a wide range of dissolution rates, we can rule out the suggestion that back-reactions had a significant influence on the net isotope effect. Similarly, we did not observe an impact of temperature, specific surface area, or degree of undersaturation on silicon isotope partitioning during dissolution, such that these can most likely also be ruled out as controlling factors. We discuss the potential impacts of the chemical composition of the dissolution medium and age of diatom opal on silicon isotope fractionation during dissolution. It appears most likely that the controlling mechanism of silicon isotope fractionation during dissolution is related to the reactivity, or potentially, aluminium content of the opal. Such a dependency would imply that silicon isotope fractionation during dissolution of diatom opal is spatially and temporally variable. However, since the isotope effects during dissolution are small, the silicon isotope composition of diatom opal appears to be robust against dissolution in the deep sea sedimentary environment.

Characteristics of Martian Crustal Materials and Implications for Magmatic Assimilation: Preliminary Re-Os Isotope and Highly Siderophile Element Abundance Data for Nakhlites and Tissint

NASA Astrophysics Data System (ADS)

Mari, N.; Riches, A. J. V.; Hallis, L. J.; Lee, M. R.

2017-07-01

This project, for the first time, aims to integrate nakhlite Os-isotope compositions and HSE abundance data with S-isotope compositions for sample fractions for which textural information is constrained prior to destructive analyses.

Isotopic Composition of Barium in Single Presolar Silicon Carbide Grains

NASA Technical Reports Server (NTRS)

Savina, M. R.; Tripa, C. E.; Pellin, M. J.; Davis, A. M.; Clayton, R. N.; Lewis, R. S.; Amari, S.

2002-01-01

We have measured Ba isotope distributions in individual presolar SiC grains. We find that the Ba isotopic composition in mainstream SiC grains is consistent with models of nucleosynthesis in low to intermediate mass asymptotic giant branch (AGB) stars. Additional information is contained in the original extended abstract.

Soil drying effects on the carbon isotope composition of soil respiration

EPA Science Inventory

Stable isotopes are used widely as a tool for determining sources of carbon (C) fluxes in ecosystem C studies. Environmental factors that change over time, such as moisture, can create dynamic changes in the isotopic composition of C assimilated by plants, and offers a unique opp...

Iron isotope behavior during fluid/rock interaction in K-feldspar alteration zone - A model for pyrite in gold deposits from the Jiaodong Peninsula, East China

NASA Astrophysics Data System (ADS)

Zhu, Zhi-Yong; Jiang, Shao-Yong; Mathur, Ryan; Cook, Nigel J.; Yang, Tao; Wang, Meng; Ma, Liang; Ciobanu, Cristiana L.

2018-02-01

Mechanisms for Fe isotope fractionation in hydrothermal mineral deposits and in zones of associated K-feldspar alteration remain poorly constrained. We have analyzed a suite of bulk samples consisting of granite displaying K-feldspar alteration, Precambrian metamorphic rocks, and pyrite from gold deposits of the Jiaodong Peninsula, East China, by multi-collector inductively-coupled plasma mass spectrometry. Pyrites from disseminated (J-type) ores show a δ56Fe variation from +0.01 to +0.64‰, overlapping with the signature of the host granites (+0.08 to +0.39‰). In contrast, pyrites from quartz veins (L-type ores) show a wide range of Fe-isotopic composition from -0.78 to +0.79‰. Negative values are never seen in the J-type pyrites. The Fe isotope signature of the host granite with K-feldspar alteration is significantly heavier than that of the bulk silicate Earth. The Fe isotopic compositions of Precambrian metamorphic rocks across the district display a narrow range between -0.16‰ and +0.19‰, which is similar to most terrestrial rocks. Concentrations of major and trace elements in bulk samples were also determined, so as to evaluate any correlation between Fe isotope composition and degree of alteration. We note that during progressive K-feldspar alteration to rocks containing >70 wt% SiO2, >75 ppm Rb, and <1.2 wt% total Fe2O3, the Fe isotope composition of the granite changes systematically. The Fe isotope signature becomes heavier as the degree of alteration increases. The extremely light Fe isotopic compositions in L-type gold deposits may be explained by Rayleigh fractionation during pyrite precipitation in an open fracture system. We note that the sulfur isotopic compositions of pyrite in the two types of ores are also different. Pyrite from J-type ores has a systematically 3.5‰-higher δ34S value (11.2‰) than those of pyrite from the L-type ores (7.7‰). There is, however, no correlation between Fe and S isotope signatures. The isotopic fractionation of sulfur is used to constrain a change in the fO2 of the hydrothermal fluids from which pyrite precipitated. This work demonstrates that the Fe isotope composition of pyrite displays a significant response to the process of pyrite precipitation in hydrothermal systems, and that systematic fractionation of iron isotopes occurs during fluid/rock reaction in the K-feldspar alteration zone of the Linglong granite. The implications of the results are that processes of mineralization and associated fluid-rock interaction, which are ubiquitously observed in porphyry-style Cu-Au-Mo and other hydrothermal deposits, may be readily traceable using Fe isotopes.

Isotopic anomalies - Chemical memory of Galactic evolution

NASA Technical Reports Server (NTRS)

Clayton, Donald D.

1988-01-01

New mechanisms for the chemical memory of isotopic anomalies are proposed which are based on the temporal change during the chemical evolution of the Galaxy of the isotopic composition of the mean ejecta from stars. Because of the differing temporal evolution of primary and secondary products of nucleosynthesis, the isotopic composition of the bulk interstellar medium changes approximately linearly with time, and thus any dust component having an age different from that of average dust will be isotopically anomalous. Special attention is given to C, O, Mg, Si, and isotopically heavy average-stellar condensates of SiC.

Continental sedimentary processes decouple Nd and Hf isotopes

NASA Astrophysics Data System (ADS)

Garçon, Marion; Chauvel, Catherine; France-Lanord, Christian; Huyghe, Pascale; Lavé, Jérôme

2013-11-01

The neodymium and hafnium isotopic compositions of most crustal and mantle rocks correlate to form the "Terrestrial Array". However, it is now well established that whereas coarse detrital sediments follow this trend, fine-grained oceanic sediments have high Hf ratios relative to their Nd isotopic ratios. It remains uncertain whether this "decoupling" of the two isotopic systems only occurs in the oceanic environment or if it is induced by sedimentary processes in continental settings. In this study, the hafnium and neodymium isotopic compositions of sediments in large rivers is expressly used to constrain the behavior of the two isotopic systems during erosion and sediment transport from continent to ocean. We report major and trace element concentrations together with Nd and Hf isotopic compositions of bedloads, suspended loads and river banks from the Ganges River and its tributaries draining the Himalayan Range i.e. the Karnali, the Narayani, the Kosi and the Marsyandi Rivers. The sample set includes sediments sampled within the Himalayan Range in Nepal, at the Himalayan mountain front, and also downstream on the floodplain and at the outflow of the Ganges in Bangladesh. Results show that hydrodynamic sorting of minerals explains the entire Hf isotopic range, i.e. more than 10 εHf units, observed in the river sediments but does not affect the Nd isotopic composition. Bedloads and bank sediments have systematically lower εHf values than suspended loads sampled at the same location. Coarse-grained sediments lie below or on the Terrestrial Array in an εHf vs. εNd diagram. In contrast, fine-grained sediments, including most of the suspended loads, deviate from the Terrestrial Array toward higher εHf relative to their εNd, as is the case for oceanic terrigenous clays. The observed Nd-Hf decoupling is explained by mineralogical sorting processes that enrich bottom sediments in coarse and dense minerals, including unradiogenic zircons, while surface sediments are enriched in fine material with radiogenic Hf signatures. The data also show that Nd-Hf isotopic decoupling increases with sediment transport in the floodplain to reach its maximum at the river mouth. This implies that the Nd-Hf isotopic decoupling observed in worldwide oceanic clays and river sediments is likely to have the same origin. Finally, we estimated the Nd-Hf isotopic composition of the present-day mantle if oceanic sediments had never been subducted and conclude that the addition of oceanic sediments with their anomalous Nd-Hf isotopic compositions has slowly shifted the composition of the Earth's mantle towards more radiogenic Hf values through time.

On the Origin of GEMS

NASA Technical Reports Server (NTRS)

Keller, L. P.; Messenger, S.

2004-01-01

GEMS (glass with embedded metal and sulfides) are a major component of anhydrous interplanetary dust particles (IDPs) their physical and chemical characteristics show marked similarities to contemporary interstellar dust. Recent oxygen isotopic measurements confirm that at least a small fraction (less than 5%) of GEMS are demonstrably presolar, while the remainder have ratios that are indistinguishable from solar values. GEMS with solar oxygen isotopic compositions either (1) had their isotopic compositions homogenized through processing in the interstellar medium (ISM), or (2) formed in the early solar system. Isotopic homogenization necessarily implies chemical homogenization, so (interstellar) GEMS compositions should reflect the average composition of dust in the local ISM. We performed a systematic examination of the bulk chemistry of GEMS in primitive IDPs in order to test this hypothesis.

Cu isotopic signature in blood serum of liver transplant patients: a follow-up study

NASA Astrophysics Data System (ADS)

Lauwens, Sara; Costas-Rodríguez, Marta; van Vlierberghe, Hans; Vanhaecke, Frank

2016-07-01

End-stage liver disease (ESLD) is life-threatening and liver transplantation (LTx) is the definitive treatment with good outcomes. Given the essential role of hepatocytes in Cu homeostasis, the potential of the serum Cu isotopic composition for monitoring a patient’s condition post-LTx was evaluated. For this purpose, high-precision Cu isotopic analysis of blood serum of ESLD patients pre- and post-LTx was accomplished via multi-collector ICP-mass spectrometry (MC-ICP-MS). The Cu isotopic composition of the ESLD patients was fractionated in favour of the lighter isotope (by about -0.50‰). Post-LTx, a generalized normalization of the Cu isotopic composition was observed for the patients with normal liver function, while it remained light when this condition was not reached. A strong decrease in the δ65Cu value a longer term post-LTx seems to indicate the recurrence of liver failure or cancer. The observed trend in favour of the heavier Cu isotopic composition post-LTx seems to be related with the restored biosynthetic capacity of the liver, the restored hepatic metabolism and/or the restored biliary secretion pathways. Thus, Cu isotopic analysis could be a valuable tool for the follow-up of liver transplant patients and for establishing the potential recurrence of liver failure.

Cu isotopic signature in blood serum of liver transplant patients: a follow-up study

PubMed Central

Lauwens, Sara; Costas-Rodríguez, Marta; Van Vlierberghe, Hans; Vanhaecke, Frank

2016-01-01

End-stage liver disease (ESLD) is life-threatening and liver transplantation (LTx) is the definitive treatment with good outcomes. Given the essential role of hepatocytes in Cu homeostasis, the potential of the serum Cu isotopic composition for monitoring a patient’s condition post-LTx was evaluated. For this purpose, high-precision Cu isotopic analysis of blood serum of ESLD patients pre- and post-LTx was accomplished via multi-collector ICP-mass spectrometry (MC-ICP-MS). The Cu isotopic composition of the ESLD patients was fractionated in favour of the lighter isotope (by about −0.50‰). Post-LTx, a generalized normalization of the Cu isotopic composition was observed for the patients with normal liver function, while it remained light when this condition was not reached. A strong decrease in the δ65Cu value a longer term post-LTx seems to indicate the recurrence of liver failure or cancer. The observed trend in favour of the heavier Cu isotopic composition post-LTx seems to be related with the restored biosynthetic capacity of the liver, the restored hepatic metabolism and/or the restored biliary secretion pathways. Thus, Cu isotopic analysis could be a valuable tool for the follow-up of liver transplant patients and for establishing the potential recurrence of liver failure. PMID:27468898

Cu isotopic signature in blood serum of liver transplant patients: a follow-up study.

PubMed

Lauwens, Sara; Costas-Rodríguez, Marta; Van Vlierberghe, Hans; Vanhaecke, Frank

2016-07-29

End-stage liver disease (ESLD) is life-threatening and liver transplantation (LTx) is the definitive treatment with good outcomes. Given the essential role of hepatocytes in Cu homeostasis, the potential of the serum Cu isotopic composition for monitoring a patient's condition post-LTx was evaluated. For this purpose, high-precision Cu isotopic analysis of blood serum of ESLD patients pre- and post-LTx was accomplished via multi-collector ICP-mass spectrometry (MC-ICP-MS). The Cu isotopic composition of the ESLD patients was fractionated in favour of the lighter isotope (by about -0.50‰). Post-LTx, a generalized normalization of the Cu isotopic composition was observed for the patients with normal liver function, while it remained light when this condition was not reached. A strong decrease in the δ(65)Cu value a longer term post-LTx seems to indicate the recurrence of liver failure or cancer. The observed trend in favour of the heavier Cu isotopic composition post-LTx seems to be related with the restored biosynthetic capacity of the liver, the restored hepatic metabolism and/or the restored biliary secretion pathways. Thus, Cu isotopic analysis could be a valuable tool for the follow-up of liver transplant patients and for establishing the potential recurrence of liver failure.

Clumped Isotope Composition of Cold-Water Corals: A Role for Vital Effects?

NASA Astrophysics Data System (ADS)

Spooner, P.; Guo, W.; Robinson, L. F.

2014-12-01

Measurements on a set of cold-water corals (mainly Desmophyllum dianthus) have suggested that their clumped isotope composition could serve as a promising proxy for reconstructing paleocean temperatures. Such measurements have also offered support for certain isotope models of coral calcification. However, there are differences in the clumped isotope compositions between warm-water and cold-water corals, suggesting that different kinds of corals could have differences in their biocalcification processes. In order to understand the systematics of clumped isotope variations in cold-water corals more fully, we present clumped isotope data from a range of cold-water coral species from the tropical Atlantic and the Southern Ocean.Our samples were either collected live or recently dead (14C ages < 1,000 yrs) with associated temperature data. They include a total of 11 solitary corals and 1 colonial coral from the Atlantic, and 8 solitary corals from the Southern Ocean. The data indicate that coral clumped isotope systematics may be more complicated than previously thought. For example, for the genus Caryophyllia we observe significant variations in clumped isotope compositions for corals which grew at the same temperature with an apparent negative correlation between Δ47 and δ18O, different to patterns previously observed in Desmophyllum. These results indicate that existing isotope models of biocalcification may not apply equally well to all corals. Clumped isotope vital effects may be present in certain cold-water corals as they are in warm-water corals, complicating the use of this paleoclimate proxy.

Cenozoic marine geochemistry of thallium deduced from isotopic studies of ferromanganese crusts and pelagic sediments

USGS Publications Warehouse

Rehkamper, M.; Frank, M.; Hein, J.R.; Halliday, A.

2004-01-01

Cenozoic records of Tl isotope compositions recorded by ferromanganese (Fe-Mn) crusts have been obtained. Such records are of interest because recent growth surfaces of Fe-Mn crusts display a nearly constant Tl isotope fractionation relative to seawater. The time-series data are complemented by results for bulk samples and leachates of various marine sediments. Oxic pelagic sediments and anoxic marine deposits can be distinguished by their Tl isotope compositions. Both pelagic clays and biogenic oozes are typically characterized by ??205Tl greater than +2.5, whereas anoxic sediments have ??205Tl of less than -1.5 (??205Tl is the deviation of the 205Tl/203Tl isotope ratio of a sample from NIST SRM 997 Tl in parts per 104). Leaching experiments indicate that the high ??205Tl values of oxic sediments probably reflect authigenic Fe-Mn oxyhydroxides. Time-resolved Tl isotope compositions were obtained from six Fe-Mn crusts from the Atlantic, Indian, and Pacific oceans and a number of observations indicate that these records were not biased by diagenetic alteration. Over the last 25 Myr, the data do not show isotopic variations that significantly exceed the range of Tl isotope compositions observed for surface layers of Fe-Mn crusts distributed globally (??205 Tl=+12.8??1.2). This indicates that variations in deep-ocean temperature were not recorded by Tl isotopes. The results most likely reflect a constant Tl isotope composition for seawater. The growth layers of three Fe-Mn crusts that are older than 25 Ma show a systematic increase of ??205Tl with decreasing age, from about +6 at 60-50 Ma to about +12 at 25 Ma. These trends are thought to be due to variations in the Tl isotope composition of seawater, which requires that the oceans of the early Cenozoic either had smaller output fluxes or received larger input fluxes of Tl with low ??205Tl. Larger inputs of isotopically light Tl may have been supplied by benthic fluxes from reducing sediments, rivers, and/or volcanic emanations. Alternatively, the Tl isotope trends may reflect the increasing importance of Tl fluxes to altered ocean crust through time. ?? 2004 Elsevier B.V. All rights reserved.

Assessment of shock effects on amphibole water contents and hydrogen isotope compositions: 1. Amphibolite experiments

NASA Astrophysics Data System (ADS)

Minitti, Michelle E.; Rutherford, Malcolm J.; Taylor, Bruce E.; Dyar, M. Darby; Schultz, Peter H.

2008-02-01

Kaersutitic amphiboles found within a subset of the Martian meteorites have low water contents and variably heavy hydrogen isotope compositions. In order to assess if impact shock-induced devolatilization and hydrogen isotope fractionation were determining factors in these water and isotopic characteristics of the Martian kaersutites, we conducted impact shock experiments on samples of Gore Mountain amphibolite in the Ames Vertical Gun Range (AVGR). A parallel shock experiment conducted on an anorthosite sample indicated that contamination of shocked samples by the AVGR hydrogen propellant was unlikely. Petrographic study of the experimental amphibolite shock products indicates that only ˜ 10% of the shock products experienced levels of damage equivalent to those found in the most highly shocked kaersutite-bearing Martian meteorites (30-35 GPa). Ion microprobe studies of highly shocked hornblende from the amphibolite exhibited elevated water contents (ΔH 2O ˜ 0.1 wt.%) and enriched hydrogen isotope compositions (Δ D ˜ + 10‰) relative to unshocked hornblende. Water and hydrogen isotope analyses of tens of milligrams of unshocked, moderately shocked, and highly shocked hornblende samples by vacuum extraction/uranium reduction and isotope ratio mass spectrometry (IRMS), respectively, are largely consistent with analyses of single grains from the ion microprobe. The mechanisms thought to have produced the excess water in most of the shocked hornblendes are shock-induced reduction of hornblende Fe and/or irreversible adsorption of hydrogen. Addition of the isotopically enriched Martian atmosphere to the Martian meteorite kaersutites via these mechanisms could explain their enriched and variable isotopic compositions. Alternatively, regrouping the water extraction and IRMS analyses on the basis of isotopic composition reveals a small, but consistent, degree of impact-induced devolatilization (˜ 0.1 wt.% H 2O) and H isotope enrichment (Δ D ˜ + 10‰). Extrapolating the shock signature of the regrouped data to grains that experienced Martian meteorite-like shock pressures suggests that shock-induced water losses and hydrogen isotope enrichments could approach 1 wt.% H 2O and Δ D = + 100‰, respectively. If these values are valid, then impact shock effects could explain a substantial fraction of the low water contents and variable hydrogen isotope compositions of the Martian meteorite kaersutites.

FE and MG Isotopic Analyses of Isotopically Unusual Presolar Silicate Grains

NASA Technical Reports Server (NTRS)

Nguyen, A. N.; Messenger, S.; Ito, M.; Rahman, Z.

2011-01-01

Interstellar and circumstellar silicate grains are thought to be Mg-rich and Fe-poor, based on astronomical observations and equilibrium condensation models of silicate dust formation in stellar outflows. On the other hand, presolar silicates isolated from meteorites have surprisingly high Fe contents and few Mg-rich grains are observed. The high Fe contents in meteoritic presolar silicates may indicate they formed by a non-equilibrium condensation process. Alternatively, the Fe in the stardust grains could have been acquired during parent body alteration. The origin of Fe in presolar silicates may be deduced from its isotopic composition. Thus far, Fe isotopic measurements of presolar silicates are limited to the Fe-54/Fe-56 ratios of 14 grains. Only two slight anomalies (albeit solar within error) were observed. However, these measurements suffered from contamination of Fe from the adjacent meteorite matrix, which diluted any isotopic anomalies. We have isolated four presolar silicates having unusual O isotopic compositions by focused ion beam (FIB) milling and obtained their undiluted Mg and Fe isotopic compositions. These compositions help to identify the grains stellar sources and to determine the source of Fe in the grains.

Isotopic composition of transpiration and rates of change in leaf water isotopologue storage in response to environmental variables.

