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Sample records for desulfurization sorbent quarterly

  1. Hot coal gas desulfurization with manganese based sorbents. Quarterly report, June--September 1994

    SciTech Connect

    Hepworth, M.T.; Slimane, R.B.

    1994-11-01

    The focus of work being performed on hot coal gas desulfurization at the Morgantown Energy Technology Center is primarily in the use of zinc titanate sorbents; however, prior studies indicated that an alternate sorbent, manganese dioxide-containing ore in mixture with alumina (75 wt% ore + 25 wt% Al{sub 2}O{sub 3}) appears to be a strong contender to zinc-based sorbents. Manganese, for example, has a lower vapor pressure in the elemental state than zinc; hence, it is not as likely to undergo zinc-depletion from the sorbent surface upon loading and regeneration cycles. Also manganese oxide is less readily reduced to the elemental state than iron; hence, the range of reduction potentials for oxygen is somewhat greater than for zinc ferrite. In addition, thermodynamic analysis of the manganese-oxygen-sulfur system shows it to be less amenable to sulfation than zinc ferrite. Also manganese chlorides are much less stable and volatile than zinc chlorides. Potential also exists for utilization of manganese at higher temperatures than zinc ferrite or zinc titanate. This Eighth Quarterly Report documents progress in pelletizing and testing via thermo-gravimetric analysis of individual pellet formulations of manganese ore/alumina combinations and also manganese carbonate/alumina with two binders, dextrin and bentonite.

  2. Hot coal gas desulfurization with manganese-based sorbents. Quarterly report, October--December 1993

    SciTech Connect

    Hepworth, M.T.; Slimane, R.B.

    1994-01-01

    The focus of work being performed on Hot Coal Gas Desulfurization at the Morgantown Energy Technology Center is primarily in the use of zinc ferrite and zinc titanate sorbents; however, prior studies indicated that an alternate sorbent, manganese dioxide-containing ore in mixture with alumina (75 wt% ore + 25 wt% Al{sub 2}O{sub 3}) may be a viable alternative to zinc-based sorbents. Manganese, for example, has a lower vapor pressure in the elemental state than zinc hence it is not as likely to undergo depletion from the sorbent surface upon loading and regeneration cycles. Also manganese oxide is less readily reduced to the elemental state than iron hence the range of reduction potentials for oxygen is somewhat greater than for zinc ferrite. In addition, thermodynamic analysis of the manganese-oxygen-sulfur system shows it to be less amenable to sulfation than zinc ferrite. Potential also exists for utilization of manganese at higher temperatures than zinc ferrite or zinc titanate. This Fifth Quarterly Report documents progress in pellet testing via thermogravimetric analysis of pellet formulation FORM4-A of a manganese ore/alumina combination. This formulation, described more fully in the Quarterly Technical Progress Report of October 15, 1993, consists of manganese carbonate combined with alundum. A 2-inch fixed-bed reactor has been fabricated and is now ready for subjecting pellets to cyclic loading and regeneration; however, a minor problem has arisen during the regeneration cycle in that sulfur tends to form and plug the exit tube during the early stage of regeneration. This problem is about to be overcome by increasing the flow rate of air during the regeneration cycle resulting in more oxidizing conditions and hence less tendency for sulfide sulfur (S{sup =}) to oxidize to the intermediate elemental form (S{sup o}) rather than to 4-valent (S{sup +4}).

  3. Hot Coal Gas Desulfurization with manganese-based sorbents. Quarterly report, April--June 1994

    SciTech Connect

    Hepworth, M.T.; Slimane, R.B.

    1994-06-01

    The focus of work being performed on Hot Coal Gas Desulfurization at the Morgantown Energy Technology Center is primarily in the use of zinc titanate sorbents; however, prior studies indicated that an alternate sorbent, manganese dioxide-containing ore in mixture with alumina (75 wt% ore + 25 wt% Al{sub 2}O{sub 3}) appears to be a strong contender to zincbased sorbents. Manganese, for example, has a lower vapor pressure in the elemental state than zinc; hence, it is not as likely to undergo zinc-depletion from the sorbent surface upon loading and regeneration cycles. Also manganese oxide is less readily reduced to the elemental state than iron; hence, the range of reduction potentials for oxygen is somewhat greater than for zinc ferrite. In addition, thermodynamic analysis of the manganese-oxygen-sulfur system shows it to be less amenable to sulfation than zinc ferrite. Also manganese chlorides are much less stable and volatile than zinc chlorides. Potential also exists for utilization of manganese at higher temperatures than zinc ferrite or zinc titanate. This Seventh Quarterly Report documents progress in bench-scale testing of a leading manganese-based sorbent pellets (FORM4-A). This formulation is a high-purity manganese carbonate-based material. This formulation was subjected to 20 consecutive cycles of sulfidation and regeneration at 900{degrees}C in a 2-inch fixed bed reactor. The sulfidation gas was a simulated Tampella U-gas with an increased hydrogen sulfide content of 3% by volume to accelerate the rate of breakthrough, arbitrarily taken as 500 ppmv. Consistent with thermo-gravimetric analysis (TGA) on individual pellets, the fixed bed tests show small improvement in capacity and kinetics with the sulfur-loading capacity being about 22% by weight of the original pellet, which corresponds to approximately 90% bed utilization!

  4. Hot gas desulfurization with sorbents containing oxides of zinc, iron, vanadium and copper. Quarterly technical progress report

    SciTech Connect

    Akyurtlu, A.

    1991-10-01

    The main objective of this research is to evaluate the desulfurization performance of novel sorbents consisting of different combinations of zinc, iron, vanadium and copper oxides; and to develop a sorbent which can reduce H{sub 2}S levels to less than 1 ppmv, which can stabilize zinc, making operations above 650{degrees}C possible, and which can produce economically recoverable amounts of elemental sulfur during regeneration. This objective will be accomplished by evaluating the sorbent performance using fixed-bed and TGA experiments supported by sorbent characterization at various reaction extents. The work done in the fourth quarter can be summarized as follows: (1) Calibration of the gas chromatograph for low and high H{sub 2}S and SO{sub 2} is completed. (2) The determination of surface areas and densities of the promoted sorbents is completed. (3) Preliminary screening of the promoted sorbents in the packed bed reactor has started.

  5. Hot Coal Gas Desulfurization with manganese based sorbents. Quarterly report, August 1, 1993--September 30, 1993

    SciTech Connect

    Hepworth, M.T.

    1993-10-01

    The focus of work being performed on Hot Coal Gas Desulfurization at the Morgantown Energy Technology Center is primarily in the use of zinc ferrite and zinc titanate sorbents; however, prior studies at the US Steel Fundamental Research Laboratories in Monroeville, PA, by E. T. Turkdogan indicated that an alternate sorbent, manganese dioxide-containing ore in mixture with alumina (75 wt % ore + 25 wt % Al{sub 2}O{sub 3}) may be a viable alternative to zinc-based sorbents. Manganese, for example, has a lower vapor pressure in the elemental state than zinc hence it is not as likely to undergo depletion from the sorbent surface upon loading and regeneration cycles. Also manganese oxide is less readily reduced to the elemental state than iron hence the range of reduction potentials for oxygen is somewhat greater than for zinc ferrite. In addition, thermodynamic analysis of the manganese-oxygen-sulfur system shows it to be less amenable to sulfation than zinc ferrite. Potential also exists for utilization of manganese at higher temperatures than zinc ferrite or zinc titanate. This report documents progress in pelletizing and testing via thermogravimetric analysis of individual pellet formulations of manganese ore/alumina combinations and also manganese carbonate/alumina with two binders, dextrin and bentonite. Preliminary results indicate that the manganese carbonate material, being of higher purity than the manganese ore, has a higher degree of sulfur capacity and more rapid absorption kinetics. A 2-inch fixed-bed reactor has been fabricated and is now ready for subjecting pellets to cyclic loading and regeneration.

  6. Enhanced durability and reactivity for zinc ferrite desulfurization sorbent. Quarterly technical progress report 8, July--September 1988

    SciTech Connect

    Jha, M.C.; Berggren, M.H.

    1988-11-14

    AMAX Research & Development Center (AMAX R&D) has been investigating methods for enhancing the reactivity and durability of the zinc ferrite desulfurization sorbent. Zinc ferrite sorbents are intended for use in desulfurization of hot coal gas in integrated gasification combined cycle (IGCC) or molten carbonate fuel cell (MCFC) applications. For the present program, the reactivity of the sorbent may be defined as its sulfur sorption capacity at the breakthrough point and at saturation in a bench-scale, fixed-bed reactor. Durability may be defined as the ability of the sorbent to maintain important physical characteristics such As size, strength, and specific surface area during 10 cycles of sulfidation and oxidation.

  7. Enhanced durability and reactivity for zinc ferrite desulfurization sorbent. Quarterly technical progress report 9, October--December 1988

    SciTech Connect

    Jha, M.C.; Berggren, M.H.

    1989-03-06

    AMAX Research & Development Center (AMAX R&D) has been investigating methods for enhancing the reactivity and durability of the zinc ferrite desulfurization sorbent. Zinc ferrite sorbents are intended for use in desulfurization of hot coal gas in integrated gasification combined cycle (IGCC) or molten carbonate fuel cell (MCFC) applications. For the present program, the reactivity of the sorbent may be defined as its sulfur sorption capacity at the breakthrough point and at saturation in a bench-scale, fixed-bed reactor. Durability may be defined as the ability of the sorbent to maintain important physical characteristics such As size, strength, and specific surface area during 10 cycles of sulfidation and oxidation.

  8. Enhanced durability and reactivity for zinc ferrite desulfurization sorbent. Quarterly technical progress report 7, April--June 1988

    SciTech Connect

    Jha, M.C.; Berggren, M.H.

    1988-08-19

    AMAX Research & Development Center (AMAX R&D) has been investigating methods for enhancing the reactivity and durability of the zinc ferrite desulfurization sorbent. Zinc ferrite sorbents are intended for use in desulfurization of hot coal gas in integrated gasification combined cycle (IGCC) or molten carbonate fuel cell (MCFC) applications. For the present program, the reactivity of the sorbent may be defined as its sulfur sorption capacity at the breakthrough point and at saturation in a bench-scale, fixed-bed reactor. Durability may be defined as the ability of the sorbent to maintain important physical characteristics such As size, strength, and specific surface area during 10 cycles of sulfidation and oxidation.

  9. LIFAC sorbent injection desulfurization demonstration project. Quarterly report No. 4, July--September 1991

    SciTech Connect

    Not Available

    1992-03-06

    In December 1990, the US Department of Energy selected 13 projects for funding under the Federal Clean Coal Technology Program (Round III). One of the projects selected was the project sponsored by LIFAC North America, (LIFAC NA), titled ``LIFAC Sorbent Injection Desulfurization Demonstration Project.`` The host site for this $17 million, three-phase project is Richmond Power and Light`s Whitewater Valley Unit No. 2 in Richmond, Indiana. The LIFAC technology uses upper-furnace limestone injection with patented humidification of the flue gas to remove 75--85% of the sulfur dioxide (SO{sub 2}) in the flue gas. In this report, progress for the period July--September 1991 is covered.

  10. LIFAC Sorbent Injection Desulfurization Demonstration Project. Quarterly report No. 12, July--September 1993

    SciTech Connect

    Not Available

    1993-12-31

    In December 1989, the U.S. Department of Energy selected 13 projects for funding under the Federal Clean Coal Technology Program (Round III). One of the projects selected was the project sponsored by LIFAC North America, (LIFAC NA), titled {open_quotes}LIFAC Sorbent Injection Desulfurization Demonstration Project.{close_quotes} The LIFAC technology uses upper-furnace limestone injection with patented humidification of the flue gas to remove 75-85% of the sulfur dioxide (SO{sub 2}) in the flue gas. The host site for this $22 million, three-phase project is Richmond Power and Light`s Whitewater Valley Unit No. 2 in Richmond, Indiana. The three project phases are: (1) Design; (2A) Long Lead Procurement; (2B) Construction; and (3) Operations. The design phase began on August 8, 1990 and was scheduled to last six months. Phase 2A, long lead procurement, overlaps the design phase and was expected to require about four months to complete. The construction phase was then to continue for another seven months, while the operations phase was scheduled to last about twenty-six months. In November 1990, after a ten (10) month negotiation period, LIFAC NA and the U.S. DOE entered into a Cooperative Agreement for the design, construction, and demonstration of the LIFAC system. This report is the twelfth Technical Progress Report covering the period July 1, 1993 through the end of September 1993. Due to the power plant`s planned outage in March 1991, and the time needed for engineering, design and procurement of critical equipment, DOE and LIFAC NA agreed to execute the Design Phase of the project in August 1990, with DOE funding contingent upon final signing of the Cooperative Agreement.

  11. Kinetics of Mn-based sorbents for hot coal gas desulfurization. Quarterly progress report, March 15, 1995--July 15, 1995

    SciTech Connect

    Hepworth, M.T.

    1995-07-15

    Hot gas desulfurization may be accomplished by using solid sorbents such as oxides of those metals that form stable sulfides. The effectiveness of a desulfurizing agent in treating such gases is related to the predicted equilibrium partial pressure of hydrogen sulfide which will be present in a phase combination of the reduced form of sulfide and oxide phases. The focus of much current work being performed by the Department of Energy on sorbent development is in the use of zinc ferrite, zinc titanate, and Z-Sorb. The latter sorbent is a commercial product consisting of ZnO, a promoter, and a proprietary supporting matrix designed to provide stability and prolong sorbent life. Although these Zn-based sorbents have been the subject of extensive pilot-scale and process development work, all sorbents produced to date still experience structural and reactive degradation over multi-cycle use at relatively moderate temperatures. An effective alternative to zinc-based sorbents could be manganese sorbents which withstand high temperature operation and also maintain structural and reactive integrity over many cycles, as investigations by Ben-Slimane and Hepworth have indicated. Thermodynamic limits may prevent MnO from achieving the low sulfur specifications of the product gas for use in a molten carbonate fuel cell, but under the correct conditions the guideline for IGCC systems can easily be achieved. Furthermore, manganese sorbents could possibly be used in conjunction with a polishing sorbent (such as zinc oxide) possessing more favorable thermodynamic properties to reach levels acceptable for fuel cell applications (< 10 ppmv). Such an arrangement may not require that the zinc sulfide be regenerated since the sulfur concentration of the cleaned gas is low enough that the zinc oxide may be discarded when exhausted.

  12. Hot Coal Gas Desulfurization with manganese-based sorbents. Second [quarterly] technical report, December 1, 1992--March 1, 1993

    SciTech Connect

    Hepworth, M.T.

    1993-03-01

    At present, the focus of work being performed on Hot Coal Gas Desulfurization is primarily in the use of zinc ferrite and zinc titanate sorbents; however studies at the US Steel Fundamental Research Laboratories in Monroeville, PA, by E. T. Turkdogan indicate that an alternate sorbent, manganese dioxide-containing ore in mixture with alumina (75 wt % ore + 25 wt % Al{sub 2}O{sub 3}) may be a preferable alternative to zinc-based sorbents. A significant domestic source of manganese in Minnesota is being explored for an in situ leach process which has potential for producing large tonnages of solutions which may be ideal for precipitation and recovery of pure manganese as a carbonate in a reactive form. In the current program the following studies will be addressed: Preparation of manganese sorbent pellets and characterization tests on pellets for strength and surface area; analysis of the thermodynamics and kinetics of sulfur removal from hot fuel gases by individual sorbent pellets (loading tests) by thermogravimetric testing; regeneration tests via TGA on individual sorbent pellets by oxidation; and bench-scale testing on sorbent beds in a two-inch diameter reactor. The developed information will be of value to METC in its determination of whether or not a manganese-based regenerable sorbent holds real promise for sulfur cleanup of hot fuel gases. This information is necessary prior to pilot-scale testing leading to commercial development is undertaken.

  13. LIFAC Sorbent Injection Desulfurization Demonstration Project. Quarterly report No. 6, January--March 1992

    SciTech Connect

    Not Available

    1992-09-01

    The LIFAC technology has similarities to other sorbent injection technologies using humidification, but employs a unique patented vertical reaction chamber located down-stream of the boiler to facilitate and control the sulfur capture and other chemical reactions. This chamber improves the overall reaction efficiency enough to allow the use of pulverized limestone rather than more expensive reagents such as lime which are often used to increase the efficiency of other sorbent injection processes. Sorbent injection is a potentially important alternative to conventional wet lime and limestone scrubbing, and this project is another effort to test alternative sorbent injection approaches. In comparison to wet systems, LIFAC, with recirculation of the sorbent, removes less sulfur dioxide - 75--85% relative to 90% or greater for conventional scrubbers - and requires more reagent material. However, if the demonstration is successful, LIFAC will offer these important advantages over wet scrubbing systems: LIFAC is relatively easy to retrofit to an existing boiler and requires less area than conventional wet FGD systems; LIFAC is less expensive to install than conventional wet FGD processes; LIFAC`s overall costs measured on a dollar-per-ton S0{sub 2} removed basis are less, an important advantage in a regulatory regime with trading of emission allocations. LIFAC produces a dry, readily disposable waste by-product versus a wet product; and LIFAC is relatively simple to operate.

  14. Desulfurization sorbent regeneration

    DOEpatents

    Jalan, V.M.; Frost, D.G.

    1982-07-07

    A spent solid sorbent resulting from the removal of hydrogen sulfide from a fuel gas flow is regenerated with a steam-air mixture. The mixture of steam and air may also include additional nitrogen or carbon dioxide. The gas mixture contacts the spent sorbent containing metal sulfide at a temperature above 500/sup 0/C to regenerate the sulfide to metal oxide or carbonate. Various metal species including the period four transition metals and the lanthanides are suitable sorbents that may be regenerated by this method. In addition, the introduction of carbon dioxide gas permits carbonates such as those of strontium, barium and calcium to be regenerated. The steam permits regeneration of spent sorbent without formation of metal sulfate. Moreover, the regeneration will proceed with low oxygen concentrations and will occur without the increase in temperature to minimize the risk of sintering and densification of the sorbent. This method may be used for high-temperature fuel cells.

  15. LIFAC Sorbent Injection Desulfurization Demonstration Project. Quarterly report No. 9, October--December 1992

    SciTech Connect

    Not Available

    1992-12-31

    Sorbent injection is a potentially important alternative to conventional wet lime and limestone scrubbing, and this project is another effort to test alternative sorbent injection approaches. In comparison to wet systems, LIFAC, with recirculation of the sorbent, removes less sulfur dioxide - 75--85% relative to 90% or greater for conventional scrubbers -- and requires more reagent material. However, if the demonstration is wet scrubbing systems: LIFAC is relatively easy to retrofit to an existing boiler and requires less area than conventional wet FGD systems. LIFAC is less expensive to install than conventional wet FGD processes. LIFAC`s overall costs measured on a dollar-per-ton SO{sub 2} removed basis are less, an important advantage in a regulatory regime with trading of emission allocations. LIFAC produces a dry, readily disposable waste by-product versus a wet product. LIFAC is relatively simple to operate.

  16. LIFAC Sorbent Injection Desulfurization Demonstration Project. Quarterly report No. 11, April--June 1993

    SciTech Connect

    Not Available

    1993-12-01

    The LIFAC technology has similarities to other sorbent injection technologies using humidification, but employs a unique patented vertical reaction chamber located down-stream of the boiler to facilitate and a 220 MW coal-fired boiler located at Kristiinankaupunki. At this facility, a slipstream (5000 SCFM) containing the calcined limestone was used to test a small-scale activation reactor (2.5 MW) in which the gas was humidified. Reactor residence times of 3 to 12 seconds resulted in SO{sub 2} removal rates up to 84%. Additional LIFAC pilot-scale tests were conducted at the 8 MW (thermal) level at the Neste Kulloo combustion laboratory to develop the relationships between the important operating and design parameters. Polish low-sulfur coal was burned to achieve 84% S0{sub 2} removal. In 1986, full-scale testing of LIFAC was conducted at Imatran Voima`s Inkoo power plant on a 250 MW utility boiler. An activation chamber was built to treat a flue gas stream representing about 70 MW. Even though the boiler was 250 MW, the 70 MW stream represented about one-half of the flue gas feeding one of the plant`s two ESP`s (i.e., each ESP receives a 125 MW gas stream). This boiler used a 1.5% sulfur coal and sulfur removal was initially 61%. By late 1987, SO{sub 2} removal rates had improved to 76%. In 1988, a LIFAC activation reactor was added to treat an additional 125 MW -- i.e., an entire flue gas/ESP stream-worth of flue gas from this same boiler. This newer activation reactor is achieving 7580% SO{sub 2} removal with Ca:S ratios between 2:1 and 2.5:1. In 1988, the first tests using high-sulfur US coals were run at the pilot scale at the Neste Kulloo Research Center, using a Pittsburgh No. 8 coal containing 3% sulfur. SO{sub 2} removal rates of 77% were achieved at a Ca:S ratio of 2:1. This LIFAC demonstration project will be conducted on a 60 MW boiler burning high-sulfur US coals to demonstrate the commercial application of the LIFAC process to US utilities.

  17. Kinetics of Mn-based sorbents for hot coal gas desulfurization. Quarterly progress report, September 15--December 15, 1994. Task 1: Literature review

    SciTech Connect

    Hepworth, M.T.

    1995-01-06

    Manganese ore as well as manganese carbonate, precipitated from aqueous solutions, combined with alumina to form indurated pellets hold promise of being a high-effective, inexpensive, regenerable sorbent for hot fuel gases. Although the thermodynamics for sulfur removal by manganese predicts somewhat higher hydrogen sulfide over-pressures (i.e. poorer degree of desulfurization) than can be accomplished with zinc-based sorbents, zinc tends to be reduced to the metallic state under coal gasification conditions resulting in loss of capacity and reactivity by volatilization of reactive surfaces. This volatilization phenomenon limits the temperatures for which desulfurization can be effectively accomplished to less than 550 C for zinc ferrite and 700 C for zinc titanate; whereas, manganese-based sorbents can be utilized at temperatures well in temperatures exceeding 700 C. Also the regeneration of manganese-based pellets under oxidizing conditions may be superior to that of zinc titanate since they can be loaded from a simulated reducing coal-derived gas and then be regenerated at higher temperatures (up to 1,300 C). The topics that will be addressed by this study include: preparation of an effective manganese-based sorbent; thermodynamics and kinetics of sulfur removal from hot fuel gases by this sorbent; analysis of kinetics and mechanisms by which sulfur is absorbed by the sorbent (i.e., whether by gaseous diffusion, surface-controlled reaction, or pore diffusion); and cyclic sulfidation and regeneration of the sorbent and recovery of the sulfur. 38 refs.

  18. Kinetics of Mn-based sorbents for hot coal gas desulfurization. Quarterly report, September 15 - December 15, 1996

    SciTech Connect

    Hepworth, M.T.

    1996-12-31

    Manganese-based sorbents have been investigated for the removal of hydrogen sulfide (the primary sulfur bearing compound) from hot coal gases prior to its use in combined cycle turbines. Four formulations of Mn-based sorbents were tested in an ambient-pressure fixed-bed reactor to determine steady state H{sub 2}S concentrations, breakthrough times and effectiveness of the sorbent when subjected to cyclic sulfidation and regeneration testing. In a previous report, the sulfidation results were presented. Manganese-based sorbents with molar ratios > 1:1 Mn:Substrate were effective in reducing the H{sub 2}S concentration in simulated coal gases to less than 100 ppmv over five cycles. Actual breakthrough time for formulation C6-2-1100 was as high as 73% of breakthrough time based on wt% Mn in sorbent. In this report, the regeneration results will be presented. Regeneration tests determined that loaded pellets can be fully regenerated in air/steam mixture at 750{degrees}C with minimal sulfate formation. 16 refs., 9 figs., 5 tabs.

  19. Kinetics of Mn-based sorbents for hot coal gas desulfurization. Quarterly report, December 15, 1993--March 15, 1997

    SciTech Connect

    Hepworth, M.T.

    1997-03-03

    Manganese-based sorbents have been investigated for the removal of hydrogen sulfide (the primary sulfur bearing compound) from hot coal gases prior to its use in combined cycle turbines. Four formulations of Mn-based sorbents were tested in an ambient-pressure fixed-bed reactor to determine steady state H{sub 2}S concentrations, breakthrough times and effectiveness of the sorbent when subjected to cyclic sulfidation and regeneration testing. In previous reports, the sulfidation and regeneration results from cyclic testing done at 600{degrees}C were presented. Manganese-based sorbents, with molar ratios > 1:1 Mn:Substrate were effective in reducing the H{sub 2}S concentration in simulated coal gases to less than 100 ppmv over five cycles. Actual breakthrough time for formulation C6-2-1100 was as high as 73% of breakthrough time based on wt% Mn in sorbent. Regeneration tests determined that loaded pellets can be fully regenerated in air/steam mixture at 750{degrees}C with minimal sulfate formation. In this report, the results from cyclic crush strength tests, Sulfur profile tests and cyclic testing at 550{degrees}C and lower flowrate cyclic testing are presented. Crush strength testing done after 5 cycles showed decreases in strength from 12.6% to 57.9%. Cyclic testing at 550{degrees}C showed pre breakthrough concentrations as low as 10 ppmv. Cyclic testing done at 2 L/min and 3 L/min did not show any significant difference in pre breakthrough concentrations or capacity.

  20. Sorbent for use in hot gas desulfurization

    DOEpatents

    Gasper-Galvin, Lee D.; Atimtay, Aysel T.

    1993-01-01

    A multiple metal oxide sorbent supported on a zeolite of substantially silicon oxide is used for the desulfurization of process gas streams, such as from a coal gasifier, at temperatures in the range of about 1200.degree. to about 1600.degree. F. The sorbent is provided by a mixture of copper oxide and manganese oxide and preferably such a mixture with molybdenum oxide. The manganese oxide and the molybdenum are believed to function as promoters for the reaction of hydrogen sulfide with copper oxide. Also, the manganese oxide inhibits the volatilization of the molybdenum oxide at the higher temperatures.

  1. Enhanced durability and reactivity for zinc ferrite desulfurization sorbent

    SciTech Connect

    Jha, M.C.; Berggren, M.H.

    1989-03-06

    AMAX Research Development Center (AMAX R D) has been investigating methods for enhancing the reactivity and durability of the zinc ferrite desulfurization sorbent. Zinc ferrite sorbents are intended for use in desulfurization of hot coal gas in integrated gasification combined cycle (IGCC) or molten carbonate fuel cell (MCFC) applications. For the present program, the reactivity of the sorbent may be defined as its sulfur sorption capacity at the breakthrough point and at saturation in a bench-scale, fixed-bed reactor. Durability may be defined as the ability of the sorbent to maintain important physical characteristics such As size, strength, and specific surface area during 10 cycles of sulfidation and oxidation.

  2. Enhanced durability and reactivity for zinc ferrite desulfurization sorbent

    SciTech Connect

    Jha, M.C.; Berggren, M.H.

    1988-11-14

    AMAX Research Development Center (AMAX R D) has been investigating methods for enhancing the reactivity and durability of the zinc ferrite desulfurization sorbent. Zinc ferrite sorbents are intended for use in desulfurization of hot coal gas in integrated gasification combined cycle (IGCC) or molten carbonate fuel cell (MCFC) applications. For the present program, the reactivity of the sorbent may be defined as its sulfur sorption capacity at the breakthrough point and at saturation in a bench-scale, fixed-bed reactor. Durability may be defined as the ability of the sorbent to maintain important physical characteristics such As size, strength, and specific surface area during 10 cycles of sulfidation and oxidation.

  3. Enhanced durability and reactivity for zinc ferrite desulfurization sorbent

    SciTech Connect

    Jha, M.C.; Berggren, M.H.

    1989-05-02

    AMAX Research Development Center (AMAX R D) has been investigating methods for enhancing the reactivity and durability of the zinc ferrite desulfurization sorbent. Zinc ferrite sorbents are intended for use in desulfurization of hot coal gas in integrated gasification combined cycle (IGCC) or molten carbonate fuel cell (MCFC) applications. For the present program, the reactivity of the sorbent may be defined as its sulfur sorption capacity at the breakthrough point and at saturation in a bench-scale, fixed-bed reactor. Durability may be defined as the ability of the sorbent to maintain important physical characteristics such As size, strength, and specific surface area during 10 cycles of sulfidation and oxidation.

  4. Enhanced durability and reactivity for zinc ferrite desulfurization sorbent

    SciTech Connect

    Jha, M.C.; Berggren, M.H.

    1988-08-19

    AMAX Research Development Center (AMAX R D) has been investigating methods for enhancing the reactivity and durability of the zinc ferrite desulfurization sorbent. Zinc ferrite sorbents are intended for use in desulfurization of hot coal gas in integrated gasification combined cycle (IGCC) or molten carbonate fuel cell (MCFC) applications. For the present program, the reactivity of the sorbent may be defined as its sulfur sorption capacity at the breakthrough point and at saturation in a bench-scale, fixed-bed reactor. Durability may be defined as the ability of the sorbent to maintain important physical characteristics such As size, strength, and specific surface area during 10 cycles of sulfidation and oxidation.

  5. LIFAC sorbent injection desulfurization demonstration project

    SciTech Connect

    Not Available

    1992-03-06

    In December 1990, the US Department of Energy selected 13 projects for funding under the Federal Clean Coal Technology Program (Round III). One of the projects selected was the project sponsored by LIFAC North America, (LIFAC NA), titled LIFAC Sorbent Injection Desulfurization Demonstration Project.'' The host site for this $17 million, three-phase project is Richmond Power and Light's Whitewater Valley Unit No. 2 in Richmond, Indiana. The LIFAC technology uses upper-furnace limestone injection with patented humidification of the flue gas to remove 75--85% of the sulfur dioxide (SO{sub 2}) in the flue gas. In this report, progress for the period July--September 1991 is covered.

  6. Hot gas desulfurization with sorbents containing oxides of zinc, iron, vanadium and copper

    SciTech Connect

    Akyurtlu, A.

    1991-10-01

    The main objective of this research is to evaluate the desulfurization performance of novel sorbents consisting of different combinations of zinc, iron, vanadium and copper oxides; and to develop a sorbent which can reduce H{sub 2}S levels to less than 1 ppmv, which can stabilize zinc, making operations above 650{degrees}C possible, and which can produce economically recoverable amounts of elemental sulfur during regeneration. This objective will be accomplished by evaluating the sorbent performance using fixed-bed and TGA experiments supported by sorbent characterization at various reaction extents. The work done in the fourth quarter can be summarized as follows: (1) Calibration of the gas chromatograph for low and high H{sub 2}S and SO{sub 2} is completed. (2) The determination of surface areas and densities of the promoted sorbents is completed. (3) Preliminary screening of the promoted sorbents in the packed bed reactor has started.

  7. Development of advanced hot-gas desulfurization sorbents. Final report

    SciTech Connect

    Jothimurugesan, K.; Adeyiga, A.A.; Gangwal, S.K.

    1997-10-01

    The objective of this project was to develop hot-gas desulfurization sorbent formulations for relatively lower temperature application, with emphasis on the temperature range from 343--538 C. The candidate sorbents include highly dispersed mixed metal oxides of zinc, iron, copper, cobalt, nickel and molybdenum. The specific objective was to develop suitable sorbents, that would have high and stable surface area and are sufficiently reactive and regenerable at the relatively lower temperatures of interest in this work. Stability of surface area during regeneration was achieved by adding stabilizers. To prevent sulfation, catalyst additives that promote the light-off of the regeneration reaction at lower temperature was considered. Another objective of this study was to develop attrition-resistant advanced hot-gas desulfurization sorbents which show stable and high sulfidation reactivity at 343 to 538 C and regenerability at lower temperatures than leading first generation sorbents.

  8. Kinetics of hot-gas desulfurization sorbents for transport reactors

    SciTech Connect

    K.C. Kwon

    2000-01-01

    Hot-gas desulfurization for the integrated gasification combined cycle (IGCC) process has been investigated by many researchers to remove effectively hydrogen sulfide with various metal oxide sorbents at elevated temperatures. Various metal oxide sorbents are formulated with metal oxides such as Fe, Co, Zn, and Ti. Initial reaction kinetics of formulated sorbents with hydrogen sulfide is studied in the presence of various amounts of moisture and hydrogen at various reaction temperatures. The objectives of this research are to study initial reaction kinetics for a sorbent-hydrogen sulfide heterogeneous reaction system, to investigate effects of concentrations of hydrogen sulfide, hydrogen, and moisture on dynamic absorption of H{sub 2}S into sorbents, to understand effects of space time of reaction gas mixtures on initial reaction kinetics of the sorbent-hydrogen sulfide system, and to evaluate effects of temperature and sorbent amounts on dynamic absorption of H{sub 2}S into sorbents. Experimental data on initial reaction kinetics of hydrogen sulfide with metal oxide sorbents were obtained with a 0.83-cm{sup 3} differential reactor. The reactivity of MCRH-67 sorbent and AHI-1 was examined. These sorbents were obtained from the Research Triangle Institute (RTI). The sorbents in the form of 70 {micro}m particles are reacted with 1,000--4,000 ppm hydrogen sulfide at 450--600 C. The range of space time of reaction gas mixtures is 0.03--0.09 s. The range of reaction duration is 4--14,400 s.

  9. Core-in-shell sorbent for hot coal gas desulfurization

    DOEpatents

    Wheelock, Thomas D.; Akiti, Jr., Tetteh T.

    2004-02-10

    A core-in-shell sorbent is described herein. The core is reactive to the compounds of interest, and is preferably calcium-based, such as limestone for hot gas desulfurization. The shell is a porous protective layer, preferably inert, which allows the reactive core to remove the desired compounds while maintaining the desired physical characteristics to withstand the conditions of use.

  10. Desulfurization sorbent development activities at METC

    SciTech Connect

    Siriwardane, R.V.

    1995-06-01

    Development of a suitable regenerable sorbent is a major barrier issue in the hot gas cleanup program for integrated gasification combined-cycle (IGCC) systems. This has been a challenging problem during the last 20 years, since many of the sorbents developed in the program could not retain their reactivity and physical integrity during repeated cycles of sulfidation and regeneration reactions. A series of promising sorbents (METC 2-10), which were capable of sustaining their reactivity and physical integrity during repeated sulfidation/ regeneration cycles, have been developed at the Morgantown Energy Technology Center (METC). These sorbents were tested both in low-pressure (260 KPa/23 psig) and high-pressure (520 KPa/60.7 psig) fixed-bed reactors at 538{degrees}C (1000{degrees}F) with simulated coal gas. High-pressure testing was continued for 20 cycles with steam regeneration. A major research goal during the last year was to lower the cost of materials utilized during the sorbent preparation. The METC 9 sorbent was prepared by substituting low-cost materials for some of the materials in METC 6 sorbent. The sulfur capacity of the two sorbents were similar during the 20-cycle testing. METC 2 sorbent was exposed to coal gas in the Modular Gas Cleanup Rig and it was later tested in the high-pressure fixed-bed reactor. The reactivity of the METC 2 sorbent was unaffected by the exposure to the coal gas. Development of these sorbents will be continued for both fluid-bed and moving-bed applications.

  11. Kinetics of Mn-based sorbents for hot coal gas desulfurization: Quarterly progress report, December 15, 1994--March 15, 1995. Task 2 -- Exploratory experimental studies: Single pellet tests; Rate mechanism analysis

    SciTech Connect

    Hepworth, M.T.

    1995-03-15

    In earlier studies, zinc ferrite and zinc titanate were developed as regenerable sorbents capable of removing hydrogen sulfide from hot fuel gases originating from coal gasification. Manganese ore as well as manganese carbonate, precipitated from aqueous solutions, combined with alumina to form indurated pellets hold promise of being a highly-effective, inexpensive, regenerable sorbent for hot fuel gases. Although the thermodynamics for sulfur removal by manganese predicts somewhat higher hydrogen sulfide over-pressures (i.e. poorer degree of desulfurization) than can be accomplished with zinc-based sorbents, zinc tends to be reduced to the metallic state under coal gasification conditions resulting in loss of capacity and reactivity by volatilization of reactive surfaces. This volatilization phenomenon limits the temperatures for which desulfurization can be effectively accomplished to less than 500 C for zinc ferrite and 700 C for zinc titanate; whereas, manganese-based sorbents can be utilized at temperatures well in temperatures exceeding 700 C. Also the regeneration of manganese-based pellets under oxidizing conditions may be superior to that of zinc titanate since they can be loaded from a simulated reducing coal-derived gas and then be regenerated at higher temperatures (up to 1,300 C). The topics that will be addressed by this study include: preparation of an effective manganese-based sorbent, thermodynamics and kinetics of sulfur removal from hot fuel gases by this sorbent, analysis of kinetics and mechanisms by which sulfur is absorbed by the sorbent (i.e., whether by gaseous diffusion, surface-controlled reaction, ore pore diffusion), and cyclic sulfidation and regeneration of the sorbent and recovery of the sulfur.

  12. Enhanced durability and reactivity for zinc ferrite desulfurization sorbent

    SciTech Connect

    Berggren, M.H.; Jha, M.C.

    1989-10-01

    AMAX Research Development Center (AMAX R D) investigated methods for enhancing the reactivity and durability of zinc ferrite desulfurization sorbents. Zinc ferrite sorbents are intended for use in desulfurization of hot coal gas in integrated gasification combined cycle (IGCC) or molten carbonate fuel cell (MCFC) applications. For this program, the reactivity of the sorbent may be defined as its sulfur sorption capacity at the breakthrough point and at saturation in a bench-scale, fixed-bed reactor. Durability may be defined as the ability of the sorbent to maintain important physical characteristics such as size, strength, and specific surface area during 10 cycles of sulfidation and oxidation. Two base case sorbents, a spherical pellet and a cylindrical extrude used in related METC-sponsored projects, were used to provide a basis for the aimed enhancement in durability and reactivity. Sorbent performance was judged on the basis of physical properties, single particle kinetic studies based on thermogravimetric (TGA) techniques, and multicycle bench-scale testing of sorbents. A sorbent grading system was utilized to quantify the characteristics of the new sorbents prepared during the program. Significant enhancements in both reactivity and durability were achieved for the spherical pellet shape over the base case formulation. Overall improvements to reactivity and durability were also made to the cylindrical extrude shape. The primary variables which were investigated during the program included iron oxide type, zinc oxide:iron oxide ratio, inorganic binder concentration, organic binder concentration, and induration conditions. The effects of some variables were small or inconclusive. Based on TGA studies and bench-scale tests, induration conditions were found to be very significant.

  13. Enhanced durability of desulfurization sorbents for fluidized-bed applications

    SciTech Connect

    Gupta, R.P.; Gangwal, S.K.

    1991-06-01

    Advanced integrated gasification combined cycle (IGCC) power systems require the development of high-temperature desulfurization sorbents capable of removing hydrogen sulfide from coal gasifier down to very low levels. The objective of this investigation was to identify and demonstrate methods for enhancing the long-term chemical reactivity and mechanical strength of zinc ferrite, a leading regenerable sorbent, for fluidized-bed applications. Fluidized sorbent beds offer significant potential in IGCC systems because of their ability to control the highly exothermic regeneration involved. However, fluidized beds require a durable, attrition-resistant sorbent in the 100--300 {mu}m size range. A bench-scale high-temperature, high- pressure (HTHP) fluidized-bed reactor (7.6-cm I.D.) system capable of operating up to 24 atm and 800{degree}C was designed, built and tested. A total of 175 sulfidation-regeneration cycles were carried out using KRW-type coal gas with various zinc ferrite formulations. A number of sorbent manufacturing techniques including spray drying, impregnation, crushing and screening, and granulation were investigated. While fluidizable sorbents prepared by crushing durable pellets and screening had acceptable sulfur capacity, they underwent excessive attrition during multicycle testing. The sorbent formulations prepared by a proprietary technique were found to have excellent attrition resistance and acceptable chemical reactivity during multicycle testing. However, zinc ferrite was found to be limited to 550{degree}C, beyond which excessive sorbent weakening due to chemical transformations, e.g., iron oxide reduction, was observed.

  14. LIFAC Sorbent Injection Desulfurization Demonstration Project

    SciTech Connect

    Not Available

    1992-01-01

    The LIFAC technology has similarities to other sorbent injection technologies using humidification, but employs a unique patented vertical reaction chamber located down-stream of the boiler to facilitate and control the sulfur capture and other chemical reactions. This chamber improves the overall reaction efficiency enough to allow the use of pulverized limestone rather than more expensive reagents such as lime which are often used to increase the efficiency of other sorbent injection processes. Sorbent injection is a potentially important alternative to conventional wet lime and limestone scrubbing, and this project is another effort to test alternative sorbent injection approaches. In comparison to wet systems, LIFAC, with recirculation of the sorbent, removes less sulfur dioxide - 75--85% relative to 90% or greater for conventional scrubbers - and requires more reagent material. However, if the demonstration is successful, LIFAC will offer these important advantages over wet scrubbing systems: LIFAC is relatively easy to retrofit to an existing boiler and requires less area than conventional wet FGD systems; LIFAC is less expensive to install than conventional wet FGD processes; LIFAC's overall costs measured on a dollar-per-ton S0{sub 2} removed basis are less, an important advantage in a regulatory regime with trading of emission allocations. LIFAC produces a dry, readily disposable waste by-product versus a wet product; and LIFAC is relatively simple to operate.

  15. Desulfurization sorbent development at the Morgantown Energy Technology Center

    SciTech Connect

    Siriwardane, R.V.; Grimm, U.; Poston, J.A.; Monaco, S.J.

    1994-10-01

    The overall objective of this project is to develop regenerable sorbents for hot gas desulfurization in IGCC systems. The major criteria for the development of novel sorbents included reasonable chemical reactivity and physical durability during repeated sulfidation and regeneration cycles. Various formulations of zinc ferrite and zinc titanate in the form of extrudates and spherical pellets have been studied at the Morgantown Energy Technology Center (METC) for removal of sulfurous gases from coal gasification gas streams. Problems of decrepitation and spalling have occurred after sulfidation and regeneration of these sorbents. Z-Sorb, a proprietary sorbent developed at Phillips Petroleum Company, showed good physical durability during testing at METC, but there was a continuous decrease in reactivity during multiple cycle tests due to steam regeneration. A series of novel sorbents containing zinc oxide have been developed at METC to address these problems. These METC-developed sorbents showed superior performance during a 20-cycle, high-pressure, fixed-bed test with steam regeneration conducted at METC. Nine sorbents were prepared, but results are given for only three.

  16. LIFAC Sorbent Injection Desulfurization Demonstration Project

    SciTech Connect

    Not Available

    1992-01-01

    Sorbent injection is a potentially important alternative to conventional wet lime and limestone scrubbing, and this project is another effort to test alternative sorbent injection approaches. In comparison to wet systems, LIFAC, with recirculation of the sorbent, removes less sulfur dioxide - 75--85% relative to 90% or greater for conventional scrubbers -- and requires more reagent material. However, if the demonstration is wet scrubbing systems: LIFAC is relatively easy to retrofit to an existing boiler and requires less area than conventional wet FGD systems. LIFAC is less expensive to install than conventional wet FGD processes. LIFAC's overall costs measured on a dollar-per-ton SO[sub 2] removed basis are less, an important advantage in a regulatory regime with trading of emission allocations. LIFAC produces a dry, readily disposable waste by-product versus a wet product. LIFAC is relatively simple to operate.

  17. Kinetics of Mn-based sorbents for hot coal gas desulfurization: Task 2, Exploratory experimental studies: Single pellet tests; Rate mechanism analysis. Quarterly report, June 15, 1996--September 15, 1996

    SciTech Connect

    Hepworth, M.T.

    1996-09-11

    Currently, the Morgantown Energy Technology Center, Department of Energy (DOE/METC) is actively investigating alternative hot fuel gas desulfurization sorbents for application to the Integrated Gasification Combined Cycle (IGCC). A sorbent must be highly active towards sulfur at high temperatures and pressures, and under varying degrees of reducing atmospheres. Also, it must regenerate nearly ideally to maintain activity over numerous cycles. Furthermore, regeneration must yield a sulfur product which is economically recoverable directly or indirectly. Several metal oxides have been investigated as regenerable sorbents for the removal of hydrogen sulfide (the primary sulfur bearing compound) from hot fuel gases. MnO was shown to have an intrinsic reaction rate approximately one order of magnitude greater than the rate or reaction with either CaO or ZnO and two orders of magnitude greater than the reaction rate with V{sub 2}0{sub 3}. Manganese also shows desulfurization potential in the temperature range of 600-700{degrees}C where metal oxides currently known to be reactive with H{sub 2}S are unsatisfactorily. In response to stability difficulties of single and binary metal oxide sorbents, increasing effort is being directed towards incorporation of an inert component into sorbent formulation as witnessed by the various Zn-titanates. Primarily, the inert component increases pore structure integrity while stabilizing the active metal oxide against reduction. This report will address testing of Mn-based sorbents in an ambient pressure fixed-bed reactor. Steady-state H{sub 2}S concentrations and breakthrough times will be presented.

  18. Hot coal gas desulfurization with manganese-based sorbents

    SciTech Connect

    Lynch, D.; Hepworth, M.T.

    1993-09-01

    The focus of work being performed on Hot Coal Gas Desulfurization is primarily in the use of zinc ferrite and zinc titanate sorbents; however, prior studies at the US Steel Fundamental Research Laboratories in Monroeville, PA, by E.T. Turkdogan indicated that an alternate sorbent, manganese dioxide-containing ore in mixture with alumina (75 wt % ore + 25 wt % Al{sub 2}/O{sub 3}) may be a viable alternative to zinc-based sorbents. Manganese, for example, has a lower vapor pressure in the elemental state than zinc hence it is not as likely to undergo depletion from the sorbent surface upon loading and regeneration cycles. Also manganese oxide is less readily reduced to the elemental state than iron hence the range of reduction potentials for oxygen is somewhat greater than for zinc ferrite. In addition, thermodynamic analysis of the manganese-oxygen-sulfur system shows it to be less amenable to sulfation than zinc ferrite. Potential also exists for utilization of manganese higher temperatures than zinc ferrite or zinc titanate. This presentation gives the thermodynamic background for consideration of manganese-based sorbents as an alternative to zinc ferrite. To date the work which has been in progress for nine months is limited at this stage to thermogravimetric testing of four formulations of manganese-alumina sorbents to determine the optimum conditions of pelletization and induration to produce reactive pellets.

  19. Enzymatic desulfurization of coal: Third quarterly report

    SciTech Connect

    Marquis, J.K.; Kitchell, J.P.

    1989-03-14

    Our current efforts to develop clean coal technology emphasize the advantages of enzymatic desulfurization techniques and have specifically addressed the potential of using partially-purified extracellular microbial enzymes or commercially available enzymes. Our work is focused on the treatment of ''model'' organic sulfur compounds such as dibenzothiophene (DBT) and ethylphenylsulfide (EPS). Furthermore, we are designing experiments to facilitate the enzymatic process by means of a hydrated organic solvent matrix. In this quarter we obtained important results both with the development of our understanding of the enzyme reaction systems and also with the microbial work at Woods Hole. 12 figs., 11 tabs.

  20. Scale-Up of Advanced Hot-Gas Desulfurization Sorbents

    SciTech Connect

    Jothimurugesan, K.; Gangwal, Santosh K.

    1996-10-14

    The overall objective of this project is to develop regenerable sorbents for hot gas desulfurization in IGCC systems. The specific objective of the project is to develop durable advanced sorbents that demonstrate a strong resistance to attrition and chemical deactivation, and high activity at temperatures as low as 343 C (650 F). A number of formulations will be prepared and screened in a 1/2-inch fixed bed reactor at high pressure (1 to 20 atm) and high temperatures using simulated coal-derived fuel-gases. Screening criteria will include, chemical reactivity, stability, and regenerability over the temperature range of 343 C to 650 C. After initial screening, at least 3 promising formulations will be tested for 25-30 cycles of absorption and regeneration. One of the superior formulations with the best cyclic performance will be selected for investigating scale up parameters. The scaled-up formulation will be tested for long term durability and chemical reactivity.

  1. Hot coal gas desulfurization with manganese-based sorbents

    SciTech Connect

    Hepworth, M.T.; Ben-Slimane, R.

    1994-12-01

    The focus of work being performed on Hot Coal Gas Desulfurization at the Morgantown Energy Technology Center is primarily in the use of zinc ferrite and zinc titanate sorbents; however, prior studies indicated that an alternate sorbent, manganese dioxide-containing ore in mixture with alumina (75 wt % ore + 25 wt % Al{sub 2}O{sub 3}) may be a viable alternative to zinc-based sorbents. Manganese, for example, has a lower vapor pressure in the elemental state than zinc hence it is not as likely to undergo depletion from the sorbent surface upon loading and regeneration cycles. Also manganese oxide is less readily reduced to the elemental state than iron hence the range of reduction potentials for oxygen is somewhat greater than for zinc ferrite. In addition, thermodynamic analysis of the manganese-oxygen-sulfur system shows it to be less amenable to sulfation than zinc ferrite. Potential also exists for utilization of manganese at higher temperatures than zinc ferrite or zinc titanate. This annual topical report documents progress in pelletizing and testing via thermo-gravimetric analysis of individual pellet formulations of manganese ore/alumina combinations and also manganese carbonate/alumina with two binders, dextrin and bentonite.

  2. SCALE-UP OF ADVANCED HOT-GAS DESULFURIZATION SORBENTS

    SciTech Connect

    K. JOTHIMURUGESAN; S.K. GANGWAL

    1998-03-01

    The objective of this study was to develop advanced regenerable sorbents for hot gas desulfurization in IGCC systems. The specific objective was to develop durable advanced sorbents that demonstrate a strong resistance to attrition and chemical deactivation, and high sulfidation activity at temperatures as low as 343 C (650 F). Twenty sorbents were synthesized in this work. Details of the preparation technique and the formulations are proprietary, pending a patent application, thus no details regarding the technique are divulged in this report. Sulfidations were conducted with a simulated gas containing (vol %) 10 H{sub 2}, 15 CO, 5 CO{sub 2}, 0.4-1 H{sub 2}S, 15 H{sub 2}O, and balance N{sub 2} in the temperature range of 343-538 C. Regenerations were conducted at temperatures in the range of 400-600 C with air-N{sub 2} mixtures. To prevent sulfation, catalyst additives were investigated that promote regeneration at lower temperatures. Characterization were performed for fresh, sulfided and regenerated sorbents.

  3. A Reusable Calcium-Based Sorbent for Desulfurizing Hot Coal Gas

    SciTech Connect

    Wheelock, T.D.; Hasler, D.J.L.

    2002-09-19

    The overall objective of this project has been to develop a superior, regenerable, calcium-based sorbent for desulfurizing hot coal gas. The sorbent should be strong, durable, inexpensive to manufacture, and capable of being reused many times. To achieve these objectives the project has focused on the development of the very promising core-in-shell sorbent.

  4. High Temperature Flue Gas Desulfurization In Moving Beds With Regenerable Copper Based Sorbents

    SciTech Connect

    Cengiz, P.A.; Ho, K.K.; Abbasian, J.; Lau, F.S.

    2002-09-20

    The objective of this study was to develop new and improved regenerable copper based sorbent for high temperature flue gas desulfurization in a moving bed application. The targeted areas of sorbent improvement included higher effective capacity, strength and long-term durability for improved process control and economic utilization of the sorbent.

  5. Characteristics and reactivity of rapidly hydrated sorbent for semidry flue gas desulfurization.

    PubMed

    Zhang, Jie; You, Changfu; Zhao, Suwei; Chen, Changhe; Qi, Haiying

    2008-03-01

    Semidry flue gas desulfurization with a rapidly hydrated sorbent was studied in a pilot-scale circulating fluidized bed (CFB) experimental facility. The desulfurization efficiency was measured for various operating parameters, including the sorbent recirculation rate and the water spray method. The experimental results show that the desulfurization efficiencies of the rapidly hydrated sorbent were 1.5-3.0 times higher than a commonly used industrial sorbent for calcium to sulfur molar ratios from 1.2 to 3.0, mainly due to the higher specific surface area and pore volume. The Ca(OH)2 content in the cyclone separator ash was about 2.9% for the rapidly hydrated sorbent and was about 0.1% for the commonly used industrial sorbent, due to the different adhesion between the fine Ca(OH)2 particles and the fly ash particles, and the low cyclone separation efficiency for the fine Ca(OH)2 particles that fell off the sorbent particles. Therefore the actual recirculation rates of the active sorbent with Ca(OH)2 particles were higher for the rapidly hydrated sorbent, which also contributed to the higher desulfurization efficiency. The high fly ash content in the rapidly hydrated sorbent resulted in good operating stability. The desulfurization efficiency with upstream water spray was 10-15% higher than that with downstream water spray. PMID:18441824

  6. Influence of Dust on High Temperature Desulfurization of Iron Oxide Sorbent

    SciTech Connect

    Zhao, J.; Huang, J.; Wu, J.; Zhang, J.; Wang, Y.

    2002-09-19

    The understanding of influence of deposited dust on desulfurization performance of sorbent is of significance for developing combined processes for simultaneous desulfurization and dust removal in hot gas cleanup. In this paper, the influence of dust from a fluidized-bed coal gasifier on iron oxide desulfurization sorbent made by a kind of waste material containing iron oxide was systemically evaluated at different temperatures (400 C-550 C) and at different quantity of dust (0.5%-5%) in a fixed-bed reactor. The result showed that dust could interact with sorbent and adversely influenced sulfur capacity and sulfidation rate of sorbent. The influence was promoted with increasing sulfidation temperature and quantity of dust. But below 450 C, the interaction could be neglected. Kinetic studies were also conducted using the grain model. Deposition of dust on the surface of the sorbent could cause the deterioration of mass transfer and the decrease of the effective diffusivities.

  7. Scale-Up of Advanced Hot-Gas desulfurization Sorbents.

    SciTech Connect

    Jothimurugesan, K.; Gangwal, S.K.

    1997-10-02

    The overall objective of this project is to develop regenerable sorbents for hot gas desulfurization in IGCC systems. The specific objective of the project is to develop durable advanced sorbents that demonstrate a strong resistance to attrition and chemical deactivation, and high activity at temperatures as low as 343 {degrees}C (650{degrees}F). A number of formulations will be prepared and screened in a one-half inch fixed bed reactor at high pressure (1 to 20 atm) and high temperatures using simulated coal-derived fuel- gases. Screening criteria will include chemical reactivity, stability, and regenerability over the temperature range of 343{degrees}C to 650{degrees}C. After initial screening, at least 3 promising formulations will be tested for 25-30 cycles of absorption and regeneration. One of the superior formulations with the best cyclic performance will be selected for investigating scale up parameters. The scaled-up formulation will be tested for long term durability and chemical reactivity.

  8. Scale-Up of Advanced Hot-Gas Desulfurization Sorbents

    SciTech Connect

    Jothimurugesan, K.; Gangwal, S.K.

    1997-04-21

    The overall objective of this project is to develop regenerable sorbents for hot gas desulfurization in IGCC systems. The specific objective of the project is to develop durable advanced sorbents that demonstrate a strong resistance to attrition and chemical deactivation, and high activity at temperatures as low as 343{degrees}C (650{degrees}F). A number of formulations will be prepared and screened in a 1/2-inch fixed bed reactor at high pressure (1 to 20 atm) and high temperatures using simulated coal-derived fuel-gases. Screening criteria will include, chemical reactivity, stability, and regenerability over the temperature range of 343{degrees}C to 650{degrees}C. After initial screening, at least 3 promising formulations will be tested for 25-30 cycles of absorption and regeneration. One of the superior formulations with the best cyclic performance will be selected for investigating scale up parameters. The scaled-up formulation will be tested for long term durability and chemical reactivity.