PubMed

Simonin, Kevin A; Roddy, Adam B; Link, Percy; Apodaca, Randy; Tu, Kevin P; Hu, Jia; Dawson, Todd E; Barbour, Margaret M

2013-12-01

During daylight hours, the isotope composition of leaf water generally approximates steady-state leaf water isotope enrichment model predictions. However, until very recently there was little direct confirmation that isotopic steady-state (ISS) transpiration in fact exists. Using isotope ratio infrared spectroscopy (IRIS) and leaf gas exchange systems we evaluated the isotope composition of transpiration and the rate of change in leaf water isotopologue storage (isostorage) when leaves were exposed to variable environments. In doing so, we developed a method for controlling the absolute humidity entering the gas exchange cuvette for a wide range of concentrations without changing the isotope composition of water vapour. The measurement system allowed estimation of (18)O enrichment both at the evaporation site and for bulk leaf water, in the steady state and the non-steady state. We show that non-steady-state effects dominate the transpiration isoflux even when leaves are at physiological steady state. Our results suggest that a variable environment likely prevents ISS transpiration from being achieved and that this effect may be exacerbated by lengthy leaf water turnover times due to high leaf water contents. © 2013 John Wiley & Sons Ltd.

Neutron radiation characteristics of plutonium dioxide fuel

NASA Technical Reports Server (NTRS)

Taherzadeh, M.

1972-01-01

The major sources of neutrons from plutonium dioxide nuclear fuel are considered in detail. These sources include spontaneous fission of several of the Pu isotopes, (alpha, n) reactions with low Z impurities in the fuel, and (alpha, n) reactions with O-18. For spontaneous fission neutrons a value of (1.95 + or - 0.07) X 1,000 n/s/g PuO2 is obtained. The neutron yield from (alpha, n) reactions with oxygen is calculated by integrating the reaction rate equation over all alpha-particle energies and all center-of-mass angles. The results indicate a neutron emission rate of (1.14 + or - 0.26) X 10,000 n/s/g PuO2. The neutron yield from (alpha, n) reactions with low Z impurities in the fuel is presented in tabular form for one part part per million of each impurity. The total neutron yield due to the combined effects of all the impurities depends upon the fractional weight concentration of each impurity. The total neutron flux emitted from a particular fuel geometry is estimated by adding the neutron yield due to the induced fission to the other neutron sources.

Source and long-term behavior of transuranic aerosols in the WIPP environment.

PubMed

Thakur, P; Lemons, B G

2016-10-01

Source and long-term behavior transuranic aerosols ((239+240)Pu, (238)Pu, and (241)Am) in the ambient air samples collected at and near the Waste Isolation Pilot Plant (WIPP) deep geologic repository site were investigated using historical data from an independent monitoring program conducted by the Carlsbad Environmental Monitoring and Research Center and an oversight monitoring program conducted by the management and operating contractor for WIPP at and near the facility. An analysis of historical data indicates frequent detections of (239+240)Pu and (241)Am, whereas (238)Pu is detected infrequently. Peaks in (239+240)Pu and (241)Am concentrations in ambient air generally occur from March to June timeframe, which is when strong and gusty winds in the area frequently give rise to blowing dust. Long-term measurements of plutonium isotopes (1985-2015) in the WIPP environment suggest that the resuspension of previously contaminated soils is likely the primary source of plutonium in the ambient air samples from WIPP and its vicinity. There is no evidence that WIPP is a source of environmental contamination that can be considered significant by any health-based standard.

Modes of planetary-scale Fe isotope fractionation

NASA Astrophysics Data System (ADS)

Schoenberg, Ronny; von Blanckenburg, Friedhelm

2006-12-01

A comprehensive set of high-precision Fe isotope data for the principle meteorite types and silicate reservoirs of the Earth is used to investigate iron isotope fractionation at inter- and intra-planetary scales. 14 chondrite analyses yield a homogeneous Fe isotope composition with an average δ56Fe/ 54Fe value of - 0.015 ± 0.020‰ (2 SE) relative to the international iron standard IRMM-014. Eight non-cumulate and polymict eucrite meteorites that sample the silicate portion of the HED (howardite-eucrite-diogenite) parent body yield an average δ56Fe/ 54Fe value of - 0.001 ± 0.017‰, indistinguishable to the chondritic Fe isotope composition. Fe isotope ratios that are indistinguishable to the chondritic value have also been published for SNC meteorites. This inner-solar system homogeneity in Fe isotopes suggests that planetary accretion itself did not significantly fractionate iron. Nine mantle xenoliths yield a 2 σ envelope of - 0.13‰ to + 0.09‰ in δ56Fe/ 54Fe. Using this range as proxy for the bulk silicate Earth in a mass balance model places the Fe isotope composition of the outer liquid core that contains ca. 83% of Earth's total iron to within ± 0.020‰ of the chondritic δ56Fe/ 54Fe value. These calculations allow to interprete magmatic iron meteorites ( δ56Fe/ 54Fe = + 0.047 ± 0.016‰; N = 8) to be representative for the Earth's inner metallic core. Eight terrestrial basalt samples yield a homogeneous Fe isotope composition with an average δ56Fe/ 54Fe value of + 0.072 ± 0.016‰. The observation that terrestrial basalts appear to be slightly heavier than mantle xenoliths and that thus partial mantle melting preferentially transfers heavy iron into the melt [S. Weyer, A.D. Anbar, G.P. Brey, C. Munker, K. Mezger and A.B. Woodland, Iron isotope fractionation during planetary differentiation, Earth and Planetary Science Letters 240(2), 251-264, 2005.] is intriguing, but also raises some important questions: first it is questionable whether the Fe isotope composition of lithospheric mantle xenoliths are representative for an undisturbed melt source, and second, HED and SNC meteorites, representing melting products of 4Vesta and Mars silicate mantles would be expected to show a similar fractionation towards heavy isotope compositions. This is not observed. Four international granitoid standards with SiO 2 contents between 60 and 70 wt.% yield δ56Fe/ 54Fe values between 0.118‰ and 0.132‰. An investigation of the alpine Bergell igneous rock suite revealed a positive correlation between Fe isotope compositions and SiO 2 contents — from gabbros and tonalites ( δ56Fe/ 54Fe ≈ 0.03 to 0.09‰) to granodiorites and silicic dykes ( δ56Fe/ 54Fe ≈ 0.14 to 0.23‰). Although in this suite δ56Fe/ 54Fe correlates with δ18O values and radiogenic isotopes, open-system behavior to explain the heavy iron is not undisputed. This is because an obvious assimilant with the required heavy Fe isotope composition has so far not been identified. Alternatively, the relatively heavy granite compositions might be obtained by fractional crystallisation of the melt. Ultimately, further detailed studies on natural rocks and the experimental determination of mineral/melt fractionation factors at magmatic conditions are required to unravel whether or not iron isotope fractionation takes place during partial mantle melting and crystal fractionation.

Crystal growth and disequilibrium distribution of oxygen isotopes in an igneous Ca-Al-rich inclusion from the Allende carbonaceous chondrite

NASA Astrophysics Data System (ADS)

Kawasaki, Noriyuki; Simon, Steven B.; Grossman, Lawrence; Sakamoto, Naoya; Yurimoto, Hisayoshi

2018-01-01

TS34 is a Type B1 Ca-Al-rich inclusion (CAI) from the Allende CV3 chondrite, consisting of spinel, melilite, Ti-Al-rich clinopyroxene (fassaite) and minor anorthite in an igneous texture. Oxygen and magnesium isotopic compositions were measured by secondary ion mass spectrometry in spots of known chemical composition in all major minerals in TS34. Using the sequence of formation from dynamic crystallization experiments and from chemical compositions of melilite and fassaite, the oxygen isotopic evolution of the CAI melt was established. Oxygen isotopic compositions of the constituent minerals plot along the carbonaceous chondrite anhydrous mineral line. The spinel grains are uniformly 16O-rich (Δ17O = -22.7 ± 1.7‰, 2SD), while the melilite grains are uniformly 16O-poor (Δ17O = -2.8 ± 1.8‰) irrespective of their åkermanite content and thus their relative time of crystallization. The fassaite crystals exhibit growth zoning overprinting poorly-developed sector zoning; they generally grow from Ti-rich to Ti-poor compositions. The fassaite crystals also show continuous variations in Δ17O along the inferred directions of crystal growth, from 16O-poor (Δ17O ∼ -3‰) to 16O-rich (Δ17O ∼ -23‰), covering the full range of oxygen isotopic compositions observed in TS34. The early-crystallized 16O-poor fassaite and the melilite are in oxygen isotope equilibrium and formed simultaneously. The correlation of oxygen isotopic compositions with Ti content in the fassaite imply that the oxygen isotopic composition of the CAI melt evolved from 16O-poor to 16O-rich during fassaite crystallization, presumably due to oxygen isotope exchange with a surrounding 16O-rich nebular gas. Formation of spinel, the liquidus phase in melts of this composition, predates crystallization of all other phases, so its 16O-rich composition is a relic of an earlier stage. Anorthite exhibits oxygen isotopic compositions between Δ17O ∼ -2‰ and -9‰, within the range of those of fassaite, indicating co-crystallization of these two minerals during the earliest to intermediate stage of fassaite growth. The melilite and fassaite yield an 26Al-26Mg mineral isochron with an initial value of (26Al/27Al)0 = (5.003 ± 0.075) × 10-5, corresponding to a relative age of 0.05 ± 0.02 Myr from the canonical Al-Mg age of CAIs. These data demonstrate that both 16O-rich and 16O-poor reservoirs existed in the solar nebula at least ∼0.05 Myr after the birth of the Solar System.

Oxygen isotope corrections for online δ34S analysis

USGS Publications Warehouse

Fry, B.; Silva, S.R.; Kendall, C.; Anderson, R.K.

2002-01-01

Elemental analyzers have been successfully coupled to stable-isotope-ratio mass spectrometers for online measurements of the δ34S isotopic composition of plants, animals and soils. We found that the online technology for automated δ34S isotopic determinations did not yield reproducible oxygen isotopic compositions in the SO2 produced, and as a result calculated δ34S values were often 1–3‰ too high versus their correct values, particularly for plant and animal samples with high C/S ratio. Here we provide empirical and analytical methods for correcting the S isotope values for oxygen isotope variations, and further detail a new SO2-SiO2 buffering method that minimizes detrimental oxygen isotope variations in SO2.

Chromium isotope heterogeneity in the mantle

NASA Astrophysics Data System (ADS)

Xia, Jiuxing; Qin, Liping; Shen, Ji; Carlson, Richard W.; Ionov, Dmitri A.; Mock, Timothy D.

2017-04-01

To better constrain the Cr isotopic composition of the silicate Earth and to investigate potential Cr isotopic fractionation during high temperature geological processes, we analyzed the Cr isotopic composition of different types of mantle xenoliths from diverse geologic settings: fertile to refractory off-craton spinel and garnet peridotites, pyroxenite veins, metasomatised spinel lherzolites and associated basalts from central Mongolia, spinel lherzolites and harzburgites from North China, as well as cratonic spinel and garnet peridotites from Siberia and southern Africa. The δ53CrNIST 979 values of the peridotites range from - 0.51 ± 0.04 ‰ (2SD) to + 0.75 ± 0.05 ‰ (2SD). The results show a slight negative correlation between δ53Cr and Al2O3 and CaO contents for most mantle peridotites, which may imply Cr isotopic fractionation during partial melting of mantle peridotites. However, highly variable Cr isotopic compositions measured in Mongolian peridotites cannot be caused by partial melting alone. Instead, the wide range in Cr isotopic composition of these samples most likely reflects kinetic fractionation during melt percolation. Chemical diffusion during melt percolation resulted in light Cr isotopes preferably entering into the melt. Two spinel websterite veins from Mongolia have extremely light δ53Cr values of - 1.36 ± 0.04 ‰ and - 0.77 ± 0.06 ‰, respectively, which are the most negative Cr isotopic compositions yet reported for mantle-derived rocks. These two websterite veins may represent crystallization products from the isotopically light melt that may also metasomatize some peridotites in the area. The δ53Cr values of highly altered garnet peridotites from southern Africa vary from - 0.35 ± 0.04 ‰ (2SD) to + 0.12 ± 0.04 ‰ (2SD) and increase with increasing LOI (Loss on Ignition), reflecting a shift of δ53Cr to more positive values by secondary alteration. The Cr isotopic composition of the pristine, fertile upper mantle is estimated as δ53Cr = - 0.14 ± 0.12 ‰, after corrections for the effects of partial melting and metasomatism. This value is in line with that estimated for the BSE (- 0.12 ± 0.10 ‰) previously.

Reassessment of the NH4 NO3 thermal decomposition technique for calibration of the N2 O isotopic composition.

PubMed

Mohn, Joachim; Gutjahr, Wilhelm; Toyoda, Sakae; Harris, Eliza; Ibraim, Erkan; Geilmann, Heike; Schleppi, Patrick; Kuhn, Thomas; Lehmann, Moritz F; Decock, Charlotte; Werner, Roland A; Yoshida, Naohiro; Brand, Willi A

2016-09-08

In the last few years, the study of N 2 O site-specific nitrogen isotope composition has been established as a powerful technique to disentangle N 2 O emission pathways. This trend has been accelerated by significant analytical progress in the field of isotope-ratio mass-spectrometry (IRMS) and more recently quantum cascade laser absorption spectroscopy (QCLAS). Methods The ammonium nitrate (NH 4 NO 3 ) decomposition technique provides a strategy to scale the 15 N site-specific (SP ≡ δ 15 N α - δ 15 N β ) and bulk (δ 15 N bulk  = (δ 15 N α  + δ 15 N β )/2) isotopic composition of N 2 O against the international standard for the 15 N/ 14 N isotope ratio (AIR-N 2 ). Within the current project 15 N fractionation effects during thermal decomposition of NH 4 NO 3 on the N 2 O site preference were studied using static and dynamic decomposition techniques. The validity of the NH 4 NO 3 decomposition technique to link NH 4 + and NO 3 - moiety-specific δ 15 N analysis by IRMS to the site-specific nitrogen isotopic composition of N 2 O was confirmed. However, the accuracy of this approach for the calibration of δ 15 N α and δ 15 N β values was found to be limited by non-quantitative NH 4 NO 3 decomposition in combination with substantially different isotope enrichment factors for the conversion of the NO 3 - or NH 4 + nitrogen atom into the α or β position of the N 2 O molecule. The study reveals that the completeness and reproducibility of the NH 4 NO 3 decomposition reaction currently confine the anchoring of N 2 O site-specific isotopic composition to the international isotope ratio scale AIR-N 2 . The authors suggest establishing a set of N 2 O isotope reference materials with appropriate site-specific isotopic composition, as community standards, to improve inter-laboratory compatibility. This article is protected by copyright. All rights reserved.

Mechanisms controlling the silicon isotopic compositions of river waters

NASA Astrophysics Data System (ADS)

Georg, R. B.; Reynolds, B. C.; Frank, M.; Halliday, A. N.

2006-09-01

It has been proposed that silicon (Si) isotopes are fractionated during weathering and biological activity leading to heavy dissolved riverine compositions. In this study, the first seasonal variations of stable isotope compositions of dissolved riverine Si are reported and compared with concomitant changes in water chemistry. Four different rivers in Switzerland were sampled between March 2004 and July 2005. The unique high-resolution multi-collector ICP-MS Nu1700, has been used to provide simultaneous interference-free measurements of 28Si, 29Si and 30Si abundances with an average limiting precision of ± 0.04‰ on δ 30Si. This precision facilitates the clarification of small temporal variations in isotope composition. The average of all the data for the 40 samples is δ 30Si = + 0.84 ± 0.19‰ (± 1σ SD). Despite significant differences in catchment lithologies, biomass, climate, total dissolved solids and weathering fluxes the averaged isotopic composition of dissolved Si in each river is strikingly similar with means of + 0.70 ± 0.12‰ for the Birs,+ 0.95 ± 0.22‰ for the Saane,+ 0.93 ± 0.12‰ for the Ticino and + 0.79 ± 0.19‰ for the Verzasca. However, the δ 30Si undergoes seasonal variations of up to 0.6‰. Comparisons between δ 30Si and physico-chemical parameters, such as the concentration of dissolved Si and other cations, the discharge of the rivers, and the resulting weathering fluxes, permits an understanding of the processes that control the Si budget and the fate of dissolved Si within these rivers. The main mechanism controlling the Si isotope composition of the mountainous Verzasca River appears to be a two component mixing between the seepage of soil/ground waters, with heavier Si produced by clay formation and superficial runoff associated with lighter Si during high discharge events. A biologically-mediated fractionation can be excluded in this particular river system. The other rivers display increasing complexity with increases in the proportion of forested and cultivated landscapes as well as carbonate rocks in the catchment. In these instances it is impossible to resolve the extent of the isotopic fractionation and contributed flux of Si contributed by biological processes as opposed to abiotic weathering. The presence of seasonal variations in Si isotope composition in mountainous rivers provides evidence that extreme changes in climate affect the overall composition of dissolved Si delivered to the oceans. The oceanic Si isotope composition is very sensitive to even small changes in the riverine Si isotope composition and this parameter appears to be more critical than plausible changes in the Si flux. Therefore, concurrent changes in weathering style may need to be considered when using the Si isotopic compositions of diatoms, sponges and radiolaria as paleoproductivity proxies.

Tracing mantle processes with Fe isotopes

NASA Astrophysics Data System (ADS)

Weyer, S.; Ionov, D.

2006-12-01

High precision Fe isotope measurements have been performed on various mantle peridotites (fertile lherzolites, harzburgites, metasomatised Fe-enriched rocks) and volcanic rocks (mainly oceanic basalts) from different localities and tectonic settings. Pimitive peridotites (Mg# = 0.894) yield delta56Fe = 0.02 and are significantly lighter than the basalts (average delta56Fe = 0.11). Furthermore, the peridotites display a negative correlation of iron isotopes with Mg#. Taken together, these findings imply that Fe isotopes fractionate during partial melting, with heavy isotopes preferentially entering the melt [1, 2]. A particularly good correlation of the Fe isotope composition and Mg# shown by poorly metasomatised spinel lherzolites of three localities (Horoman, Kamchatka and Lherz) was used to model Fe isotope fractionation during partial melting, resulting in alphamantle-melt = 1.0003. This value implies higher Fe isotope fractionation between residual mantle and mantle-derived melts (i.e. Delta56Femantle-melt = 0.2-0.3) than the observed difference between the peridotites and the basalts in this study. Our data on plagioclase lherzolites from Horoman and spinel lherzolites from other localities indicate that the difference in Fe isotope composition between mantle and basalts may be reduced by partial re-equilibration between the isotopically heavy basalts and the isotopically light depleted lithospheric mantle during melt ascent. Besides partial melting, the Fe isotope composition of mantle peridotites can also be significantly modified by metasomatic events. At two localities (Tok, Siberia and Tariat, Mongolia) Fe isotopes correlates with the Fe concentration of the peridotites, which was increased up to 14.5% FeO by melt percolation. Such processes can be accompanied by chromatographic effects and produce a range of Fe isotope compositions in the percolation columns, from extremely light to heavy (delta56Fe = -0.42 to +0.17). We propose that Fe isotopes can be used as a sensitive tracer to identify such metasomatic processes in the mantle. [1] Weyer et al. (2005) EPSL 240: 251-264 [2] Williams et al. (2005) EPSL 235 : 435-452

The Molybdenum Isotope System as a Tracer of Slab Input in Subduction Zones: An Example From Martinique, Lesser Antilles Arc

NASA Astrophysics Data System (ADS)

Gaschnig, Richard M.; Reinhard, Christopher T.; Planavsky, Noah J.; Wang, Xiangli; Asael, Dan; Chauvel, Catherine

2017-12-01

Molybdenum isotopes are fractionated by Earth-surface processes and may provide a tracer for the recycling of crustal material into the mantle. Here, we examined the Mo isotope composition of arc lavas from Martinique in the Lesser Antilles arc, along with Cretaceous and Cenozoic Deep Sea Drilling Project sediments representing potential sedimentary inputs into the subduction zone. Mo stable isotope composition (defined as δ98Mo in ‰ deviation from the NIST 3134 standard) in lavas older than ˜7 million years (Ma) exhibits a narrow range similar to and slightly higher than MORB, whereas those younger than ˜7 Ma show a much greater range and extend to unusually low δ98Mo values. Sediments from DSDP Leg 78A, Site 543 have uniformly low δ98Mo values whereas Leg 14, Site 144 contains both sediments with isotopically light Mo and Mo-enriched black shales with isotopically heavy Mo. When coupled with published radiogenic isotope data, Mo isotope systematics of the lavas can be explained through binary mixing between a MORB-like end-member and different sedimentary compositions identified in the DSDP cores. The lavas older than ˜7 Ma were influenced by incorporation of isotopically heavy black shales into the mantle wedge. The younger lavas are the product of mixing isotopically light sedimentary material into the mantle wedge. The change in Mo isotope composition of the lavas at ˜7 Ma is interpreted to reflect the removal of the Cretaceous black shale component due to the arrival of younger ocean crust where the age-equivalent Cretaceous sediments were deposited in shallower oxic waters. Isotopic fractionation of Mo during its removal from the slab is not required to explain the observed systematics in this system.