  9. Characteristics and reactivity of rapidly hydrated sorbent for semidry flue gas desulfurization

    SciTech Connect

    Jie Zhang; Changfu You; Suwei Zhao; Changhe Chen; Haiying Qi

    2008-03-01

    The semidry flue gas desulfurization (FGD) process has many advantages over the wet FGD process for moving sulfur dioxide emissions from pulverized coal-fired power plants. Semidry FGD with a rapidly hydrated sorbent was studied in a pilot-scale circulating fluidized bed (CFB) experimental facility. The sorbent was made from lumps of lime and coal fly ash. The desulfurization efficiency was measured for various operating parameters, including the sorbent recirculation rate and the water spray method. The experimental results show that the desulfurization efficiencies of the rapidly hydrated sorbent were 1.5-3.0 times higher than a commonly used industrial sorbent for calcium to sulfur molar ratios from 1.2 to 3.0, mainly due to the higher specific surface area and pore volume. The Ca(OH){sub 2} content in the cyclone separator ash was about 2.9% for the rapidly hydrated sorbent and was about 0.1% for the commonly used industrial sorbent, due to the different adhesion between the fine Ca(OH){sub 2} particles and the fly ash particles, and the low cyclone separation efficiency for the fine Ca(OH){sub 2} particles that fell off the sorbent particles. Therefore the actual recirculation rates of the active sorbent with Ca(OH){sub 2} particles were higher for the rapidly hydrated sorbent, which also contributed to the higher desulfurization efficiency. The high fly ash content in the rapidly hydrated sorbent resulted in good operating stability. The desulfurization efficiency with upstream water spray was 10-15% higher than that with downstream water spray. 20 refs., 7 figs., 1 tab.

  10. Adhesive carrier particles for rapidly hydrated sorbent for moderate-temperature dry flue gas desulfurization.

    PubMed

    Li, Yuan; You, Changfu; Song, Chenxing

    2010-06-15

    A rapidly hydrated sorbent for moderate-temperature dry flue gas desulfurization was prepared by rapidly hydrating adhesive carrier particles and lime. The circulation ash from a circulating fluidized bed boiler and chain boiler ash, both of which have rough surfaces with large specific surface areas and specific pore volumes, can improve the adhesion, abrasion resistance, and desulfurization characteristics of rapidly hydrated sorbent when used as the adhesive carrier particles. The adhesion ability of sorbent made from circulation ash is 67.4% higher than that of the existing rapidly hydrated sorbent made from fly ash, the abrasion ratio is 76.2% lower, and desulfurization ability is 14.1% higher. For sorbent made from chain boiler ash, the adhesion ability is increased by 74.7%, the desulfurization ability is increased by 30.3%, and abrasion ratio is decreased by 52.4%. The abrasion ratios of the sorbent made from circulation ash having various average diameters were all about 9%, and their desulfurization abilities were similar (approximately 150 mg/g). PMID:20481549

  11. Hot coal gas desulfurization with manganese-based sorbents. Annual report, September 1992--September 1993

    SciTech Connect

    Hepworth, M.T.

    1993-12-01

    The focus of work being performed on Hot Coal Gas Desulfurization at the Morgantown Energy Technology Center is primarily in the use of zinc ferrite and zinc titanate sorbents; however, prior studies at the US Steel Fundamental Research Laboratories in Monroeville, PA, by E. T. Turkdogan indicated that an alternate sorbent, manganese dioxide-containing ore in mixture with alumina (75 wt % ore + 25 wt % Al{sub 2}O{sub 3}) may be a viable alternative to zinc-based sorbents. Manganese, for example, has a lower vapor pressure in the elemental state than zinc hence it is not as likely to undergo depletion from the sorbent surface upon loading and regeneration cycles. Also manganese oxide is less readily reduced to the elemental state than iron hence the range of reduction potentials for oxygen is somewhat greater than for zinc ferrite. In addition, thermodynamic analysis of the manganese-oxygen-sulfur system shows it to be less amenable to sulfation than zinc ferrite. Potential also exists for utilization of manganese at higher temperatures than zinc ferrite or zinc titanate. This Annual Topical Report documents progress in pelletizing and testing via thermo-gravimetric analysis of individual pellet formulations of manganese ore/ alumina combinations and also manganese carbonate/alumina with two binders, dextrin and bentonite. It includes the prior Quarterly Technical Reports which indicate that the manganese carbonate material, being of higher purity than the manganese ore, has a higher degree of sulfur capacity and more rapid absorption kinetics. A 2-inch fixed-bed reactor has been fabricated and is now ready for subjecting pellets to cyclic loading and regeneration.

  12. Pore structure and reactivity changes in hot coal gas desulfurization sorbents

    SciTech Connect

    Sotirchos, S.V.

    1991-05-01

    The primary objective of the project was the investigation of the pore structure and reactivity changes occurring in metal/metal oxide sorbents used for desulfurization of hot coal gas during sulfidation and regeneration, with particular emphasis placed on the effects of these changes on the sorptive capacity and efficiency of the sorbents. Commercially available zinc oxide sorbents were used as model solids in our experimental investigation of the sulfidation and regeneration processes.

  13. Characterization and fixed-bed testing of a nickel-based hot gas desulfurization sorbent

    SciTech Connect

    Gasper-Galvin, L.D.; Swisher, J.H.; Hammerbeck, K.

    1994-10-01

    The objective of this project was to (1) extend a preliminary investigation completed earlier on dispersed nickel sorbents by developing new processing methods, characterizing sorbent materials more extensively, and evaluating the materials in fixed bed reactor tests, and (2) to determine the feasibility of using dispersed nickel sorbents with reductive regeneration for hot gas desulfurization. One of the properties of nickel that is somewhat unique is that it forms a liquid sulfide at sufficiently high temperatures with high sulfur potentials or H{sub 2}S levels. A eutectic exists in the Ni-S phase diagram at 637 C and a composition of 33.4 wt% or 21.5 wt% S. Under controlled conditions, the formation of a liquid phase can be used to advantage in hot gas desulfurization. Sorbent preparation, the experimental unit, and experimental procedure are described. Results from the sorbent, 24Ni-7Cu-Al{sub 2}O{sub 3}, are given.

  14. Enhanced durability of high-temperature desulfurization sorbents for fluidized-bed applications. [Zinc titanate

    SciTech Connect

    Gupta, R.P.; Gangwal, S.K.

    1992-01-01

    The objectives of this project are to identify and demonstrate methods for enhancing long-term chemical reactivity and attrition resistance of zinc ferrite and zinc titanate sorbents to be employed for desulfurization of hot coal-derived gases in a high-temperature, high-pressure (HTHP) fluid-bed reactor. The sorbent formulation specified for study during the base period of this project was zinc ferrite. Zinc titanate sorbents are being studied under two options to the base contract. Specific objectives of the zinc titanate sorbent development work are the following: The effect of following process variables was investigated o the performance of zinc titanate sorbents: Method of sorbent preparation, Composition of fuel gas, Zn to Ti ratio of the sorbent, Sulfidation temperature, and Superficial gas velocity. The effect of first three variables has been covered in RTI's 1991 paper (Gupta and Gangwal, 1991b), while the effect of temperature and superficial gas velocity is described here.

  15. Enhanced durability of high-temperature desulfurization sorbents for fluidized-bed applications

    SciTech Connect

    Gupta, R.P.; Gangwal, S.K.

    1992-11-01

    The objectives of this project are to identify and demonstrate methods for enhancing long-term chemical reactivity and attrition resistance of zinc ferrite and zinc titanate sorbents to be employed for desulfurization of hot coal-derived gases in a high-temperature, high-pressure (HTHP) fluid-bed reactor. The sorbent formulation specified for study during the base period of this project was zinc ferrite. Zinc titanate sorbents are being studied under two options to the base contract. Specific objectives of the zinc titanate sorbent development work are the following: The effect of following process variables was investigated o the performance of zinc titanate sorbents: Method of sorbent preparation, Composition of fuel gas, Zn to Ti ratio of the sorbent, Sulfidation temperature, and Superficial gas velocity. The effect of first three variables has been covered in RTI`s 1991 paper (Gupta and Gangwal, 1991b), while the effect of temperature and superficial gas velocity is described here.

  16. Advanced sulfur control concepts in hot-gas desulfurization technology. Quarterly report, April 1--June 30, 1997

    SciTech Connect

    Harrison, D.P.

    1997-12-31

    Three areas of research were pursued during the past quarter. Experimental CeO{sub 2} sulfidation and regeneration tests examined the effect of SO{sub 2} concentration and gas flow rate on the production of elemental sulfur during regeneration. The maximum number of cycles using a single sorbent charge was increased to 13, and initial tests using a second source of CeO{sub 2} (from Molycorp, Inc.) were carried out. In the process analysis effort, a third case study based on single-stage desulfurization using CeO{sub 2} sorbent was added. Capital and operating costs for this option were estimated under base case conditions. The sensitivity of the annual levelized cost of all three cases to variations in sorbent durability, sorbent unit cost, O{sub 2} and N{sub 2} unit cost, and capital cost was examined. As the sorbent cost was reduced, based on smaller sorbent replacement rate and/or smaller sorbent unit cost, the annual levelized cost of all three processes decreased, and the cerium process became more attractive. For example, at a sorbent replacement rate of 0.1% of the sorbent circulation rate, both cerium processes should be less costly than the single-stage zinc sorbent process. As the sorbent replacement rate approaches zero (infinite sorbent lifetime), income from the sulfur by-product and export steam produced by the cerium processes exceeds the other process costs and a profit of $2 to 2.5 million appears possible. In contrast, the annual levelized cost of the zinc-based process at zero sorbent replacement rate is about $5 million.

  17. Characterization and optimization of sorbents utilized for emission control during coal gasification. 1997 Fourth quarter research report, October 1, 1997--December 31, 1997

    SciTech Connect

    Huque, Z.; Mei, D.; Zhou, J.

    1997-12-31

    Advanced integrated gasification combined cycle and pressurized fluidized bed combustion power system requires both hot gas desulfurization and particulate filtration to improve system thermal efficiency and overall performance. Few metal oxides were evaluated to be the sorbent candidate for hot gas desulfurization process. The use of waste iron oxide as a disposable metal oxide sorbent will alleviate the constraints imposed on iron oxides including the degradation of sulfur capacity and its physical attrition required for a regenerable sorbent. The very low cost of waste iron oxides and the elimination of the investment associated with sorbent regeneration make it attractive to replace currently developed sorbent candidates. However, the use of waste iron oxides indicates a significant increase of dust loading for particulate filtration. The slower the reaction rate the iron oxide and coal ash mixture is, the longer residence time and higher iron oxide to coal ratio are required. One of the key issue of the use of waste iron oxides as a disposable sorbent material relies on the capability of particulate filtration efficiency. The current back pulse cleaning of the dust cake had been evaluated; and the preliminary test results indicated that the simultaneous operation of hot gas desulfurization and particulate filtration is feasible. A parametric testing will be performed on hot gas desulfurization and particulate independently first. The independent test results will help optimize the test design and evaluation of the integration of hot gas desulfurization testing and particulate filtration testing to be completed in the first two quarters 1998.

  18. Experimental study on the reuse of spent rapidly hydrated sorbent for circulating fluidized bed flue gas desulfurization.

    PubMed

    Li, Yuan; Zheng, Kai; You, Changfu

    2011-11-01

    Rapidly hydrated sorbent, prepared by rapidly hydrating adhesive carrier particles and lime, is a highly effective sorbent for moderate temperature circulating fluidized bed flue gas desulfurization (CFB-FGD) process. The residence time of fine calcium-containing particles in CFB reactors increases by adhering on the surface of larger adhesive carrier particles, which contributes to higher sorbent calcium conversion ratio. The circulation ash of CFB boilers (α-adhesive carrier particles) and the spent sorbent (β and γ-adhesive carrier particles) were used as adhesive carrier particles for producing the rapidly hydrated sorbent. Particle physical characteristic analysis, abrasion characteristics in fluidized bed and desulfurization characteristics in TGA and CFB-FGD systems were investigated for various types of rapidly hydrated sorbent (α, β, and γ-sorbent). The adhesion ability of γ-sorbent was 50.1% higher than that of α-sorbent. The abrasion ratio of β and γ-sorbent was 16.7% lower than that of α-sorbent. The desulfurization abilities of the three sorbent in TGA were almost same. The desulfurization efficiency in the CFB-FGD system was up to 95% at the bed temperature of 750 °C for the β-sorbent. PMID:21928832

  19. Continuous Operation of Spray-Dried Zinc Based Sorbent in a Hot Gas Desulfurization Process Consisting of a Transport Desulfurizer and a Fluidized Regenerator

    SciTech Connect

    Yi, C-K.; Jo, S-H.; Jin, G-T.; Son, J-E.; Han, M-H.; Ryu, C-K.

    2002-09-19

    We see the sorbent reaction performance in a HGD process consisting of a transport desulfurizer and a fluidized regenerator in this study. We have obtained the solid hold-up and solid circulation rate necessary to reach the target desulfurization efficiency. A major obstacle for fluidized- or transport bed sorbent developments is sorbent durability withstanding attrition. Continuous operation only makes similar conditions of real processes such as rapid temperature swing, chemical transformations between sulfidation and regeneration, stresses induced by fluidization and continuous particle circulation between two reactors. Therefore, an integrated system of transport desulfurizer and bubbling regenerator is operated continuously more than 150 hours to see system reliability, sorbent reaction characteristics, sorbent morphology before and after test.

  20. DISPOSAL OF SPENT SORBENT FROM DRY FGD (FLUE GAS DESULFURIZATION) PROCESSES

    EPA Science Inventory

    The report gives results of a study of sintering and leaching mechanisms of fly ash/spent sodium sorbent mixtures from a dry injection flue gas desulfurization (FGD) process. It includes an estimate of the economics of pelletizing and sintering to handle the fly ash and spent sor...

  1. Method for reducing sulfate formation during regeneration of hot-gas desulfurization sorbents

    DOEpatents

    Bissett, Larry A.; Strickland, Larry D.; Rockey, John M.

    1994-01-01

    The regeneration of sulfur sorbents having sulfate forming tendencies and used for desulfurizing hot product gas streams such as provided by coal gasification is provided by employing a two-stage regeneration method. Air containing a sub-stoichiometric quantity of oxygen is used in the first stage for substantially fully regenerating the sorbent without sulfate formation and then regeneration of the resulting partially regenerated sorbent is completed in the second stage with air containing a quantity of oxygen slightly greater than the stoichiometric amount adequate to essentially fully regenerate the sorbent. Sulfate formation occurs in only the second stage with the extent of sulfate formation being limited only to the portion of the sulfur species contained by the sorbent after substantially all of the sulfur species have been removed therefrom in the first stage.

  2. Iron blast furnace slag/hydrated lime sorbents for flue gas desulfurization.

    PubMed

    Liu, Chiung-Fang; Shih, Shin-Min

    2004-08-15

    Sorbents prepared from iron blast furnace slag (BFS) and hydrated lime (HL) through the hydration process have been studied with the aim to evaluate their reactivities toward SO2 under the conditions prevailing in dry or semidry flue gas desulfurization processes. The BFS/HL sorbents, having large surface areas and pore volumes due to the formation of products of hydration, were highly reactive toward SO2, as compared with hydrated lime alone (0.24 in Ca utilization). The sorbent reactivity increased as the slurrying temperature and time increased and as the particle size of BFS decreased; the effects of the liquid/solid ratio and the sorbent drying conditions were negligible. The structural properties and the reactivity of sorbent were markedly affected by the BFS/HL ratio; the sorbent with 30/70 ratio had the highest 1 h utilization of Ca, 0.70, and SO2 capture, 0.45 g SO2/g sorbent. The reactivity of a sorbent was related to its initial specific surface area (Sg0) and molar content of Ca (M(-1)); the 1 h utilization of Ca increased almost linearly with increasing Sg0/M. The results of this study are useful to the preparation of BFS/HL sorbents with high reactivity for use in the dry and semidry processes to remove SO2 from the flue gas. PMID:15382877

  3. Enhanced durability and reactivity for zinc ferrite desulfurization sorbent. Volume 1, Bench-scale testing and analysis

    SciTech Connect

    Jha, M.C.; Berggren, M.H.

    1989-05-02

    AMAX Research & Development Center (AMAX R&D) has been investigating methods for enhancing the reactivity and durability of the zinc ferrite desulfurization sorbent. Zinc ferrite sorbents are intended for use in desulfurization of hot coal gas in integrated gasification combined cycle (IGCC) or molten carbonate fuel cell (MCFC) applications. For the present program, the reactivity of the sorbent may be defined as its sulfur sorption capacity at the breakthrough point and at saturation in a bench-scale, fixed-bed reactor. Durability may be defined as the ability of the sorbent to maintain important physical characteristics such As size, strength, and specific surface area during 10 cycles of sulfidation and oxidation.

  4. Enhanced durability of high-temperature desulfurization sorbents for moving-bed applications

    SciTech Connect

    Ayala, R.E.

    1991-08-01

    The objective of this contract was to identify and test fabrication methods and sorbent chemical compositions that enhance the long-term chemical reactivity and mechanical strength of zinc ferrite and other novel sorbents for moving-bed, high-temperature desulfurization of coal-derived gases. Desired properties to be enhanced for moving-bed sorbent materials are: (1) high chemical reactivity (sulfur absorption rate and total sulfur capacity), (2) high mechanical strength (pellet crush strength and attrition resistance), and (3) suitable pellet morphology (e.g., pellet size, shape, surface area, and average specific pore volume). In addition, it is desired to maintain the sorbent properties over extended cyclic use in moving- bed systems.

  5. Enhanced durability of desulfurization sorbents for fluidized-bed applications

    SciTech Connect

    Gupta, R.P.; Gangwal, S.K.

    1993-08-01

    To the most important findings of this 100-cycle test, ZT-4 consistently reduced the H{sub 2}S content of coal gas from 11,400 ppmv to less than 20 ppmv at 750{degree}C. The sorbent exhibited deactivation over 100 cycles with most of the activity decline occurring in the first 50 cycles. This deactivation was found to correlate with decreases in the BET area, pore volume, and internal porosity. The best correlation, as expected with small particles, was with the BET surface area. Formation of zinc silicate in the sorbent structure is believed to be a potential cause of deactivation. Despite deactivation, the sorbent became more attrition-resistant after 100 cycles of testing with negligible material loss from the reactor. No evidence of zinc loss from the sorbent was found despite its operation at 750{degree}C for 100 cycles.

  6. Microbial stabilization of sulfur-laden sorbents. [Quarterly] technical report, March 1, 1993--May 31, 1993

    SciTech Connect

    Miller, K.W.

    1993-09-01

    Clean coal technologies that involve limestone for in situ sulfur capture generate lime/limestone products laden with sulfur at various oxidation states. If sulfur is completely stabilized as sulfate, the spent sorbent is ready for commercial utilization as gypsum. However, the presence of reduced sulfur species requires additional processing. Thermal oxidation of reduced sulfur frequently results in undesirable release of SO{sub 2}. Microbial oxidation might provide an inexpensive and effective alternative. Sorbents laden with reduced forms of sulfur such as sulfide or sulfite can serve as growth substrates for sulfur-oxidizing bacteria, which convert all sulfur to sulfate. The goals of this project are the following: (1) to optimize conditions for sulfate generation from sulfide, thiosulfate, and sulfite; (2) to test and optimize the effectiveness of microbial processing on spent sorbents from flue gas desulfurization, coal gasification, and fluidized bed combustion; (3) to search for hyperalkalinophilic thiobacilli, which would be effective up to pH 11. This quarter, temperature, nitrogen, and phosphate requirements for sulfate generation on thiosulfate were optimized with respect to two named strains and two promising isolates. Spent sorbents from three different power plants were tested for sulfite and thiosulfate contents, in preparation for bioprocessing.

  7. Hot coal gas desulfurization with manganese-based sorbents. Final report, September 1992--December 1994

    SciTech Connect

    Hepworth, M.T.; Slimane, R.B.

    1994-11-01

    The focus of much current work being performed by the Morgantown Energy Technology Center (METC) of the Department of Energy on hot coal-derived fuel gas desulfurization is in the use of zinc-based sorbents. METC has shown interest in formulating and testing manganese-based pellets as alternative effective sulfur sorbents in the 700 to 1200{degree}C temperature range. To substantiate the potential superiority of Mn-based pellets, a systematic approach toward the evaluation of the desulfurizing power of single-metal sorbents is developed based on thermodynamic considerations. This novel procedure considered several metal-based sorbents and singled out manganese oxide as a prime candidate sorbent capable of being utilized under a wide temperature range, irrespective of the reducing power (determined by CO{sub 2}/CO ratio) of the fuel gas. Then, the thermodynamic feasibility of using Mn-based pellets for the removal of H{sub 2}S from hot-coal derived fuel gases, and the subsequent oxidative regeneration of loaded (sulfided) pellets was established. It was concluded that MnO is the stable form of manganese for virtually all commercially available coal-derived fuel gases. In addition, the objective of reducing the H{sub 2}S concentration below 150 ppMv to satisfy the integrated gasification combined cycle system requirement was shown to be thermodynamically feasible. A novel process is developed for the manufacture of Mn-based spherical pellets which have the desired physical and chemical characteristics required.

  8. Process for the manufacture of an attrition resistant sorbent used for gas desulfurization

    DOEpatents

    Venkataramani, Venkat S.; Ayala, Raul E.

    2003-09-16

    This process produces a sorbent for use in desulfurization of coal gas. A zinc titanate compound and a metal oxide are mixed by milling the compounds in an aqueous medium, the resulting mixture is dried and then calcined, crushed, sleved and formed into pellets for use in a moving-bed reactor. Metal oxides suitable for use as an additive in this process include: magnesium oxide, magnesium oxide plus molybdenum oxide, calcium oxide, yttrium oxide, hafnium oxide, zirconium oxide, cupric oxide, and tin oxide. The resulting sorbent has a percentage of the original zinc or titanium ions substituted for the oxide metal of the chosen additive.

  9. Enhanced durability of desulfurization sorbents for fluidized-bed applications

    SciTech Connect

    Gupta, R.P.; Gangwal, S.K.

    1992-11-01

    To extend the operating temperature range and further improve the durability of fluidizable sorbents, zinc titanate, another leading regenerable sorbent, was selected for development in the later part of this project. A number of zinc titanate formulations were prepared in the 50 to 300 {mu}m range using granulation and spray drying methods. Important sorbent preparation variables investigated included zinc to titanium ratio, binder type, binder amount, and various chemical additives such as cobalt and molybdenum. A number of sorbents selected on the basis of screening tests were subjected to bench-scale testing for 10 cycles at high temperature, high pressure (HTHP) conditions using the reactor system designed and constructed during the base program. This reactor system is capable of operation either as a 2.0 in. or 3.0 in. I.D. bubbling bed and is rated up to 20 atm operation at 871{degrees}C. Bench-scale testing variables included sorbent type, temperature (550 to 750{degrees}C), gas type (KRW or Texaco gasifier gas), steam content of coal gas, and fluidizing gas velocity (6 to 15 cm/s). The sorbents prepared by spray drying showed poor performance in terms of attrition resistance and chemical reactivity. On the other hand, the granulation method proved to be very successful. For example, a highly attrition-resistant zinc titanate formulation, ZT-4, prepared by granulation exhibited virtually no zinc loss and demonstrated a constant high reactivity and sulfur capacity over 10 cycles, i.e., approximately a 60 percent capacity utilization, with Texaco gas at 750{degrees}C, 15 cm/s fluidizing velocity and 15 atm pressure. The commercial potential of the granulation method for zinc titanate manufacture was demonstrated by preparing two 80 lb batches of sorbent with zinc to titanium mol ratios of 0.8 and 1.5.

  10. Enhanced durability of desulfurization sorbents for fluidized-bed applications

    SciTech Connect

    Gupta, R.P.; Gangwal, S.K.

    1992-11-01

    To extend the operating temperature range and further improve the durability of fluidizable sorbents, zinc titanate, another leading regenerable sorbent, was selected for development in the later part of this project. A number of zinc titanate formulations were prepared in the 50 to 300 [mu]m range using granulation and spray drying methods. Important sorbent preparation variables investigated included zinc to titanium ratio, binder type, binder amount, and various chemical additives such as cobalt and molybdenum. A number of sorbents selected on the basis of screening tests were subjected to bench-scale testing for 10 cycles at high temperature, high pressure (HTHP) conditions using the reactor system designed and constructed during the base program. This reactor system is capable of operation either as a 2.0 in. or 3.0 in. I.D. bubbling bed and is rated up to 20 atm operation at 871[degrees]C. Bench-scale testing variables included sorbent type, temperature (550 to 750[degrees]C), gas type (KRW or Texaco gasifier gas), steam content of coal gas, and fluidizing gas velocity (6 to 15 cm/s). The sorbents prepared by spray drying showed poor performance in terms of attrition resistance and chemical reactivity. On the other hand, the granulation method proved to be very successful. For example, a highly attrition-resistant zinc titanate formulation, ZT-4, prepared by granulation exhibited virtually no zinc loss and demonstrated a constant high reactivity and sulfur capacity over 10 cycles, i.e., approximately a 60 percent capacity utilization, with Texaco gas at 750[degrees]C, 15 cm/s fluidizing velocity and 15 atm pressure. The commercial potential of the granulation method for zinc titanate manufacture was demonstrated by preparing two 80 lb batches of sorbent with zinc to titanium mol ratios of 0.8 and 1.5.

  11. Hot coal gas desulfurization with manganese-based sorbents

    SciTech Connect

    Hepworth, M.T.; Ben-Slimane, R.

    1995-11-01

    The primary major deposit of manganese in the US which can be readily mined by an in situ process is located in the Emily district of Minnesota. The US Bureau of Mines Research Centers at both the Twin Cities and Salt Lake City have developed a process for extracting and refining manganese in the form of a high-purity carbonate product. This product has been formulated into pellets by a multi-step process of drying, calcination, and induration to produce relatively high-strength formulations which are capable of being used for hot fuel gas desulfurization. These pellets, which have been developed at the University of Minnesota under joint sponsorship of the US Department of Energy and the US Bureau of Mines, appear superior to other, more expensive, formulations of zinc titanate and zinc ferrite which have previously been studied for multi-cycle loading (desulfurization) and regeneration (evolution of high-strength SO{sub 2} and restoration of pellet reactivity). Although these other formulations have been under development for the past twelve years, their prices still exceed $7 per pound. If manganese pellets perform as predicted in fixed bed testing, and if a significant number of utilities which burn high-sulfur coals incorporate combined-cycle gasification with hot coal gas desulfurization as a viable means of increasing conversion efficiencies, then the potential market for manganese pellets may be as high as 200,000 tons per year at a price not less than $3 per pound. This paper discusses the role of manganese pellets in the desulfurization process with respect to the integrated gasification combined-cycle (IGCC) for power generation.

  12. Regenerative Cu/La zeolite supported desulfurizing sorbents

    NASA Technical Reports Server (NTRS)

    Voecks, Gerald E. (Inventor); Sharma, Pramod K. (Inventor)

    1991-01-01

    Efficient, regenerable sorbents for removal of H2S from fluid hydrocarbons such as diesel fuel at moderate condition comprise a porous, high surface area aluminosilicate support, suitably a synthetic zeolite, and most preferably a zeolite having a free lattice opening of at least 6 Angstroms containing from 0.1 to 0.5 moles of copper ions, lanthanum ions or their mixtures. The sorbent removes sulfur from the hydrocarbon fuel in high efficiency and can be repetitively regenerated without loss of activity.

  13. Pore structure and reactivity changes in hot coal gas desulfurization sorbents. Final report, September 1987--January 1991

    SciTech Connect

    Sotirchos, S.V.