Trihalomethanes formed from natural organic matter isolates: Using isotopic and compositional data to help understand sources

USGS Publications Warehouse

Bergamaschi, Brian A.; Fram, Miranda S.; Fujii, Roger; Aiken, George R.; Kendall, Carol; Silva, Steven R.

2000-01-01

Over 20 million people drink water from the Sacramento-San Joaquin Delta despite problematic levels of natural organic matter (NOM) and bromide in Delta water, which can form trihalomethanes (THMs) during the treatment process. It is widely believed that NOM released from Delta peat islands is a substantial contributor to the pool of THM precursors present in Delta waters. Dissolved NOM was isolated from samples collected at five channel sites within the Sacramento-San Joaquin Rivers and Delta, California, USA, and from a peat island agricultural drain. To help understand the sources of THM precursors, samples were analyzed to determine their chemical and isotopic composition, their propensity to form THMs, and the isotopic composition of the THMs.The chemical composition of the isolates was quite variable, as indicated by significant differences in carbon-13 nuclear magnetic resonance spectra and carbon-to-nitrogen concentration ratios. The lowest propensity to form THMs per unit of dissolved organic carbon was observed in the peat island agricultural drain isolate, even though it possessed the highest fraction of aromatic material and the highest specific ultraviolet absorbance. Changes in the chemical and isotopic composition of the isolates and the isotopic composition of the THMs suggest that the source of the THMs precursors was different between samples and between isolates. The pattern of variability in compositional and isotopic data for these samples was not consistent with simple mixing of river- and peat-derived organic material.

Coordinated Petrography and Oxygen Isotopic Compositions of Al-Rich Chondrules from CV3 Chondrites

NASA Astrophysics Data System (ADS)

Zhang, M. M.; Lin, Y. T.; Tang, G. Q.; Li, X. H.

2017-07-01

In this study, we coordinated the petrology, bulk compositions and oxygen isotope compositions of 12 ARCs from Allende and Leoville and Ningqiang chondrites in order to elucidate any potential genetic relationships between ARCs, CAIs and FMCs.

Paleoclimate Reconstruction at Lamanai, Belize Using Oxygen-Isotope Tropical Dendrochronology

NASA Astrophysics Data System (ADS)

Prentice, A.; Webb, E. A.; White, C. D.; Graham, E.

2009-05-01

Tropical dendrochronology can be complicated because many trees growing in these areas lack distinct visible annual rings. However, the oxygen-isotope composition of wood growing in tropical regions can provide a record of seasonal fluctuations in the amount of precipitation even when visible rings are absent. Variations in the oxygen-isotope compositions of cellulose as the trees grow can be related to the relative timing of wet and dry seasons and used to identify periods of drought. In this study, the oxygen-isotope composition was determined for cellulose extracted from living trees at the site of Lamanai, Belize to assess the variation in oxygen-isotope values that result from heterogeneity within individual tree rings and seasonal fluctuations in amount of precipitation. In temperate regions, the latewood rings that form during periods of reduced growth are traditionally selected for oxygen-isotope analysis of cellulose because their oxygen-isotope compositions are more directly influenced by climate and precipitation during the growing season. However, in tropical isotope dendrochronology, when visible rings are present, detailed sampling of both the light coloured earlywood and the denser latewood is required. At Lamanai, a seasonal signal was evident in the oxygen- isotope composition of the cellulose when tree rings were sectioned in very small increments (approximately every mm), sub-sampling both earlywood and latewood. However, the visible rings did not always correspond with minimum or maximum oxygen-isotope values. As a result, the amplitude of the oxygen-isotope signal obtained by considering only latewood samples is smaller than that obtained from fine-increment sampling. Hence, the oxygen-isotope values of latewood samples alone did not provide accurate data for climate reconstruction. Multiple series of latewood samples extracted from different cross-sections of the same tree did not consistently show the same trends in oxygen isotope values, which can differ by up to 2 permil around the circumference of the same ring. This indicates that even when visible rings are present in tropical trees, the rings may not be annual or continuous. However, the amplitude of variation in the oxygen-isotope values of cellulose from both early and latewood can be related to seasonal signals across the modern tree rings. These signals will be compared to the oxygen-isotope composition of tree ring cellulose extracted from a wood sample excavated from an ancient tomb at the site of Lamanai to assess the preservation of the cellulose- isotope signal in this artefact. If similar oxygen-isotope patterns are preserved in ancient cellulose they can be used as a proxy to determine past climate conditions, such as those experienced by the ancient Maya populations in Belize.

Boron Isotopic Composition Correlates with Ultra-Structure in a - Sea Coral Lophelia Pertusa: Implications for Biomineralization and - PH

NASA Astrophysics Data System (ADS)

Blamart, D.; Rollion-Bard, C.; Meibom, A.; Cuif, J.; Juillet-Leclerc, A.; Dauphin, Y.; Douarin, M.

2007-12-01

The geochemistry (stable isotopes and trace elements) of biogenic carbonates has been widely used for more than fifty years to reconstruct past climatic variability. During this time, the studies were mainly based on bulk sampling limiting sometimes the interpretations of the geochemical data as paleoclimatic proxies. Recently, high spatial resolution sampling techniques, such as micro-mill and SIMS, have been employed in the study of C, O and B isotopic compositions and trace elements (Mg, Sr) in the skeletons of a variety of (deep-sea) coral species. These studies have documented dramatic 'vital effects' and uncovered a systematic relationship between skeletal ultra-structure and stable isotopic composition. The formation of skeleton corals follows a universal two-step growth process. At the tips of the skeletal structures, the mineralizing cell layer produces centers of calcification (COC) or, equivalently, Early Mineralization Zone (EMZ). These EMZ are subsequently overgrown by fibrous aragonite(FA) consisting of cyclically added layers. The EMZ are characterized by systematically lighter C and O isotopic compositions compared with the adjacent FA. A number of geochemical models have been proposed, in which this systematic stable isotopic difference between EMZ and FA is ascribed to a biologically induced variation in the pH of a proposed Extra-cytoplasmic Calcifying Fluid (ECF) reservoir. In these models, relatively high pH conditions during the formation of EMZ result in relatively light C and O isotopic compositions compared with FA, which form under generally lower pH conditions. A direct test of such models would be possible if the Boron isotopic composition, which is pH sensitive, of EMZ and FA could be measured. We performed ion microprobe d11B measurements for EMZ and FA in Lophelia pertusa, a deep-sea coral common in the North-East Atlantic Ocean. We observe a systematic difference in B isotopic composition between the EMZ and FA skeleton. In EMZ, the measured δ11B values are consistently low. Fibrous aragonite is characterized by systematically higher d11B values, but also display B isotopic heterogeneity associated with specific growth bands in the calyx wall. The magnitude of the observed B isotopic variations cannot be explained by changes in environmental conditions and are likely caused by biological processes involved in the biomineralization of new skeleton; i.e. 'vital' effects. The observed B isotopic variations are opposite to the predictions of geochemical models for vital effects. Our data indicate that pH variations are not responsible for the observed stable isotopic fractionations. Geochemical models therefore do not provide an adequate framework within which to understand coral skeletal formation. Without a better understanding of these processes, which require experiments, the use of B isotopic composition to reconstruct paleo-pH variations in the oceans must be considered problematic - at least as far as Lophelia pertusa is concerned.

Chapter 16Tracing Nitrogen Sources and Cycling in Catchments

USGS Publications Warehouse

Kendall, Carol

1998-01-01

This chapter focuses on the uses of isotopes to understand water chemistry.I Isotopic compositions generally cannot be interpreted successfully in the absence of other chemical and hydrologic data. The chapter focusses on uses of isotopes in tracing sources and cycling of nitrogen in the water-component of forested catchment, and on dissolved nitrate in shallow waters, nutrient uptake studies in agricultural areas, large-scale tracer experiments, groundwater contamination studies, food-web investigations, and uses of compound-specific stable isotope techniques. Shallow waters moving along a flowpath through a relatively uniform material and reacting with minerals probably do not achieve equilibrium but gradually approach some steady-state composition. The chapter also discusses the use of isotopic techniques to assess impacts of changes in land-management practices and land use on water quality. The analysis of individual molecular components for isotopic composition has much potential as a method for tracing the source, biogeochemistry, and degradation of organic liquids and gases because different materials have characteristic isotope spectrums or biomarkers.

Tracing fluid transfer across subduction zones using iron and zinc stable isotopes

NASA Astrophysics Data System (ADS)

Williams, H. M.; Debret, B.; Pons, M. L.; Bouilhol, P.

2016-12-01

In subduction zones, serpentinite devolatilization within the downgoing slab and the fluids released play a fundamental role in volatile transfer as well as the redox evolution of the sub-arc mantle. Constraining subduction-related serpentinite devolatilisation is essential in order to better understand of the nature and composition of slab-derived fluids and fluid/rock interactions. Fe and Zn stable isotopes can trace fluid composition and speciation as isotope partitioning is driven by changes in oxidation state, coordination, and bonding environment. In the case of serpentinite devolatilisation, Fe isotope fractionation should reflect changes in Fe redox state and the formation of Fe-Cl- and SO42- complexes (Hill et al., GCA 2010); Zn isotope fractionation should be sensitive to complexation with CO32-, HS- and SO42- anions (Fujii et al., GCA 2011). We targeted samples from Western Alps ophiolite complexes, interpreted as remnants of serpentinized oceanic lithosphere metamorphosed and devolatilized during subduction (Hattori and Guillot, G3 2007; Debret et al., Chem. Geol. 2013). A striking negative correlation is present between bulk serpentinite Fe isotope composition and Fe3+/Fetot, with the highest grade samples displaying the heaviest Fe isotope compositions and lowest Fe3+/Fetot (Debret et al., Geology, 2016). The same samples also display a corresponding variation in Zn isotopes, with the highest grade samples displaying isotopically light compositions (Pons et al., in revision). The negative correlation between Fe and Zn isotopes and decrease in Fe3+/Fetot can explained by serpentinite sulfide breakdown and the release of fluids enriched in isotopically light Fe and heavy Zn sulphate complexes. The migration of these SOX-bearing fluids from the slab to the slab-mantle interface or mantle wedge has important implications for the redox evolution of the sub-arc mantle and the transport of metals from the subducting slab.

Improvement of 2,4-dinitrophenylhydrazine derivatization method for carbon isotope analysis of atmospheric acetone.

PubMed

Wen, Sheng; Yu, Yingxin; Guo, Songjun; Feng, Yanli; Sheng, Guoying; Wang, Xinming; Bi, Xinhui; Fu, Jiamo; Jia, Wanglu

2006-01-01

Through simulation experiments of atmospheric sampling, a method via 2,4-dinitrophenylhydrazine (DNPH) derivatization was developed to measure the carbon isotopic composition of atmospheric acetone. Using acetone and a DNPH reagent of known carbon isotopic compositions, the simulation experiments were performed to show that no carbon isotope fractionation occurred during the processes: the differences between the predicted and measured data of acetone-DNPH derivatives were all less than 0.5 per thousand. The results permitted the calculation of the carbon isotopic compositions of atmospheric acetone using a mass balance equation. In this method, the atmospheric acetone was collected by a DNPH-coated silica cartridge, washed out as acetone-DNPH derivatives, and then analyzed by gas chromatography/combustion/isotope ratio mass spectrometry (GC/C/IRMS). Using this method, the first available delta13C data of atmospheric acetone are presented. Copyright 2006 John Wiley & Sons, Ltd.

Determination of chemical purity and isotopic composition of natural and carbon-13-labeled arsenobetaine bromide standards by quantitative(1)H-NMR.

PubMed

Le, Phuong-Mai; Ding, Jianfu; Leek, Donald M; Mester, Zoltan; Robertson, Gilles; Windust, Anthony; Meija, Juris

2016-10-01

In this study, we report the characterization of three arsenobetaine-certified reference materials by quantitative NMR. We have synthesized an arsenobetaine bromide high-purity standard of natural isotopic composition (ABET-1) and two carbon-13-labeled isotopic standards (BBET-1 and CBET-1). Assignments of the chemical purity and isotopic composition are not trivial in the case of arsenobetaine, and in this study we utilized quantitative(1)H-NMR techniques for the determination of the mass fractions (chemical purity). The isotopic purity of all three standards was also assessed by NMR from the carbon-13 satellite signals. The standards are non-hygroscopic, high-purity (ca. 0.99 g/g), and the carbon-13 enrichment for both isotopic standards is x((13)C)≈0.99. These standards are designed for use as primary calibrators for mass spectrometric determination of arsenobetaine in environmental samples.

Fabrication of thorium bearing carbide fuels

DOEpatents

Gutierrez, Rueben L.; Herbst, Richard J.; Johnson, Karl W. R.

1981-01-01

Thorium-uranium carbide and thorium-plutonium carbide fuel pellets have been fabricated by the carbothermic reduction process. Temperatures of 1750.degree. C. and 2000.degree. C. were used during the reduction cycle. Sintering temperatures of 1800.degree. C. and 2000.degree. C. were used to prepare fuel pellet densities of 87% and >94% of theoretical, respectively. The process allows the fabrication of kilogram quantities of fuel with good reproducibility of chemicals and phase composition. Methods employing liquid techniques that form carbide microspheres or alloying-techniques which form alloys of thorium-uranium or thorium-plutonium suffer from limitation on the quantities processed of because of criticality concerns and lack of precise control of process conditions, respectively.

Isotopic Analysis of Fingernails as a USGS Open House Demonstration of the Use of Stable Isotopes in Foodweb Studies

NASA Astrophysics Data System (ADS)

Silva, S. R.; Kendall, C.; Young, M. B.; Choy, D.

2011-12-01

The USGS Isotope Tracers Project uses stable isotopes and tritium to add a unique dimension of chemical information to a wide range of environmental investigations. The use and application of isotopes is usually an unfamiliar and even esoteric topic to the general public. Therefore during three USGS open house events, as a public outreach effort, we demonstrated the use of stable isotopes by analyzing nitrogen and carbon isotopes from very small fragments of fingernail from willing participants. We titled the exhibit "You Are What You Eat". The results from all participants were plotted on a graph indicating the general influence of different food groups on the composition of body tissues as represented by fingernails. All participants were assigned a number and no personal-identification information was collected. A subset of participants provided us with an estimate of the number of days a week various foods were eaten and if they were vegetarians, vegans or non-vegetarians. Volunteers from our research group were on hand to explain and discuss fundamental concepts such as how foods attain their isotopic composition, the difference between C3 and C4 plants, the effects of assimilation, trophic enrichment, and the various uses of stable isotopes in environmental studies. The results of the fingernail analyses showed the variation of the range of isotopic compositions among about 400 people at each event, the distinct influence of C4 plants (mainly corn and cane sugar) on our carbon isotopic composition, and the isotopic differences between vegetarians and non vegetarians among other details (http://wwwrcamnl.wr.usgs.gov/isoig/projects/fingernails/). A poll of visitors attending the open house event in 2006 indicated that "You Are What You Eat" was among the most popular exhibits. Following the first two open house events we were contacted by a group of researchers from Brazil who had completed a very similar study. Our collaboration resulted in a publication in the American Journal of Physical Anthropology (Nardoto et al., 2006). This study found that despite global trends toward dietary homogenization, regional differences in food resources and dietary preferences were recorded in the carbon and nitrogen isotopic compositions of fingernails.

Sea surface salinity of the Eocene Arctic Azolla event using innovative isotope modeling

NASA Astrophysics Data System (ADS)

Speelman, E. N.; Sewall, J. O.; Noone, D.; Huber, M.; Sinninghe Damste, J. S.; Reichart, G. J.

2009-04-01

With the realization that the Eocene Arctic Ocean was covered with enormous quantities of the free floating freshwater fern Azolla, new questions regarding Eocene conditions facilitating these blooms arose. Our present research focuses on constraining the actual salinity of, and water sources for, the Eocene Arctic basin through the application of stable water isotope tracers. Precipitation pathways potentially strongly affect the final isotopic composition of water entering the Arctic Basin. Therefore we use the Community Atmosphere Model (CAM3), developed by NCAR, combined with a recently developed integrated isotope tracer code to reconstruct the isotopic composition of global Eocene precipitation and run-off patterns. We further addressed the sensitivity of the modeled hydrological cycle to changes in boundary conditions, such as pCO2, sea surface temperatures (SSTs) and sea ice formation. In this way it is possible to assess the effect of uncertainties in proxy estimates of these parameters. Overall, results of all runs with Eocene boundary conditions, including Eocene topography, bathymetry, vegetation patterns, TEX86 derived SSTs and pCO2 estimates, show the presence of an intensified hydrological cycle with precipitation exceeding evaporation in the Arctic region. Enriched, precipitation weighted, isotopic values of around -120‰ are reported for the Arctic region. Combining new results obtained from compound specific isotope analyses (δD) on terrestrially derived n-alkanes extracted from Eocene sediments, and model outcomes make it possible to verify climate reconstructions for the middle Eocene Arctic. Furthermore, recently, characteristic long-chain mid-chain ω20 hydroxy wax constituents of Azolla were found in ACEX sediments. δD values of these C32 - C36 diols provide insight into the isotopic composition of the Eocene Arctic surface water. As the isotopic signature of the runoff entering the Arctic is modelled, and the final isotopic composition of the surface waters can be deduced from the isotopic composition of the diols, we can calculate the degree of mixing between freshwater (isotopically light) and seawater (isotopically heavy) in the surface waters. This way we quantify Eocene Arctic surface water salinity, which in turn will shed light on the degree of (seasonal) mixing and stratification.

Return to the Strangelove Ocean?: Preliminary results of carbon and oxygenisotope compositions of post-impact sediments, IODP Expedition 364 "Chicxulub Impact Crater"

NASA Astrophysics Data System (ADS)

Yamaguchi, K. E.; Ikehara, M.; Hayama, H.; Takiguchi, S.; Masuda, S.; Ogura, C.; Fujita, S.; Kurihara, E.; Matsumoto, T.; Oshio, S.; Ishihata, K.; Fuchizawa, Y.; Noda, H.; Sakurai, U.; Yamane, T.; Morgan, J. V.; Gulick, S. P. S.

2017-12-01

The Chicxulub crater in the northern Yucatan Peninsula, Mexico was formed by the asteroid impact at the Cretaceous-Paleogene boundary (66.0 Ma). In early 2016 the IODP Exp. 364 successfully drilled the materials from the topographic peak ring within the crater that was previously identified by seismological observations. A continuous core was recovered. The 112m-thick uppermost part of the continuous core (505.7-1334.7 mbsf) is post-impact sediments, including the PETM, that are mainly composed of carbonate with intercalation of siliciclastics and variable contents of organic carbon. More than 300 samples from the post-impact section were finely powdered for a variety of geochemical analysis. Here we report their carbon and oxygen isotope compositions of the carbonate fraction (mostly in the lower part of the analyzed section) and carbon and nitrogen isotope compositions of organic matter (mostly in the middle-upper part of the analyzed section). Isotope mass spectrometer Isoprime was used for the former analysis, and EA-irMS (elemental analyzer - isotope ratio mass spectrometer) was used for the latter analysis, both at CMCR, Kochi Univ. Depth profile of oxygen isotope compositions of carbonate fraction is variable and somewhat similar to those of Zachos et al. (2001; Science). Carbon isotope compositions of carbonate and organic carbon in the lower part of the analyzed section exhibit some excursions that could correspond to the hyperthemals in the early Paleogene. Their variable nitrogen isotope compositions reflect temporal changes in the style of biogeochemical cycles involving denitrification and nitrogen fixation. Coupled temporal changes in the carbon isotope compositions of organic and carbonate carbon immediately after the K-Pg boundary might support a Strangelove ocean (Kump, 1991; Geology), however high export production (Ba/Ti, nannoplankton and calcisphere blooms, high planktic foram richness, and diverse and abundant micro- and macrobenthic organisms) at the base of the Danian limestone cored during Exp. 364 contradict a Strangelove Ocean.

Nickel isotopic composition of the mantle

NASA Astrophysics Data System (ADS)

Gall, Louise; Williams, Helen M.; Halliday, Alex N.; Kerr, Andrew C.

2017-02-01

This paper presents a detailed high-precision study of Ni isotope variations in mantle peridotites and their minerals, komatiites as well as chondritic and iron meteorites. Ultramafic rocks display a relatively large range in δ60 Ni (permil deviation in 60 Ni /58 Ni relative to the NIST SRM 986 Ni isotope standard) for this environment, from 0.15 ± 0.07‰ to 0.36 ± 0.08‰, with olivine-rich rocks such as dunite and olivine cumulates showing lighter isotope compositions than komatiite, lherzolite and pyroxenite samples. The data for the mineral separates shed light on the origin of these variations. Olivine and orthopyroxene display light δ60 Ni whereas clinopyroxene and garnet are isotopically heavy. This indicates that peridotite whole-rock δ60 Ni may be controlled by variations in modal mineralogy, with the prediction that mantle melts will display variable δ60 Ni values due to variations in residual mantle and cumulate mineralogy. Based on fertile peridotite xenoliths and Phanerozoic komatiite samples it is concluded that the upper mantle has a relatively homogeneous Ni isotope composition, with the best estimate of δ60Nimantle being 0.23 ± 0.06‰ (2 s.d.). Given that >99% of the Ni in the silicate Earth is located in the mantle, this also defines the Ni isotope composition of the Bulk Silicate Earth (BSE). This value is nearly identical to the results obtained for a suite of chondrites and iron meteorites (mean δ60 Ni 0.26 ± 0.12‰ and 0.29 ± 0.10‰, respectively) showing that the BSE is chondritic with respect to its Ni isotope composition, with little to no Ni mass-dependent isotope fractionation resulting from core formation.

In Situ Carbon Isotope Analysis by Laser Ablation MC-ICP-MS.

PubMed

Chen, Wei; Lu, Jue; Jiang, Shao-Yong; Zhao, Kui-Dong; Duan, Deng-Fei

2017-12-19

Carbon isotopes have been widely used in tracing a wide variety of geological and environmental processes. The carbon isotope composition of bulk rocks and minerals was conventionally analyzed by isotope ratio mass spectrometry (IRMS), and, more recently, secondary ionization mass spectrometry (SIMS) has been widely used to determine carbon isotope composition of carbon-bearing solid materials with good spatial resolution. Here, we present a new method that couples a RESOlution S155 193 nm laser ablation system with a Nu Plasma II MC-ICP-MS, with the aim of measuring carbon isotopes in situ in carbonate minerals (i.e., calcite and aragonite). Under routine operating conditions for δ 13 C analysis, instrumental bias generally drifts by 0.8‰-2.0‰ in a typical analytical session of 2-3 h. Using a magmatic calcite as the standard, the carbon isotopic composition was determined for a suite of calcite samples with δ 13 C values in the range of -6.94‰ to 1.48‰. The obtained δ 13 C data are comparable to IRMS values. The combined standard uncertainty for magmatic calcite is <0.3‰ (1s). No significant matrix effects have been identified in calcite with the amplitude of chemical composition variation (i.e., MnO, SrO, MgO, or FeO) up to 2.5 wt %. Two modern corals were investigated using magmatic calcite as the calibration standard, and the average δ 13 C values for both corals are similar to the bulk IRMS values. Moreover, coral exhibits significant heterogeneity in carbon isotope compositions, with differences up to 4.85‰ within an individual coral. This study indicates that LA-MC-ICP-MS can serve as an appropriate method to analyze carbon isotopes of carbonate minerals in situ.

Compound-specific Isotope Analysis of Cyanobacterial Pure cultures and Microbial Mats: Effects of Photorespiration?

NASA Technical Reports Server (NTRS)

Jahnke, L. L.; Summons, R. E.

2006-01-01

Microbial mats are considered modern homologs of Precambrian stromatolites. The carbon isotopic compositions of organic matter and biomarker lipids provide clues to the depositional environments of ancient mat ecosystems. As the source of primary carbon fixation for over two billion years, an understanding of cyanobacterial lipid biosynthesis, associated isotopic discriminations, and the influence of physiological factors on growth and isotope expression is essential to help us compare modern microbial ecosystems to their ancient counterparts. Here, we report on the effects of photorespiration (PR) on the isotopic composition of cyanobacteria and biomarker lipids, and on potential PR effects associated with the composition of various microbial mats. The high light, high O2 and limiting CO2 conditions often present at the surface of microbial mats are known to support PR in cyanobacteria. The oxygenase function of ribulose bisphosphate carboxylase/oxygenase can result in photoexcretion of glycolate and subsequent degration by heterotrophic bacteria. We have found evidence which supports an isotopic depletion (increased apparent E) scaled to O2 level associated with growth of Phormidium luridum at low CO2 concentrations (less than 0.04%). Similar to previous studies, isotopic differences between biomass and lipid biomarkers, and between lipid classes were positively correlated with overall fractionation, and should provide a means of estimating the influence of PR on overall isotopic composition of microbial mats. Several examples of microbial mats growing in the hydrothermal waters of Yellowstone National Park and the hypersaline marine evaporation ponds at Guerrero Negro, Baja Sur Mexico will be compared with a view to PR as a possible explanation of the relatively heavy C-isotope composition of hypersaline mats.

Characterization of Representative Materials in Support of Safe, Long Term Storage of Surplus Plutonium in DOE-STD-3013 Containers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Narlesky, Joshua E.; Stroud, Mary Ann; Smith, Paul Herrick

2013-02-15

The Surveillance and Monitoring Program is a joint Los Alamos National Laboratory/Savannah River Site effort funded by the Department of Energy-Environmental Management to provide the technical basis for the safe, long-term storage (up to 50 years) of over 6 metric tons of plutonium stored in over 5,000 DOE-STD-3013 containers at various facilities around the DOE complex. The majority of this material is plutonium that is surplus to the nuclear weapons program, and much of it is destined for conversion to mixed oxide fuel for use in US nuclear power plants. The form of the plutonium ranges from relatively pure metalmore » and oxide to very impure oxide. The performance of the 3013 containers has been shown to depend on moisture content and on the levels, types and chemical forms of the impurities. The oxide materials that present the greatest challenge to the storage container are those that contain chloride salts. Other common impurities include oxides and other compounds of calcium, magnesium, iron, and nickel. Over the past 15 years the program has collected a large body of experimental data on 54 samples of plutonium, with 53 chosen to represent the broader population of materials in storage. This paper summarizes the characterization data, moisture analysis, particle size, surface area, density, wattage, actinide composition, trace element impurity analysis, and shelf life surveillance data and includes origin and process history information. Limited characterization data on fourteen nonrepresentative samples is also presented.« less

Uncertainty quantification in fission cross section measurements at LANSCE

DOE PAGES

Tovesson, F.

2015-01-09

Neutron-induced fission cross sections have been measured for several isotopes of uranium and plutonium at the Los Alamos Neutron Science Center (LANSCE) over a wide range of incident neutron energies. The total uncertainties in these measurements are in the range 3–5% above 100 keV of incident neutron energy, which results from uncertainties in the target, neutron source, and detector system. The individual sources of uncertainties are assumed to be uncorrelated, however correlation in the cross section across neutron energy bins are considered. The quantification of the uncertainty contributions will be described here.

What is the iron isotope composition of the Moon?

NASA Astrophysics Data System (ADS)

Poitrasson, F.; Zambardi, T.; Magna, T.; Neal, C. R.

2016-12-01

It is difficult to estimate the bulk chemical and isotopic composition of the Moon because of severe limitations in our sampling. As a result, there is currently a debate on the bulk Fe isotope composition of the Moon despite the constraints on the lunar accretion modes or differentiation processes it may provide. For this, a proper mass balance estimation of essential planetary reservoirs is required. For instance, the dichotomy in δ57Fe between low- and high-Ti mare basalt varieties as a consequence of differences in degree of fractional crystallization of their respective lunar mantle sources should be rigorously tested. To investigate this, we performed new iron isotope measurements of 33 bulk lunar mare basalts and highland rocks, including KREEP-related materials. The new data show significant Fe isotope differences between high-Ti and low-Ti mare basalts, yielding mean δ57FeIRMM-014=0.277±0.020‰ and δ57FeIRMM-014=0.127±0.020‰, respectively. Assuming that lunar basalts mirror the iron isotope composition of their respective mantle protoliths, the estimated relative proportion of the low-Ti and high-Ti mantle source suggests that the lunar upper mantle should be close to δ57Fe=0.14±0.03‰. At present, it is unclear whether the bulk lunar Fe isotope composition is indistinguishable from that of the Earth (δ57FeIRMM-014=0.10±0.03‰), when estimated solely from mare basalts data, or if it is twice as heavy relative to chondrites, as initially proposed. A large scatter at δ57Fe=0.08±0.19‰ for ferroan anorthosites, Mg-suite rocks and a KREEP basalt imparts more complexities for global isotopic view of the Moon. A better understanding of the cause of Fe isotope heterogeneity among the lunar highland rocks will likely allow to better estimate the bulk Moon composition, and possibly to improve our knowledge about the genesis of the lunar crust itself.

Low-resolution gamma-ray spectrometry for an information barrier based on a multi-criteria template-matching approach

NASA Astrophysics Data System (ADS)

Göttsche, Malte; Schirm, Janet; Glaser, Alexander

2016-12-01

Gamma-ray spectrometry has been successfully employed to identify unique items containing special nuclear materials. Template information barriers have been developed in the past to confirm items as warheads by comparing their gamma signature to the signature of true warheads. Their development has, however, not been fully transparent, and they may not be sensitive to some relevant evasion scenarios. We develop a fully open template information barrier concept, based on low-resolution measurements, which, by design, reduces the extent of revealed sensitive information. The concept is based on three signatures of an item to be compared to a recorded template. The similarity of the spectrum is assessed by a modification of the Kolmogorov-Smirnov test to confirm the isotopic composition. The total gamma count rate must agree with the template as a measure of the projected surface of the object. In order to detect the diversion of fissile material from the interior of an item, a polyethylene mask is placed in front of the detector. Neutrons from spontaneous and induced fission events in the item produce 2.223 MeV gamma rays from neutron capture by hydrogen-1 in the mask. This peak is detected and its intensity scales with the item's fissile mass. The analysis based on MCNP Monte Carlo simulations of various plutonium configurations suggests that this concept can distinguish a valid item from a variety of invalid ones. The concept intentionally avoids any assumptions about specific spectral features, such as looking for specific gamma peaks of specific isotopes, thereby facilitating a fully unclassified discussion. By making all aspects public and allowing interested participants to contribute to the development and benchmarking, we enable a more open and inclusive discourse on this matter.

Isotope and trace element insights into heterogeneity of subridge mantle

NASA Astrophysics Data System (ADS)

Mallick, Soumen; Dick, Henry J. B.; Sachi-Kocher, Afi; Salters, Vincent J. M.

2014-06-01

Geochemical data for abyssal peridotites are used to determine the relationship to mid-ocean ridge basalts from several locations at ridge segments on the SW Indian Ridge (SWIR), the Mid-Cayman-Rise (MCR), and the Mid-Atlantic Ridge (MAR). Based on chemical and petrological criteria peridotites are categorized as being either dominantly impregnated with melt or being residual after recent melting. Those that are considered impregnated with melt also have isotopic compositions similar to the basalts indicating impregnation by an aggregate MORB melt. A SWIR and MCR residual peridotite Nd-isotopic compositions partly overlap the Nd-isotopic compositions of the basalts but extend to more radiogenic compositions. The differences between peridotite and basalt Nd-isotopic compositions can be explained by incorporating a low-solidus component with enriched isotopic signature in the subridge mantle: a component that is preferentially sampled by the basalts. At the MAR, peridotites and associated basalts have overlapping Nd-isotopic compositions, suggesting a more homogeneous MORB mantle. The combined chemistry and petrography indicates a complex history with several depletion and enrichment events. The MCR data indicate that a low-solidus component can be a ubiquitous component of the asthenosphere. Residual abyssal peridotites from limited geographic areas also show significant chemical variations that could be associated with initial mantle heterogeneities related to events predating the ridge-melting event. Sm-Nd model ages for possible earlier depletion events suggest these could be as old as 2.4 Ga. This article was corrected on 9 JULY 2014. See the end of the full text for details.

Triple Oxygen Isotope Constraints on Seawater δ18O and Temperature

NASA Astrophysics Data System (ADS)

Hayles, J.; Shen, B.; Homann, M.; Yeung, L.

2017-12-01

One point of contention among geoscientists is whether the 18O/16O ratio of seawater is roughly constant, or if it varies considerably throughout geologic time. On one hand, the oxygen isotope composition of the ocean is thought to be well buffered by high- and low-temperature interactions between seawater and seafloor rocks. If these interactions do not vary on billion-year timescales, the oxygen-isotope compositions of marine sedimentary rocks mostly relate to changes in seawater temperature and global ice volume. On the other hand, long-term cooling of the planetary interior would alter these water-rock interactions leading to a secular change in the oxygen isotope composition of seawater. Models suggest that this secular change would enrich seawater with heavy oxygen isotopes over time. In this study, we present new, high precision, triple-oxygen-isotope (18O/16O, 17O/16O) analyses of marine chert samples from 3.45 Ga to 460Ma. The results of these analyses are paired with a new theoretical quartz-water equilibrium curve and a simplified seawater model to provide possible pairings of δ'18O and Δ'17O for the water which these samples could have formed in equilibrium with. Analysis of the new sample data, in addition to published chert triple oxygen isotope compositions, shows a general trend of older chert samples being progressively incompatible with waters possessing a modern-like seawater triple oxygen isotope composition. Implications on constraining the secular evolution of seawater δ18O and temperature will be discussed.

Impact of topography, climate and moisture sources on isotopic composition (δ18O &δD) of rivers in the Pyrenees: Implications for topographic reconstructions in small orogens

NASA Astrophysics Data System (ADS)

Huyghe, Damien; Mouthereau, Frédéric; Sébilo, Mathieu; Vacherat, Arnaud; Ségalen, Loïc; Richard, Patricia; Biron, Philippe; Bariac, Thierry

2018-02-01

Understanding how orogenic topography controls the spatial distribution and isotopic composition of precipitation is critical for paleoaltitudinal reconstructions. Here, we determine the isotopic composition (δ18O and δD) of 82 small rivers and springs from small catchments in the Pyrenees. Calculation of the deuterium excess (d-excess) parameter allows the distinction of four distinct isotopic provinces with d-excess values of between 15 and 22‰ in the northwest, between 7 and 14‰ in the central northern Pyrenees and between 3 and 11‰ in the northeast. The southern Pyrenees have a homogenous d-excess signature ranging from 7 to 14‰. Our results show significant local moisture recycling and/or rain amount effect in the northwestern Pyrenees, and control by evaporation processes during rainfall events in the southern Pyrenees and for low elevated samples of the northeast of the range. Based on the distribution of d-excess values, we estimate contrasting isotope lapse rates of -2.9/-21.4‰/km (δ18O/δD) in the northwest, -2.7/-21.4‰/km (δ18O/δD) in the north central and -3.7/-31.7‰/km (δ18O/δD) in the northeastern Pyrenees. The southern Pyrenees show distinctly higher lapse rates of -9.5/-77.5‰/km (δ18O/δD), indicating that in this area the altitudinal effect in not the only parameter driving isotopic composition of rivers. Despite their relatively low topographic gradient, the Pyrenees exert a direct control on the isotopic composition of river waters, especially on their northern side. The variations in isotopic composition-elevation relationships documented along the strike of the range are interpreted to reflect an increasing continentality effect driven by wind trajectories parallel to the range, and mixing with Mediterranean air masses. Despite these effects, the measurable orographic effect on precipitation in the Pyrenees proves that the isotopic composition approach for reconstructing past topography is applicable to low-elevation orogens.

DN/DG Screening of Environmental Swipe Samples: FY2016 Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Glasgow, David C.; Croft, Stephen; Venkataraman, Ramkumar

The Delayed Neutron Delayed Gamma (DNDG) technique provides a new analytical capability to the International Atomic Energy Agency (IAEA) for detecting undeclared nuclear activities. IAEA’s Long Term R&D (LTRD) plan has a stated high urgency need to develop elemental and isotopic signatures of nuclear fuel cycle activities and processes (LTRD 2.2). The new DNDG capability is used to co-detect both uranium and plutonium as an extension of a DN only method that is already being utilized by the IAEA for the analysis of swipes to inform on undeclared nuclear activities. Analytical method involving irradiation of swipe samples potentially containing tracemore » quantities of fissile material in a thermal neutron field, followed by the counting of delayed neutrons, is a well-known technique in the field of safeguards and nonproliferation. It is used for detecting the presence of microscopic amounts of fissile material, (typically a linear combination of 233U, 235U, 239Pu, and 241Pu)and quantifying it in terms of the equivalent mass of 235U. The delayed neutron (DN) technique is very sensitive and is been routinely employed at the High Flux Isotope Reactor (HFIR) facility at Oak Ridge National Laboratory (ORNL). Both uranium and plutonium are of high safeguards value. However, the DN technique is not well suited for distinguishing between U and Pu isotopes since the decay curves overlap closely. The delayed gamma (DG) technique will help detect the presence of 239Pu in a mixture of U and Pu. Thus the DNDG approach combines the best of both worlds; the sensitivity of DN counting and the isotopic specificity of DG counting. The present work seeks to build on the delayed neutron and delayed gamma methods that have been developed at ORNL. It is recognized that the distribution profile of heavy fission products remains fairly invariant for the fissile nuclides whereas the distribution of light fission products varies from one isotope to another. That is, the ratio of the yield of a light fission fragment to a heavy fission fragments is isotope specific. Measurement of the ratio of the net full energy peak (FEP) from low/high mass fission products is an elegant way to characterize the fraction of fissile materials present in a mixture. By empirically calibrating the ratio of the net FEP as a function of known concentration of the binary mixture, one can determine the fraction of fissile isotopes in an unknown sample. In the work done in fiscal year (FY) 2016, samples of single fissile material isotopes as well as binary mixtures were irradiated in a well thermalized irradiation field in the HFIR. Delayed neutron counting was performed using the neutron counter at the HFIR Neutron Activation Analysis (NAA) laboratory. Delayed gamma counting was performed using a shielded high purity germanium (HPGe) detector. Delayed neutron decay curve results highlighted the difficulty of distinguishing between U and Pu isotopes, and the need for including the delayed gamma component. Based on delayed gamma spectrometry, twelve ratios of low mass/high fission product gamma ray FEP have been identified as valid candidates. Linearity of the ratios, as a function of 239Pu fraction in 235U+ 239Pu mixtures, was confirmed for the low mass/high mass candidates that were selected. The DNDG method we are spearheading allows not only the presence of total fissile content to be detected, but whether the material is predominantly U or predominantly Pu, or a mixture. This provides additional SG relevant information.« less

Hydrogen Isotope Measurements of Organic Acids and Alcohols by Pyrolysis-GC-MS-TC-IRMS

NASA Technical Reports Server (NTRS)

Socki, Richard A.; Fu, Qi; Niles, Paul B.

2011-01-01

One possible process responsible for methane generation on Mars is abiotic formation by Fischer-Tropsch-type (FTT) synthesis during serpentinization reactions. Measurement of carbon and hydrogen isotopes of intermediary organic compounds can help constrain the origin of this methane by tracing the geochemical pathway during formation. Of particular interest within the context of this work is the isotopic composition of organic intermediaries produced on the surfaces of mineral catalysts (i.e. magnetite) during hydrothermal experiments, and the ability to make meaningful and reproducible hydrogen isotope measurements. Reported here are results of experiments to characterize the hydrogen isotope composition of low molecular weight organic acids and alcohols. The presence of these organic compounds has been suggested by others as intermeadiary products made during mineral surface catalyzed reactions. This work compliments our previous study characterizing the carbon isotope composition of similar low molecular weight intermediary organic compounds (Socki, et al, American Geophysical Union Fall meeting, Abstr. #V51B-2189, Dec., 2010). Our hydrogen isotope measurements utilize a unique analytical technique combining Pyrolysis-Gas Chromatograph-Mass Spectrometry-High Temperature Conversion-Isotope Ratio Mass Spectrometry (Py-GC-MS-TC-IRMS). Our technique is unique in that it carries a split of the pyrolyzed GC-separated product to a Thermo DSQ-II? quadrupole mass spectrometer as a means of making qualitative and semi-quantitative compositional measurements of separated organic compounds, therefore both chemical and isotopic measurements can be carried out simultaneously on the same sample.

Isotopic coherence of refractory inclusions from CV and CK meteorites: Evidence from multiple isotope systems

NASA Astrophysics Data System (ADS)

Shollenberger, Quinn R.; Borg, Lars E.; Render, Jan; Ebert, Samuel; Bischoff, Addi; Russell, Sara S.; Brennecka, Gregory A.

2018-05-01

Calcium-aluminum-rich inclusions (CAIs) are the oldest dated materials in the Solar System and numerous previous studies have revealed nucleosynthetic anomalies relative to terrestrial rock standards in many isotopic systems. However, most of the isotopic data from CAIs has been limited to the Allende meteorite and a handful of other CV3 chondrites. To better constrain the isotopic composition of the CAI-forming region, we report the first Sr, Mo, Ba, Nd, and Sm isotopic compositions of two CAIs hosted in the CK3 desert meteorites NWA 4964 and NWA 6254 along with two CAIs from the CV3 desert meteorites NWA 6619 and NWA 6991. After consideration of neutron capture processes and the effects of hot-desert weathering, the Sr, Mo, Ba, Nd, and Sm stable isotopic compositions of the samples show clearly resolvable nucleosynthetic anomalies that are in agreement with previous results from Allende and other CV meteorites. The extent of neutron capture, as manifested by shifts in the observed 149Sm-150Sm isotopic composition of the CAIs is used to estimate the neutron fluence experienced by some of these samples and ranges from 8.40 × 1013 to 2.11 × 1015 n/cm2. Overall, regardless of CAI type or host meteorite, CAIs from CV and CK chondrites have similar nucleosynthetic anomalies within analytical uncertainty. We suggest the region that CV and CK CAIs formed was largely uniform with respect to Sr, Mo, Ba, Nd, and Sm isotopes when CAIs condensed and that CAIs hosted in CV and CK meteorites are derived from the same isotopic reservoir.