    1991-05-01

    The primary objective of the project was the investigation of the pore structure and reactivity changes occurring in metal/metal oxide sorbents used for desulfurization of hot coal gas during sulfidation and regeneration, with particular emphasis placed on the effects of these changes on the sorptive capacity and efficiency of the sorbents. Commercially available zinc oxide sorbents were used as model solids in our experimental investigation of the sulfidation and regeneration processes.

  14. Elemental sulfur recovery from desulfurization sorbents in advanced power systems

    SciTech Connect

    Dorchak, T.P.; Gangwal, S.K.; Turk, B.S.

    1995-12-31

    Regenerable metal oxide sorbents, such as zinc titanate, are being developed to efficiently remove hydrogen sulfide (H{sub 2}S) from coal gas in advanced power systems. Dilute air regeneration of the sorbents produces a tailgas containing a few percent sulfur dioxide (SO{sub 2}). Catalytic reduction of the SO{sub 2} to elemental sulfur with a coal gas slipstream using the Direct Sulfur Recovery Process (DSRP) is a leading first-generation technology. Currently the DSRP is undergoing field testing at gasifier sites. The objective of this study is to develop second-generation processes that produce elemental sulfur with limited use of coal gas. Novel approaches that were evaluated to produce elemental sulfur from sulfided sorbents include (1) SO{sub 2} regeneration, (2) substoichiometric oxidation, (3) steam regeneration followed by H{sub 2}S oxidation, and (4) steam-air regeneration. Experimental results at high temperature and high pressure demonstrate that, with simple sorbent modifications, direct regeneration to elemental sulfur is feasible without the use of coal gas.

  15. Mechanistic and kinetic studies of high-temperature coal gas desulfurization sorbents

    SciTech Connect

    Lew, S.; Flytzani-Stephanopoulos, M.; Sarofim, A.F.

    1991-10-01

    The overall objective of this project was to investigate the properties of and evaluate mixed oxides of zinc and titanium for hot fuel gas desulfurization. Uncombined ZnO was also investigated as a base case. Detailed investigation of the reduction and sulfidation reactions of Zn-Ti-O sorbents was performed. The intrinsic kinetics and the product layer diffusion rates in reduction and sulfidation were determined. Kinetic experiments with sorbents containing various Zn/Ti atomic ratios were performed. Chemical phase and structural transformations were followed by various methods. The results were compared to similar experiments performed with ZnO. The purpose of these experiments was to determine how the presence of titanium dioxide affects the reduction and sulfidation of ZnO. This information would be used to identify and select the sorbent composition that gives the best combination of low reduction rate and acceptable sulfidation performance at temperatures exceeding 600{degree}C. (VC)

  16. Durable zinc ferrite sorbent pellets for hot coal gas desulfurization

    DOEpatents

    Jha, Mahesh C.; Blandon, Antonio E.; Hepworth, Malcolm T.

    1988-01-01

    Durable, porous sulfur sorbents useful in removing hydrogen sulfide from hot coal gas are prepared by water pelletizing a mixture of fine zinc oxide and fine iron oxide with inorganic and organic binders and small amounts of activators such as sodium carbonate and molybdenite; the pellets are dried and then indurated at a high temperature, e.g., 1800.degree. C., for a time sufficient to produce crush-resistant pellets.

  17. Durable zinc oxide-containing sorbents for coal gas desulfurization

    DOEpatents

    Siriwardane, Ranjani V.

    1996-01-01

    Durable zinc-oxide containing sorbent pellets for removing hydrogen sulfide from a gas stream at an elevated temperature are made up to contain titania as a diluent, high-surface-area silica gel, and a binder. These materials are mixed, moistened, and formed into pellets, which are then dried and calcined. The resulting pellets undergo repeated cycles of sulfidation and regeneration without loss of reactivity and without mechanical degradation. Regeneration of the pellets is carried out by contacting the bed with an oxidizing gas mixture.

  18. Desulfurization characteristics of rapidly hydrated sorbents with various adhesive carrier particles for a semidry CFB-FGD system.

    PubMed

    You, Changfu; Li, Yuan

    2013-03-19

    Semidry flue gas desulfurization (FGD) experiments were conducted using rapidly hydrated sorbents with four different adhesive carrier particles: circulation ash from a circulating fluidized bed boiler (CFBB circulation ash), fly ash from the first electrical field of the electrostatic precipitator of a circulating fluidized bed boiler (CFBB ESP ash), fly ash from a chain boiler (chain boiler ash), and river sand smaller than 1 mm. The influences of various adhesive carrier particles and operating conditions on the desulfurization characteristics of the sorbents were investigated, including sprayed water, reaction temperature, and the ratio of calcium to sulfur (Ca/S). The experimental results indicated that the rapidly hydrated sorbents had better desulfurization characteristics by using adhesive carrier particles which possessed better pore, adhesion, and fluidization characteristics. The desulfurization efficiency of the system increased as the reaction temperature decreased, it improved from 35% to 90% as the mass flow rate of the sprayed water increased from 0 to 10 kg/h, and it increased from 65.6% to 82.7% as Ca/S increased from 1.0 to 2.0. Based on these findings, a new semidry circulating fluidized bed (CFB)-FGD system using rapidly hydrated sorbent was developed. Using the rapidly hydrated sorbent, this system uses a cyclone separator instead of an ESP or a bag filter to recycle the sorbent particles, thereby decreasing the system flow resistance, saving investment and operating costs of the solids collection equipment. PMID:23398211

  19. Advanced sulfur control concepts in hot-gas desulfurization technology. Quarterly report, April--June 1994

    SciTech Connect

    Harrison, D.P.

    1994-07-01

    The primary objective of this research project is the direct production of elemental sulfur during the regeneration of known high temperature desulfurization sorbents. The contract was awarded to LSU on April 12, 1994, and this quarterly report covers accomplishments during the first 2 1/2 months of the project. Effort during the initial 2 1/2 month period has been limited to Tasks 1 and 2, and involves a search of the literature to identify concepts for producing elemental sulfur during regeneration of known metal oxide sorbents and a thermodynamic evaluation of these concepts. While searching and evaluating the literature is a continuing process, concentrated effort on that phase is now complete and a detailed summary is included in this report. Three possible concepts for the direct production of elemental sulfur were identified in the LSU proposal, and the literature search has not uncovered any additional concepts. Thus, the three concepts being investigated involve: (1) regeneration with SO{sub 2}, (2) regeneration with mixtures Of 02 and H{sub 2}O, and (3) regeneration with H{sub 2}O. While concept (3) directly produces H{sub 2}S instead of elemental sulfur, the concept is included because the possibility exists for converting H{sub 2}S to elemental sulfur using the Claus process. Each of the concepts will ultimately be compared to the Direct Sulfur Recovery Process (DSRP) under development by RTI. DSRP involves initial sorbent regeneration to SO{sub 2}, and the inclusion of additional processing steps to reduce the SO{sub 2} to elemental sulfur.

  20. Hot coal gas desulfurization with manganese-based sorbents

    SciTech Connect

    Hepworth, M.T.; Ben-Slimane, R.

    1994-10-01

    In this paper, the physical and chemical behavior of several sorbent formulations fabricated from a manganese-containing compound, alundum (Al{sub 2}O{sub 3}), and a binder are addressed. The thermodynamic feasibility of hydrogen sulfide (H{sub 2}S)-removal from hot-simulated coal-gases using these sorbents and their subsequent regeneration with air are established. A formulation, FORM4-A, which consists of MnCO{sub 3}, alundum, and bentonite exhibits the best combination of capacity and reactivity; whereas, FORM1-A, which consists of Mn-ore, alundum, and dextrin exhibits the best combination of strength and reactivity. One important finding is that the capacity of the pellets for sulfur pickup from a H{sub 2}/H{sub 2}S mixture (at 950{degrees}C) and the kinetics of reduction, sulfidation and regeneration (at 1000{degrees}C) improve with recycling without compromising the strength. The leading formulation, FORM4-A, was subjected to 20 consecutive cycles of sulfidation and regeneration at 900{degrees}C in a 2-inch fixed bed reactor. The sulfidation gas was a simulated Tampella U-gas with an increased hydrogen sulfide content of 3% by volume to accelerate the rate of breakthrough, arbitrarily taken as 500 ppmv. Consistent with thermo-gravimetric analysis (TGA) on individual pellets, the fixed bed tests show small improvement in capacity and kinetics with the sulfur-loading capacity being about 22% by weight of the original pellet, which corresponds to approximately 90% bed utilization.

  1. A biomass-supported Na2CO3 sorbent for flue gas desulfurization.

    PubMed

    Shang, Hongshan; Ouyang, Ti; Yang, Fan; Kou, Yuan

    2003-06-01

    A novel sorbent for SO2 removal has been investigated. The sorbent is obtained by conventional incipient wetness impregnation of abandoned biomaterials (straw or dried leaves) with an aqueous solution of Na2CO3. A material with the composition 80 wt % Na2CO3/straw shows a desulfurization activity which is both higher and faster than that of the reference sample Na2CO3/gamma-Al2O3. The breakthrough and stoichiometric SO2 adsorption efficiencies for 80 wt % Na2CO3/straw reach 48.9% and 80.6%, respectively, at a temperature of 80 degrees C. The adsorption efficiencies are almost constant in the temperature range 70 to 300 degrees C. According to IR and XPS analysis the main products observed on the spent sorbent are sulfite below 150 degrees C and sulfate at 300 degrees C. The Na2CO3 in 80 wt % Na2CO3/straw can potentially be recycled by the oxidation of the straw with concomitant reduction of the sulfite species to elemental sulfur, making the proposed process CO2 neutral. PMID:12831049

  2. Enhanced durability of high-temperature desulfurization sorbents for moving-bed applications. Base Program: Development and testing of zinc ferrite sorbents

    SciTech Connect

    Ayala, R.E.

    1991-08-01

    The objective of this contract was to identify and test fabrication methods and sorbent chemical compositions that enhance the long-term chemical reactivity and mechanical strength of zinc ferrite and other novel sorbents for moving-bed, high-temperature desulfurization of coal-derived gases. Desired properties to be enhanced for moving-bed sorbent materials are: (1) high chemical reactivity (sulfur absorption rate and total sulfur capacity), (2) high mechanical strength (pellet crush strength and attrition resistance), and (3) suitable pellet morphology (e.g., pellet size, shape, surface area, and average specific pore volume). In addition, it is desired to maintain the sorbent properties over extended cyclic use in moving- bed systems.

  3. Enhanced durability of high-temperature desulfurization sorbents for moving-bed applications. Option 2 Program: Development and testing of zinc titanate sorbents

    SciTech Connect

    Ayala, R.E.

    1993-04-01

    One of the most advantageous configurations of the integrated gasification combined cycle (IGCC) power system is coupling it with a hot gas cleanup for the more efficient production of electric power in an environmentally acceptable manner. In conventional gasification cleanup systems, closely heat exchangers are necessary to cool down the fuel gases for cleaning, sometimes as low as 200--300{degree}F, and to reheat the gases prior to injection into the turbine. The result is significant losses in efficiency for the overall power cycle. High-temperature coal gas cleanup in the IGCC system can be operated near 1000{degree}F or higher, i.e., at conditions compatible with the gasifier and turbine components, resulting is a more efficient overall system. GE is developing a moving-bed, high-temperature desulfurization system for IGCC power systems in which mixed-metal oxides are currently being used as desulfurization sorbents. The objective of this contract is to identify and test fabrication methods and sorbent chemical compositions that enhance the long-term chemical reactivity and mechanical durability of zinc ferrite and other novel sorbents for moving-bed, high-temperature desulfurization of coal-derived gases. Zinc ferrite was studied under the base program of this contract. In the next phase of this program novel sorbents, particularly zinc titanate-based sorbents, are being studied under the remaining optional programs. This topical report summarizes only the work performed under the Option 2 program. In the course of carrying out the program, more than 25 zinc titanate formulations have been prepared and characterized to identify formulations exhibiting enhanced properties over the baseline zinc titanate formulation selected by the US Department of Energy.

  4. Mechanistic and kinetic studies of high-temperature coal gas desulfurization sorbents. Final report, July 1988--July 1991

    SciTech Connect

    Lew, S.; Flytzani-Stephanopoulos, M.; Sarofim, A.F.

    1991-10-01

    The overall objective of this project was to investigate the properties of and evaluate mixed oxides of zinc and titanium for hot fuel gas desulfurization. Uncombined ZnO was also investigated as a base case. Detailed investigation of the reduction and sulfidation reactions of Zn-Ti-O sorbents was performed. The intrinsic kinetics and the product layer diffusion rates in reduction and sulfidation were determined. Kinetic experiments with sorbents containing various Zn/Ti atomic ratios were performed. Chemical phase and structural transformations were followed by various methods. The results were compared to similar experiments performed with ZnO. The purpose of these experiments was to determine how the presence of titanium dioxide affects the reduction and sulfidation of ZnO. This information would be used to identify and select the sorbent composition that gives the best combination of low reduction rate and acceptable sulfidation performance at temperatures exceeding 600{degree}C. (VC)

  5. Enhanced durability for high-temperature desulfurization sorbents for moving-bed applications -- Option 3 program: Development and testing of additional zinc titanate sorbents. Final report, September 1992--May 1996

    SciTech Connect

    Ayala, R.E.; Chuck, T.L.

    1996-12-31

    GE is developing a moving-bed, high-temperature desulfurization system for the integrated gasification combined-cycle (IGCC) power cycle in which zinc-based regenerable sorbents are currently being used as desulfurization sorbents. Zinc titanate and other zinc-based oxides are being considered as sorbents for use in the Clean Coal Technology Demonstration Program at Tampa Electric Co.`s Polk Power Station. A key to success in the development of high-temperature desulfurization systems is the matching of sorbent properties for the selected process operating conditions, namely, sustainable desulfurization kinetics, high sulfur capacity, and mechanical durability over multiple cycles. Additionally, the sulfur species produced during regeneration of the sorbent must be in a form compatible with sulfur recovery systems, such as sulfuric acid or elemental sulfur processes. The objective of this contract is to identify and test sorbent fabrication methods and chemical compositions that enhance the long-term chemical reactivity and mechanical strength of zinc titanate and other novel sorbents for moving-bed, high-temperature desulfurization of coal-derived gases. A parametric study on the use of calcium sulfate additives to zinc titanate was conducted for zinc titanates having a 2:1 and 1.5:1 zinc-to-titanium molar ratio, and they showed a beneficial effect on crush strength of fresh 2:1 zinc titanate sorbents. In addition, a test procedure was developed to screen sorbent formulations based on resistance to spalling and pellet breakage induced by zinc sulfate formation in the presence of sulfur dioxide and excess oxygen conditions.

  6. Bench-scale demonstration of hot-gas desulfurization technology. First quarterly report, 1997

    SciTech Connect

    1997-07-01

    The U.S. Department of Energy (DOE), Federal Energy Technology Center (FETC), is sponsoring research in advanced methods for controlling contaminants in hot coal gasifier gas (coal-derived fuel-gas) streams of integrated gasification combined-cycle (IGCC) power systems. The hot gas cleanup work seeks to eliminate the need for expensive heat recovery equipment, reduce efficiency losses due to quenching, and minimize wastewater treatment costs. Hot-gas desulfurization research has focused on regenerable mixed-metal oxide sorbents that can reduce the sulfur in coal-derived fuel-gas to less than 20 ppmv and can be regenerated in a cyclic manner with air for multicycle operation. Zinc titanate (Zn{sub 2}TiO{sub 4} or ZnTiO{sub 3}), formed by a solid-state rea of zinc oxide (ZnO) and titanium dioxide (TiO{sub 2}), is currently one of the leading sorbents.

  7. Molecular biological enhancement of coal desulfurization: Cloning and expression of the sulfoxide/sulfone/sulfonate/sulfate genes in Pseudomonads and Thiobacillae. Eleventh quarterly report

    SciTech Connect

    Krawiec, S.

    1992-08-01

    Research continues on desulfurization of coal using microorganisms. Topics reported on this quarter include: desulfurization with N1-36 (presumptively identified as Rhodochrous erythropolis), pulsed-field gel electrophoresis of chromosomal DNA`s of Thiobacillus spp., and fresh isolates with the presumptive capacity to desulfurize dibenzothiophenes.

  8. [TDA`s hot gas desulfurization sorbent]. TDA Inc./FETC CRADA No. 97-F003, final report

    SciTech Connect

    Berry, D.A.

    1997-11-14

    This report describes the results of a Cooperative Research and Development Agreement (CRADA) between TDA Incorporated and the Federal Energy Technology Center (FETC) in Morgantown, West Virginia. The objective of this CRADA was to evaluate the performance of TDA`s hot gas desulfurization (HGD) sorbent for use in fossil fuel gasification processes. This particular sorbent, TNT-MB was developed for use in moving-bed HGD reactors in an integrated gasification combined cycle (IGCC) power plant. Two separate tests were conducted; a 10-cycle test, and a low-temperature scoping test. All 10 cycles absorbed H{sub 2}S for the prescribed 125 minutes without breakthrough. The H{sub 2}S concentration remained below 50 ppmv throughout the 125 minute test period. The sorbent showed an increase in attrition resistance from 1.8% (fresh) to 0.87% (reactor inlet) and 0.64% (reactor outlet) after 10 cycles. The results of an additional attrition test are also contained in this report.

  9. Desulfurization behavior of iron-based sorbent with MgO and TiO{sub 2} additive in hot coal gas

    SciTech Connect

    Weiren Bao; Zong-you Zhang; Xiu-rong Ren; Fan Li; Li-ping Chang

    2009-07-15

    The sulfidation behaviors of iron-based sorbent with MgO and MgO-TiO{sub 2} are studied under different isothermal conditions from 623 to 873 K in a fixed bed reactor. The results of sorbents sulfidation experiments indicate that the sorbents with MgO and TiO{sub 2} additives are more attractive than those without additives for desulfurization of hot coal gas. The sulfur capacity (16.17, 18.45, and 19.68 g S/100 g sorbent) of M1F, M3F, and M5F sorbent containing 1, 3, and 5% MgO, respectively, is obviously bigger than that (15.02 g S/100 g sorbent) of M0F without additive. The feasible sulfidation temperature range for M3F sorbent is 773-873 K. The M3F sorbent is optimally regenerated at the temperature of 873 K, under the gas containing 2% oxygen, 15% steam and N{sub 2}, in the space velocity of 2500 h{sup -1}. The sorbent regenerated is also well performed in the second sulfidation (the effective sulfur capacities of 17.98 g S/100 g sorbents and the efficiency of removal sulfur of 99%). The capacity to remove sulfur decreases with steam content increasing in feeding gas from 0 to 10%, but it can restrain the formation of carbon and iron carbide. The addition of TiO{sub 2} in sorbent can shift the optimal sulfidation temperature lower. The iron-based sorbent with 3% MgO and 10% TiO{sub 2} (MFT) is active to the deep removal of H{sub 2}S and COS, especially in the temperature range of 673-723 K. The sulfur removal capacity of MFT sorbent is 21.60 g S/100 g sorbent. 16 refs., 12 figs., 8 tabs.

  10. Bench-scale development of mild gasification char desulfurization; [Quarterly] report, September 1--November 30, 1993

    SciTech Connect

    Knight, R.A.

    1994-03-01

    This goal of this project is to scale up a process, developed under a previous ICCI grant, for desulfurization of mild gasification char by treatment with hydrogen-rich process-derived fuel gas at 650{degree}--760{degree}C and 7-15 atm. The char can be converted into a low-sulfur metallurgical form coke. In the prior study, IBC-105 coal with 4.0 wt % sulfur was converted to chars with less than 1.0 wt % sulfur in a laboratory-scale batch reactor. The susceptibility of the char to desulfurization was correlated with physicochemical char properties and mild gasification conditions. Acid pretreatment of the coal prior to mild gasification was also shown to significantly enhance subsequent sulfur removal. In this study, IGT is conducting continuous bench-scale tests in a 1-lb/h fluidized-bed reactor to determine the preferred process conditions and obtain steady-state data necessary for process design and scale-up. The desulfurized chars are to be used to produce low-sulfur form coke, which will be evaluated for density, reactivity, and strength properties relevant to utilization in blast furnaces. During the first quarter, 180 lb (82 kg) of IBC-105 coal was obtained and subjected to crushing, and sizing to prepare 49 lb (22 kg) of material for test operation.

  11. KINETICS OF Mn-BASED SORBENTS FOR HOT COAL GAS DESULFURIZATION

    SciTech Connect

    J.J. BERNS; K.A. SADECKI; M.T. HEPWORTH

    1997-09-15

    Mixed manganese oxide sorbents have been investigated for high-temperature removal of hydrogen sulfide (the primary sulfur bearing compound) from hot coal gases. The sorbents were screened by thermodynamic equilibrium considerations for sulfidation. Preliminary experimental work using thermogravimetric analysis (TGA) indicated titania to be a superior substrate than alumina. Four formulations showing superior reactivity in a TGA were then tested in an ambient pressure fixed-bed reactor to determine steady state H 2 S concentrations, breakthrough times and effectiveness of the sorbent when subjected to cyclic sulfidation and regeneration testing. Eight tests were conducted with each test consisting of five cycles of sulfidation and regeneration. Sulfidation occurred at 600 o C using a simulated coal gas at an empty-bed space velocity of approximately 12,000 per hour. Manganese-based sorbents with molar ratios > 1:1 Mn:Substrate were effective in reducing the H 2 S concentration in simulated coal gases to less than 100 ppmv over five cycles. Actual breakthrough time for formulation C6-2-1100 was as high as 73% of breakthrough time based on wt% Mn in sorbent at 600 o C. Regeneration tests determined that loaded pellets can be essentially completely regenerated in an air/steam mixture at 750 o C with minimal sulfate formation. The leading formulation (designated C6-2) from the fixed-bed tests was then further tested under varying sorbent induration temperature, sulfidation temperature and superficial gas velocity. Four tests were conducted with each test consisting of four cycles of sulfidation and regeneration. Results showed that the induration temperature of the sorbent and the reaction temperature greatly affected the H 2 S removal capacity of the sorbent while the superficial gas velocity between 1090 and 1635 cm/min had minimal affect on the sorbent's breakthrough capacity. Testing showed that the sorbent's strength was a strong function of the sorbent induration

  12. Novel dry-desulfurization process using Ca(OH)2/fly ash sorbent in a circulating fluidized bed.

    PubMed

    Matsushima, Norihiko; Li, Yan; Nishioka, Masateru; Sadakata, Masayoshi; Qi, Haiying; Xu, Xuchang

    2004-12-15

    A dry-desulfurization process using Ca(OH)2/fly ash sorbent and a circulating fluidized bed (CFB) was developed. Its aim was to achieve high SO2 removal efficiency without humidification and production of CaSO4 as the main byproduct. The CaSO4 produced could be used to treat alkalized soil. An 83% SO2 removal rate was demonstrated, and a byproduct with a high CaSO4 content was produced through baghouse ash. These results indicated that this process could remove SO2 in flue gas with a high efficiency under dry conditions and simultaneously produce soil amendment. It was shown that NO and NO2 enhanced the SO2 removal rate markedly and that NO2 increased the amount of CaSO4 in the final product more than NO. These results confirmed that the significant effects of NO and NO2 on the SO2 removal rate were due to chain reactions that occurred under favorable conditions. The amount of baghouse ash produced increased as the reaction progressed, indicating that discharge of unreacted Ca(OH)2 from the reactor was suppressed. Hence, unreacted Ca(OH)2 had a long residence time in the CFB, resulting in a high SO2 removal rate. It was also found that 350 degrees C is the optimum reaction temperature for dry desulfurization in the range tested (320-380 degrees C). PMID:15669351

  13. KINETICS OF Mn-BASED SORBENTS FOR HOT COAL GAS DESULFURIZATION

    SciTech Connect

    K.A. SADECKI; M.T. HEPWORTH

    1997-06-15

    Manganese-based sorbents have been investigated for the removal of hydrogen sulfide (the primary sulfur bearing compound) from hot coal gases. Four formulations of Mn-based sorbents were tested in an ambient-pressure fixed-bed reactor to determine steady state H2S concentrations, breakthrough times and effectiveness of the sorbent when subjected to cyclic sulfidation and regeneration testing. In previous reports, the sulfidation and regeneration results from cyclic testing done at 550 and 600 °C were presented. Manganese-based sorbents with molar ratios > 1:1 Mn:Substrate were effective in reducing the H2S concentration in simulated coal gases to less than 100 ppmv over five cycles. Actual breakthrough time for formulation C6-2-1100 was as high as 73% of breakthrough time based on wt% Mn in sorbent at 600 °C. Regeneration tests determined that loaded pellets can be essentially completely regenerated in air/steam mixture at 750 °C with minimal sulfate formation. In this report, the performance of the leading formulation (designated C6-2) was investigated for high temperature removal of H2S from simulated coal-derived fuel gas under varying sorbent induration temperature, reaction temperature, and superficial gas velocity. Sulfidation experiments were performed in an ambient pressure fixed-bed reactor between 500 °C and 600 °C. Four tests were conducted with each test consisting of four cycles of sulfidation and regeneration. Results showed that the induration temperature of the sorbent and the reaction temperature greatly affected the H2S removal capacity of the sorbent while the superficial gas velocity between 1090 and 1635 cm/min had minimal affect on the sorbent's breakthrough capacity. Sorbent also showed 30 to 53% loss of its strength over four cycles of sulfidation and regeneration. The former being sorbent indurated at 1115 °C and the prior being sorbent indurated at 1100 °C.

  14. Scale-up of advanced hot-gas desulfurization sorbents. [Semi-annual report], October 1, 1995--March 31, 1996

    SciTech Connect

    Jothimurugesan, K.; Adeyiga, A.A.; Gangwal, S.K.

    1996-08-01

    The overall objective of this project is to develop regenerable sorbents for hot gas desulfurization in IGCC systems. The specific objective of the project is to develop durable advanced sorbents that demonstrate a strong resistance to attrition and chemical deactivation, and high activity at temperatures as low as 343 {degrees}C(650{degrees}F). A number of formulations will be prepared and screened in a 1/2-inch fixed bed reactor at high pressure (1 to 20 atm) and high temperatures using simulated coal-derived fuel-gases. Screening criteria will include, chemical reactivity, stability, and regenerability over the temperature range of 343{degrees}C to 650{degrees}C. After initial screening, at least 3 promising formulations will be tested for 25-30 cycles of absorption and regeneration. One of the superior formulations with the best cyclic performance will be selected for investigating scale up parameters. The scaled-up formulation will be tested for long term durability and chemical reactivity. Accomplishments for this period are presented for the following tasks: optimization of preparation; investigation of scale-up; and preparation of 100 lb batch.

  15. Testing of zinc titanate desulfurization sorbents for moving-bed applications

    SciTech Connect

    Ayala, R.E.; Gal, E.; Gupta, R.P.

    1993-09-01

    Sorbents developed for moving-bed systems must comply with a minimum of chemical and mechanical durability performance characteristics in order to be considered acceptable for long-term operation. Among the desired properties, a sorbent must have: (1) High chemical reactivity, as measured by the rate of sulfur absorption and the total sulfur loading on the sorbent. (2) High mechanical strength, as measured by the pellet crush strength and the attrition resistance; (3) Suitable pellet morphology, as given by pellet size and shape to promote good bulk flow ability and seasonable porosity to increase reactivity. Formulation 2A1.7M (UCI designation L-3787M) was selected by DOE as the baseline formulation for performance evaluation of Option 3 sorbents. This baseline formulation is a rounded zinc titanate sorbent containing a 2:1 Zn:Ti molar ratio, 1.7% molybdenum (equivalent to 2.5% MoO{sub 3}), and 3% bentonite binder that had been previously tested under the Option 2 program. Zinc titanate sorbents were prepared by UCI as rounded spherical or ellipsoidal pellets. The fabrication procedure is targeted at achieving a balance of mechanical strength (crush strength and attrition resistance) and chemical reactivity by controlling the pellet internal porosity.