Large Carbonate Associated Sulfate isotopic variability between brachiopods, micrite, and other sedimentary components in Late Ordovician strata

NASA Astrophysics Data System (ADS)

Present, Theodore M.; Paris, Guillaume; Burke, Andrea; Fischer, Woodward W.; Adkins, Jess F.

2015-12-01

Carbonate Associated Sulfate (CAS) is trace sulfate incorporated into carbonate minerals during their precipitation. Its sulfur isotopic composition is often assumed to track that of seawater sulfate and inform global carbon and oxygen budgets through Earth's history. However, many CAS sulfur isotope records based on bulk-rock samples are noisy. To determine the source of bulk-rock CAS variability, we extracted CAS from different internal sedimentary components micro-drilled from well-preserved Late Ordovician and early Silurian-age limestones from Anticosti Island, Quebec, Canada. Mixtures of these components, whose sulfur isotopic compositions vary by nearly 25‰, can explain the bulk-rock CAS range. Large isotopic variability of sedimentary micrite CAS (34S-depleted from seawater by up to 15‰) is consistent with pore fluid sulfide oxidation during early diagenesis. Specimens recrystallized during burial diagenesis have CAS 34S-enriched by up to 9‰ from Hirnantian seawater, consistent with microbial sulfate reduction in a confined aquifer. In contrast to the other variable components, brachiopods with well-preserved secondary-layer fibrous calcite-a phase independently known to be the best-preserved sedimentary component in these strata-have a more homogeneous isotopic composition. These specimens indicate that seawater sulfate remained close to about 25‰ (V-CDT) through Hirnantian (end-Ordovician) events, including glaciation, mass extinction, carbon isotope excursion, and pyrite-sulfur isotope excursion. The textural relationships between our samples and their CAS isotope ratios highlight the role of diagenetic biogeochemical processes in setting the isotopic composition of CAS.

Bioconversion of Coal: Hydrologic indicators of the extent of coal biodegradation under different redox conditions and coal maturity, Velenje Basin case study, Slovenia

NASA Astrophysics Data System (ADS)

Kanduč, Tjaša; Grassa, Fausto; Lazar, Jerneja; Jamnikar, Sergej; Zavšek, Simon; McIntosh, Jennifer

2014-05-01

Underground mining of coal and coal combustion for energy has significant environmental impacts. In order to reduce greenhouse gas emissions, other lower -carbon energy sources must be utilized. Coalbed methane (CBM) is an important source of relatively low-carbon energy. Approximately 20% of world's coalbed methane is microbial in origin (Bates et al., 2011). Interest in microbial CBM has increased recently due to the possibility of stimulating methanogenesis. Despite increasing interest, the hydrogeochemical conditions and mechanisms for biodegradation of coal and microbial methane production are poorly understood. This project aims to examine geochemical characteristics of coalbed groundwater and coalbed gases in order to constrain biogeochemical processes to better understand the entire process of coal biodegradation of coal to coalbed gases. A better understanding of geochemical processes in CBM areas may potentially lead to sustainable stimulation of microbial methanogenesis at economical rates. Natural analogue studies of carbon dioxide occurring in the subsurface have the potential to yield insights into mechanisms of carbon dioxide storage over geological time scales (Li et al., 2013). In order to explore redox processes related to methanogenesis and determine ideal conditions under which microbial degradation of coal is likely to occur, this study utilizes groundwater and coalbed gas samples from Velenje Basin. Determination of the concentrations of methane, carbondioxide, nitrogen, oxygen, argon was performed with homemade NIER mass spectrometer. Isotopic composition of carbon dioxide, isotopic composition of methane, isotopic composition of deuterium in methane was determined with Europa-Scientific IRMS with an ANCA-TG preparation module and Thermo Delta XP GC-TC/CF-IRMS coupled to a TRACE GC analyzer. Total alkalinity of groundwater was measured by Gran titration. Major cations were analyzed by ICP-OES and anions by IC method. Isotopic composition of dissolved inorganic carbon was determined by MultiflowBio preparation module. The stable isotope composition of sulphur was determined with a Europa Scientific 20-20 continuous flow IRMS ANCA-SL preparation module. Concentrations of tritium were determined with the electrolytic enrichment method. PHREEQC for Windows was used to perform thermodynamic modelling. The average coalbed gas composition in the coalbed seam is approximately carbon dioxide: methane > 2:1, where a high proportion of CO2 is adsorbed on the lignite structure, while methane is present free in coal fractures. It can be concluded that isotopic composition of carbon in methane from -70.4‰ to -50.0‰ is generated via acetate fermentation and via reduction of carbon dioxide, while isotopic composition of carbon in methane values range from -50.0‰ to -18.8‰, thermogenic methane can be explained by secondary processes, causing enrichment of residual methane with the heavier carbon isotope. Isotopic composition of deuterium in methane range from -343.9‰ to -223.1‰. Isotopic composition of carbon in carbon dioxide values at excavation fields range from -11.0‰ to +5‰ and are endogenic and microbial in origin. The major ion chemistry, redox conditions, stable isotopes and tritium measured in groundwater from the Velenje Basin, suggest that the Pliocene and Triassic aquifers contain distinct water bodies. Groundwater in the Triassic aquifer is dominated by hydrogen carbonate, calcium, magnesium and isotopic composition of dissolved inorganic carbon indicating degradation of soil organic matter and dissolution of carbonate minerals, similar to surface waters. In addition, groundwater in the Triassic aquifer has isotopic composition of oxygen and isotopic composition of deuterium values which plot near surface waters on the local and global meteoric water lines and detectable tritium reflects recent recharge. In contrast, groundwater in the Pliocene aquifers is enriched in magnesium, sodium, calcium, potassium, and silica and has alkalinity and isotopic composition of dissolved inorganic carbon values with low sulphate and nitrate concentrations. These waters have likely been influenced by sulfate reduction and microbial methanogenesis associated with coal seams and dissolution of feldspars and magnesium-rich clay minerals. Pliocene aquifer waters are also depleted in heavier oxygen isotope and heavier deuterium isotope and have tritium concentrations near the detection limit, suggesting these waters are older. References Bates, B.L., McIntosh J.C., Lohse K.A., Brooks P.D. 2011: Influence of groundwater flowpaths, residence times, and nutrients on the extent of microbial methanogenesis in coal beds: Powder River Basin, USA, Chemical geology, 284, 45-61. Li, W., Cheng Y., Wang L., Zhou H., Wang H., Wang L. 2013: Evaluating the security of geological coalbed sequestration of supercritical CO2 reservoirs: The Haishiwan coalfield, China as a natural analogue, International Journal of Greenhouse Gas Control, 13, 102-111.

Noble gases in the moon

NASA Technical Reports Server (NTRS)

Manuel, O. K.; Srinivasan, B.; Hennecke, E. W.; Sinclair, D. E.

1972-01-01

The abundance and isotopic composition of helium, neon, argon, krypton, and xenon which were released by stepwise heating of lunar fines (15601.64) and (15271.65) were measured spectrometrically. The results of a composition of noble gases released from the lunar fines with noble gases in meteorites and in the earth are presented along with the isotopic composition of noble gases in lunar fines, in meteorites, and in the atmosphere. A study of two isotopically distinct components of trapped xenon in carbonaceous chondrites is also included.

Stable Isotope Characteristics of Jarosite: The Acidic Aqueous History of Mars

NASA Technical Reports Server (NTRS)

Earl, Lyndsey D.

2005-01-01

The Mars Rover Opportunity found jarosite (Na(+) or K(+))Fe3SO4(OH)6 at the Meridiani Planum site. This mineral forms from the evaporation of an aqueous acidic sulfate brine. Oxygen isotope compositions may characterize formation conditions but subsequent isotope exchange may have occurred between the sulfate and hydroxide of jarosite and water. The rate of oxygen isotope exchange depends on the acidity and temperature of the brine, but it has not been investigated in detail. We performed laboratory experiments to determine the rate of oxygen isotope exchange under varying acidities and temperatures to learn more about this process. Barium sulfate samples were precipitated weekly from acidic sodium sulfate brines. The oxygen isotope composition of the precipitated sulfate was obtained using a Finnigan MAT253 Isotope Ratio Mass-Spectrometer. The results show that water was trapped in barium sulfate during precipitation. Trapped water may exchange with sulfate when exposed to high temperatures, thus changing the isotope composition of sulfate and the observed fractionation factor of oxygen isotope exchange between sulfate and water. The results of our research will contribute to the understanding of oxygen isotope exchange rates between water and sulfate under acidic conditions and provide experimental knowledge for the dehydration of barium sulfate samples.

Thallium-isotopic compositions of euxinic sediments as a proxy for global manganese-oxide burial

NASA Astrophysics Data System (ADS)

Owens, Jeremy D.; Nielsen, Sune G.; Horner, Tristan J.; Ostrander, Chadlin M.; Peterson, Larry C.

2017-09-01

Thallium (Tl) isotopes are a new and potentially powerful paleoredox proxy that may track bottom water oxygen conditions based on the global burial flux of manganese oxides. Thallium has a residence time of ∼20 thousand years, which is longer than the ocean mixing time, and it has been inferred that modern oxic seawater is conservative with respect to both concentration and isotopes. Marine sources of Tl have nearly identical isotopic values. Therefore, the Tl sinks, adsorption onto manganese oxides and low temperature oceanic crust alteration (the dominant seawater output), are the primary controls of the seawater isotopic composition. For relatively short-term, ∼million years, redox events it is reasonable to assume that the dominant mechanism that alters the Tl isotopic composition of seawater is associated with manganese oxide burial because large variability in low temperature ocean crust alteration is controlled by long-term, multi-million years, average ocean crust production rates. This study presents new Tl isotope data for an open ocean transect in the South Atlantic, and depth transects for two euxinic basins (anoxic and free sulfide in the water column), the Cariaco Basin and Black Sea. The Tl isotopic signature of open ocean seawater in the South Atlantic was found to be homogeneous with ε205Tl = -6.0 ± 0.3 (±2 SD, n = 41) while oxic waters from Cariaco and the Black Sea are -5.6 and -2.2, respectively. Combined with existing data from the Pacific and Arctic Oceans, our Atlantic data establish the conservatism of Tl isotopes in the global ocean. In contrast, partially- and predominantly-restricted basins reveal Tl isotope differences that vary between open-ocean (-6) and continental material (-2) ε205Tl, scaling with the degree of restriction. Regardless of the differences between basins, Tl is quantitatively removed from their euxinic waters below the chemocline. The burial of Tl in euxinic sediments is estimated to be an order of magnitude less than each of the modern ocean outputs and imparts no isotopic fractionation. Thallium removal into pyrite appears to be associated with a small negative fractionation between -1 and -3 ε205Tl, which renders Tl-depleted waters below the chemocline enriched in isotopically-heavy Tl. Due to the quantitative removal of Tl from euxinic seawater, Tl isotope analyses of the authigenic fraction of underlying euxinic sediments from both the Black Sea and Cariaco Basin capture the Tl isotope value of the oxic portion of their respective water column with no net isotope fractionation. Since the Tl isotope composition of seawater is largely dictated by the relative fraction of Mn-oxide burial versus oceanic crust alteration, we contend that the Tl isotope composition of authigenic Tl in black shales, deposited under euxinic conditions but well-connected to the open ocean, can be utilized to reconstruct the Tl isotope composition of seawater, and thus to reconstruct the global history of Mn-oxide burial.

Iron isotope composition of particles produced by UV-femtosecond laser ablation of natural oxides, sulfides, and carbonates.

PubMed

d'Abzac, Francois-Xavier; Beard, Brian L; Czaja, Andrew D; Konishi, Hiromi; Schauer, James J; Johnson, Clark M

2013-12-17

The need for femtosecond laser ablation (fs-LA) systems coupled to MC-ICP-MS to accurately perform in situ stable isotope analyses remains an open question, because of the lack of knowledge concerning ablation-related isotopic fractionation in this regime. We report the first iron isotope analysis of size-resolved, laser-induced particles of natural magnetite, siderite, pyrrhotite, and pyrite, collected through cascade impaction, followed by analysis by solution nebulization MC-ICP-MS, as well as imaging using electron microscopy. Iron mass distributions are independent of mineralogy, and particle morphology includes both spheres and agglomerates for all ablated phases. X-ray spectroscopy shows elemental fractionation in siderite (C-rich agglomerates) and pyrrhotite/pyrite (S-rich spheres). We find an increase in (56)Fe/(54)Fe ratios of +2‰, +1.2‰, and +0.8‰ with increasing particle size for magnetite, siderite, and pyrrhotite, respectively. Fe isotope differences in size-sorted aerosols from pyrite ablation are not analytically resolvable. Experimental data are discussed using models of particles generation by Hergenröder and elemental/isotopic fractionation by Richter. We interpret the isotopic fractionation to be related to the iron condensation time scale, dependent on its saturation in the gas phase, as a function of mineral composition. Despite the isotopic variations across aerosol size fractions, total aerosol composition, as calculated from mass balance, confirms that fs-LA produces a stoichiometric sampling in terms of isotopic composition. Specifically, both elemental and isotopic fractionation are produced by particle generation processes and not by femtosecond laser-matter interactions. These results provide critical insights into the analytical requirements for laser-ablation-based stable isotope measurements of high-precision and accuracy in geological samples, including the importance of quantitative aerosol transport to the ICP.

Methane transport mechanisms and isotopic fractionation in emergent macrophytes of an Alaskan tundra lake

NASA Technical Reports Server (NTRS)

Chanton, Jeffrey P.; Martens, Christopher S.; Kelley, Cheryl A.; Crill, Patrick M.; Showers, William J.

1992-01-01

The stable carbon isotopic composition of methane associated with and emitted by the two dominant emergent macrophytes abundant in the many Alaskan tundra lakes, Carex rostrata and Arctophila fulva, is determined. The carbon isotopic composition of the methane was -58.6 +/- 0.5 (n=2) for Arctophila and -66.6 +/- 2.5 (n=6) for Carex. The methane emitted by these species is depleted in C-13 by 12 per mil for Arctophila and 18 per mil for Carex relative to methane withdrawn from plant stems 1-2 cm below the waterline. The results suggest more rapid transport of (C-12)H4 relative to (C-13)H4 through plants to the atmosphere. Plant stem methane concentrations ranged from 0.2 to 4.0 percent in Arctophila, with an isotopic composition of -46.1 +/- 4.3 percent (n=8). Carex stem methane concentrations ranged from 150 to 1200 ppm, with an isotopic composition of -48.3 +/- 1.4 per mil (n=3).

U-Pb systematics in iron meteorites - Uniformity of primordial lead

NASA Astrophysics Data System (ADS)

Gopel, C.; Manhes, G.; Allegre, C. J.

1985-08-01

Pb isotopic compositions and U-Pb abundances were determined in the metal phase of six iron meteorites: Canyon Diablo IA, Toluca IA, Odessa IA, Youndegin IA, Deport IA, and Mundrabilla An. Prior to complete dissolution, samples were subjected to a series of leachings and partial dissolutions. Isotopic compositions and abundances of the etched Pb indicate a contamination by terrestrial Pb which is attributable to previous cutting of the meteorite. Pb isotopic compositions measured in the decontaminated samples are identical within 0.2 percent and essentially confirm the primordial Pb value defined by Tatsumoto et al. (1973). These data invalidate more radiogenic Pb isotopic compositions published for iron meteorites, which are the result of terrestrial Pb contamination introduced mainly by analytical procedure. The results of this study support the idea of a solar nebula which was isotopically homogeneous for Pb 4.55 Ga ago. The new upper limit for U-abundance in iron meteorites, 0.001 ppb, is in agreement with its expected thermodynamic solubility in the metal phase.

The Chlorine Isotopic Composition Of Lunar UrKREEP

NASA Technical Reports Server (NTRS)

Barnes, J. J.; Tartese, R.; Anand, M.; McCubbin, F. M.; Neal, C. R.; Franchi, I. A.

2016-01-01

Since the long standing paradigm of an anhydrous Moon was challenged there has been a renewed focus on investigating volatiles in a variety of lunar samples. However, the current models for the Moon’s formation have yet to fully account for its thermal evolution in the presence of H2O and other volatiles. When compared to chondritic meteorites and terrestrial rocks, lunar samples have exotic chlorine isotope compositions, which are difficult to explain in light of the abundance and isotopic composition of other volatile species, especially H, and the current estimates for chlorine and H2O in the bulk silicate Moon. In order to better understand the processes involved in giving rise to the heavy chlorine isotope compositions of lunar samples, we have performed a comprehensive in situ high precision study of chlorine isotopes, using NanoSIMS (Nanoscale Secondary Ion Mass Spectrometry) of lunar apatite from a suite of Apollo samples covering a range of geochemical characteristics and petrologic types.

Hydrogen isotope fractionation during lipid biosynthesis by Haloarcula marismortui

NASA Astrophysics Data System (ADS)

Dirghangi, Sitindra S.; Pagani, Mark

2013-10-01

We studied the controls on the fractionation of hydrogen isotopes during lipid biosynthesis by Haloarcula marismortui, a halophilic archaea, in pure culture experiments by varying organic substrate, the hydrogen isotope composition (D/H) of water, temperature, and salinity. Cultures were grown on three substrates: succinate, pyruvate and glycerol with known hydrogen isotope compositions, and in water with different hydrogen isotopic compositions. All culture series grown on a particular substrate show strong correlations between δDarchaeol and δDwater. However, correlations are distinctly different for cultures grown on different substrates. Our results indicate that the metabolic pathway of substrate exerts a fundamental influence on the δD value of lipids, likely by influencing the D/H composition of NADPH (nicotinamide adenine dinucleotide phosphate), the reducing agent that contributes hydrogen to carbon atoms during lipid biosynthesis. Temperature and salinity have smaller, but similar effects on δDlipid, primarily due to the way temperature and salinity influence growth rate, as well as temperature effects on the activity of enzymes.

Fe isotope composition of bulk chondrules from Murchison (CM2): Constraints for parent body alteration, nebula processes and chondrule-matrix complementarity

NASA Astrophysics Data System (ADS)

Hezel, Dominik C.; Wilden, Johanna S.; Becker, Daniel; Steinbach, Sonja; Wombacher, Frank; Harak, Markus

2018-05-01

Chondrules are a major constituent of primitive meteorites. The formation of chondrules is one of the most elusive problems in cosmochemistry. We use Fe isotope compositions of chondrules and bulk chondrites to constrain the conditions of chondrule formation. Iron isotope compositions of bulk chondrules are so far only known from few studies on CV and some ordinary chondrites. We studied 37 chondrules from the CM chondrite Murchison. This is particularly challenging, as CM chondrites contain the smallest chondrules of all chondrite groups, except for CH chondrites. Bulk chondrules have δ56Fe between -0.62 and +0.24‰ relative to the IRMM-014 standard. Bulk Murchison has as all chondrites a δ56Fe of 0.00‰ within error. The δ56Fe distribution of the Murchison chondrule population is continuous and close to normal. The width of the δ56Fe distribution is narrower than that of the Allende chondrule population. Opaque modal abundances in Murchison chondrules is in about 67% of the chondrules close to 0 vol.%, and in 33% typically up to 6.5 vol.%. Chondrule Al/Mg and Fe/Mg ratios are sub-chondritic, while bulk Murchison has chondritic ratios. We suggest that the variable bulk chondrule Fe isotope compositions were established during evaporation and recondensation prior to accretion in the Murchison parent body. This range in isotope composition was likely reduced during aqueous alteration on the parent body. Murchison has a chondritic Fe isotope composition and a number of chondritic element ratios. Chondrules, however, have variable Fe isotope compositions and chondrules and matrix have complementary Al/Mg and Fe/Mg ratios. In combination, this supports the idea that chondrules and matrix formed from a single reservoir and were then accreted in the parent body. The formation in a single region also explains the compositional distribution of the chondrule population in Murchison.

Re-Os isotopic evidence for an enriched-mantle source for the Noril'sk-type, ore-bearing intrusions, Siberia

USGS Publications Warehouse

Walker, R.J.; Morgan, J.W.; Horan, M.F.; Czamanske, G.K.; Krogstad, E.J.; Fedorenko, V.A.; Kunilov, V.E.