  16. Anion-exchange resin-based desulfurization process. Quarterly technical progress report, October 1, 1992--December 31, 1992

    SciTech Connect

    Sheth, A.C.; Dharmapurikar, R.

    1992-12-31

    Under DOE Grant No. DE-FG22-90PC90309, the University of Tennessee Space Institute (UTSI) is contracted to further develop its anion-exchange, resin-based desulfurization concept to desulfurize alkali metal sulfates. From environmental as well as economic viewpoints, it is necessary to remove soluble sulfates from the wastes created by flue gas desulfurization systems. In order to do this economically, a low-cost desulfurization process for spent sorbents is necessary. UTSI`s anion-exchange resin-based desulfurization concept is believed to satisfy these requirements. During the reporting period, October 1, 1992--December 31, 1992, UTSI has completed the batch mode experiments to evaluate the performance enhancement effect caused by organic acids on the resin`s exhaustion efficiency. At present, batch mode experiments are being conducted to locate the position of the CO{sub 3}= and SO{sub 4}= ions in the affinity chart, and also reviewing/assessing the ASPEN Code`s capabilities for use in the development of the Best Process Schematic and related economics.

  17. Advanced sulfur control concepts for hot gas desulfurization technology. Quarterly report, October--December 1994

    SciTech Connect

    Harrison, D.P.

    1995-01-01

    The goal is the development of simpler and economically superior processing of regenerable sorbents used for control of hydrogen sulfide in hot, high-pressure gas streams in advanced power generating systems. The improved processing will produce an elemental sulfur byproduct. Progress during the past quarter was limited by delays in identifying an appropriate analytical instrument for measuring the concentration of sulfur species (S{sub x}(g), H{sub 2}S, and SO{sub 2} in the regeneration product gas. The ability to carry out this analysis on a real-time basis is an important component of the overall project and we feel that a satisfactory gas analysis procedure should be available before forging ahead with other experimental activities. The primary accomplishment, therefore, was the completion and submission of the Task 3 Project Plan. This plan, which assumed a satisfactory solution to sulfur analysis problem, is included in this quarterly report.

  18. Bench-scale testing of novel high-temperature desulfurization sorbents: Final report

    SciTech Connect

    Gangwal, S.K.; Harkins, S.M.; Stogner, J.M.; Woods, M.C.; Rogers, T.N.

    1988-12-01

    Extrudates of regenerable mixed-metal oxide sorbents including zinc ferrite, copper-modified zinc ferrite, zinc titanate, copper aluminate, copper-iron aluminate, and copper manganate were prepared and tested for their potential to remove hydrogen sulfide (H/sub 2/S) from coal gasifier gas in a high-temperature high-pressure (HTHP) fixed-bed reactor. The zinc containing sorbents were found to be more promising than those containing combinations of copper, aluminum, iron, and manganese. Reductions in H/sub 2/S concentration were achieved depending on sorbent, reactor temperature, and steam concentration. The copper-modified zinc ferrite sorbent reduced the H/sub 2/S concentration to less than 1 ppmv at up to 1100/degree/F with 20 volume % steam in the gas. The zinc ferrite sorbent showed no apparent loss in capacity over 15 sulfidation-regeneration cycles but underwent significant strength reduction in a coal-derived gas with 15% or less steam due to soot formation. Zinc titanate exhibited excellent strength and capacity retention at steam levels as low as 5% and temperatures as high as 1350/degree/F. 13 refs., 64 figs., 75 tabs.

  19. Molecular biology of coal bio-desulfurization; Quarterly technical progress report, October 1--December 31, 1990

    SciTech Connect

    Young, K.D.; Gallagher, J.R.

    1991-01-25

    The aim of this project is to use the techniques of molecular genetics to identify, clone, sequence, and enhance the expression of proteins which remove sulfur covalently bound to coal. This includes the movement and expression of these proteins into bacterial species which may be more useful in the industrial application of a biological desulfurization process. This quarter we finalized the initial cloning and sequencing of the dibenzothiophene (DBT) metabolic (``dox``) genes from strain C18. In addition, we constructed several mutations in single dox genes and have begun to dissect the contribution of each gene product in the DBT degradation pathway. Using a probe derived from DNA adjacent to a transposon which inactivated DBT metabolism, the DBT active genes from A15 have been cloned and identified on cosmids. We have also electroporated Thiobacillus ferrooxidans with a plasmid containing a chloramphenicol resistant transposon. Colonies of T. ferrooxidans resistant to chloramphenicol were obtained.

  20. EVALUATION OF DRY SORBENTS AND FABRIC FILTRATION FOR FGD (FLUE GAS DESULFURIZATION)

    EPA Science Inventory

    The report gives results of a study to assess the use of baghouses (fabric filtration) to control air pollutant emissions (particularly SOx) from large utility combustion sources. The assessment included sorbent costs, and system capital, operating, and disposal costs. SO2 would ...

  1. Advanced sulfur control concepts for hot gas desulfurization technology. Quarterly report, January 1995--March 1995

    SciTech Connect

    Harrison, D.P.

    1995-04-01

    Research continued on hot gas desulfurization. Antek Instruments reported success in the use of a quartz capillary tube having a diameter of about 0.005 inches and a length of 6 inches to reduce the pressure of a 600{degrees}C gas stream from 15 atm to 1 atm. This capillary tube will be incorporated into the Antek R-6000 elemental sulfur analyzer; an order was placed for the modified instrument during the latter stages of the quarter. SO{sub 2} and H{sub 2}S analysis will be accomplished by modifying an existing Shimadzu GC-14A gas chromatograph. Repairs to both the electrobalance and the furnace temperature controller were accomplished and a manifold system capable of feeding N{sub 2}, O{sub 2}, H{sub 2}, and H{sub 2}O was constructed. A number of calibration and scoping tests were completed, and atmospheric pressure testing of the regeneration of FeS with O{sub 2}/N{sub 2}, H{sub 2}O/N{sub 2} and O{sub 2}/H{sub 2}O/N{sub 2} atmosphere is scheduled to get underway early in the next quarter. Key components of the reactor system, including the data acquisition computer, furnace and temperature controller, gas feed manifold, high pressure syringe pump, and back pressure regulators, were last used in a fixed-bed reactor study. Primary effort during the quarter was devoted to correcting problems with the data acquisition system and reassembling the components for the high pressure electrobalance. Scoping and calibration testing of this unit is scheduled to get underway early in the following quarter.

  2. Investigation on durability and reactivity of promising metal oxide sorbents during sulfidation and regeneration. Quarterly report, April--June 1995

    SciTech Connect

    Kwon, K.C.

    1995-07-01

    Hot-gas desulfurization for the integrated gasification combined cycle (IGCC) process has been investigated by many researchers to remove effectively hydrogen sulfide with various metal oxide sorbents at high pressures and high temperatures. Metal oxides such as zinc titanate oxides, zinc ferrite oxide, copper oxide, manganese oxide and calcium oxide, were found to be promising sorbents in comparison with other removal methods such as membrane separations and reactive membrane separations. Removal reaction of H{sub 2}S from coal gas mixtures with ZT-4 or other promising sorbents of fine solid particles, and regeneration reaction of sulfur-loaded sorbents will be carried on in a batch reactor or a continuous differential reactor. The objectives of this research project are to find intrinsic initial reaction kinetics for the metal oxide-hydrogen sulfide heterogeneous reaction system, to obtain effects of concentrations of coal gas components such as hydrogen, carbon monoxide, carbon dioxide, oxygen, nitrogen and moisture on equilibrium reaction rate constants of the reaction system at various reaction temperatures and pressures, to identify regeneration kinetics of sulfur-loaded metal oxide sorbents, and to formulate promising metal oxide sorbents for the removal of sulfur from coal gas mixtures. Promising durable metal oxide sorbents of high-sulfur-absorbing capacity will be formulated by mixing active metal oxide powders with inert metal oxide powders and calcining these powder mixtures, or impregnating active metal oxide sorbents on supporting metal oxide matrixes. The Research Triangle Institute, a sub-contractor of this research project, will also prepare promising metal oxide sorbents for this research project, plan experiments on removal of sulfur compounds from coal gases with metal oxide sorbents as well as regeneration of sulfur-loaded metal oxide sorbents, and review experimental results.

  3. Fixed bed testing of a molybdenum-promoted zinc titanate sorbent for hot gas desulfurization

    SciTech Connect

    Mei, J.S.; Gasper-Galvin, L.; Everitt, C.E.; Katta, S.

    1993-09-01

    The experimental test program for the molybdenum-promoted zinc titanate with Zn/Ti ratio of 1.91, consists of two series of test: six half-cycle (sulfidation phase) parametric tests and four multi-cycle (sulfidation and regeneration phase) tests. Results of the parametric tests were utilized to select the optimum conditions for multi-cycle tests. The intent of the multi-cycle test series was to demonstrate durability and regenerability of the molybdenum-promoted zinc titanate sorbent. During the parametric tests, sorbent bed temperature and linear velocity were varied. However, system pressure was fixed at 150 psia (1.03 MPa) for sulfidation test phases and 50 psia (0.34 MPa) for regeneration test phases for both single and multi-cycle tests. Figure 2 shows the effect of gas flow rate and temperature on hydrogen sulfide removal during the half-cycle (sulfidation) parametric tests. Simulated KRW coal gas which contained 15 vol% H{sub 2}, 21 vol% CO, 9.0 vol% H{sub 2}O and 800 ppmv H{sub 2}S was used during the parametric tests. As can be seen from the data, sorbent efficiency and capacity were only weak functions of bed temperature. However, increasing the space velocity substantially reduced sorbent efficiency and capacity as indicated on the rapid breakthrough of H{sub 2}S for the high space velocity. Breakthrough period is defined here as corresponding to H{sub 2}S concentration of 200 ppmv in exit gas.

  4. [Reparation and desulfurization of Na2CO3/straw sorbents for removing SO2 from flue gas].

    PubMed

    Shang, Hongshan; Yang, Fan; Kou, Yuan

    2003-11-01

    A series of SO2 sorbents 5%-90% (mass percent) Na2CO3/straw were prepared by conventional incipient wetness impregnation of straw with an aqueous solution of Na2CO3. It was showed that small particle size (< or = 0.28 mm) of the straw and low flow rate (40 mL/min) of the feed gas favor the removal of SO2, while temperature (70 degrees C-300 degrees C) has little effect on the desulfurization efficiency. Based on XRD, SEM and ATR-IR analysis it can be concluded that the Na2CO3 on the surface of the straw is mainly in an amorphous state. The unique structural features of the straw and its interaction with Na2CO3 lead to the amorphous structure having greater surface area (12.14 m2/g) and pore volume (0.093 cm3/g) with a high loading of Na2CO3. PMID:14768568

  5. INVESTIGATION ON DURABILITY AND REACTIVITY OF PROMISING METAL OXIDE SORBENTS DURING SULFIDATION AND REGENERATION. QUARTERLY AND FINAL REPORT

    SciTech Connect

    K.C. KWON

    1998-08-01

    Hot-gas desulfurization for the integrated gasification combined cycle (IGCC) process has been investigated by many researchers to remove effectively hydrogen sulfide with various metal oxide sorbents at high pressures and high temperatures. Metal oxides such as zinc titanate oxides, zinc ferrite oxide, copper oxide, manganese oxide and calcium oxide, were found to be promising sorbents in comparison with other removal methods such as membrane separations and reactive membrane separations. Some metal oxide sorbents exhibited the quite favorable performance in terms of attrition resistance and sulfur capacity. Experiments on removal reaction of H{sub 2}S from coal gas mixtures with formulated metal oxide sorbents were conducted in a batch reactor or a differential reactor. The objectives of this research project are to formulate promising metal oxide sorbents for removal of sulfur from coal gas mixtures, to find initial reaction kinetics for the metal oxide-hydrogen sulfide heterogeneous reaction system, to obtain effects of hydrogen, nitrogen and moisture on dynamic absorption and equilibrium absorption at various absorption temperatures. Promising durable metal oxide sorbents with high-sulfur-absorbing capacity were formulated by mixing active metal oxide powders with inert metal oxide powders, and calcining these powder mixtures. The Research Triangle Institute (RTI), a sub-contractor of this research project, will also prepare promising metal oxide sorbents for this research project, plan experiments on removal of sulfur compounds from coal gases with metal oxide, and review experimental results.

  6. Bench-scale demonstration of hot-gas desulfurization technology. Quarterly report, October 1 - December 31, 1994

    SciTech Connect

    1994-12-31

    The U.S. Department of Energy (DOE), Morgantown Energy Technology Center (METC), is sponsoring research in advanced methods for controlling contaminants in hot coal gasifier gas (coal gas) streams of integrated gasification combined-cycle (IGCC) power systems. The programs focus on hot-gas particulate removal and desulfurization technologies that match or nearly match the temperatures and pressures of the gasifier, cleanup system, and power generator. The work seeks to eliminate the need for expensive heat recovery equipment, reduce efficiency losses due to quenching, and minimize wastewater treatment costs. Hot-gas desulfurization research has focused on regenerable mixed-metal oxide sorbents which can reduce the sulfur in coal gas to less than 20 ppmv and can be regenerated in a cyclic manner with air for multicycle operation. Zinc titanate (Zn{sub 2}TiO{sub 4} or ZnTiO{sub 3}), formed by a solid-state reaction of zinc (ZnO) and titanium dioxide (TiO{sub 2}), is currently one of the leading sorbents. This report summarizes the highlights and accomplishments of the October slipstream test run of the Zinc Titanate Fluid Bed Desulfurization/Direct Sulfur Recovery Process (ZTFBD/DSRP) Mobile Laboratory at the Department of Energy`s Morgantown Energy Technology Center. Although the run had to be shortened due to mechanical problems with METC`s gasifier, there was sufficient on-stream time to demonstrate highly successful operation of both the zinc titanate fluid bed desulfurization and the DSRP with actual coal gas.

  7. LIFAC sorbent injection desulfurization demonstration project. Final report, volume II: Project performance and economics

    SciTech Connect

    1996-01-01

    This publication discusses the demonstration of the LIFAC sorbent injection technology at Richmond Power and Light`s Whitewater Valley Unit No. 2, performed under the auspices of the U.S. Department of Energy`s (DOE) Clean Coal Technology Program. LIFAC is a sorbent injection technology capable of removing 75 to 85 percent of a power plant`s SO{sub 2} emissions using limestone at calcium to sulfur molar ratios of between 2 and 2.5 to 1. The site of the demonstration is a coal-fired electric utility power plant located in Richmond, Indiana. The project is being conducted by LIFAC North America (LIFAC NA), a joint venture partnership of Tampella Power Corporation and ICF Kaiser Engineers, in cooperation with DOE, RP&L, and Research Institute (EPRI), the State of Indiana, and Black Beauty Coal Company. The purpose of Public Design Report Volume 2: Project Performance and Economics is to consolidate, for public use, the technical efficiency and economy of the LIFAC Process. The report has been prepared pursuant to the Cooperative Agreement No. DE-FC22-90PC90548 between LIFAC NA and the U.S. Department of Energy.

  8. Investigation on durability and reactivity of promising metal oxide sorbents during sulfidation and regeneration. Quarterly report, October--December 1994

    SciTech Connect

    Kwon, K.C.

    1995-01-01

    Hot-gas desulfurization for the integrated gasification combined cycle (IGCC) process has been investigated by many researchers to remove effectively hydrogen sulfide with various metal oxide sorbents at high pressures and high temperatures. Metal oxides such as zinc titanate oxides, zinc ferrite oxide, copper oxide, manganese oxide and calcium oxide, were found to be promising sorbents in comparison with other removal methods such as membrane separations and reactive membrane separations. Some metal oxide sorbents exhibited the quite favorable performance in terms of attrition resistance and sulfur capacity. Removal reaction of H{sub 2}S from coal gas mixtures with ZT-4 or other promising sorbents of fine solid particles, and regeneration reaction of sulfur-loaded sorbents will be carried on in a batch reactor or a continuous differential reactor. The objectives of this research project are to find intrinsic initial reaction kinetics for the metal oxide-hydrogen sulfide heterogeneous reaction system, to obtain effects of concentrations of coal gas components such as hydrogen, carbon monoxide, carbon dioxide, oxygen, nitrogen and moisture on equilibrium reaction rate constants of the reaction system at various reaction temperatures and pressures, to identify regeneration kinetics of sulfur-loaded metal oxide sorbents, and to formulate promising metal oxide sorbent for the removal of sulfur from coal gas mixtures. Promising durable metal oxide sorbents of high-sulfur-absorbing capacity will be formulated by mixing active metal oxide powders with inert metal oxide powders and calcining these powder mixtures, or impregnating active metal oxide sorbents on supporting metal oxide matrixes.

  9. Porous desulfurization sorbent pellets containing a reactive metal oxide and an inert zirconium compound

    SciTech Connect

    Gardner, Todd H.; Gasper-Galvin, Lee D.

    1996-12-01

    Sorbent pellets for removing hydrogen sulfide from coal gas are prepared by combining a reactive oxide, in particular zinc oxide, with a zirconium compound such as an oxide, silicate, or aluminate of zirconium, and an inorganic binder and pelletizing and calcining the mixture. Alternately, the zinc oxide may be replaced by copper oxide or a combination of copper, molybdenum, and manganese oxides. The pellet components may be mixed in dry form, moistened to produce a paste, and converted to pellets by forming an aqueous slurry of the components and spray drying the slurry, or the reactive oxide may be formed on existing zirconium-containing catalyst-carrier pellets by infusing a solution of a salt of the active metal onto the existing pellets and firing at a high temperature to produce the oxide. Pellets made according to this invention show a high reactivity with hydrogen sulfide and durability such as to be useful over repeated cycles of sorption and regeneration.

  10. Desulfurization of coal with hydroperoxides of vegetable oils. [Quarterly] report, September 1--November 30, 1994

    SciTech Connect

    Smith, G.V.; Gaston, R.D.; Song, Ruozhi; Cheng, Jianjun

    1994-12-31

    This project proposes a new method for removing organic sulfur from Illinois coals using readily available farm products. It proposes to use air and vegetable oils to disrupt the coal matrix, oxidize sulfur forms, increase volatiles, and desulfurize coal. This will be accomplished by impregnating coals with polyunsaturated oils, converting the oils to their hydroperoxides, and heating. Since these oils are relatively inexpensive and easily applied, this project could lead to a cost effective method for removing organic sulfur from coals. Moreover, the oils are environmentally safe; they will produce no noxious products and will improve burning qualities of the solid products. Preliminary experiments showed that EBC 104 coal catalyzes the formation of hydroperoxides in safflower oil and that more sulfur is extracted from the treated than untreated coal. During this first quarter the requirement of an added photosensitizer has been eliminated, the catalytic effect of coal has been confirmed, and the existence of a complex set of reactions revealed. These reactions between the oxygen, oil, hydroperoxides, and coal are hydroperoxide formation, which is catalyzed by the coal surface and by heat, an unknown coal-hydroperoxide reaction, and oil polymerization. Additionally, diffusion phenomena must be playing a role because oil polymerization occurs, but the importance of diffusion is difficult to assess because less polymerization occurs when coal is present. The first task has been completed and we are now ready to determine the ability of linseed oil hydroperoxides to oxidize organic sulfur in EBC 108 coal.

  11. A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report 17, July--September 1993

    SciTech Connect

    Harrison, D.P.

    1993-10-01

    Phase II research involves a scale-up from microgram to gram quantities of sorbent and a switch from the electrobalance reactor to a fixed-bed reactor with capability for feed and product gas analysis. Parameters being studied in Phase II are essentially the same as in Phase I. The reactor response is being studied as a function of calcination and carbonation temperature and pressure, composition of the calcination and carbonation feed gas, and space velocity during the carbonation cycle. Multicycle tests are also being conducted to extend the information on sorbent durability. During the current quarter, reactor modifications to permit easier addition and removal of sorbent to and from the reactor were accomplished. It is now possible to remove sorbent after a run in discrete axial sections which will permit characterization of the sorbent as a function of axial position. Tracer response tests in which the chromatograph response to step function injections of hydrogen to flowing nitrogen under non-reactive conditions were carried out to evaluate the lag time between feeding reactive gases to the reactor and their appearance in the product gas sample. Fourteen additional calcination/carbonation reaction tests were completed this quarter, and the effects of carbonation background gas composition, sorbent particle size, calcination temperature, calcination gas flow rate, and calcination gas composition were studied. In addition, the first multicycle test involving complete calcination/carbonation cycles was carried out.

  12. Advanced sulfur control concepts in hot-gas desulfurization technology. Quarterly report, October 1--December 31, 1997

    SciTech Connect

    Harrison, D.P.

    1997-12-31

    This quarter, the authors turned their attention to sorbent durability studies by beginning a multicycle run. By the end of the quarter, nineteen complete cycles had been completed with little or no evidence of sorbent deactivation. Prebreakthrough H{sub 2}S concentrations below the thermal conductivity detector limit of about 100 ppmv were achieved in all cycles. The time, t{sub 0.5}, required for the H{sub 2}S concentration in the product gas to reach 0.5% (50% of the inlet concentration) varied only between 97 and 106 minutes in the 19 cycles. Significant, t{sub 0.5} for the 19th cycle was 103 minutes, among the largest of all cycles. SO{sub 2} breakthrough during regeneration showed similar good reproducibility. t{sub 0.5} for regeneration only varied between 20.6 and 22.9 minutes. The concentration of elemental sulfur (considered as S{sub 2}) in the product gas exceeded 10% for more than 15 minutes in each cycle. By the end of December, the sorbent had been exposed continuously to temperatures ranging from 600 to 800 C for more than one month in gas compositions ranging from 100% H{sub 2} to air, and from 1% H{sub 2}S/10% H{sub 2}N{sub 2} to 12% SO{sub 2}/N{sub 2}. Between regeneration and sulfidate, the system was purged by nitrogen. The sorbent was at the highest temperature of 800 for about 90% of that time. These sorbent durability results are considered to be quite favorable.

  13. A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report 19, January--March, 1994

    SciTech Connect

    Harrison, D.P.

    1994-04-01

    This research project is investigating the technical feasibility of a high-temperature, high-pressure (HTHP) process for the bulk separation of CO{sub 2} from coal-derived gas. Indirect evidence which suggested that the water-gas shift reaction occurred simultaneously with CO{sub 2} removal was found. Occurrence of the simultaneous reactions created the possibility of a direct one-step process for the manufacture of hydrogen from coal-gas while at the same time separating a concentrated stream of CO{sub 2}. Previous quarterly reports have described the design, construction, and commissioning of the fixed-bed reactor, development of analytical procedures, and results of a number of tests using dolomite sorbent precursor. During the current quarter, additional tests were carried out to study the effects of calcination gas composition, temperature, and space velocity using the standard dolomite sorbents. Alternate sorbents were tested to provide direct comparison of dolomite and limestone performance. Tests were performed using an empty reactor and reactor packed with commercial shift catalyst to learn more of the characteristics of the shift reaction in the absence of carbonation. Toward the end of the quarter, emphasis changed to sorbent durability and a number of multicycle tests were completed.

  14. Novel sorbents for high temperature regenerative H/sub 2/S removal. Quarterly report No. 4, November 1984-January 1985

    SciTech Connect

    Flytzani-Stephanopoulos, M.; Gavalas, G.R.; Sharma, P.K.

    1985-03-01

    The overall objective of this program is to develop improved regenerable sorbents for the high-temperature desulfurization of coal-derived gas streams. The aim is to reduce the H/sub 2/S level, preferably in a single stage, from a few percent down to 1 ppM. The specific objectives of this project are to synthesize, characterize and test two classes of sorbents. One consists of eutectic mixtures of metal oxides (e.g., ZnO-V/sub 2/O/sub 5/, CuMoO/sub 4/-MoO/sub 3/) in the form of a melt coating the pore surface of a high surface area solid support. The second class of sorbents includes unsupported mixed oxides, in the form of solid solutions or solid compounds, e.g., Zn-Fe/sub x/-O/sub y/, Cu-Fe/sub x/-O/sub y/, prepared as highly dispersed microcrystalline solids. The principal characteristics of both classes of sorbents are rapid kinetics of absorption, high absorption capacity and good regenerability. During this reporting period, parametric studies of sulfidation/regeneration with the mixed oxide sorbents CFA (Cu-Fe-Al-O) and CM (Cu-Mo-Al-O) both prepared in porous, microcrystalline form were performed. These two types of sorbents were identified in our previous work as very efficient, high performance materials for single-stage H/sub 2/S removal at temperatures higher than 600/sup 0/C. Experimental procedures and results are discussed. 15 refs., 4 figs., 4 tabs.

  15. LIFAC sorbent injection desulfurization demonstration project. Quarterly report No. 3, April--June 1991

    SciTech Connect

    Not Available

    1991-12-31

    LIFAC combines upper-furnace limestone injection followed by post-furnace humidification in an activation reactor located between the air preheater and the ESP. The process produces a dry and stable waste product that is partially removed from the bottom of the activation reactor and partially removed at the ESP.

  16. LIFAC Sorbent Injection Desulfurization Demonstration Project. Quarterly report No. 5, October--December 1991

    SciTech Connect

    Not Available

    1991-12-31

    LIFAC combines upper-furnace limestone injection followed by post- furnace humidification in an activation reactor located between the air preheater and the ESP. The process produces a dry and stable waste product that is partially removed from the bottom of the activation reactor and partially removed at the ESP. In November 1990, after a ten (10) month negotiation period, LIFAC NA and the US DOE entered into a Cooperative Agreement for the design, construction, and demonstration of the LIFAC system. This report is the fifth Technical Progress Report covering the period October 1, 1991 through the end of December 1991. Due to the power plant`s planned outage schedule, and the time needed for engineering, design and procurement of critical equipment, DOE and LIFAC NA agreed to execute the Design Phase of the project in August 1990, with DOE funding contingent upon final signing of the Cooperative Agreement.

  17. Bench-scale demonstration of hot-gas desulfurization technology. Quarterly report, January 1--March 31, 1998

    SciTech Connect

    1998-12-31

    At the start of the current project, the DSRP (Direct Sulfur Recovery Process) technology was at the bench-scale development stage with a skid-mounted system ready for field testing. The process had been extended to fluidized-bed operation in the Stage 1 reactor. A preliminary economic study for a 100 MW plant in which the two-stage DSRP was compared to conventional processes indicated the economic attractiveness of the DSRP. Through bench-scale development, both fluidized-bed zinc titanate and DSRP technologies have been shown to be technically and economically attractive. The demonstrations prior to the start of this project, however, had only been conducted using simulated (rather than real) coal gas and simulated regeneration off-gas. Thus, the effect of trace contaminants in real coal gases on the sorbent and DSRP catalyst was not known. Also, the zinc titanate desulfurization unit and DSRP had not been demonstrated in an integrated manner. The overall goal of this project is to continue further development of the zinc titanate desulfurization and DSRP technologies by scale-up and field testing (with actual coal gas) of the zinc titanate fluidized-bed reactor system, and the Direct Sulfur Recovery Process.

  18. Performance of a novel synthetic Ca-based solid sorbent suitable for desulfurizing flue gases in a fluidized bed

    SciTech Connect

    Pacciani, R.; Muller, C.R.; Davidson, J.F.; Dennis, J.S.; Hayhurst, A.N.