1994-01-01

Magmatic Cu-Ni sulfide ores and spatially associated ultramafic and mafic rocks from the Noril'sk I, Talnakh, and Kharaelakh intrusions are examined for Re-Os isotopic systematics. Neodymium and lead isotopic data also are reported for the ultramafic and mafic rocks. The Re-Os data for most samples indicate closed-system behavior since the ca. 250 Ma igneous crystallization age of the intrusions. There are small but significant differences in the initial osmium isotopic compositions of samples from the three intrusions. Ores from the Noril'sk I intrusion have ??Os values that vary from +0.4 to +8.8, but average +5.8. Ores from the Talnakh intrusion have ??Os values that range from +6.7 to +8.2, averaging +7.7. Ores from the Kharaelakh intrusion have ??Os values that range from +7.8 to +12.9, with an average value of +10.4. The osmium isotopic compositions of the ore samples from the Main Kharaelakh orebody exhibit minimal overlap with those for the Noril'sk I and Talnakh intrusions, indicating that these Kharaelakh ores were derived from a more radiogenic source of osmium than the other ores. Combined osmium and lead data for major orebodies in the three intrusions plot in three distinct fields, indicating derivation of osmium and lead from at least three isotopically distinct sources. Some of the variation in lead isotopic compositions may be the result of minor lower-crustal contamination. However, in contrast to most other isotopic and trace element data, Os-Pb variations are generally inconsistent with significant crustal contamination or interaction with the subcontinental lithosphere. Thus, the osmium and lead isotopic compositions of these intrusions probably reflect quite closely the compositions of their mantle source, and suggest that these two isotope systems were insensitive to lithospheric interaction. Ultramafic and mafic rocks have osmium and lead isotopic compositions that range only slightly beyond the compositions of the ores. These rocks also have relatively uniform ??{lunate}Nd values that range only from -0.8 to + 1.1. This limited variation in neodymium isotopic composition may reflect the characteristics of the mantle sources of the rocks, or it may indicate that somehow similar proportions of crust contaminated the parental melts. The osmium, lead, and neodymium isotopic data for these rocks most closely resemble the mantle sources of certain ocean island basalts (OIB), such as some Hawaiian basalts. Hence, these data are consistent with derivation of primary melts from a mantle source similar to that of some types of hotspot activity. The long-term Re/Os enrichment of this and similar mantle sources, relative to chondritic upper mantle, may reflect 1. (1) incorporation of recycled oceanic crust into the source more than 1 Ga ago, 2. (2) derivation from a mantle plume that originated at the outer core-lower mantle interface, or 3. (3) persistence of primordial stratification of rhenium and osmium in the mantle. ?? 1994.

Isotope Geochemistry for Comparative Planetology of Exoplanets

NASA Technical Reports Server (NTRS)

Mandt, K. E.; Atreya, S.; Luspay-Kuti, A.; Mousis, O.; Simon, A.; Hofstadter, M. D.

2017-01-01

Isotope geochemistry has played a critical role in understanding processes at work in and the history of solar system bodies. Application of these techniques to exoplanets would be revolutionary and would allow comparative planetology with the formation and evolution of exoplanet systems. The roadmap for comparative planetology of the origins and workings of exoplanets involves isotopic geochemistry efforts in three areas: (1) technology development to expand observations of the isotopic composition of solar system bodies and expand observations to isotopic composition of exoplanet atmospheres; (2) theoretical modeling of how isotopes fractionate and the role they play in evolution of exoplanetary systems, atmospheres, surfaces and interiors; and (3) laboratory studies to constrain isotopic fractionation due to processes at work throughout the solar system.

Stable-isotope fingerprints of biological agents as forensic tools.

PubMed

Horita, Juske; Vass, Arpad A

2003-01-01

Naturally occurring stable isotopes of light elements in chemical and biological agents may possess unique "stable-isotope fingerprints" depending on their sources and manufacturing processes. To test this hypothesis, two strains of bacteria (Bacillus globigii and Erwinia agglomerans) were grown under controlled laboratory conditions. We observed that cultured bacteria cells faithfully inherited the isotopic composition (hydrogen, carbon, and nitrogen) of media waters and substrates in predictable manners in terms of bacterial metabolism and that even bacterial cells of the same strain, which grew in media water and substrates of different isotopic compositions, have readily distinguishable isotopic signatures. These "stable-isotopic fingerprints" of chemical and biological agents can be used as forensic tools in the event of biochemical terrorist attacks.

Magnesium isotope compositions of Solar System materials determined by double spiking

NASA Astrophysics Data System (ADS)

Hin, R.; Lai, Y. J.; Coath, C.; Elliott, T.

2015-12-01

As a major element, magnesium is of interest for investigating large scale processes governing the formation and evolution of rocky planetary bodies. Determining the Mg isotope composition of the Earth and other planetary bodies has hence been a topic of interest ever since mass-dependent fractionation of 'non-traditional' stable isotopes has been used to study high-temperature processes. Published results, however, suffer from disagreement on the Mg isotope compositions of the Earth and chondrites [1-5], which is attributed to residual matrix effects. Nonetheless, most recent studied have converged towards a homogeneous (chondritic) Mg isotope composition in the Solar System [2-5]. However, in several of the recent studies there is a hint of a systematic difference of about 0.02-0.06‰ in the 26Mg/24Mg isotope compositions of chondrites and Earth. Such difference, however, is only resolvable by taking standard errors, which assumes robust data for homogenous sample sets. The discrepancies between various studies unfortunately undermine the confidence in such robustness and homogeneity. The issues with matrix effects during isotopic analyses can be overcome by using a double spike approach. Such methodology generally requires three isotope ratios to solve for three unknowns, a requirement that cannot be met for Mg. However, using a newly developed approach, we present Mg isotope compositions obtained by critical mixture double spiking. This new approach should allow greater confidence in the robustness of the data and hence enable improvement of. Preliminary data indicate that chondrites have a resolvable ~0.04‰ lighter 26Mg/24Mg than (ultra)mafic rocks from Earth, Mars and the eucrite parent body, which appear indistinguishable from each other. It seems implausible that this difference is caused by magmatic process such as partial melting or crystallisation. More likely, Mg isotopes are fractionated by a non-magmatic process during the formation of planets, e.g. by vapour-condensate fractionation. [1] Wiechert and Halliday, 2007. EPSL 256, 360-371. [2] Bourdon et al., 2010. GCA 74, 5069-5083. [3] Teng et al., 2010. GCA 74, 4150-4166. [4] Chakrabarti and Jacobsen, 2010. EPSl 293, 349-358. [5] Von Strandmann, 2011. GCA 75, 5247-5268.

Equilibrium and non-equilibrium controls on the abundances of clumped isotopologues of methane during thermogenic formation in laboratory experiments: Implications for the chemistry of pyrolysis and the origins of natural gases

NASA Astrophysics Data System (ADS)

Shuai, Yanhua; Douglas, Peter M. J.; Zhang, Shuichang; Stolper, Daniel A.; Ellis, Geoffrey S.; Lawson, Michael; Lewan, Michael D.; Formolo, Michael; Mi, Jingkui; He, Kun; Hu, Guoyi; Eiler, John M.

2018-02-01

Multiply isotopically substituted molecules ('clumped' isotopologues) can be used as geothermometers because their proportions at isotopic equilibrium relative to a random distribution of isotopes amongst all isotopologues are functions of temperature. This has allowed measurements of clumped-isotope abundances to be used to constrain formation temperatures of several natural materials. However, kinetic processes during generation, modification, or transport of natural materials can also affect their clumped-isotope compositions. Herein, we show that methane generated experimentally by closed-system hydrous pyrolysis of shale or nonhydrous pyrolysis of coal yields clumped-isotope compositions consistent with an equilibrium distribution of isotopologues under some experimental conditions (temperature-time conditions corresponding to 'low,' 'mature,' and 'over-mature' stages of catagenesis), but can have non-equilibrium (i.e., kinetically controlled) distributions under other experimental conditions ('high' to 'over-mature' stages), particularly for pyrolysis of coal. Non-equilibrium compositions, when present, lead the measured proportions of clumped species to be lower than expected for equilibrium at the experimental temperature, and in some cases to be lower than a random distribution of isotopes (i.e., negative Δ18 values). We propose that the consistency with equilibrium for methane formed by relatively low temperature pyrolysis reflects local reversibility of isotope exchange reactions involving a reactant or transition state species during demethylation of one or more components of kerogen. Non-equilibrium clumped-isotope compositions occur under conditions where 'secondary' cracking of retained oil in shale or wet gas hydrocarbons (C2-5, especially ethane) in coal is prominent. We suggest these non-equilibrium isotopic compositions are the result of the expression of kinetic isotope effects during the irreversible generation of methane from an alkyl precursor. Other interpretations are also explored. These findings provide new insights into the chemistry of thermogenic methane generation, and may provide an explanation of the elevated apparent temperatures recorded by the methane clumped-isotope thermometer in some natural gases. However, it remains unknown if the laboratory experiments capture the processes that occur at the longer time and lower temperatures of natural gas formation.

Evaluating climate model performance in the tropics with retrievals of water isotopic composition from Aura TES

NASA Astrophysics Data System (ADS)

Field, Robert; Kim, Daehyun; Kelley, Max; LeGrande, Allegra; Worden, John; Schmidt, Gavin

2014-05-01

Observational and theoretical arguments suggest that satellite retrievals of the stable isotope composition of water vapor could be useful for climate model evaluation. The isotopic composition of water vapor is controlled by the same processes that control water vapor amount, but the observed distribution of isotopic composition is distinct from amount itself . This is due to the fractionation that occurs between the abundant H216O isotopes (isotopologues) and the rare and heavy H218O and HDO isotopes during evaporation and condensation. The fractionation physics are much simpler than the underlying moist physics; discrepancies between observed and modeled isotopic fields are more likely due to problems in the latter. Isotopic measurements therefore have the potential for identifying problems that might not be apparent from more conventional measurements. Isotopic tracers have existed in climate models since the 1980s but it is only since the mid 2000s that there have been enough data for meaningful model evaluation in this sense, in the troposphere at least. We have evaluated the NASA GISS ModelE2 general circulation model over the tropics against water isotope (HDO/H2O) retrievals from the Aura Tropospheric Emission Spectrometer (TES), alongside more conventional measurements. A small ensemble of experiments was performed with physics perturbations to the cumulus and planetary boundary layer schemes, done in the context of the normal model development process. We examined the degree to which model-data agreement could be used to constrain a select group of internal processes in the model, namely condensate evaporation, entrainment strength, and moist convective air mass flux. All are difficult to parameterize, but exert strong influence over model performance. We found that the water isotope composition was significantly more sensitive to physics changes than precipitation, temperature or relative humidity through the depth of the tropical troposphere. Among the processes considered, this was most closely, and fairly exclusively, related to mid-tropospheric entrainment strength. This demonstrates that water isotope retrievals have considerable potential alongside more conventional measurements for climate model evaluation and development.

Triple oxygen isotope composition of photosynthetic oxygen

NASA Astrophysics Data System (ADS)

van der Meer, Anne; Kaiser, Jan

2013-04-01

The measurement of biological production rates is essential for our understanding how marine ecosystems are sustained and how much CO2 is taken up through aquatic photosynthesis. Traditional techniques to measure marine production are laborious and subject to systematic errors. A biogeochemical approach based on triple oxygen isotope measurements in dissolved oxygen (O2) has been developed over the last few years, which allows the derivation of gross productivity integrated over the depth of the mixed layer and the time-scale of O2 gas exchange (Luz and Barkan, 2000). This approach exploits the relative 17O/16O and 18O/16O isotope ratio differences of dissolved O2 compared to atmospheric O2 to work out the rate of biological production. Two parameters are key for this calculation: the isotopic composition of dissolved O2 in equilibrium with air and the isotopic composition of photosynthetic oxygen. Recently, a controversy has emerged in the literature over these parameters (Kaiser, 2011) and one of the goals of this research is to provide additional data to resolve this controversy. In order to obtain more information on the isotopic signature of biological oxygen, laboratory experiments have been conducted to determine the isotopic composition of oxygen produced by different phytoplankton cultures.

Magnesium Isotopes as a Tracer of Crustal Materials in Volcanic Arc Magmas in the Northern Cascade Arc

NASA Astrophysics Data System (ADS)

Brewer, Aaron W.; Teng, Fang-Zhen; Mullen, Emily

2018-03-01

Fifteen North Cascade Arc basalts and andesites were analyzed for Mg isotopes to investigate the extent and manner of crustal contributions to this magmatic system. The δ26Mg of these samples vary from within the range of ocean island basalts (the lightest being -0.33 ± 0.07‰) to heavier compositions (as heavy as -0.15 ± 0.06‰). The observed range in chemical and isotopic composition is similar to that of other volcanic arcs that have been assessed to date in the circum-pacific subduction zones and in the Caribbean. The heavy Mg isotope compositions are best explained by assimilation and fractional crystallization within the deep continental crust with a possible minor contribution from the addition of subducting slab-derived fluids to the primitive magma. The bulk mixing of sediment into the primitive magma or mantle source and the partial melting of garnet-rich peridotite are unlikely to have produced the observed range of Mg isotope compositions. The results show that Mg isotopes may be a useful tracer of crustal input into a magma, supplementing traditional methods such as radiogenic isotopic and trace element data, particularly in cases in which a high fraction of crustal material has been added.

Silurian shale origin for light oil, condensate, and gas in Algeria and the Middle East

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zumberge, J.E.; Macko, S.

1996-01-01

Two of the largest gas fields in the world, Hasi R'Mel, Algeria and North Dome, Qatar, also contain substantial condensate and light oil reserves. Gas to source rock geochemical correlation is difficult due to the paucity of molecular parameters in the former although stable isotope composition is invaluable. However, by correlating source rocks with light oils and condensates associated with gas production using traditional geochemical parameters such as biomarkers and isotopes, a better understanding of the origin of the gas is achieved. Much of the crude oil in the Ghadames/Illizi Basins of Algeria has long been thought to have beenmore » generated from Silurian shales. New light oil discoveries in Saudi Arabia have also been shown to originate in basal euxinic Silurian shales. Key sterane and terpane biomarkers as well as the stable carbon isotopic compositions of the C15+ saturate and aromatic hydrocarbon fractions allow for the typing of Silurian-sourced, thermally mature light oils in Algeria and the Middle East. Even though biomarkers are often absent due to advanced thermal maturity, condensates can be correlated to the light oils using (1) carbon isotopes of the residual heavy hydrocarbon fractions, (2) light hydrocarbon distributions (e.g., C7 composition), and (3) compound specific carbon isotopic composition of the light hydrocarbons. The carbon isotopes of the C2-C4 gas components ran then be compared to the associated condensate and light oil isotopic composition.« less

Planetary and meteoritic Mg/Si and δ30 Si variations inherited from solar nebula chemistry

NASA Astrophysics Data System (ADS)

Dauphas, Nicolas; Poitrasson, Franck; Burkhardt, Christoph; Kobayashi, Hiroshi; Kurosawa, Kosuke

2015-10-01

The bulk chemical compositions of planets are uncertain, even for major elements such as Mg and Si. This is due to the fact that the samples available for study all originate from relatively shallow depths. Comparison of the stable isotope compositions of planets and meteorites can help overcome this limitation. Specifically, the non-chondritic Si isotope composition of the Earth's mantle was interpreted to reflect the presence of Si in the core, which can also explain its low density relative to pure Fe-Ni alloy. However, we have found that angrite meteorites display a heavy Si isotope composition similar to the lunar and terrestrial mantles. Because core formation in the angrite parent-body (APB) occurred under oxidizing conditions at relatively low pressure and temperature, significant incorporation of Si in the core is ruled out as an explanation for this heavy Si isotope signature. Instead, we show that equilibrium isotopic fractionation between gaseous SiO and solid forsterite at ∼1370 K in the solar nebula could have produced the observed Si isotope variations. Nebular fractionation of forsterite should be accompanied by correlated variations between the Si isotopic composition and Mg/Si ratio following a slope of ∼1, which is observed in meteorites. Consideration of this nebular process leads to a revised Si concentration in the Earth's core of 3.6 (+ 6.0 / - 3.6) wt% and provides estimates of Mg/Si ratios of bulk planetary bodies.

Stable water isotopic composition of the Antarctic subglacial Lake Vostok: implications for understanding the lake's hydrology.

PubMed

Ekaykin, Alexey A; Lipenkov, Vladimir Y; Kozachek, Anna V; Vladimirova, Diana O

2016-01-01

We estimated the stable isotopic composition of water from the subglacial Lake Vostok using two different sets of samples: (1) water frozen on the drill bit immediately after the first lake unsealing and (2) water frozen in the borehole after the unsealing and re-drilled one year later. The most reliable values of the water isotopic composition are: -59.0 ± 0.3 ‰ for oxygen-18, -455 ± 1 ‰ for deuterium and 17 ± 1 ‰ for d-excess. This result is also confirmed by the modelling of isotopic transformations in the water which froze in the borehole, and by a laboratory experiment simulating this process. A comparison of the newly obtained water isotopic composition with that of the lake ice (-56.2 ‰ for oxygen-18, -442.4 ‰ for deuterium and 7.2 ‰ for d-excess) leads to the conclusion that the lake ice is very likely formed in isotopic equilibrium with water. In turn, this means that ice is formed by a slow freezing without formation of frazil ice crystals and/or water pockets. This conclusion agrees well with the observed physical and chemical properties of the lake's accreted ice. However, our estimate of the water's isotopic composition is only valid for the upper water layer and may not be representative for the deeper layers of the lake, so further investigations are required.

Silurian shale origin for light oil, condensate, and gas in Algeria and the Middle East

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zumberge, J.E.; Macko, S.

Two of the largest gas fields in the world, Hasi R`Mel, Algeria and North Dome, Qatar, also contain substantial condensate and light oil reserves. Gas to source rock geochemical correlation is difficult due to the paucity of molecular parameters in the former although stable isotope composition is invaluable. However, by correlating source rocks with light oils and condensates associated with gas production using traditional geochemical parameters such as biomarkers and isotopes, a better understanding of the origin of the gas is achieved. Much of the crude oil in the Ghadames/Illizi Basins of Algeria has long been thought to have beenmore » generated from Silurian shales. New light oil discoveries in Saudi Arabia have also been shown to originate in basal euxinic Silurian shales. Key sterane and terpane biomarkers as well as the stable carbon isotopic compositions of the C15+ saturate and aromatic hydrocarbon fractions allow for the typing of Silurian-sourced, thermally mature light oils in Algeria and the Middle East. Even though biomarkers are often absent due to advanced thermal maturity, condensates can be correlated to the light oils using (1) carbon isotopes of the residual heavy hydrocarbon fractions, (2) light hydrocarbon distributions (e.g., C7 composition), and (3) compound specific carbon isotopic composition of the light hydrocarbons. The carbon isotopes of the C2-C4 gas components ran then be compared to the associated condensate and light oil isotopic composition.« less

Interactions between surface waters in King George Island, Antarctica - a stable isotope perspective

NASA Astrophysics Data System (ADS)

Perşoiu, Aurel; Bădăluşă, Carmen

2017-04-01

In this paper we present a first study of the isotopic composition of surface waters in the southern peninsulas (Barton, Fildes, Weaver and Potter) of King George Island, Antarctica. We have collected > 200 samples of snow and snowmelt, water (lake, river and spring), ice (glacier ice and permafrost) from the four peninsulas in February 2016 and analyzed them for their oxygen and hydrogen stable isotopic composition. Samples from lake water (50+) indicate a clear west-east depletion trend, suggesting a rain-out process as air masses are moving westward (and are progressively depleted in heavy isotopes) from their origin in the Drake Passage. In both Fildes and Barton Peninsulas, permafrost samples have the heaviest isotopic composition, most probably due to preferential incorporation of heavy isotopes in the ice during freezing (and no fractionation during melting). As permafrost melts, the resulting water mixes with isotopically lighter infiltrated snowmelt, and thus the groundwater has a lower isotopic composition. Further, lake and river (the later fed by lakes) water has the lightest isotopic composition, being derived mostly from the melting of light snow and glacier ice. It seems feasible to separate isotopically water in lakes/rivers (largely fed by melting multi-year glaciers and snow) and water from melting of snow/ground ice This preliminary study suggests that it is possible to separate various water sources in the southern peninsulas of King George Island, and this separation could be used to study permafrost degradation, as well as feeding and migration patterns in the bird fauna, with implications for protection purposes. Acknowledgments. The National Institute of Research and Development for Biological Sciences (Bucharest, Romania) and the Korean polar institute financially supported fieldwork in King George Island. We thank the personal at King Sejong (South Korea), Belingshaussen (Russia) and Carlini (Argentina) stations in King George Island for logistic supports.

PALOMA : an isotope analyzer using static mass spectrometry, coupled with cryogenic and chemical trapping, for the MSL mission to Mars

NASA Astrophysics Data System (ADS)

Chassefiere, E.; Jambon, A.; Berthelier, J.-J.; Goulpeau, G.; Leblanc, F.; Montmessin, F.; Sarda, P.; Agrinier, P.; Fouchet, T.; Waite, H.

The technique of GCMS analysis has to be completed by static mass spectrometry for precise in-situ measurements of the isotopic composition of planetary atmospheres (noble gases, stable isotopes), and volatile outgassed products from solid sample pyrolysis. Static mass spectrometry, coupled with gas separation by cryo-separation and gettering, is commonly used in the laboratory to study volatiles extracted from terrestrial and meteoritic samples. Such an instrument (PALOMA) is presently developed in our laboratories, and it will be coupled with a Pyr-GCMS analyzer (MACE), built by a US consortium of science laboratories and industrials (University of Michigan, Southwest Research Institute, JPL, Ball Aerospace). The MACE/PALOMA experiment will be proposed on the NASA Mars Science Laboratory mission, planned to be launched in 2009. The scientific objectives of PALOMA, coupled with MACE, may be listed as follows : (i) search for isotopic signatures of past life in atmosphere, rock, dust and ice samples, with emphasis on carbon, nitrogen and hydrogen; (ii) accurately measure isotopic composition of atmospheric noble gases, and stable isotopes, in order to better constrain past escape, surface interaction, outgassing history and climate evolution; (iii) precisely measure diurnal/ seasonal variations of isotopic ratios of H2O, CO2, and N2, for improving our understanding of present and past climate, and of the role of water cycle. Main measurement objectives are : (i) C, H, O, N isotopic composition in both organic evolved samples (provided by MACE pyrolysis system) and atmosphere with high accuracy (a few per mil at 1-s level); (ii) noble gas (He, Ne, Ar, Kr, Xe) and stable (C, H, O, N) isotope composition in atmosphere with high accuracy (a few per mil at 1-s level); (iii) molecular and isotopic composition of inorganic evolved samples (salts, hydrates, nitrates, {ldots}), including ices; (iv) diurnal and seasonal monitoring of D/H in water vapor, and water ice.

Spatiotemporal patterns of plant water isotope values from a continental-scale sample network in Europe as a tool to improve hydroclimate proxies

NASA Astrophysics Data System (ADS)

Nelson, D. B.; Kahmen, A.

2016-12-01

The hydrogen and oxygen isotopic composition of water available for biosynthetic processes in vascular plants plays an important role in shaping the isotopic composition of organic compounds that these organisms produce, including leaf waxes and cellulose in leaves and tree rings. Characterizing changes in large scale spatial patterns of precipitation, soil water, stem water, and leaf water isotope values over time is therefore useful for evaluating how plants reflect changes in the isotopic composition of these source waters in different environments. This information can, in turn, provide improved calibration targets for understanding the environmental signals that plants preserve. The pathway of water through this continuum can include several isotopic fractionations, but the extent to which the isotopic composition of each of these water pools varies under normal field conditions and over space and time has not been systematically and concurrently evaluated at large spatial scales. Two season-long sampling campaigns were conducted at nineteen sites throughout Europe over the 2014 and 2015 growing seasons to track changes in the isotopic composition of plant-relevant waters. Samples of precipitation, soil water, stem water, and leaf water were collected over more than 200 field days and include more than 500 samples from each water pool. Measurements were used to validate continent-wide gridded estimates of leaf water isotope values derived from a combination of mechanistic and statistical modeling conducted with temperature, precipitation, and relative humidity data. Data-model comparison shows good agreement for summer leaf waters, and substantiates the incorporation of modeled leaf waters in evaluating how plants respond to hydroclimate changes at large spatial scales. These results also suggest that modeled leaf water isotope values might be used in future studies in similar ecosystems to improve the coverage density of spatial or temporal data.

The stable Cr isotopic compositions of chondrites and silicate planetary reservoirs

NASA Astrophysics Data System (ADS)

Schoenberg, Ronny; Merdian, Alexandra; Holmden, Chris; Kleinhanns, Ilka C.; Haßler, Kathrin; Wille, Martin; Reitter, Elmar

2016-06-01

The depletion of chromium in Earth's mantle (∼2700 ppm) in comparison to chondrites (∼4400 ppm) indicates significant incorporation of chromium into the core during our planet's metal-silicate differentiation, assuming that there was no significant escape of the moderately volatile element chromium during the accretionary phase of Earth. Stable Cr isotope compositions - expressed as the ‰-difference in 53Cr/52Cr from the terrestrial reference material SRM979 (δ53/52CrSRM979 values) - of planetary silicate reservoirs might thus yield information about the conditions of planetary metal segregation processes when compared to chondrites. The stable Cr isotopic compositions of 7 carbonaceous chondrites, 11 ordinary chondrites, 5 HED achondrites and 2 martian meteorites determined by a double spike MC-ICP-MS method are within uncertainties indistinguishable from each other and from the previously determined δ53/52CrSRM979 value of -0.124 ± 0.101‰ for the igneous silicate Earth. Extensive quality tests support the accuracy of the stable Cr isotope determinations of various meteorites and terrestrial silicates reported here. The uniformity in stable Cr isotope compositions of samples from planetary silicate mantles and undifferentiated meteorites indicates that metal-silicate differentiation of Earth, Mars and the HED parent body did not cause measurable stable Cr isotope fractionation between these two reservoirs. Our results also imply that the accretionary disc, at least in the inner solar system, was homogeneous in its stable Cr isotopic composition and that potential volatility loss of chromium during accretion of the terrestrial planets was not accompanied by measurable stable isotopic fractionation. Small but reproducible variations in δ53/52CrSRM979 values of terrestrial magmatic rocks point to natural stable Cr isotope variations within Earth's silicate reservoirs. Further and more detailed studies are required to investigate whether silicate differentiation processes, such as partial mantle melting and crystal fractionation, can cause stable Cr isotopic fractionation on Earth and other planetary bodies.

Absolute Isotopic Abundance Ratios and the Accuracy of Δ47 Measurements

NASA Astrophysics Data System (ADS)

Daeron, M.; Blamart, D.; Peral, M.; Affek, H. P.

2016-12-01

Conversion from raw IRMS data to clumped isotope anomalies in CO2 (Δ47) relies on four external parameters: the (13C/12C) ratio of VPDB, the (17O/16O) and (18O/16O) ratios of VSMOW (or VPDB-CO2), and the slope of the triple oxygen isotope line (λ). Here we investigate the influence that these isotopic parameters exert on measured Δ47 values, using real-world data corresponding to 7 months of measurements; simulations based on randomly generated data; precise comparisons between water-equilibrated CO2 samples and between carbonate standards believed to share quasi-identical Δ47 values; reprocessing of two carbonate calibration data sets with different slopes of Δ47 versus T. Using different sets of isotopic parameters generally produces systematic offsets as large as 0.04 ‰ in final Δ47 values. What's more, even using a single set of isotopic parameters can produce intra- and inter-laboratory discrepancies in final Δ47 values, if some of these parameters are inaccurate. Depending on the isotopic compositions of the standards used for conversion to "absolute" values, these errors should correlate strongly with either δ13C or δ18O, or more weakly with both. Based on measurements of samples expected to display identical Δ47 values, such as 25°C water-equilibrated CO2 with different carbon and oxygen isotope compositions, or high-temperature standards ETH-1 and ETH-2, we conclude that the isotopic parameters used so far in most clumped isotope studies produces large, systematic errors controlled by the relative bulk isotopic compositions of samples and standards, which should be one of the key factors responsible for current inter-laboratory discrepancies. By contrast, the isotopic parameters of Brand et al. [2010] appear to yield accurate Δ47 values regardless of bulk isotopic composition. References:Brand, Assonov and Coplen [2010] http://dx.doi.org/10.1351/PAC-REP-09-01-05

Mass dependent fractionation of stable chromium isotopes in mare basalts: Implications for the formation and the differentiation of the Moon

NASA Astrophysics Data System (ADS)

Bonnand, Pierre; Parkinson, Ian J.; Anand, Mahesh

2016-02-01

We present the first stable chromium isotopic data from mare basalts in order to investigate the similarity between the Moon and the Earth's mantle. A double spike technique coupled with MC-ICP-MS measurements was used to analyse 19 mare basalts, comprising high-Ti, low-Ti and KREEP-rich varieties. Chromium isotope ratios (δ53Cr) for mare basalts are positively correlated with indices of magmatic differentiation such as Mg# and Cr concentration which suggests that Cr isotopes were fractionated during magmatic differentiation. Modelling of the results provides evidence that spinel and pyroxene are the main phases controlling the Cr isotopic composition during fractional crystallisation. The most evolved samples have the lightest isotopic compositions, complemented by cumulates that are isotopically heavy. Two hypotheses are proposed to explain this fractionation: (i) equilibrium fractionation where heavy isotopes are preferentially incorporated into the spinel lattice and (ii) a difference in isotopic composition between Cr2+ and Cr3+ in the melt. However, both processes require magmatic temperatures below 1200 °C for appreciable Cr3+ to be present at the low oxygen fugacities found in the Moon (IW -1 to -2 log units). There is no isotopic difference between the most primitive high-Ti, low-Ti and KREEP basalts, which suggest that the sources of these basalts were homogeneous in terms of stable Cr isotopes. The least differentiated sample in our sample set is the low-Ti basalt 12016, characterised by a Cr isotopic composition of -0.222 ± 0.025‰, which is within error of the current BSE value (-0.124 ± 0.101‰). The similarity between the mantles of the Moon and Earth is consistent with a terrestrial origin for a major fraction of the lunar Cr. This similarity also suggests that Cr isotopes were not fractionated by core formation on the Moon.

Using semi-continuous, in-situ measurements of nitrous oxide isotopic composition at a suburban site to track emission processes

NASA Astrophysics Data System (ADS)

Harris, Eliza; Henne, Stephan; Christoph, Hüglin; Christoph, Zellweger; Béla, Tuzson; Erkan, Ibraim; Lukas, Emmenegger; Joachim, Mohn

2017-04-01

Nitrous oxide (N2O) is a potent greenhouse gas and the strongest ozone-destroying substance emitted this century. The atmospheric N2O mole fraction has been increasing at a rate of 0.2-0.3% per year over the past decades due to anthropogenic emissions; in addition, recent results suggest that the rate of increase is rising - therefore effective mitigation of N2O emissions is a critical point for environmental policy. However, N2O sources are poorly defined and disperse, complicating the development of targeted mitigation strategies. Online isotopic measurements using preconcentration and laser spectroscopy [1,2,3] have great potential to unravel spatial and temporal variations in sources, sinks and chemistry of trace gases such as N2O. Semi-continuous, real-time measurements of N2O isotopic composition (δ18O, site preference [SP = 14N15N16O - 15N14N16O] and δ15Nbulk) were performed at the suburban site of Dübendorf, Switzerland, for 19 months between July 2014 and February 2016. The data precision reached 0.1‰ in the final months, thus the results could clearly identify nocturnal build-up of N2O, with a corresponding decrease in δ18O, SP and δ15Nbulk due to isotopically depleted anthropogenic sources. Daily mean source isotopic composition was calculated by considering the measured and the background mole fraction and isotopic composition. Delta values of the mean emission source were highest in winter, with a seasonal cycle of 12, 8 and 5‰ for δ18O, SP and δ15Nbulk respectively. The chemical and meteorological parameters controlling source isotopic composition were considered using data from the Swiss National Air Pollution Monitoring Network (NABEL) as well as a transport regime cluster analysis. A clear spatial distribution for source isotopic composition was observed for δ18O, as well as a significant relationship with the level of urban pollution, indicating δ18O may be a strong indicator of combustion/industrial vs. agricultural N2O. In contrast, δ15Nbulk and particularly SP appear to vary too strongly in response to other factors affecting emission processes to provide a useful distinction between source categories on a regional scale - these isotopocules may however be useful to distinguish emission pathways on a local scale. For comparison, FLEXPART-COSMO transport simulations [4] were combined with emissions from the EDGAR inventory and estimates of source isotopic composition from literature, to simulate N2O isotopic composition at the sampling site. The model was able to capture variability in N2O mole fraction adequately (R2 = 0.34; p <<0.01). However, the measured variability in source isotopic composition was 1-2 orders of magnitude larger than simulated, illustrating that our knowledge of isotopic source signatures - in particular technical N2O sources - is still too limited to successfully model variations in ambient N2O isotopic composition. [1] Mohn et al. (2012) Atmospheric Measurement Techniques, doi:10.5194/amt-5-1601-2012 [2] Harris et al. (2014) Analytical Chemistry, doi: 10.1021/ac403606u. [3] Röckmann et al. (2016) Atmospheric Chemistry and Physics, doi:10.5194/acp-16-10469-2016. [4] Henne et al. (2016) Atmospheric Chemistry and Physics, doi:10.5194/acp-16-3683-2016.

Evidence for a nonmagmatic component in potassic hydrothermal fluids of porphyry cu-Au-Mo systems, Yukon, Canada

NASA Astrophysics Data System (ADS)

Selby, David; Nesbitt, Bruce E.; Creaser, Robert A.; Reynolds, Peter H.; Muehlenbachs, Karlis

2001-02-01

Isotopic (H, Sr, Pb, Ar) and fluid inclusion data for hydrothermal fluids associated with potassic alteration from three Late Cretaceous porphyry Cu occurrences, west central Yukon, suggest a nonmagmatic fluid component was present in these hydrothermal fluids. Potassic stage quartz veins contain a dominant assemblage of saline and vapor-rich fluid inclusions that have δD values between -120 and -180‰. Phyllic stage quartz veins are dominated by vapor-rich fluid inclusions and have δD values that overlap with but are, on average, heavier (-117 to -132‰) than those in potassic stage quartz veins. These δD values are significantly lower than those from plutonic quartz phenocrysts (-91 to -113‰), and from values typically reported for primary fluids from porphyry-style mineralization (-40 to -100‰). The initial Sr ( 87Sr/ 86Sr i) isotopic values for the plutons are 0.7055 (Casino), 0.7048 (Mt. Nansen), and 0.7055 (Cash). The 87Sr/ 86Sr i compositions of hydrothermal K-feldspar ranges from magmatic Sr i values to more radiogenic compositions (Casino: 0.70551-0.70834, n = 8; Mt. Nansen: 0.7063-0.7070, n = 4; Cash: 0.7058, n = 1). The fluid inclusion waters from potassic quartz veins have 87Sr/ 86Sr i values that are similar to those of co-existing hydrothermal K-feldspar. The Pb isotopic compositions of hydrothermal K-feldspar show a weak positive correlation with Sr i for identical samples. Fluid inclusion waters of phyllic quartz veins also have Sr i compositions more radiogenic than the plutons. The Pb isotopic composition of pyrite and bornite from phyllic alteration veins are similar to, or more radiogenic than, hydrothermal K-feldspar Pb isotopic values. Hydrothermal K-feldspar samples yield 40Ar/ 39Ar ages (Casino = 71.9 ± 0.7 to 73.4 ± 0.8 Ma; Mt. Nansen = 68.2 ± 0.7 and 69.5 ± 0.6 Ma; Cash = 68.3 ± 0.8 Ma) similar to the U-Pb zircon, K-Ar biotite and Re-Os molybdenite ages of the Late Cretaceous plutons, with the age spectra indicating no excess 40Ar or disturbance. The 40Ar/ 36Ar values (285-292) of the K-feldspar samples are similar to the atmospheric compositions (295 ± 5) during Late Cretaceous time. The H, Sr, Pb, and Ar isotopic compositions of hydrothermal K-feldspar and quartz vein fluid inclusion waters that characterize the potassic hydrothermal fluids show evidence for an exotic component in addition to magmatic water (fluid). This component has a low δD, radiogenic Sr and Pb, and an atmospheric Ar composition. The inheritance of pre-existing isotope compositions from the host rocks, postpotassic alteration isotope exchange, or the replenishment of the magma chamber with magma of different isotopic composition cannot explain the isotope data. We suggest that to generate the observed H, Sr, Pb, and Ar isotope compositions, crustal fluids must be a component (15-94%) of potassic hydrothermal fluids in porphyry mineralization in the deposits studied.

Osmium uptake, distribution, and 187Os/188Os and 187Re/188Os compositions in Phaeophyceae macroalgae, Fucus vesiculosus: Implications for determining the 187Os/188Os composition of seawater

NASA Astrophysics Data System (ADS)

Racionero-Gómez, B.; Sproson, A. D.; Selby, D.; Gannoun, A.; Gröcke, D. R.; Greenwell, H. C.; Burton, K. W.

2017-02-01

The osmium isotopic composition (187Os/188Os) of seawater reflects the balance of input from mantle-, continental- and anthropogenic-derived sources. This study utilizes the Phaeophyceae, Fucus vesiculosus, to analyse its Os abundance and uptake, as well as to assess if macroalgae records the Os isotope composition of the seawater in which it lives. The data demonstrates that Os is not located in one specific biological structure within macroalgae, but is found throughout the organism. Osmium uptake was measured by culturing F. vesiculosus non-fertile tips with different concentrations of Os with a known 187Os/188Os composition (∼0.16), which is significantly different from the background isotopic composition of local seawater (∼0.94). The Os abundance of cultured non-fertile tips show a positive correlation to the concentration of the Os doped seawater. Moreover, the 187Os/188Os composition of the seaweed equalled that of the culture medium, strongly confirming the possible use of macroalgae as a biological proxy for the Os isotopic composition of the seawater.

Optimizing isotope substitution in graphene for thermal conductivity minimization by genetic algorithm driven molecular simulations

NASA Astrophysics Data System (ADS)

Davies, Michael; Ganapathysubramanian, Baskar; Balasubramanian, Ganesh

2017-03-01

We present results from a computational framework integrating genetic algorithm and molecular dynamics simulations to systematically design isotope engineered graphene structures for reduced thermal conductivity. In addition to the effect of mass disorder, our results reveal the importance of atomic distribution on thermal conductivity for the same isotopic concentration. Distinct groups of isotope-substituted graphene sheets are identified based on the atomic composition and distribution. Our results show that in structures with equiatomic compositions, the enhanced scattering by lattice vibrations results in lower thermal conductivities due to the absence of isotopic clusters.

Revising Estimates of the Methane Production Pathway in Peatland Porewater Using Intramolecular Isotopic Analyses of Acetate

NASA Astrophysics Data System (ADS)

Thomas, B.; Arthur, M. A.; Freeman, K. H.

2007-12-01

Stable isotopic measurements of methane and carbon dioxide are routinely applied to environmental samples to assess the relative importance of methane production by either aceticlastic or hydrogenotrophic methanogenesis. Such estimates rely upon assumptions about isotopic fractionation during methane production and oxidation. Rigorous isotope-based pathway estimates require knowledge of the carbon isotopic composition of both carbon dioxide and acetate. In practice, technical barriers have limited measurements of the isotopic composition of whole acetate in natural samples. Yet, the estimate of whole acetate isotopic values, even when available, may not represent accurately the composition of the methyl carbon, which is, in fact, the precursor to methane. It is exceedingly rare to find carbon isotopic measurements of acetate-methyl in the literature, and, to our knowledge, the d13C of the acetate-methyl precursor to methane has never before been reported from peatland porewater samples. Extremely 13C-depleted methane, -70 permil VPDB, and 13C-enriched carbon dioxide from acidic northern peat bogs are typically interpreted as signatures of hydrogenotrophic methanogenesis. The hypothesized dominance of methane production from hydrogen in acidic bogs contrasts with the vast majority of freshwater wetlands in which aceticlastic methanogenesis dominates. Using a new technique for the online analysis of the intramolecular carbon isotopic composition of acetate in natural samples, we find the acetate-methyl in peat porewaters can be significantly depleted relative to bulk organic matter. In porewater profiles from both winter and summer, acetate is as much as 15 permil depleted relative to bulk carbon. We hypothesize that acetate- methyl isotopic depletion results from conditions that favor autotrophic acetogenesis and subsequent acetate consumption by aceticlastic methanogens. Porewater depth profiles during winter and summer illustrate depth- dependent increases in the fraction of methane derived from carbon dioxide, with deeper peat dominated by hydrogenotrophic methanogenesis, but shallow peat dominated by aceticlastic methanogens. Significant aceticlastic methane production from autotrophically produced acetate challenges the ability of hydrogen isotopic measurements of methane to represent the pathway of methanogenesis. Supplementing our field observations, intramolecular acetate measurements of incubation experiments confirm that an aceticlastic methanogen can facilitate significant acetate-carboxyl exchange with DIC. This novel technique confirms two caveats associated with whole acetate carbon isotopic data: 1, the carboxyl carbon isotopic composition may not accurately reflect the composition of the parent molecule, and 2, the acetate methyl may be derived from inorganic carbon or the fractionation effect of fermentation in acidic porewaters may be significant.

Methane clumped isotopes: Progress and potential for a new isotopic tracer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Douglas, Peter M. J.; Stolper, Daniel A.; Eiler, John M.