    2009-08-05

    The extent and mechanism of sulfation and carbonation of limestone, dolomite, and chalk, were compared with a novel, synthetic sorbent (85 wt % CaO and 15 wt % Ca{sub 12}A{sub l14}O{sub 33}), by means of experiments undertaken in a small, electrically heated fluidized bed. The sorbent particles were used either (I) untreated, sieved to two particle sizes and reacted with two different concentrations of SO{sub 2}, or (ii) after being cycled 20 times between carbonation, in 15 vol % CO{sub 2} in N2, and calcination, in pure N2, at 750 degrees C. The uptake of untreated limestone and dolomite was generally low (<0.2 g(SO{sub 2})/g(sorbent)), confirming previous results, However, the untreated chalk and the synthetic sorbent were found to be substantially more reactive with SO{sub 2}, and their final uptake was significantly higher (>0.5 g(SO{sub 2})/g(sorbent)) and essentially independent of the particle size. Here, comparisons are made on the basis of the sorbents in the calcined state. The capacities for the uptake of SO{sub 2}, on a basis of unit mass of calcined sorbent, were comparable for the chalk and the synthetic sorbent. However, previous work has demonstrated the ability of the synthetic sorbent to retain its capacity for CO{sub 2} over many cycles of carbonation and calcination: much more so than natural sorbents such as chalk and limestone. Accordingly, the advantage of the synthetic sorbent is that it could be used to remove CO{sub 2} from flue gases and, at the end of its life, to remove SO{sub 2} on a once-through basis.

  19. DEVELOPMENT AND PILOT PLANT EVALUATION OF SILICA-ENHANCED LIME SORBENTS FOR DRY FLUE GAS DESULFURIZATION (JOURNAL VERSION)

    EPA Science Inventory

    The paper discusses recent work on lime enhancement and testing at the bench-scale, followed by evaluation of the more promising sorbents in a pilot plant to develop low cost, retrofittable flue gas cleaning technology specifically the development of highly reactive sorbents. Con...

  20. Management of dry flue gas desulfurization by-products in underground mines. Quarterly report, October 1--December 31, 1995

    SciTech Connect

    1997-05-01

    On September 30, 1993, the U.S. Department of Energy - Morgantown Energy Technology Center (DOE-METC) and Southern Illinois University at Carbondale (SITJC) entered into a cooperative research agreement entitled {open_quotes}Management of Dry Flue Gas Desulfurization By-Products in Underground Mines{close_quotes} (DE-FC21-93MC-30252). Under the agreement SIUC will develop and demonstrate two technologies for the placement of coal combustion by-products in abandoned underground coal mine workings, and assess the environmental impact of such underground placements. This report discusses the technical progress achieved during the period October 1 - December 31, 1995. Rapid Aging Test columns were placed in operation during the second quarter of 1995, and some preliminary data were acquired during this quarter. These data indicate that the highly caustic pH is initially generated in the pneumatic mix, but that such pH is short lived. The initial pH rapidly declines to the range of 8 to 9. Leachates in this pH range will have little or no effect on environmental concerns. Dedicated sampling equipment was installed in the groundwater monitoring wells at the proposed placement site at the Peabody Number 10 mine. Also, the groundwater monitoring wells were {open_quotes}developed{close_quotes} during the quarter to remove the fines trapped in the sand pack and screen. A new procedure was used in this process, and proved successful. A series of tests concerning the geotechnical characteristics of the pneumatic mixes were conducted. Results show that both moisture content and curing time have a direct effect on the strength of the mixes. These are, of course, the expected general results. The Christmas holidays and the closing of the University during an extended period affected the progress of the program during the quarter. However, the program is essentially on schedule, both technically and fiscally, and any delays will be overcome during the first quarter of 1996.

  1. Investigation on durability and reactivity of promising metal oxide sorbents during sulfidation and regeneration. Quarterly report, July 1 - September 30, 1995

    SciTech Connect

    1995-12-31

    Hot-gas desulfurization for the integrated gasification combined cycle process has been investigated by many to remove effectively hydrogen sulfide with various metal oxide sorbents at high pressures and high temperatures. Metal oxides such as zinc titanate oxides, zinc ferrite oxide, copper oxide, manganese oxide and calcium oxide, were found to be promising sorbents in comparison with other removal methods such as membrane separations and reactive membrane separations. Some metal oxide sorbents exhibited the quite favorable performance in terms of attrition resistance and sulfur capacity. Removal reaction of H{sub 2}S from coal gas mixtures with ZT-4 or other promising sorbents of fine solid particles, and regeneration reaction of sulfur-loaded sorbents will be carried on in a batch reactor or a continuous differential reactor. The objectives of this project are to find intrinsic initial reaction kinetics for the metal oxide-hydrogen sulfide heterogeneous reaction system, to obtain effects of concentrations of coal gas components such as hydrogen, carbon monoxide, carbon dioxide, nitrogen and moisture on equilibrium reaction rate constants of the reaction system at various reaction temperatures and pressures, to identify regeneration kinetics of sulfur-loaded metal oxide sorbents, and to formulate promising metal oxide sorbents for the removal of sulfur from coal gas mixtures. Promising durable metal oxide sorbents of high-sulfur- absorbing capacity will be formulated by mixing active metal oxide powders with inert metal oxide powders and calcining these powder mixtures, or impregnating active metal oxide sorbents on supporting metal oxide matrixes. The Research Triangle Institute will also prepare promising metal oxide sorbents for this research project, plan experiments on removal of sulfur compounds from coal gases with metal oxide sorbents as well as regeneration of sulfur-loaded metal oxide sorbents, and review experimental results. 1 ref., 10 figs., 11 tabs.

  2. Molecular biology of coal bio-desulfurization; Quarterly technical progress report, January 1, 1991--March 31, 1991

    SciTech Connect

    Young, K.D.; Gallagher, J.R.

    1991-04-17

    The aim of this project is to use the techniques of molecular genetics to identify, clone, sequence, and enhance the expression of proteins which remove sulfur covalently bound to coal. This includes the movement and expression of these proteins into bacterial species which may be more useful in the industrial application of a biological desulfurization process. This quarter, several mutants were constructed to inactivate specific cloned C18 dox genes. These mutants were consistent with the phenotypes expected if these genes participated in an oxidative degradation DBT. The dox genes from strain A15 have been isolated in several cosmid clones, one of which can transfer the DBT metabolic trait to our laboratory Pseudomonas strain. DBT desulfurizing strains of Rhodococcus rhodochrous (IGTS8 and IGTS85) were obtained. Bioavailability assays confirmed the ability of these isolates to remove sulfur from DBT. Several mutants of IGTS8 were isolated that had lost the ability to use DBT as a sole sulfur source. These mutants were investigated as preferred recipients of the gene libraries. Multiple trials are underway to discover a mechanism by which DNA can be successfully introduced into the Rhodococcus strains. 1 tab.

  3. Advanced sulfur control concepts in hot-gas desulfurization technology. Quarterly report, January 1--March 31, 1998

    SciTech Connect

    Harrison, D.P.

    1998-08-01

    The last six cycles of a 25-cycle sorbent durability test were completed, final installation of the flame photometric detector was accomplished, and fifteen tests whose aim was to determine the minimum prebreakthrough H{sub 2}S concentration over reduced CeO{sub 2} were performed. There was little, if any, evidence of sorbent deterioration in the durability test. During the durability test the author confirmed that, when using pre-reduced sorbent and a clean system, the prebreakthrough H{sub 2}S concentration was less than 100 ppmv, the detection limit of the thermal conductivity detector (TCD). Consequently, a more sensitive flame photometric detector (FPD) which permitted measurements of H{sub 2}S concentrations of 1 ppmv or less was installed. The FPD and TCD were connected in parallel so that, when desired, the entire H{sub 2}S breakthrough curve could be measured. Most of the quarter was devoted to conducting reduction-sulfidation tests to determine the minimum prebreakthrough H{sub 2}S concentrations which could be achieved using prereduced CeO{sub 2}. Fifteen runs involving variations in reduction-sulfidation temperature, H{sub 2}S concentration in the feed gas, and feed gas volumetric flow rate were completed. In all tests the prebreakthrough H{sub 2}S concentration was less than 10 ppmv, and in many of the tests the H{sub 2}S concentration was equal to or less than 1 ppmv for an extended time period.

  4. Hot coal gas desulfurization with manganese-based sorbents. Progress report, April 1, 1993--June 30, 1993

    SciTech Connect

    Hepworth, M.T.

    1993-07-15

    Focus of work is primarily in use of zinc ferrite and zinc titanate sorbents; however, an alternate sorbent, manganese dioxide-containing ore in mixture with alumina (75 wt % ore + 25 wt % Al{sub 2}O{sub 3}) may be a viable alternative to zinc-based sorbents. Manganese, for example, has a lower vapor pressure in the elemental state than zinc, hence it is not as likely to undergo depletion from the sorbent surface upon loading and regeneration cycles. Also manganese oxide is less readily reduced to the elemental state than iron hence the range of reduction potentials for oxygen is somewhat greater than for zinc ferrite. Thermodynamic analysis of the system shows it to be less amenable to sulfation than zinc ferrite. Potential also exists for utilization of manganese higher temperatures than zinc ferrite or titanate. This report gives the thermodynamic background for consideration of manganese-based sorbents as an alternative to zinc ferrite. To date the work is limited to thermogravimetric testing of four formulations of manganese-alumina sorbents to determine the optimum conditions of pelletization and enduration to produce reactive pellets.

  5. Kinetics of MN-based sorbents for hot coal gas desulfurization. Semiannual report, December 15, 1996--March 15, 1997

    SciTech Connect

    Hepworth, M.T.

    1997-03-01

    Manganese-based sorbents have been investigated for the removal of hydrogen sulfide (the primary sulfur bearing compound) from hot coal gases prior to its use in combined cycle turbines. Four formulations of Mn-based sorbents were tested in an ambient-pressure fixed-bed reactor to determine steady state H{sub 2}S concentrations, breakthrough times and effectiveness of the sorbent when subjected to cyclic sulfidation and regeneration testing. In previous reports, the sulfidation and regeneration results from cyclic testing done at 600{degrees}C were presented. Manganese-based sorbents with molar ratios >1:1 Mn:substrate were effective in reducing the H{sub 2}S concentration in simulated coal gases to less than 100 ppmv over five cycles. Actual breakthrough time for formulation C6-2-1100 was as high as 73% of breakthrough time based on wt% Mn in sorbent. Regeneration tests determined that loaded pellets can be fully regenerated in air/steam mixture at 750{degrees}C with minimal sulfate formation. In this report, the results from the cyclic crush strength tests, sulfur profile test, and cyclic testing done after 5 cycles showed decreases in strength from 12.6% to 57.9%. Cyclic testing at 550{degrees}C showed pre-breakthrough concentrations as low as 10 ppmv. Cyclic testing done at 2 L/min and 3 L/min did not show any significant difference in pre-breakthrough concentrations or capacity.

  6. Enzymatic desulfurization of coal. Second quarterly report, October 1--December 15, 1988

    SciTech Connect

    Marquis, J.K.; Kitchell, J.P.

    1988-12-15

    Our current efforts to develop clean coal technology emphasize the advantages of enzymatic desulfurization techniques and have specifically addressed the potential of using partially-purified extracellular microbial enzymes or commercially available enzymes. Our work is focused on the treatment of ``model`` organic sulfur compounds such as dibenzothiophene (DBT) and ethylphenylsulfide (EPS). Furthermore, we are designing experiments to facilitate the enzymatic process by means of a hydrated organic solvent matrix.

  7. Enzymatic desulfurization of coal. Fourth quarterly report, March 16--June 15, 1989

    SciTech Connect

    Boyer, Y.N.; Crooker, S.C.; Kitchell, J.P.; Nochur, S.V.; Marquis, J.K.

    1989-06-16

    Our current efforts to develop clean coal technology emphasize the advantages of enzymatic desulfurization techniques and have specifically addressed the potential of using partially-purified extracellular microbial enzymes as well as commercially available enzymes. Our work is focused on the treatment of ``model`` organic sulfur compounds such as dibenzothiophene (DBT) and ethylphenylsulfide (EPS). Furthermore, we are designing experiments to facilitate the enzymatic process by means of a hydrated organic solvent matrix.

  8. Enzymatic desulfurization of coal. First quarterly report, May 5--September 30, 1988

    SciTech Connect

    Marquis, J.K.; Kitchell, J.P.

    1988-10-07

    Our current efforts to develop clean coal technology, emphasize the advantages of enzymatic desulfurization techniques and have specifically addressed the potential of using partially-purified extracellular microbial enzymes or commercially available enzymes. Our work is focused on the treatment of ``model`` organic sulfur compounds such as dibenzothiophene (DBT) and ethylphenylsulfide (EPS). Furthermore, we are designing experiments to facilitate the enzymatic process by means of a hydrated organic solvent matrix.

  9. Desulfurization of coal: enhanced selectivity using phase transfer catalysts. Quarterly report, March 1 - May 31, 1996

    SciTech Connect

    Palmer, S.R.; Hippo, E.J.

    1996-12-31

    Due to environmental problems related to the combustion of high sulfur Illinois coal, there continues to be interest in the development in viable pre-combustion desulfurization processes. Recent studies by the authors have obtained very good sulfur removals but the reagents that are used are too expensive. Use of cheaper reagents leads to a loss of desired coal properties. This study investigated the application phase transfer catalysts to the selective oxidation of sulfur in coal using air and oxygen as oxidants. The phase transfer catalyst is expected to function as a selectivity moderator by permitting the use of milder reaction conditions that otherwise necessary. This would enhance the sulfur selectivity and help retain the heating value of the coal. The use of certain coal combustion wastes for desulfurization, and the application of cerium (IV) catalyzed air oxidation for selective sulfur oxidation are also being studied. If successful, this project could lead to the rapid development of a commercially viable desulfurization process. This would significantly improve the marketability of Illinois coal.

  10. An attrition-resistant zinc titanate sorbent for sulfur. [Quarterly] technical report, March 1, 1993--May 31, 1993

    SciTech Connect

    Swisher, J.H.

    1993-09-01

    In the continuing search for good sorbent materials to remove sulfur from hot, coal-derived gases, zinc titanate sorbents have shown great promise. The objective of this project is to extend the work of prior investigators by developing improvements in the compressive strength and, therefore, the cycle life of these sorbents without a significant loss in chemical reactivity. During the third quarter, the preparation and properties of sorbents with a nominal composition of 50% Zn{sub 2}TiO{sub 4} and 50% TiO{sub 2} were studied. In differential thermogravimetric tests of reactivity, specimens sintered at 850 and 900{degrees}C both gave two identical sulfidation-regeneration cycles. Specimens sintered at lower temperatures showed evidence of degradation during the second cycle. Materials of this composition had lower crush strengths than for the composition 75% Zn{sub 2}TiO{sub 4} -- 25% TiO{sub 2} reported earlier, but higher values than reported by other investigators. Future work will include the preparation and properties of a lot of material with a coarser structure and larger pores, and microscopic studies on all three lots of material.

  11. Management of dry flue gas desulfurization by-products in underground mines. Quarterly report, October--December 1994

    SciTech Connect

    Chugh, Y.; Dutta, D.; Esling, S.; Ghafoori, N.; Paul, B.; Sevim, H.; Thomasson, E.

    1995-01-01

    On September 30, 1993, the US Department of Energy, Morgantown Energy Technology Center and Southern Illinois University at Carbondale (SIUC) entered into a cooperative agreement entitled ``Management of Dry Flue Gas Desulfurization By-Products in Underground Mines`` (DE-FC21-93MC30252). Under the agreement, Southern Illinois University at Carbondale will develop and demonstrate several technologies for the placement of coal combustion residues in abandoned coal mines, and will assess the environmental impact of such underground residues placement. The major event during the quarter was the demonstration of the SEEC, Inc. technology for loading and transporting coal combustion residues in the SEEC developed Collapsible Intermodal Containers (CIC). The demonstration was held on November 17, 1994, at the Illinois Power Company Baldwin power plant, and was attended by about eighty (80) invited guest. Also during the quarter meetings were held with Peabody Coal Company officials to finalize the area in the Peabody No. 10 mine to be used for the placement of coal combustion residues. Work under the Materials Handling and Systems Economics area continued, particularly in refining the costs and systems configuration and in economic evaluation of various systems using equipment leasing rather than equipment purchases. Likewise, work progressed on residues characterization, with some preparations being made for long-term testing.

  12. Desulfurization of coal with hydroperoxides of vegetable oils. [Quarterly progress report], December 1, 1994--February 28, 1995

    SciTech Connect

    Smith, G.V.; Gaston, R.D.; Song, Ruozhi; Cheng, Jianjun; Shi, Feng; Gholson, K.L.; Ho, K.K.

    1995-12-31

    This project proposes a new method for removing organic sulfur from Illinois coals using readily available farm products. It proposes to use air and vegetable oils to disrupt the coal matrix, oxidize sulfur forms, increase volatiles, and desulfurize coal. This will be accomplished by impregnating coals with polyunsaturated oils, converting the oils to their hydroperoxides, and heating. Since these oils are relatively inexpensive and easily applied, this project could lead to a cost effective method for removing organic sulfur from coals. Moreover, the oils are environmentally safe; they will produce no noxious products and will improve burning qualities of the solid products. Preliminary experiments showed that IBC 104 coal catalyzes the formation of hydroperoxides in safflower oil and that more sulfur is extracted from the treated than untreated coal. During the first quarter the requirement of an added photosensitizer was eliminated, the catalytic effect of coal was confirmed, and the existence of a complex set of reactions was revealed. During this second quarter working with IBC-108 coal (2.3% organic S. 0.4% pyrite S), the effects of different ratios of oil:coal, different extraction solvents, and different temperatures were examined. A new pretreatment which combines alkali with linseed oil was discovered. Best organic sulfur removal is approximately 26% using alkali pretreatment combined with linseed oil at 1OO{degree}C. BTU loses can be kept to a minimum of 3% with proper use of solvents.

  13. Management of dry flue gas desulfurization by-products in underground mines. Quarterly technical progress report, April 1995--June 1995

    SciTech Connect

    Chugh, Y.P.; Dutta, D.; Esling, S.

    1995-07-01

    On September 30, 1993, the U.S. Department of Energy-Morgantown Energy Technology Center and Southern Illinois University at Carbondale (SIUC) entered into a cooperative research agreement entitled {open_quotes}Management of Dry Flue Gas Desulfurization By-Products in Underground Mines{close_quotes} (DE-FC21-93MC30252). Under the agreement Southern Illinois University at Carbondale will develop and demonstrate several technologies for the placement of coal combustion residues in abandoned coal mines, and will assess the environmental impact of such underground residues placement. Previous quarterly Technical Progress Reports have set forth the specific objectives of the program, and a discussion of these is not repeated here. Rather, this report discusses the technical progress made during the period April 1 - June 30, 1995. A final topical report on the SEEC, Inc. demonstration of its technology for the transporting of coal combustion residues was completed during the quarter, although final printing of the report was accomplished early in July, 1995. The SEEC technology involves the use of Collapsible Intermodal Containers (CIC`s) developed by SEEC, and the transportation of such containers - filled with fly ash or other coal combustion residues - on rail coal cars or other transportation means. Copies of the final topical report, entitled {open_quotes}The Development and Testing of Collapsible Intermodal Containers for the Handling and Transport of Coal Combustion Residues{close_quotes} were furnished to the Morgantown Energy Technology Center. The Rapid Aging Test colums were placed in operation during the quarter. This test is to determine the long-term reaction of both the pneumatic and hydraulic mixtures to brine as a leaching material, and simulates the conditions that will be encountered in the actual underground placement of the coal combustion residues mixtures. The tests will continue for about one year.

  14. Reduction of spalling in mixed metal oxide desulfurization sorbents by addition of a large promoter metal oxide

    DOEpatents

    Poston, James A.

    1997-01-01

    Mixed metal oxide pellets for removing hydrogen sulfide from fuel gas mixes derived from coal are stabilized for operation over repeated cycles of desulfurization and regeneration reactions by addition of a large promoter metal oxide such as lanthanum trioxide. The pellets, which may be principally made up of a mixed metal oxide such as zinc titanate, exhibit physical stability and lack of spalling or decrepitation over repeated cycles without loss of reactivity. The lanthanum oxide is mixed with pellet-forming components in an amount of 1 to 10 weight percent.

  15. Reduction of spalling in mixed metal oxide desulfurization sorbents by addition of a large promoter metal oxide

    DOEpatents

    Poston, J.A.

    1997-12-02

    Mixed metal oxide pellets for removing hydrogen sulfide from fuel gas mixes derived from coal are stabilized for operation over repeated cycles of desulfurization and regeneration reactions by addition of a large promoter metal oxide such as lanthanum trioxide. The pellets, which may be principally made up of a mixed metal oxide such as zinc titanate, exhibit physical stability and lack of spalling or decrepitation over repeated cycles without loss of reactivity. The lanthanum oxide is mixed with pellet-forming components in an amount of 1 to 10 weight percent.

  16. Advanced sulfur control concepts in hot-gas desulfurization technology. Quarterly report, April 1--June 30, 1998

    SciTech Connect

    Harrison, D.P.

    1998-09-01

    Twenty-five reduction/sulfidation tests plus one sulfidation/regeneration test were completed during the quarter. The reduction/sulfidation tests examined the behavior of six cerium oxide sorbents from different sources with reaction variables of temperature, pressure, gas composition and flow rate. Most significantly, steam was added to the sulfidation feed gas for the first time. Tests using pre-reduced sorbents and tests in which reduction and sulfidation occurred simultaneously were performed. Prebreakthrough H{sub 2}S concentrations less than 10 ppmv were obtained over a range of reaction conditions with prebreakthrough concentrations as low as 1 ppmv achieved at the most favorable conditions. The general response to reaction variables was as expected except when feed rate was varied. In some of these cases the FPD breakthrough time did not correspond to expectation. The single regeneration run was conducted at 600 C and 2 atm using 12% SO{sub 2} in N{sub 2} at a feet rate of 400 sccm. This was the first regeneration test at other than 1 atm pressure; favorable results were obtained. The only experimental objective remaining is additional high pressure regeneration testing.

  17. Cross-flow, filter-sorbent catalyst for particulate, SO{sub 2} and NO{sub x} control. Seventh quarterly technical progress report

    SciTech Connect

    Benedek, K.; Flytzani-Stephanopoulos, M.

    1992-01-01

    This report describes work performed on a new concept for integrated pollutant control: a cross-flow filter comprised of layered, gas permeable membranes that act as a particle filter, an SO {sub 2} sorbent, and a NO {sub x} reduction catalyst. One critical element of the R&D program is the development of mixed metal oxide materials that serve as combined SO {sub 2} sorbents and NO {sub x} reduction catalysts. In this seventh quarterly progress report, we summarize the performance characteristics of three promising sorbent/catalyst materials tested in powder form.

  18. Modification of ZnO-TiO{sub 2} high-temperature desulfurization sorbent by ZrO{sub 2} addition

    SciTech Connect

    Sasaoka, Eiji; Sada, Norimasa; Manabe, Akifumi; Uddin, M.A.; Sakata, Yusaku

    1999-03-01

    To develop a highly reactive and easily regenerable zinc oxide high-temperature desulfurization sorbent, a modification of ZnO-TiO{sub 2} by addition of ZrO{sub 2} was studied. The metal oxides ZnO-TiO{sub 2}-ZrO{sub 2} were prepared by a coprecipitation method: the amount of ZnO was a fixed 50 mol % of the sample. In this study, it was found that the addition of 5 or 10 mol % ZrO{sub 2} to 50 mol % of ZnO-50 mol % TiO{sub 2} greatly improved the reactivity for H{sub 2}S removal. Furthermore, the addition of ZrO{sub 2} improved its regenerability: the temperature for the regeneration of the sample was decreased to ca. 40 C in the absence of H{sub 2}O and ca. 75 C in the presence of 10% H{sub 2}O by the addition of 10% ZrO{sub 2}.

  19. Effects of CO and CO2 on the desulfurization of H2S using a ZnO sorbent: a density functional theory study.

    PubMed

    Ling, Lixia; Zhao, Zhongbei; Wang, Baojun; Fan, Maohong; Zhang, Riguang

    2016-04-20

    The density functional theory (DFT) method has been performed to study the effects of CO and CO2 on the desulfurization of H2S over a ZnO sorbent. It shows that COS is inevitably formed on the ZnO(101[combining macron]0) surface, which tends to be adsorbed onto the surface via a S-C bond binding with either a long or a short Zn-O bond. Potential energy profiles for the COS formation via reactions between H2S and CO, and H2S and CO2 on the ZnO(101[combining macron]0) surface have been constructed. In the presence of CO, the dissociated active S of H2S reacting with CO leads to the formation of COS, and the activation energy of the rate-determining step is 87.7 kJ mol(-1). When CO2 is present, the linear CO2 is first transferred to active CO2 in a triplet state, and then combines with active S to form COS with the highest energy barrier of 142.4 kJ mol(-1). Rate constants at different temperatures show that the formation of COS via the reaction of CO and H2S is easier than that of CO2 and H2S over the ZnO surface. PMID:27048981

  20. A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report No. 15, January 1993--March 1993

    SciTech Connect

    Harrison, D.P.

    1993-04-01

    Phase I research, in which an electrobalance reactor was used to establish the technical feasibility of the regenerable sorbent process, was completed in March 1992 and results have been fully described in earlier quarterly reports. In Phase I, the calcination and carbonation characteristics of three calcium sorbents were studied as a function of calcination and carbonation temperature and pressure, mol fraction CO{sub 2} in the carbonation gas, and carbonation background gas composition. Desirable reaction conditions required for high reactivity and good sorbent durability were determined. Multicycle tests consisting of as many as ten complete calcination and carbonation cycles were completed. Indirect evidence which suggested that the water-gas shift reaction occurred simultaneously with CO{sub 2} removal was found. Occurrence of the simultaneous reactions created the possibility of a direct one-step process for the manufacture of hydrogen from coal-gas while at the same time separating a concentrated stream of CO{sub 2}. The concentrated CO{sub 2} stream could be quite significant if, in the future, environmental regulations restrict atmospheric CO{sub 2} emissions.

  1. A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report No. 18, October 1993--December 1993

    SciTech Connect

    Harrison, D.P.

    1994-01-01

    This research project is investigating the technical feasibility of a high-temperature, high-pressure (HTHP) process for the bulk separation of CO{sub 2} from coal-derived gas. Phase I research, in which an electrobalance reactor was used to establish the technical feasibility of the regenerable sorbent process, was completed in March 1992 and results have been fully described in earlier quarterly reports. In Phase I, the calcination and carbonation characteristics of three calcium sorbents were studied as a function of calcination and carbonation temperature and pressure, mol fraction CO{sub 2} in the carbonation gas, and carbonation background gas composition. Desirable reaction conditions required for high reactivity and good sorbent durability were determined. Multicycle tests consisting of as many as ten complete calcination and carbonation cycles were completed. Indirect evidence which suggested that the water-gas shift reaction occurred simultaneously with CO{sub 2} removal was found. Occurrence of the simultaneous reactions created the possibility of a direct one-step process for the manufacture of hydrogen from coal-gas while at the same time separating a concentrated stream of CO{sub 2}. The concentrated CO{sub 2} stream could be quite significant if, in the future, environmental regulations restrict atmospheric CO{sub 2}, emissions.

  2. Enzymatic desulfurization of coal. Seventh quarterly report, December 16, 1989--March 15, 1990

    SciTech Connect

    Boyer, Y.N.; Crooker, S.C.; Kitchell, J.P.; Nochur, S.V.

    1990-03-23

    Our experimental approach focuses on the use of enzymes which catalyze the addition of oxygen to organic compounds. In tailoring the application of these enzymes to coal processing, we are particularly interested in ensuring that oxidation occurs at sulfur and not at carbon-carbon bonds. Previous studies with DBT have shown that the reaction most frequently observed in microbial oxidative pathways is one in which DBT is oxidized at ring carbons. These reactions, as we have said, are accompanied by a considerable decrease in the energy content of the compound. In addition, microbial pathways have been identified in which the sulfur atom is sequentially oxidized to sulfoxide, to sulfone, to sulfonate, and finally to sulfuric acid. In this case, the fuel value of the desulfurized compounds is largely retained. We are evaluating the potential of commercially available enzymes to perform this function.

  3. Enzymatic desulfurization of coal. Fifth quarterly report, June 16--September 15, 1989

    SciTech Connect

    Boyer, Y.N.; Crooker, S.C.; Kitchell, J.P.; Nochur, S.V.; Marquis, J.K.