The isotopic composition of methane is of longstanding geochemical interest, with important implications for understanding hydrocarbon systems, atmospheric greenhouse gas concentrations, the global carbon cycle, and life in extreme environments. Recent analytical developments focusing on multiply substituted isotopologues (‘clumped isotopes’) are opening a potentially valuable new window into methane geochemistry. When methane forms in internal isotopic equilibrium, clumped isotopes can provide a direct record of formation temperature, making this property particularly valuable for identifying different methane origins. However, it has also become clear that in certain settings methane clumped isotope measurements record kinetic rather than equilibrium isotope effects. Here wemore » present a substantially expanded dataset of methane clumped isotope analyses, and provide a synthesis of the current interpretive framework for this parameter. We review different processes affecting methane clumped isotope compositions, describe the relationships between conventional isotope and clumped isotope data, and summarize the types of information that this measurement can provide in different Earth and planetary environments.« less

Oxygen-isotope, X-ray-diffraction and scanning-electron-microscope examinations of authigenic-layer-silicate minerals from Mississippian and Pennsylvanian sandstones in the Michigan Basin

USGS Publications Warehouse

Zacharias, K.F.; Sibley, D.F.; Westjohn, D.B.; Weaver, T. L.

1993-01-01

Oxygen-isotope compositions of authigenic-layer silicates (<2-micrometer fraction) extracted from Mississippian and Pennsylvanian sandstones in the Lower Peninsula of Michigan were determined. Petrographic and scanning-electron-microscope examinations, and X-ray diffractograms show that chlorite and kaolinite are the most common authigenic-layer silicates in Mississippian sandstones. The range of oxygen-isotope compositions of chlorite and kaolinite are +10.3 to +11.9 and +12.9 to +19.3 pars per thousand (per mil) (relative to Standard Mean Ocean Water), respectively. Kaolinite is the only authigenic-isotopic compositions of kaolinite range from +16.8 to +19.0 per mil.

Development of particle induced gamma-ray emission methods for nondestructive determination of isotopic composition of boron and its total concentration in natural and enriched samples.

PubMed

Chhillar, Sumit; Acharya, Raghunath; Sodaye, Suparna; Pujari, Pradeep K

2014-11-18

We report simple particle induced gamma-ray emission (PIGE) methods using a 4 MeV proton beam for simultaneous and nondestructive determination of the isotopic composition of boron ((10)B/(11)B atom ratio) and total boron concentrations in various solid samples with natural isotopic composition and enriched with (10)B. It involves measurement of prompt gamma-rays at 429, 718, and 2125 keV from (10)B(p,αγ)(7)Be, (10)B(p, p'γ)(10)B, and (11)B(p, p'γ)(11)B reactions, respectively. The isotopic composition of boron in natural and enriched samples was determined by comparing peak area ratios corresponding to (10)B and (11)B of samples to natural boric acid standard. An in situ current normalized PIGE method, using F or Al, was standardized for total B concentration determination. The methods were validated by analyzing stoichiometric boron compounds and applied to samples such as boron carbide, boric acid, carborane, and borosilicate glass. Isotopic compositions of boron in the range of 0.247-2.0 corresponding to (10)B in the range of 19.8-67.0 atom % and total B concentrations in the range of 5-78 wt % were determined. It has been demonstrated that PIGE offers a simple and alternate method for total boron as well as isotopic composition determination in boron based solid samples, including neutron absorbers that are important in nuclear technology.

Stalagmite geochemistry and the timing of the last interglacial-glacial transition in Central Europe (NE Hungary)

NASA Astrophysics Data System (ADS)

Siklosy, Z.; Demeny, A.; Pilet, S.; Leel-Ossy, Sz.; Lin, K.; Shen, C.-C.

2009-04-01

Speleothems can provide accurate chronologies for reconstructions of climate change by combination of U/Th dating and climate-related geochemical compositions. Geochemical studies of speleothems from Central Europe are mostly based on stable C and O isotope analyses, thus, complex geochemical studies combining isotope and trace element measurements are needed for more reliable climate models for this transitional area between oceanic and continental regions. We present stable H-C-O isotope and trace element records obtained on speleothems covering the Last Interglacial (MIS 5e) and the transition to MIS 5d. A stalagmite from Baradla Cave grew from 127.5 to 110 ka. Accelerated growth rates have been detected by U/Th age data in the 127 to 126 ka and 119 to 117 ka parts. Trace element compositions and 230Th/232Th ratios suggest changes in the hydrological regime, whereby early calcite precipitates formed in fissures during the dry and cold glacial period were dissolved by the starting flux of infiltrating meteoric water (producing elevated dissolved ion concentration but low detrital Th component), then the increasing amount of dripwater during the interglacial period resulted in trace element dilution. Temperature and precipitation amount variations are also reflected by the stable isotope compositions. Oxygen isotope composition shows a continuous increase from 127.5 ka until about 118 ka most probably related to temperature rise, whereas C isotope values are shifted in negative direction suggesting increasing humidity in accordance with trace element contents. The presumably warmest period at ca. 118 ka is associated with rather arid climate as indicated by peak d18O values coinciding with the highest dD values of fluid inclusion water. This is followed by a pronounced negative shift in both O and H isotope values, similarly to recent Alpine studies (Meyer et al., 2008), most probably related to cooling. Hydrogen isotope compositions of fluid inclusion water evaluated together with calculated oxygen isotope compositions of water indicate warming and increasing significance of summer precipitation at the latest period of the last interglacial, then increasing importance of winter precipitation and/or changes in oceanic source composition during the cooling phase. The good agreement with other (Alpine and marine) records indicate a synchronous climate change. However, after a negative shift in the wet/warm phase (increasing soil activity), C isotope values start to increase already at about 119 ky BP, warning to the use of the two isotope systems as event correlation tools. In conclusion, our combined isotope and trace element study indicate a complex pattern of temperature and humidity variations during and right after the Last Interglacial. Acknowledgements — This study was financially supported by the Hungarian Scientific Research Fund (OTKA T 049713). Measurements of U-Th isotopic compositions and and 230Th dates were supported by the National Science Council grants (94-2116-M002-012, 97-2752-M002-004-PAE & -005-PAE to C.C.S.). [Meyer, M.; Spötl, C.; Mangini, A. (2008): The demise of the Last Interglacial recorded in isotopically dated speleothems from the Alps. Quaternary Science Reviews, 27, 476-496.

Carbon isotope geochemistry and geobiology

NASA Technical Reports Server (NTRS)

Desmarais, D.

1985-01-01

Carbon isotope fractionation values were used to understand the history of the biosphere. For example, plankton analyses confirmed that marine extinctions at the end of the Cretaceous period were indeed severe (see Hsu's article in Sundquist and Broeker, 1984). Variations in the isotopic compositions of carbonates and evaporitic sulfates during the Paleozoic reflect the relative abundances of euxinic (anoxic) marine environments and organic deposits from terrestrial flora. The carbon isotopic composition of Precambrian sediments suggest that the enzyme ribulose bisphosphate carboxylase has existed for perhaps 3.5 billion years.

Calcium and Titanium Isotope Fractionation in CAIS: Tracers of Condensation and Inheritance in the Early Solar Protoplanetary Disk

NASA Technical Reports Server (NTRS)

Simon, J. I.; Jordan, M. K.; Tappa, M. J.; Kohl, I. E.; Young, E. D.

2016-01-01

The chemical and isotopic compositions of calcium-aluminum-rich inclusions (CAIs) can be used to understand the conditions present in the protoplantary disk where they formed. The isotopic compositions of these early-formed nebular materials are largely controlled by chemical volatility. The isotopic effects of evaporation/sublimation, which are well explained by both theory and experimental work, lead to enrichments of the heavy isotopes that are often exhibited by the moderately refractory elements Mg and Si. Less well understood are the isotopic effects of condensation, which limits our ability to determine whether a CAI is a primary condensate and/or retains any evidence of its primordial formation history.

MCNP5 CALCULATIONS REPLICATING ARH-600 NITRATE DATA

DOE Office of Scientific and Technical Information (OSTI.GOV)

FINFROCK SH

This report serves to extend the previous document: 'MCNP Calculations Replicating ARH-600 Data' by replicating the nitrate curves found in ARH-600. This report includes the MCNP models used, the calculated critical dimension for each analyzed parameter set, and the resulting data libraries for use with the CritView code. As with the ARH-600 data, this report is not meant to replace the analysis of the fissile systems by qualified criticality personnel. The M CNP data is presented without accounting for the statistical uncertainty (although this is typically less than 0.001) or bias and, as such, the application of a reasonable safetymore » margin is required. The data that follows pertains to the uranyl nitrate and plutonium nitrate spheres, infinite cylinders, and infinite slabs of varying isotopic composition, reflector thickness, and molarity. Each of the cases was modeled in MCNP (version 5.1.40), using the ENDF/B-VI cross section set. Given a molarity, isotopic composition, and reflector thickness, the fissile concentration and diameter (or thicknesses in the case of the slab geometries) were varied. The diameter for which k-effective equals 1.00 for a given concentration could then be calculated and graphed. These graphs are included in this report. The pages that follow describe the regions modeled, formulas for calculating the various parameters, a list of cross-sections used in the calculations, a description of the automation routine and data, and finally the data output. The data of most interest are the critical dimensions of the various systems analyzed. This is presented graphically, and in table format, in Appendix B. Appendix C provides a text listing of the same data in a format that is compatible with the CritView code. Appendices D and E provide listing of example Template files and MCNP input files (these are discussed further in Section 4). Appendix F is a complete listing of all of the output data (i.e., all of the analyzed dimensions and the resulting k{sub eff} values).« less

SRNL Development of Recovery Processes for Mark-18A Heavy Actinide Targets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Allender, Jeffrey S.; Bridges, Nicholas J.; Loftin, Bradley M.

2015-07-14

Savannah River National Laboratory (SRNL) and Oak Ridge National Laboratory (ORNL) are developing plans for the recovery of rare and unique isotopes contained within heavy-actinide target assemblies, specifically the Mark-18A. Mark-18A assemblies were irradiated in Savannah River Site (SRS) reactors in the 1970s under extremely high neutron-flux conditions and produced, virtually, the world's supply of plutonium-244, an isotope of key importance to high-precision actinide measurement and other scientific and nonproliferation uses; and curium highly enriched in heavy isotopes (e.g., curium-246 and curium-248). In 2015 and 2016, SRNL is pursuing tasks that would reduce program risk and budget requirements, including furthermore » characterization of unprocessed targets; engineering studies for the use of the SRNL Shielded Cells Facility (SCF) for recovery; and development of onsite and offsite shipping methods including a replacement for the heavy (70 ton) cask previously used for onsite transfer of irradiated items at SRS. A status update is provided for the characterization, including modeling using the Monte Carlo N-Particle Transport Code (MCNP); direct non-destructive assay measurements; and cask design.« less

Spatial, seasonal, and source variability in the stable oxygen and hydrogen isotopic composition of tap waters throughout the USA

USGS Publications Warehouse

Landwehr, Jurate M.; Coplen, Tyler B.; Stewart, David W.

2013-01-01

To assess spatial, seasonal, and source variability in stable isotopic composition of human drinking waters throughout the entire USA, we have constructed a database of δ18O and δ2H of US tap waters. An additional purpose was to create a publicly available dataset useful for evaluating the forensic applicability of these isotopes for human tissue source geolocation. Samples were obtained at 349 sites, from diverse population centres, grouped by surface hydrologic units for regional comparisons. Samples were taken concurrently during two contrasting seasons, summer and winter. Source supply (surface, groundwater, mixed, and cistern) and system (public and private) types were noted. The isotopic composition of tap waters exhibits large spatial and regional variation within each season as well as significant at-site differences between seasons at many locations, consistent with patterns found in environmental (river and precipitation) waters deriving from hydrologic processes influenced by geographic factors. However, anthropogenic factors, such as the population of a tap’s surrounding community and local availability from diverse sources, also influence the isotopic composition of tap waters. Even within a locale as small as a single metropolitan area, tap waters with greatly differing isotopic compositions can be found, so that tap water within a region may not exhibit the spatial or temporal coherence predicted for environmental water. Such heterogeneities can be confounding factors when attempting forensic inference of source water location, and they underscore the necessity of measurements, not just predictions, with which to characterize the isotopic composition of regional tap waters. Published 2013. This article is a U.S. Government work and is in the public domain in the USA.

On the origin and composition of Theia: Constraints from new models of the Giant Impact

NASA Astrophysics Data System (ADS)

Meier, M. M. M.; Reufer, A.; Wieler, R.

2014-11-01

Knowing the isotopic composition of Theia, the proto-planet which collided with the Earth in the Giant Impact that formed the Moon, could provide interesting insights on the state of homogenization of the inner Solar System at the late stages of terrestrial planet formation. We use the known isotopic and modeled chemical compositions of the bulk silicate mantles of Earth and Moon and combine them with different Giant Impact models, to calculate the possible ranges of isotopic composition of Theia in O, Si, Ti, Cr, Zr and W in each model. We compare these ranges to the isotopic composition of carbonaceous chondrites, Mars, and other Solar System materials. In the absence of post-impact isotopic re-equilibration, the recently proposed high angular momentum models of the Giant Impact ("impact-fission", Cúk, M., Stewart, S.T. [2012]. Science 338, 1047; and "merger", Canup, R.M. [2012]. Science 338, 1052) allow - by a narrow margin - for a Theia similar to CI-chondrites, and Mars. The "hit-and-run" model (Reufer, A., Meier, M.M.M., Benz, W., Wieler, R. [2012]. Icarus 221, 296-299) allows for a Theia similar to enstatite-chondrites and other Earth-like materials. If the Earth and Moon inherited their different mantle FeO contents from the bulk mantles of the proto-Earth and Theia, the high angular momentum models cannot explain the observed difference. However, both the hit-and-run as well as the classical or "canonical" Giant Impact model naturally explain this difference as the consequence of a simple mixture of two mantles with different FeO. Therefore, the simplest way to reconcile the isotopic similarity, and FeO dissimilarity, of Earth and Moon is a Theia with an Earth-like isotopic composition and a higher (∼20%) mantle FeO content.

Multiple enrichment of the Carpathian-Pannonian mantle: Pb-Sr-Nd isotope and trace element constraints

NASA Astrophysics Data System (ADS)

Rosenbaum, Jeffrey M.; Wilson, Marjorie; Downes, Hilary

1997-07-01

Pb isotope compositions of acid-leached clinopyroxene and amphibole mineral separates from spinel peridotite mantle xenoliths entrained in Tertiary-Quaternary alkali basalts from the Carpathian-Pannonian Region of eastern Europe provide important constraints on the processes of metasomatic enrichment of the mantle lithosphere in an extensional tectonic setting associated with recent subduction. Principal component analysis of Pb-Sr-Nd isotope and rare earth element compositions of the pyroxenes is used to identify the geochemical characteristics of the original lithospheric mantle protolith and a spectrum of infiltrating metasomatic agents including subduction-related aqueous fluids and silicate melts derived from a subduction-modified mantle wedge which contains a St. Helena-type (HIMU) plume component. The mantle protolith is highly depleted relative to mid-ocean ridge basalt-source mantle with Pb-Nd-Sr isotope compositions consistent with an ancient depletion event. Silicate melt infiltration into the protolith accounts for the primary variance in the Pb-Sr-Nd isotope compositions of the xenoliths and has locally generated metasomatic amphibole. Infiltration of aqueous fluids has introduced radiogenic Pb and Sr without significantly perturbing the rare earth element signature of the protolith. The Pb isotope compositions of the fluid-modified xenoliths suggest that they reacted with aqueous fluids released from a subduction zone which had equilibrated with sediment derived from an ancient basement terrain. We propose a model for mantle lithosphere evolution consistent with available textural and geochemical data for the xenolith population. The Pb-Sr-Nd isotope compositions of both alkaline mafic magmas and rare, subduction-related, calc-alkaline basaltic andesites from the region provide important constraints for the nature of the asthenospheric mantle wedge and confirm the presence of a HIMU plume component. These silicate melts contribute to the metasomatism of the mantle lithosphere rather than being derived therefrom.

Stable Isotopes as Indicators of Groundwater Recharge Mechanisms in Arid and Semi-arid Australia

NASA Astrophysics Data System (ADS)

Harrington, G. A.; Herczeg, A. L.

2001-05-01

The isotopic compositions of soil water and groundwaters in arid and semi-arid zones are always different from the mean composition of rainfall. Although evaporative processes always remove the lighter isotopes (1H and 16O) to the vapour phase, arid zone groundwaters are invariably depleted in the heavy isotopes (2H and 18O) relative to mean present day rainfall. We compare two sites, one in semi-arid South Australia and the other in arid Central Australia that have a similar mean annual rainfall (250 to 300 mm/a), very high potential evapotranspiration (2500 and 3500 mm/a respectively) but very different rainfall patterns (winter dominated versus summer monsoonal). We aim to evaluate whether inferences from groundwater \\delta2H and \\delta18O reveal information about palaeorecharge, or recharge mechanisms or a combination of both. Recharge to the unconfined limestone aquifer in the Mallee area of South Australia occurs annually via widespread (diffuse) infiltration of winter dominant rainfall. This process is reflected in soil and groundwater isotopic compositions that plot relatively close to both the Local Meteoric Water Line and the volume-weighted mean composition of winter rainfall, and have a deuterium excess (\\delta2H-8.\\delta18O) of between +2 and +8 for the freshest samples. Groundwater recharge to the arid Ti-Tree Basin occurs predominantly by inputs of partially-evaporated surface water from ephemeral rivers and flood-plains following rare, high-intensity storms that are derived from monsoonal activity to the north of Australia. These extreme events result in groundwater and soil water stable isotope compositions being significantly depleted in the heavy isotopes relative to the mean composition of rainfall and a deuterium excess of between minus 8 and +3 in the freshest groundwaters.

Large-scale drivers of Caucasus climate variability in meteorological records and Mt El'brus ice cores

NASA Astrophysics Data System (ADS)

Kozachek, Anna; Mikhalenko, Vladimir; Masson-Delmotte, Valérie; Ekaykin, Alexey; Ginot, Patrick; Kutuzov, Stanislav; Legrand, Michel; Lipenkov, Vladimir; Preunkert, Susanne

2017-05-01

A 181.8 m ice core was recovered from a borehole drilled into bedrock on the western plateau of Mt El'brus (43°20'53.9'' N, 42°25'36.0'' E; 5115 m a.s.l.) in the Caucasus, Russia, in 2009 (Mikhalenko et al., 2015). Here, we report on the results of the water stable isotope composition from this ice core with additional data from the shallow cores. The distinct seasonal cycle of the isotopic composition allows dating by annual layer counting. Dating has been performed for the upper 126 m of the deep core combined with 20 m from the shallow cores. The whole record covers 100 years, from 2013 back to 1914. Due to the high accumulation rate (1380 mm w.e. year-1) and limited melting, we obtained isotopic composition and accumulation rate records with seasonal resolution. These values were compared with available meteorological data from 13 weather stations in the region and also with atmosphere circulation indices, back-trajectory calculations, and Global Network of Isotopes in Precipitation (GNIP) data in order to decipher the drivers of accumulation and ice core isotopic composition in the Caucasus region. In the warm season (May-October) the isotopic composition depends on local temperatures, but the correlation is not persistent over time, while in the cold season (November-April), atmospheric circulation is the predominant driver of the ice core's isotopic composition. The snow accumulation rate correlates well with the precipitation rate in the region all year round, which made it possible to reconstruct and expand the precipitation record at the Caucasus highlands from 1914 until 1966, when reliable meteorological observations of precipitation at high elevation began.

[Effect of microorganisms and seasonal factors on the isotope composition of organic carbon from Black Sea suspensions].

PubMed

Ivanov, M V; Lein, A Iu; Miller, Iu M; Iusunov, S K; Pimenov, N V; Wehrli, B; Rusanov, I I; Zehnder, A

2000-01-01

The isotopic composition of particulate organic carbon (POC) from the Black Sea deep-water zone was studied during a Russian-Swiss expedition in May 1998. POC from the upper part of the hydrogen sulfide zone (the C-layer) was found to be considerably enriched with the 12C isotope, as compared to the POC of the oxycline and anaerobic zone. In the C-layer waters, the concurrent presence of dissolved oxygen and hydrogen sulfide and an increased rate of dark CO2 fixation were recorded, suggesting that the change in the POC isotopic composition occurs at the expense of newly formed isotopically light organic matter of the biomass of autotrophic bacteria involved in the sulfur cycle. In the anaerobic waters below the C-layer, the organic matter of the biomass of autotrophs is consumed by the community of heterotrophic microorganisms; this results in weighting of the POC isotopic composition. Analysis of the data obtained and data available in the literature allows an inference to be made about the considerable seasonable variability of the POC delta 13C value, which depends on the ratio of terrigenic and planktonogenic components in the particulate organic matter.