    1989-11-07

    Our experimental approach focuses on the use of enzymes which catalyze the addition of oxygen to organic compounds. In tailoring the application of these enzymes to coal processing, we are particularly interested in ensuring that oxidation occurs at sulfur and not at carbon-carbon bonds. Previous studies with DBT have shown that the reaction most frequently observed in microbial oxidative pathways is one in which DBT is oxidized at ring carbons. These reactions, as we have said, are accompanied by a considerable decrease in the energy content of the compound. In addition, microbial pathways have been identified in which the sulfur atom is sequentially oxidized to sulfoxide, to sulfone, to sulfonate, and finally to sulfuric acid. In this case, the fuel value of the desulfurized compounds is largely retained. We are evaluating the potential of commercially available enzymes to selectively catalyze oxidation at sulfur.

  4. Enzymatic desulfurization of coal. Sixth quarterly report, September 16--December 15, 1989

    SciTech Connect

    Boyer, Y.N.; Crooker, S.C.; Kitchell, J.P.; Nochur, S.V.

    1989-12-14

    Our experimental approach focuses on the use of enzymes which catalyze the addition of oxygen to organic compounds., In tailoring the application of these enzymes to coal processing, we are particularly interested in ensuring that oxidation occurs at sulfur and not at carbon-carbon bonds. Previous studies with DBT have shown that the reaction most frequently observed in microbial oxidative pathways is one in which DBT is oxidized at ring carbons. These reactions, as we have said, are accompanied by a considerable decrease in the energy content of the compound. In addition, microbial pathways have been identified in which the sulfur atom is sequentially oxidized to sulfoxide, to sulfone, to sulfonate, and finally to sulfuric acid. In this case, the fuel value of the desulfurized compounds is largely retained. We are evaluating the potential of commercially available enzymes to perform this function.

  5. Management of dry flue gas desulfurization by-products in underground mines. Quarterly report, January--March 1995

    SciTech Connect

    Chugh, Y.; Dutta, D.; Esling, S.

    1995-04-01

    On September 30, 1993, the U.S. Department of Energy, Morgantown Energy Technology Center and Southern Illinois University at Carbondale (SIUC) entered into a cooperative research agreement entitled {open_quotes}Management of Dry Flue Gas Desulfurization By-Products in Underground Mines{close_quotes} (DE-FC21-93MC 30252). Under the agreement Southern Illinois University at Carbondale will develop and demonstrate several technologies for the placement of coal combustion residues in abandoned coal mines, and will assess the environmental impact of such underground residues placement. Previous quarterly Technical Progress Reports have set forth the specific objectives of the program, as well as the management plan and the test plan for the overall program, and a discussion of these will not be repeated here. Rather, this report, will set forth the technical progress made during the period January 1 through March 31, 1995. The demonstration of the SEEC, Inc. technology for the transporting of coal combustion residues was completed with the unloading and final disposition of the three Collapsible Intermodal Containers (CIC). The loading and transport by rail of the three CIC`s was quire successful; however some difficulties were encountered in the unloading of the containers. A full topical report on the entire SEEC demonstration is being prepared. As a result of the demonstration some modifications of the SEEC concept may be undertaken. Also during the quarter the location of the injection wells at the Peabody No. 10 mine demonstration site were selected. Peabody Coal Company has developed the specifications for the wells and sought bids for the actual drilling. It is expected that the wells will be drilled early in May.

  6. Advanced sulfur control concepts for hot-gas desulfurization technology. Quarterly progress report, October 1--December 31, 1996

    SciTech Connect

    1997-06-01

    Good progress was made on both the experimental and process modelling fronts during the past quarter. All experimental tests used the fixed-bed laboratory reactor to study the sulfidation of CeO{sub 2} with H{sub 2}S and the regeneration of Ce{sub 2}O{sub 2}S using SO{sub 2}. A number of experimental problems were solved (or at least alleviated) during the quarter including malfunctioning mass flow controllers, excessive bed pressure drop, and elimination of the H{sub 2}S plateau during early stages of sulfidation tests. Most CeO{sub 2} sulfidation tests were carried out a 800{degrees}C and 5 atm using a sulfidation gas containing 1% H{sub 2}S, 10 % H{sub 2}, balance N{sub 2}. At these conditions sulfidation of CeO{sub 2} was rapid and complete. Sulfur material balance closure was satisfactory, and, except for the unexpected H{sub 2}S plateau during the prebreakthrough period, the sulfidation results were as expected. Near the end of the quarter, the cause of the H{sub 2}S plateau was tentatively identified as being due to reaction between H{sub 2} and elemental sulfur deposited downstream of the sorbent in the bottom of the reactor and in tubing leading to the gas chromatograph. The sulfur deposits occurred during regeneration tests, and chemically cleaning the lines between regeneration and sulfidation coupled with reducing the temperature of the transfer line during sulfidation greatly reduced the H{sub 2}S plateau. A brief examination of the effect of sulfidation temperature between 700 and 850{degrees}C showed relatively little temperature effect, although the slope of the active portion of the breakthrough curve was somewhat smaller at 700{degrees}C, which is consistent with a smaller reaction rate at this temperature.

  7. Management of dry flue gas desulfurization by-products in underground mines. Quarterly report, April 1--June 30, 1996

    SciTech Connect

    1997-05-01

    On September 30, 1993, the US Department of Energy - Morgantown Energy Technology Center (DOE-METC) and Southern Illinois University at Carbondale (SIUC) entered into a cooperative research agreement entitled {open_quotes}Management of Dry Flue Gas Desulfurization By-Products in Underground Mines{close_quotes} (DE-FC21-93MC30252). Under the agreement Southern Illinois University at Carbondale will develop and demonstrate two technologies for the placement of coal combustion residues in abandoned underground coal mines, and will assess the environmental impact of these technologies for the management of coal combustion by-products. The two technologies for the underground placement that will be developed and demonstrated are: (1) pneumatic placement, using virtually dry materials, and (2) hydraulic placement, using a {open_quotes}paste{close_quotes} mixture of materials with about 70% solids. Phase II of the overall program began April 1, 1996. The principal objective of Phase II is to develop and fabricate the equipment for placing the coal combustion by-products underground, and to conduct a demonstration of the technologies on the surface. Therefore, this quarter has been largely devoted to developing specifications for equipment components, visiting fabrication plants throughout Southern Illinois to determine their capability for building the equipment components in compliance with the specifications, and delivering the components in a timely manner.

  8. Management of dry flue gas desulfurization by-products in underground mines. Quarterly report, July 1 - September 30, 1996

    SciTech Connect

    1996-12-31

    On September 30, 1996, the U.S. Department of Energy-Morgantown Energy Technology Center and Souther Illinois University at Carbondale (SIUC) entered into a cooperative research agreement entitled ``Management of Dry Flue Gas Desulfurization By-Products in Underground Mines``. Under the agreement SIUC will develop and demonstrate two technologies for the placement of coal combustion by-products in abandoned underground coal mines, and will assess the environmental impact of these technologies for the management of coal combustion by-products. The two technologies for the underground placement that will be developed and demonstrated are: (1) pneumatic placement, using virtually dry materials, and (2) hydraulic placement, using a ``paste`` mixture of materials with about 70% solids. Phase II of the overall program began April 1, 1996. The principal objective of Phase II is to develop and fabricate the equipment for both the pneumatic and hydraulic placement technologies, and to conduct a surface demonstration-test of both technologies. During the current quarter the main thrust was to develop the equipment necessary for the program. Shop drawings were completed for the pneumatic placement equipment, and purchase orders issued for many of the component parts. The final pneumatic placement system will be assembled in the SIUC Carterville facility.

  9. Advanced sulfur control concepts for hot gas desulfurization technology. Quarterly report, April--June 1995

    SciTech Connect

    Harrison, D.P.

    1995-07-01

    Delivery of the Antek R-6000 total sulfur analyzer and modifications of the Shimadzu GC-14A gas chromatograph are scheduled for early July. Installation and calibration of these instruments will follow shortly. The atmospheric pressure electrobalance was used during the quarter for studies of the regeneration of FeS with O{sub 2}/N{sub 2} gas mixtures. Some anomalies in the data initially obtained required adjustment of balance sensitivity, reduction of sample size, and recalibration of the air rotameter. The authors are now confident that they can routinely obtain accurate and reproducible data with this unit. Definitive tests of effects of temperature, O{sub 2} concentration, and gas flow rate will be done next quarter. The high pressure electrobalance was put into service, and calibration experiments were started. Decomposition of CuSO{sub 4}{center_dot}5H{sub 2}O produced agreement with expected results. Heating of FeS in an O{sub 2}/N{sub 2} gas stream gave results in qualitative agreement with experiments using the atmospheric pressure electrobalance. Initial tests on effects of temperature, O{sub 2} concentration, and gas flow rate on the regeneration of FeS were done. Results were generally in agreement with expectations and with previous experiments on the atmospheric apparatus. Possible problems arose when the lowest range of the air mass flow controller was used. Fluctuation of the electrobalance signal in the early part of the regeneration experiment was an additional problem. Effort during the next quarter will focus on these problems and on definitive tests for FeS regeneration at elevated pressure. The Alonized fixed bed reactor pressure vessel was successfully leak tested early in the quarter. Other components of the fixed bed reactor system continued to arrive. Construction will begin in July along with installation of the analytical instruments.

  10. Kinetics of MN based sorbents for hot coal gas. Quarterly report, September--December 1996

    SciTech Connect

    1996-12-31

    Manganese-based sorbents have been investigated for the removal of hydrogen sulfide (the primary sulfur bearing compound) from hot coal gases prior to its use in combined cycle turbines. Four formulations of Mn-based sorbents were tested in an ambient-pressure fixed-bed reactor to determine steady state H{sub 2}S concentrations, breakthrough times and effectiveness of the sorbent when subjected to cyclic sulfidation and regeneration testing. In a previous report, the sulfidation results were presented. Manganese-based sorbents with molar ratios > 1:1 Mn:Substrate were effective in reducing the H{sub 2}S concentration in simulated coal gases to less than 100 ppmv over five cycles. Actual breakthrough time for formulation C6-2-1100 was as high as 73% of breakthrough time based on wt% Mn in sorbent. In this report, the regeneration results will be presented. Regeneration tests determined that loaded pellets can be fully regenerated in air/steam mixture at 750{degrees}C with minimal sulfate formation. 16 refs., 9 figs., 5 tabs.

  11. A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report 13, October 1992--December 1992

    SciTech Connect

    Harrison, D.P.

    1993-01-01

    The original contract f or two years was awarded in September 1989 as a result of solicitation number DE-RA21-89MC26040 entitled ``Novel Concepts for Bulk Separation of Gases in Coal Gasification Systems.`` Two no-cost extensions without a change in the statement of work extended the performance period by six months to March 1992. At that time a two-year contract extension with an enlarged scope of work and additional funding was approved so that the research is now scheduled to end in March 1994. Phase I research, in which an electrobalance reactor was used to establish the technical feasibility of the regenerable sorbent process, was completed in March 1992 and results have been fully described in earlier quarterly reports. In Phase I, the calcination and carbonation characteristics of three calcium sorbents were studied as a function of calcination and carbonation temperature and pressure, mol fraction CO{sub 2} in the carbonation gas, and carbonation background gas composition. Desirable reaction conditions required for high reactivity and good sorbent durability were determined. Multicycle tests consisting of as many as ten complete calcination and carbonation cycles were completed. Indirect evidence which suggested that the water-gas shift reaction occurred simultaneously with CO{sub 2} removal was found. Occurrence of the simultaneous reactions created the possibility of a direct one-step process for the manufacture of hydrogen from coal-gas while at the same time separating a concentrated stream of CO{sub 2} The concentrated CO{sub 2} stream could be quite significant if, in the future, environmental regulations restrict atmospheric CO{sub 2} emissions.

  12. Advanced sulfur control concepts in hot gas desulfurization technology. Quarterly report, April 1--June 30, 1996

    SciTech Connect

    1997-05-01

    Experimental effort during the past quarter was restricted to the fixed-bed reactor. Effort during April was devoted to the sulfidation and regeneration of cerium oxide. Sulfidation tests were plagued by over-sulfidation, i.e., the quantity of H{sub 2}S removed from the gas phase exceeded the stoichiometric amount associated with the conversion of CeO{sub 2} to Ce{sub 2}O{sub 2}S. This was initially attributed to the formation of Ce{sub 2}S{sub 3} which was found to be thermodynamically possible in the highly reducing feed gas. However, the addition of steam to the feed gas to prevent Ce{sub 2}S{sub 3} formation did not eliminate the over-sulfidation problem. Later tests indicated that the apparent over-sulfidation was due to reaction between H{sub 2}S and the walls of the reaction vessel. Apparently the alonizing treatment to passivate the reactor walls was either ineffective at the reaction conditions or had deteriorated with use to the point that protection was no longer viable. Limited Ce{sub 2}O{sub 2}S regeneration results, although very qualitative, were quite favorable. In one regeneration test in an O{sub 2}-N{sub 2} atmosphere, no SO{sub 2} or H{sub 2}S were detected by the chromatograph in the regeneration product. Significant amounts of total sulfur were detected, and the test had to be terminated prematurely when elemental sulfur caused the product line leading to the chromatograph to plug. Experimental tests during May and June examined the regeneration of FeS as a function of temperature, gas feed composition, and gas flow rate. Complete regeneration was achieved with as much as 75% of the sulfur liberated in elemental form. Low regeneration temperature and large ratios of H{sub 2}O to O{sub 2} in the feed gas promote the formation of elemental sulfur. A number of changes in the reactor system were made during the quarter, including improvements to the sulfur condenser and filters on the reactor product line leading to the gas chromatograph.

  13. Theoretical approach for enhanced mass transfer effects in-duct flue gas desulfurization processes. Volume 1, Dry sorbent injection: Final report

    SciTech Connect

    Jozewicz, W.; Rochelle, G.T.

    1992-01-29

    This report presents the results of fundamental mass transfer testing for in-duct removal of SO{sub 2}. Following this initial part of an experimental program, it became clear that the amount of initial moisture on the sorbent strongly affected the extent of Ca(OH){sub 2} conversion. Novel techniques aimed at increasing sorbent utilization were investigated and are described. Major novel technique investigated and reported on here was the reaction with SO{sub 2} of sorbents with initial free moisture (damp sorbents). The duct injection process using damp solids has the following steps: preparation of sorbent as a slurry, blending of the slurry with dry recycle materials to create damp solids, injection of the solids into the duct, reaction and drying of the solids with flue gas in the duct, collection in particulate control equipment, and finally recycle of dry solids with some bleed to disposal. The moisture content of the solids at each step affects system performance. Various factors favor high moisture whereas others favor low moisture. (VC)

  14. Interactions between trace metals, sodium and sorbents in combustion. Quarterly report No. 4, July 1, 1995--September 30, 1995

    SciTech Connect

    Wendt, J.O.L.; Davis, S.

    1995-10-15

    The proposed research is directed at an understanding of how to exploit interactions between sodium, toxic metals and sorbents, in order to optimize sorbents injection procedures, which can be used to capture and transform these metals into environmentally benign forms. The research will use a 17kW downflow, laboratory combustor, to yield data that can be interpreted in terms of fundamental kinetic mechanisms. Metals to be considered are lead, cadmium, and arsenic. Sorbents will be kaolinite, bauxite, and limestone. The role of sulfur will also be determined.

  15. Stabilization and/or regeneration of spent sorbents from coal gasification. [Quarterly] technical report, December 1, 1991--February 29, 1992

    SciTech Connect

    Abbasian, J.; Hill, A.H.; Wangerow, J.R.

    1992-08-01

    The objective of this investigation is to determine the effects of SO, partial pressure and reaction temperature on the conversion of sulfide containing solid wastes from coal gasifiers to stable and environmentally acceptable calcium-sulfate, while preventing the release of sulfur dioxide through undesirable side reactions during the stabilization step. An additional objective of this program is to investigate the use of the Spent Sorbent Regeneration Process (SSRP) to regenerate spent limestone, from a fluidized-bed gasifier with in-bed sulfur capture, for recycling to the gasifier. To achieve these objectives, selected samples of partially sulfided sorbents will be reacted with oxygen at a variety of operating conditions under sufficient S0{sub 2} partial pressure to prevent release of sulfur from the solids during stabilization that reduces the overall sorbent utilization. Partially sulfided limestone will also be regenerated with water to produce calcium hydroxide and release sulfur as H{sub 2}S. The regenerated sorbent will be dewatered, dried and pelletized. The reactivity of the regenerated sorbent toward H{sub 2}S will also be determined.

  16. Effect of solids concentration distribution on the flue gas desulfurization process

    SciTech Connect

    Jie Zhang; Changfu You; Haiying Qi; Changhe Chen; Xuchang Xu

    2006-06-15

    A dry flue gas desulfurization (FGD) process at 600-800{sup o}C was studied in a pilot-scale circulating fluidized bed (CFB) experimental facility. Various fresh sorbent distribution types and internal structures were modeled numerically to investigate their effect on the gas-solid flow and sulfate reaction characteristics. Experimental results show that, after the fresh sorbent supply was stopped, the desulfurization efficiency declined rapidly even though the sorbent recirculation was maintained. Therefore, the fresh sorbent is the main contributor to the desulfurization process and the primary effect of the recirculated sorbent was to evenly distribute the fresh sorbent and to prolong the sorbent particle residence time. The numerical results demonstrate that the desulfurization efficiency varied greatly for the various fresh sorbent bottom injection methods. The desulfurization efficiency of the bottom-even injection method was 1.5 times that of the bottom two-sided injection method. Internal structures effectively improved the fresh sorbent solids concentration distribution and the desulfurization efficiency. Optimized internal structures increased the desulfurization efficiency of the bottom two-sided injection method by 46%, so that it was very close to that of the bottom-even injection method with only a 4.6% difference. 16 refs., 6 figs., 2 tabs.

  17. Effect of solids concentration distribution on the flue gas desulfurization process.

    PubMed

    Zhang, Jie; You, Changfu; Qi, Haiying; Chen, Changhe; Xu, Xuchang

    2006-06-15

    A dry flue gas desulfurization (FGD) process at 600-800 degrees C was studied in a pilot-scale circulating fluidized bed (CFB) experimental facility. Various fresh sorbent distribution types and internal structures were modeled numerically to investigate their effect on the gas-solid flow and sulfate reaction characteristics. Experimental results show that, after the fresh sorbent supply was stopped, the desulfurization efficiency declined rapidly even though the sorbent recirculation was maintained. Therefore, the fresh sorbent is the main contributor to the desulfurization process and the primary effect of the recirculated sorbent was to evenly distribute the fresh sorbent and to prolong the sorbent particle residence time. The numerical results demonstrate thatthe desulfurization efficiency varied greatly for the various fresh sorbent bottom injection methods. The desulfurization efficiency of the bottom-even injection method was 1.5 times that of the bottom two-sided injection method. Internal structures effectively improved the fresh sorbent solids concentration distribution and the desulfurization efficiency. Optimized internal structures increased the desulfurization efficiency of the bottom two-sided injection method by 46%, so that it was very close to that of the bottom-even injection method with only a 4.6% difference. PMID:16830575

  18. Biocatalytic desulfurization

    SciTech Connect

    Monticello, D.J. )

    1994-02-01

    Biocatalytic desulfurization (BDS) has many advantages compared to traditional refinery desulfurization processes, including: lower capital and operating costs, low-temperature and low-pressure operation and no hydrogen requirement. Biotechnology has developed from an art into a science in recent years. The HPI is familiar with an artful' application of biotechnology in the biotreatment of refinery wastes, and has experimented with other technologies for over 50 years. This paper discusses the following: biorefining, sulfur management, conventional solutions, bioprocessing precedents, new biotechnology tools, microbial desulfurization, biocatalytic desulfurization, specificity, biodesulfurization conceptual design, development issues, and implementation.

  19. Desulfurization of Illinois coals with hydroperoxides of vegetable oils and alkali, Quarterly report, March 1 - May 31, 1996

    SciTech Connect

    Smith, G.V.; Gaston, R.D.; Song, R.; Cheng, J.; Shi, F.; Wang, Y.

    1996-12-31

    Organic sulfur is removed from coals by treatment with aqueous base, air, and vegetable oils with minimal loss of BTU. Such results were revealed during exploratory experiments on an ICCI funded project to remove organic sulfur from Illinois coals with hydroperoxides of vegetable oils. In fact, prewashing IBC-108 coal with dilute alkali prior to treating with linseed oil and air results in 26% removal of sulfur. This new method is being investigated by treating coals with alkali, impregnating coals with polyunsaturated oils, converting the oils to their hydroperoxides, and heating. Since these oils are relatively inexpensive and easily applied, this project could lead to a cost effective method for removing organic sulfur from coals. During the first quarter the selection of base fro pretreatment and extraction was completed. NaOH is better than NH{sub 4}OH for the pretreatment and Na{sub 2}CO{sub 3} is better than NaOH for the oil extraction. During the second quarter the effectiveness of linseed oil and NaOH for sulfur removal from IBC-108 coal was further tested by pretreating the coal with two base concentrations at four different times followed by treatment with linseed oil at 125{degrees}C for three different times and finally washing with 5% Na{sub 2}CO{sub 3} and methanol. During this third quarter more experimental parameters were systematically varied in order to study the effectiveness of linseed oil and NaOH for sulfur removal from IBC- 108 coal.

  20. Development of novel copper-based sorbents for hot-gas cleanup. [Quarterly] technical report, September 1--November 30, 1993

    SciTech Connect

    Abbasian, J.; Hill, A.H.; Flytzani-Stephanopoulos, M.; Li Li

    1994-03-01

    The objective of this investigation is to evaluate two novel copper-based sorbents, namely copper-chromium and copper-cerium, for their effectiveness in removing hydrogen sulfide from fuel gas in the temperature range of 650{degree} to 850{degree}C. Such high temperatures will be required for the new generation of gas turbines (inlet >750{degree}C) in Integrated Gasification Combined Cycle (IGCC) systems. The effect of pre-reduction on the performance of the sorbents as well as the rate of different reactions occurring in cyclic sulfidation/regeneration, were studied in a thermogravimetric analyzer (TGA). Sulfidation was conducted with and without H{sub 2} and H{sub 2}O, and with and without pre-reduction in H{sub 2} or H{sub 2}/H{sub 2}O. The results of these tests indicate that reduction and regeneration of both sorbents occurs rapidly. Sulfidation of CuCr{sub 2}O{sub 4}, in H{sub 2}O-free and H{sub 2}-/H{sub 2}O-free gas indicates the possible sulfidation of both copper and chromium. Small quantities of SO{sub 2}, were released during sulfidation suggesting the possible oxidation of H{sub 2}S by the sorbent. Regeneration of the CuCr{sub 2}O{sub 4} was complete while regeneration of the CuO-CeO{sub 2} indicated possible limited sulfate formation.

  1. Coal desulfurization in a rotary kiln combustor. Quarterly report No. 1, April 16, 1990--July 15, 1990

    SciTech Connect

    Cobb, J.T. Jr.

    1990-08-15

    BCR National Laboratory (BCRNL) has initiated a project aimed at evaluating the technical and economic feasibility of using a rotary kiln, suitably modified, to burn Pennsylvania anthracite wastes, co-fired with high-sulfur bituminous coal. Limestone will be injected into the kiln for sulfur control, to determine whether high sulfur capture levels can be achieved with high sorbent utilization. The principal objectives of this work are: (1) to prove the feasibility of burning anthracite refuse, with co-firing of high-sulfur bituminous coal and with limestone injection for sulfur emissions control, in a rotary kiln fitted with a Universal Energy International (UEI) air injector system; (2) to determine the emissions levels of SO{sub x} and NO{sub x} and specifically to identify the Ca/S ratios that are required to meet New Source Performance Standards; (3) to evaluate the technical and economic merits of a commercial rotary kiln combustor in comparison to fluidized bed combustors; and, (4) to ascertain the need for further work, including additional combustion tests, prior to commercial application, and to recommend accordingly a detailed program towards this end.

  2. Pyrite surface characterization and control for advanced fine coal desulfurization technologies. Ninth quarterly technical progress report, September 1, 1992-- December 31, 1992

    SciTech Connect

    Wang, X.H.; Leonard, J.W.; Parekh, B.K.; Jiang, C.L.

    1992-12-31

    This is the 9th quarterly technical progress report for the project entitled ``Pyrite surface characterization and control for advanced fine coal desulfurization technologies``, DE-FG22-90PC90295. The work presented in this report was performed from September 1, 1992 to November 31, 1992. The objective of the project is to conduct extensive fundamental studies on the surface chemistry of pyrite oxidation and flotation and to understand how the alteration of the coal-pyrite surface affects the efficiency of pyrite rejection in coal flotation. During this reporting period, the surface oxidation of pyrite in various electrolytes was investigated. It has been demonstrated, for the first time, that borate, a pH buffer and electrolyte used by many previous investigators in studying sulfide mineral oxidation, actively participates in the surface oxidation of pyrite. In borate solutions, the surface oxidation of pyrite is tronly enhanced. The anodic oxidation potential of pyrite is lowered by more than 0.4 volts. The initial reaction of the borate enhanced pyrite oxidation can be described by:FeS{sub 2} + B(OH){sub 4}{sup =} ------> [S{sub 2}Fe-B(OH){sub 4}]{sub surf} + e. This reaction is irreversible and is controlled by the mass-transfer of borate species from the solution to the surface. It has been shown that the above reaction inhibits the adsorption of xanthate on pyrite. Comparative studies have been made with other sulfide minerals. The solution chemistry of the iron-borate systems have been studied to understand the electrochemical results.

  3. High-volume, high-value usage of flue gas desulfurization (FGD) by-products in underground mines: Phase 1 -- Laboratory investigations. Quarterly report, July--September 1995

    SciTech Connect

    1996-01-01

    Efforts primarily focused on Subtask 2.2, Chemical and Mineralogical Characterization and Subtask 4.3, Selection and Testing of Transport System. As part of Subtask 2.2, samples were collected from the Freeman United Crown Mine III FBC disposal facility representing a verity of ages and weathering. A laboratory scale transport system has been built at the CAER to evaluate the potential of pneumatic transport for flue gas desulfurization material (FGDM) emplacement and to provide essential data for the mine emplacement demonstration as part of the Subtask 4.3 effort. The system is modeled after shotcreting systems and has the advantage that the material can be remotely placed without the need for forms. The test program is focusing on determining the pneumatic conditions necessary to maximize the strength of the emplaced FGDM under anticipated mine curing conditions while minimizing dust formation. Work on Subtask 4.1, Mine Selection, also proceeded during the quarter. A new mine site, located in the south-central section of the Pikeville quadrangle, Pike County, Kentucky, was examined for the field study. The proposed fill site is in the Middle Pennsylvanian Breathitt Formation Middle Amburgy coal bed, a coal previously mined by Costain elsewhere on the property. Efforts on Subtask 4.2, Hydrologic Monitoring Plan, focused primarily on theoretical issues concerning the effects of the mining and backfill activity on the ground water and surface water due to uncertainties in the location of the final field site. There are three major concerns about the effects of the mining activity: changes in the ground water flow field, changes in ground water quality, and consequential induced changes on stream flow.

  4. Advanced sulfur control concepts in hot-gas desulfurization technology. Quarterly technical progress report, July--September 1995

    SciTech Connect

    Harrison, D.P.

    1995-10-01

    Both the Antek total sulfur analyzer and the modifications to the Shimadzu GC-14A gas chromatograph to be used for analysis for SO{sub 2} and H{sub 2}S were delivered during the quarter. Problems were faced during the installation and calibration phases of both instruments. By the end of the quarter we believe that the GC problems have been solved, but problems remain with the Antek analyzer. It appears that too much sulfur (as SO{sub 2}) reaches the UV detector and causes it to become saturated. This shows up as a maximum in the instrument calibration curve. At 200 psia, the capillary flow restrictor allows a total flow rate of about 180 sccm, and the maximum occurs at about 1 % H{sub 2}S in the calibration gas. Reducing the pressure so that the total flow is reduced to about 25 sccm shifts the calibration curve maximum to about 5.7% H{sub 2}S. It appears that we must reduce the total flow rate to the detector or provide additional dilution. This may be accomplished by increasing the resistance of the capillary restrictor, by diverting a portion of the flow leaving the pyrotube to vent, or adding an inert such as N{sub 2} to the gases exiting the pyrotube. We are in contact with Antek representatives about the problem. Both the atmospheric pressure and high pressure electrobalances were used during the quarter to study the regeneration of FeS in atmospheres of O{sub 2}/N{sub 2} or H{sub 2}O/N{sub 2}. In the atmospheric pressure unit the effects of temperature (600 - 800{degrees}C), flow rate (130 - 500 sccm), and reactive gas mol fraction (0.005 to 0.03 O{sub 2} and 0.1 to 0.5 H{sub 2}O) are being studied. Regeneration tests completed to date in the high pressure unit have utilized only O{sub 2}/N. and the parameters studied include temperature (600 - 800{degrees}C), flow rate (500 - 1000 sccm), pressure (1 - 15 atm) ad O{sub 2} mol fraction (0.005 - 0.03).

  5. Zinc titanate sorbents

    DOEpatents

    Gupta, Raghubir P.; Gangwal, Santosh K.; Jain, Suresh C.

    1998-01-01

    The present invention provides a zinc titanate sorbent material useful in desulfurization applications. The zinc titanate material is in the form of generally spherical particles of substantially uniform chemical distribution. The sorbent material is capable of absorbing sulfur compounds from a gaseous feed in an amount of at least about 15 weight percent based on the weight of the sorbent. The sorbent material is prepared by a process including: (a) forming a zinc oxide/titanium dioxide dry blend, (b) preparing a substantially uniform aqueous slurry comprising the zinc oxide/titanium dioxide dry blend, organic binder, and at least about 1 weight percent inorganic binder based on the solids weight of the slurry, (c) spray drying the slurry to produce substantially spherical particles, and (d) calcining the particles at a temperature of between about 750.degree. C. to about 950.degree. C. The dry blend is formed by mixing between about 0.5 to about 2 parts zinc oxide having a median particle size of less than about 0.5 .mu., and about 1 part titanium dioxide having a median particle size of less than about 1 .mu.. The slurry contains substantially no free silica and may be prepared by the process including (1) preparing an aqueous solution of organic binder, (2) adding the dry blend to the aqueous solution of organic binder, and (3) adding the inorganic binder to the solution of organic binder, and blend. Additional reagents, such as a surfactant, may also be incorporated into the sorbent material. The present invention also provides a process for desulfurizing a gaseous stream. The process includes passing a gaseous stream through a reactor containing an attrition resistant zinc titanate sorbent material of the present invention.

  6. Zinc titanate sorbents

    DOEpatents

    Gupta, R.P.; Gangwal, S.K.; Jain, S.C.

    1998-02-03

    The present invention provides a zinc titanate sorbent material useful in desulfurization applications. The zinc titanate material is in the form of generally spherical particles of substantially uniform chemical distribution. The sorbent material is capable of absorbing sulfur compounds from a gaseous feed in an amount of at least about 15 weight percent based on the weight of the sorbent. The sorbent material is prepared by a process including: (a) forming a zinc oxide/titanium dioxide dry blend, (b) preparing a substantially uniform aqueous slurry comprising the zinc oxide/titanium dioxide dry blend, organic binder, and at least about 1 weight percent inorganic binder based on the solids weight of the slurry, (c) spray drying the slurry to produce substantially spherical particles, and (d) calcining the particles at a temperature of between about 750 to about 950 C. The dry blend is formed by mixing between about 0.5 to about 2 parts zinc oxide having a median particle size of less than about 0.5 microns, and about 1 part titanium dioxide having a median particle size of less than about 1 micron. The slurry contains substantially no free silica and may be prepared by the process including (1) preparing an aqueous solution of organic binder, (2) adding the dry blend to the aqueous solution of organic binder, and (3) adding the inorganic binder to the solution of organic binder, and blend. Additional reagents, such as a surfactant, may also be incorporated into the sorbent material. The present invention also provides a process for desulfurizing a gaseous stream. The process includes passing a gaseous stream through a reactor containing an attrition resistant zinc titanate sorbent material of the present invention.

  7. Management of dry flue gas desulfurization by-products in underground mines. Quarterly report, August 1--October 31, 1997

    SciTech Connect

    Chugh, Y.P.

    1997-12-31

    The objective of this project was to develop and demonstrate two technologies for the placement of coal combustion by-products in abandoned underground coal mines, and to assess the environmental impact of these technologies for the management of CCB materials. The two technologies for the underground placement that were to be developed and demonstrated are: (1) pneumatic placement using virtually dry CCB products, and (2) hydraulic placement using a paste mixture of CCB products with about 70% solids. The period covered by this report is the second quarter of Phase 3 of the overall program. During this period over 8,000 tons of CCB mixtures was injected using the hydraulic paste technology. This amount of material virtually filled the underground opening around the injection well, and was deemed sufficient to demonstrate fully the hydraulic injection technology. By the end of this quarter about 2,000 tons of fly ash had been placed underground using the pneumatic placement technology. While the rate of injection of about 50 tons per hour met design criteria, problems were experienced in the delivery of fly ash to the pneumatic demonstration site. The source of the fly ash, the Archer Daniels Midland Company power plant at Decatur, Illinois is some distance from the demonstration site, and often sufficient tanker trucks are not available to haul enough fly ash to fully load the injection equipment. Further, on some occasions fly ash from the plant was not available. The injection well was plugged three times during the demonstration. This typically occurred due to cementation of the FBC ash in contact with water. After considerable deliberations and in consultation with the technical project officer, it was decided to stop further injection of CCB`s underground using the developed pneumatic technology.

  8. A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report, October--December 1991

    SciTech Connect

    Silaban, A.; Narcida, M.; Harrison, D.P.

    1992-02-01

    The expected commercialization of coal gasification technology in the US and world-wide will create a need for advanced gas purification and separation processes capable of operating at higher temperatures and in more hostile environments than is common today. For example, a high-temperature, high-pressure process capable of separating CO{sub 2} from coal-derived gas may find application in purifying synthesis gas for H{sub 2}, NH{sub 3}, or CH{sub 3}OH production. High temperature CO{sub 2} removal has the potential for significantly improving the operating efficiency of integrated gasification-molten carbonate fuel cells for electric power generation. This study proved the technical feasibility of a CO{sub 2}-separation process based upon the regenerable noncatalytic gas-solid reaction between CaO and CO{sub 2} to form CACO{sub 3}. Such a process operating at 650{degree}C and 15 atm with 15% CO{sub 2} in the coal gas has the potential for removing in excess of 99% of the CO{sub 2} fed. Selection of a sorbent precursor which, upon calcination, produces high-porosity CaO is important for achieving rapid and complete reaction. The addition of magnesium to the sorbent appears to improve the multicycle durability at a cost of reduced CO{sub 2} capacity per unit mass of sorbent. Reaction conditions, principally calcination and carbonation temperatures, are important factors in multicycle durability. Reaction pressure and CO{sub 2} concentration are important in so far as the initial rapid reaction rate is concerned, but are relatively unimportant in terms of sorbent capacity and durability. Indirect evidence for the simultaneous occurrence of the shift reaction and CO{sub 2}-removal reaction creates the possibility of a direct one-step process for the production of hydrogen from coal-derived gas.

  9. Confined zone dispersion flue gas desulfurization demonstration. Volume 1, Quarterly report No. 6, February 1, 1992--April 30, 1992

    SciTech Connect

    Not Available

    1993-01-15

    This is the sixth quarterly report for this project and it covers work performed on Phase 3a of the project from February 1, 1992 through April 30, 1992. Extension of the parametric test period through June 1992 provides an opportunity to regain most of the schedule slippage, but only if the modifications needed for continuous operation of the CZD system are installed concurrent with the extended test period. These modifications include automation of the lime preparation and transfer system, automatic injection control, and related instrumentation and controls as necessary to integrate the operation of the CZD system with Seward Station Boiler No. 15. Early installation of these modifications would permit testing, debugging and adjustment of the automatic control system during the parametric test period. Results of current testing indicate that considerable testing and adjustment will be required to optimize operation of the CZD system after it is automated for continuous operation. Therefore, we intend to incorporate in Phase 3a(parametric testing) the system modifications needed for continuous automatic operation that were originally included in Phase 3b. Phase 3b would then be limited only to the one-year continuous demonstration.

  10. Confined zone dispersion flue gas desulfurization demonstration. Quarterly report No. 8, August 17, 1992--November 16, 1992

    SciTech Connect

    Not Available

    1993-09-27

    The CZD process involves injecting a finely atomized slurry of reactive lime into the flue gas duct work of a coal-fired utility boiler. The principle of the confined zone is to form a wet zone of slurry droplets in the middle of the duct confined in an envelope of hot gas between the wet zone and the duct walls. The lime slurry reacts with part of the SO{sub 2} in the gas, and the reaction products dry to form solid particles. A solids collector, typically an electrostatic precipitator (ESP) downstream from the point of injection, captures the reaction products along with the fly ash entrained in the flue gas. The goal of this demonstration is to prove the technical and economic feasibility of the CZD technology on a commercial scale. The process is expected to achieve 50% SO{sub 2} removal at lower capital and O&M costs than other systems. To achieve its objectives, the project is divided into the following three phases: Phase 1: Design and Permitting, Phase 2: Construction and Start-up, Phase 3: Operation and Disposition. Phase 1 activities were completed on January 31, 1991. Phase 2 activities were essentially concluded on July 31, 1991, and Phase 3a, Parametric Testing, was initiated on July 1, 1991. This Quarterly Technical Progress Report covers Phase 3b activities from August 17, 1992 through November 16, 1992.

  11. Hot Gas Desulfurization Using Transport Reactors

    SciTech Connect

    Moorehead, E.L.

    1996-12-31

    Sierra Pacific Power Company is building a 100 MW, IGCC power plant based on KRW fluid bed gasifier technology that utilizes transport reactors for hot gas desulfurization and sorbent regeneration. Use of a transport absorber avoids the need for pre-filtration of dust-laden gasifier effluent, while a transport regenerator allows for the use of 100% air without the need for heat exchange equipment. Selection of transport reactors for hot gas desulfurization using a proprietary sorbent, based on testing performed in a transport reactor test unit (TRTU) at the M. W. Kellogg Technology Development Center and in a fixed bed reactor at Morgantown Energy Technology Center (METC), is outlined. The results obtained in these two test facilities and reasons for selecting transport reactors for the IGCC power plant in preference to either fixed bed or fluidized bed reactors are discussed. This paper reviews the evolution of the hot gas desulfurization system designs and includes selected results on H{sub 2}S absorption and regeneration of sulfided sorbent over several absorption/regeneration cycles conducted in the TRTU and the METC fixed bed reactor. The original design for the Sierra Pacific Project was based on fixed bed reactors with zinc ferrite as the sorbent. Owing to the high steam requirements of this sorbent, zinc titanate was selected and tested in a fixed bed reactor and was found unacceptable due to loss of strength on cyclic absorption/regeneration operation. Another sorbent evaluated was Z-Sorb{reg_sign}, a proprietary sorbent developed by Phillips Petroleum Company, was found to have excellent sulfur capacity, structural strength and regenerability. Steam was found unsuitable as fixed bed regenerator diluent, this results in a requirement for a large amount of inert gas, whereas a transport regenerator requires no diluent. The final Sierra design features transport reactors for both desulfurization and regeneration steps using neat air. 3 refs., 3 figs., 2 tabs.

  12. Confined zone dispersion flue gas desulfurization demonstration. Volume 1, Quarterly report No. 5, November 1, 1991--January 31, 1992

    SciTech Connect

    Not Available

    1992-12-31

    This is the fifth quarterly report for this project. This project is divided into three phases. Phase 1, which has been completed, involved design, engineering, and procurement for the CZD system, duct and facility modifications, and supporting equipment. Phase 2, also completed, included equipment acquisition and installation, facility construction, startup, and operator training for parametric testing. Phase 3 broadly covers testing, operation and disposition, but only a portion of Phase 3 was included in Budget Period 1. That portion was concerned with parametric testing of the CZD system to establish the optimum conditions for an extended, one-year, continuous demonstration. As of December 31, 1991, the following goals have been achieved. (1) Nozzle Selection - A modified Spraying Systems Company (SSC) atomizing nozzle has been selected for the one-year continuous CZD demonstration. (2) SO{sub 2} and NO{sub x} Reduction - Preliminary confirmation of 50% SO{sub 2} reduction has been achieved, but the NO{sub x} reduction target cannot be confirmed at this time. (3) Lime Selection - Testing indicated an injection rate of 40 to 50 gallons per minute with a lime slurry concentration of 8 to 10% to achieve 50% SO{sub 2} reduction. There has been no selection of the lime to be used in the one year demonstration. (4) ESP Optimization - Tests conducted to date have shown that lime injection has a very beneficial effect on ESP performance, and little adjustment may be necessary. (5) SO{sub 2} Removal Costs - Testing has not revealed any significant departure from the bases on which Bechtel`s original cost estimates (capital and operating) were prepared. Therefore, SO{sub 2} removal costs are still expected to be in the range of $300/ton or less.

  13. Advanced sulfur control concepts in hot-gas desulfurization technology. Quarterly report 14, July--October 1997

    SciTech Connect

    Harrison, D.P.

    1997-10-01

    Experimental work during the quarter was limited to a series of CeO{sub 2} reduction tests using an atmospheric pressure electrobalance reactor. Both Rhonc-Poulenc and Molycorp CeO{sub 2} were tested over a temperature range of 600 to 1000{degrees}C in various reducing gas compositions. Experimental results are in reasonable agreement with equilibrium calculations of the oxygen partial pressure from CHEMQ coupled with earlier experimental results from Bevan and Kordis. Weight loss corresponding to the reduction of CeO{sub 2} to CeO{sub 1.86} was observed at 1000{degrees} in an atmosphere of 40% H{sub 2}, 3.5% CO{sub 2}, balance He. Helium was used as the carrier gas instead of nitrogen to reduce aerodynamic noise, and the H{sub 2} and CO{sub 2} concentrations were chosen since this mixture results in oxygen partial pressure similar to those expected in Shell gas. The experimental value of CeO{sub 1.86} compares quite favorably to the predicted value of CeO{sub 1.83}. One unexpected results was a weight loss of about 9% from Rhone-Poulenc CeO{sub 2} in an inert atmosphere at 600{degrees}C. BET surface area measurements of nine samples were performed consisting of as-received CeO{sub 2} (both Rhone Poulenc and Molycorp), as-received Al{sub 2}O{sub 3}, both CeO{sub 2} samples with Al{sub 2}O{sub 3} as initially charged to the reactor, and both CeO{sub 2}-Al{sub 2}O{sub 3} mixtures after multicycle sulfidation-regeneration tests. The BET surface area of the Rhone-Poulenc CeO{sub 2} was about 20 times larger than the surface area of Molycorp CeO{sub 2} which explains differences in sulfidation performance reported earlier. Finally a more complete search of the literature for thermodynamic data for cerium compounds was carried out. It appears that the free energy of formation of CeO{sub 2} as a function of temperature is well defined.

  14. Adsorption and Ultrasound-Assisted Sorbent Regeneration

    SciTech Connect

    Yuhe Wang; Liping Ma; Ralph T. Yang

    2006-09-30

    This work was conducted for the department of Energy. In this work, we developed a class of new sorbents that were highly sulfur selective and had high sulfur capacities. The study consisted of two sections. Development of the new sorbents is described in Section 1, and Section was a fundamental study, conducted for a better understanding for desulfurization of jet fuels. More details of the results are given blow separately for the two sections.

  15. Development of novel copper-based sorbents for hot-gas cleanup. [Quarterly] technical report, December 1, 1991--February 29, 1992

    SciTech Connect

    Abbasian, J.; Hill, A.H.; Wangerow, J.R.; Flytzani-Stephanopoulos, M.; Bo, L.; Patel, C.

    1992-08-01

    The objective of this investigation is to evaluate several novel copper-based binary oxides for their suitability as regenerable sorbents for hot gas cleanup application in the temperature range of 650{degrees} to 850{degrees}C. To achieve this objective, several novel copper-based binary oxide sorbents will be prepared. Experimental tests will be conducted at ambient pressure to determine the stability, sulfidation capacity, regenerability, and sulfidation kinetics of the novel sorbents. Tests will also be conducted at high pressure for the determination of the sulfidation reactivity, regenerability, and durability of the sorbents. The attrition characteristics of the sorbents will also be determined.

  16. A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report 11, April 1992--June 1992

    SciTech Connect

    Harrison, D.P.

    1992-08-01

    This research project is investigating the technical feasibility of a high-temperature, high-pressure (HTHP) process for the bulk separation of CO{sub 2} from coal-derived gas. Phase I research, which utilized an electrobalance reactor, was completed during the previous quarter and final experimental results have been reported. Phase II research involves a switch from the electrobalance reactor to a laboratory-scale fixed-bed reactor having feed and product gas analysis capability. Initial effort during Phase II has been limited to project planning including the design and construction of the fixed-bed reactor, developing specifications for gas analysis, and ordering the gas chromatograph system. These activities are described in the present report.

  17. Zirconia-silica based mesoporous desulfurization adsorbents

    NASA Astrophysics Data System (ADS)

    Palomino, Jessica M.; Tran, Dat T.; Kareh, Ana R.; Miller, Christopher A.; Gardner, Joshua M. V.; Dong, Hong; Oliver, Scott R. J.

    2015-03-01

    We report a series of mesoporous silicate sorbent materials templated by long-chain primary alkylamines that display record level of desulfurization of the jet fuel JP-8. Pure silica frameworks and those with a Si:Zr synthesis molar ratio ranging from 44:1 to 11:1 were investigated. The optimum sorbent was identified as dodecylamine-templated silica-zirconia synthesized from a gel with Si:Zr molar ratio of 15:1. With an optimized silver loading of 11 wt.%, a saturation adsorption capacity of 39.4 mgS g-1 and a silver efficiency of 1.21 molS mol Ag-1 were observed for JP-8. This sorbent displayed exceptional regenerability, maintaining 86% of its initial capacity in model fuel after solvent regeneration with diethyl ether. Low-cost, portable and reusable sorbents for the desulfurization of JP-8 jet fuel are needed to make solid oxide fuel cells (SOFCs) a reality for military power needs. SOFCs require ultra-low sulfur content fuel, which traditional desulfurization methods cannot achieve.

  18. Low temperature SO{sub 2} removal with solid sorbents in a circulating fluidized bed absorber. Final report

    SciTech Connect

    Lee, S.K.; Keener, T.C.

    1994-10-10

    A novel flue gas desulfurization technology has been developed at the University of Cincinnati incorporating a circulating fluidized bed absorber (CFBA) reactor with dry sorbent. The main features of CFBA are high sorbent/gas mixing ratios, excellent heat and mass transfer characteristics, and the ability to recycle partially utilized sorbent. Subsequently, higher SO{sub 2} removal efficiencies with higher overall sorbent utilization can be realized compared with other dry sorbent injection scrubber systems.

  19. Aerogel sorbents

    DOEpatents

    Begag, Redouane; Rhine, Wendell E; Dong, Wenting

    2016-04-05

    The current invention describes methods and compositions of various sorbents based on aerogels of various silanes and their use as sorbent for carbon dioxide. Methods further provide for optimizing the compositions to increase the stability of the sorbents for prolonged use as carbon dioxide capture matrices.

  20. LIFAC sorbent injection desulfurization demonstration project

    SciTech Connect

    Not Available

    1991-01-01

    LIFAC combines upper-furnace limestone injection followed by post-furnace humidification in an activation reactor located between the air preheater and the ESP. The process produces a dry and stable waste product that is partially removed from the bottom of the activation reactor and partially removed at the ESP.

  1. LIFAC Sorbent Injection Desulfurization Demonstration Project

    SciTech Connect

    Not Available

    1991-01-01

    LIFAC combines upper-furnace limestone injection followed by post- furnace humidification in an activation reactor located between the air preheater and the ESP. The process produces a dry and stable waste product that is partially removed from the bottom of the activation reactor and partially removed at the ESP. In November 1990, after a ten (10) month negotiation period, LIFAC NA and the US DOE entered into a Cooperative Agreement for the design, construction, and demonstration of the LIFAC system. This report is the fifth Technical Progress Report covering the period October 1, 1991 through the end of December 1991. Due to the power plant's planned outage schedule, and the time needed for engineering, design and procurement of critical equipment, DOE and LIFAC NA agreed to execute the Design Phase of the project in August 1990, with DOE funding contingent upon final signing of the Cooperative Agreement.

  2. Desulfurization of hot fuel gas produced from high-chlorine Illinois coals. Technical report, March 1, 1992--May 31, 1992

    SciTech Connect

    O`Brien, W.S.; Gupta, R.P.

    1992-10-01

    New coal gasification processes are now being developed which can generate electricity with high thermal efficiency either in an integrated gasification combined cycle (IGCC) or in a fuel cell (MCFC). Both of these new coal-to-electricity pathways require that the coal-derived fuel gas be at a high temperature and be free of potential pollutants, such as sulfur compounds. Unfortunately, some high-sulfur Illinois coals also contain significant chlorine which converts into hydrogen chloride (HCl) in the coal-gas. This project investigates the effect of HCl, in concentrations typical of a gasifier fed by high-chlorine Illinois coals, on zinc-titanate sorbents that are currently being developed for H{sub 2}S and COS removal from hot coal gas. This study is designed to identify any deleterious changes in the sorbent caused by the HCI, both in absorptive operation and in the regeneration cycle, and will pave the way to modify the sorbent formulation or the process operating procedure to remove HCl along with the H{sub 2}S and COS from hot coal gas. This will negate any harmful consequences of utilizing high-chlorine Illinois coal in these processes. The work activity during the third quarter of this project involved the performance of the second block-set of experiments in the bench-scale fluidized-bed reactor. These experiments were designed to study the effect of HCl in the desulfurization of a low-Btu fuel gas. Nine single-cycle experiments were performed, at operating temperature of 538, 650, and 750{degrees}C, with HCl concentrations of 0, 200, and 800 ppMv. The presence of HCl in the coal gas significantly enhanced the desulfurization efficacy of the sorbent. A 10-cycle sulfidation-regeneration sequence is currently being performed at 650{degrees}C with 800 ppMv HCl in the simulated fuel gas to determine any adverse effects on the sorbent structure or its desulfurization capability.

  3. Effect of operating parameters and reactor structure on moderate temperature dry desulfurization

    SciTech Connect

    Jie Zhang; Changfu You; Haiying Qi; Bo Hou; Changhe Chen; Xuchang Xu

    2006-07-01

    A moderate temperature dry desulfurization process at 600-800 C was studied in a pilot-scale circulating fluidized bed flue gas desulfurization (CFB-FGD) experimental facility. The desulfurization efficiency was investigated for various operating parameters. Structural improvements in key parts of the CFB-FGD system, i.e., the cyclone separator and the distributor, were made to improve the desulfurization efficiency and flow resistance. The experimental results show that the desulfurization efficiency increased rapidly with increasing temperature above 600 C due to enhanced gas diffusion and the shift of the equilibrium for the carbonate reaction. The sorbent sulfated gradually after quick carbonation of the sorbent with a long particle residence time necessary to realize a high desulfurization ratio. A reduced solids concentration in the bed reduced the particle residence time and the desulfurization efficiency. A single-stage cyclone separator produced no improvement in the desulfurization efficiency compared with a two-stage cyclone separator. Compared with a wind cap distributor, a large hole distributor reduced the flow resistance which reduced the desulfurization efficiency due to the reduced bed pressure drop and worsened bed fluidization. The desulfurization efficiency can be improved by increasing the collection efficiency of fine particles to prolong their residence time and by improving the solids concentration distribution to increase the gas-solid contact surface area. 16 refs., 9 figs.

  4. Effect of operating parameters and reactor structure on moderate temperature dry desulfurization.

    PubMed

    Zhang, Jie; You, Changfu; Qi, Haiying; Hou, Bo; Chen, Changhe; Xu, Xuchang

    2006-07-01

    A moderate temperature dry desulfurization process at 600-800 degrees C was studied in a pilot-scale circulating fluidized bed flue gas desulfurization (CFB-FGD) experimental facility. The desulfurization efficiency was investigated for various operating parameters, such as bed temperature, CO2 concentration, and solids concentration. In addition, structural improvements in key parts of the CFB-FGD system, i.e., the cyclone separator and the distributor, were made to improve the desulfurization efficiency and flow resistance. The experimental results show that the desulfurization efficiency increased rapidly with increasing temperature above 600 degrees C due to enhanced gas diffusion and the shift of the equilibrium for the carbonate reaction. The sorbent sulfated gradually after quick carbonation of the sorbent with a long particle residence time necessary to realize a high desulfurization ratio. A reduced solids concentration in the bed reduced the particle residence time and the desulfurization efficiency. A single-stage cyclone separator produced no improvement in the desulfurization efficiency compared with a two-stage cyclone separator. Compared with a wind cap distributor, a large hole distributor reduced the flow resistance which reduced the desulfurization efficiency due to the reduced bed pressure drop and worsened bed fluidization. The desulfurization efficiency can be improved by increasing the collection efficiency of fine particles to prolong their residence time and by improving the solids concentration distribution to increase the gas-solid contact surface area. PMID:16856750

  5. Investigation and demonstration of dry carbon-based sorbent injection for mercury control. Quarterly technical report, July 1, 1996--September 31, 1996

    SciTech Connect

    Hunt, T.; Sjostrom, S.; Smith, J.

    1996-11-06

    The overall objective of this two phase program is to investigate the use of dry carbon-based sorbents for mercury control. This information is important to the utility industry in anticipation of pending regulations. During Phase I, a bench-scale field test device that can be configured as an electrostatic precipitator, a pulse-jet baghouse, or a reverse-gas baghouse has been designed, built and integrated with an existing pilot-scale facility at PSCo`s Comanche Station. Up to three candidate sorbents will be injected into the flue gas stream upstream of the test device to and mercury concentration measurements will be made to determine the mercury removal efficiency for each sorbent. During the Phase II effort, component integration for the most promising dry sorbent technology shall be tested at the 5000 acfm pilot-scale.

  6. Investigation on durability and reactivity of promising metal oxide sorbents during sulfidation and regeneration. Quarterly report, January 1 - March 31, 1996

    SciTech Connect

    1996-12-31

    Research activities and efforts of this research project were concentrated on conducting experiments on initial reaction rates of hydrogen sulfide with the formulated sorbents, and developing a reaction rate equation containing a reaction rate constant in terms of disappearance of H{sub 2}S, a reaction order with respect to hydrogen sulfide, and a reaction order with respect to the TU-24 metal oxide sorbent.

  7. Sorbent suppliers

    SciTech Connect

    Vedder, M.

    1994-03-01

    Sorbents are used to absorb or contain spilled and leaking chemicals, oils, lubricants and other process fluids. They are commonly used around the base of machinery in industrial applications, and in remediating oil spills on land and water. Sorbents are made from biodegradable, inorganic or synthetic materials. Organic materials include corn cobs, wood pulp, paper fiber and cotton. Inorganic materials include clay, perlite, expanded silicates and expanded mica. Synthetic sorbents are made from petroleum- or plastic-based materials such as polyurethane, polyethylene or polypropylene. Sorbents are available in a variety of forms, including pads, rolls, booms, pillows and loose particulate.

  8. Advanced low-temperature sorbents

    SciTech Connect

    Ayala, R.E.; Venkataramani, V.S.; Abbasian, J.; Hill, A.H.

    1995-12-01

    A number of promising technologies are currently being optimized for coal-based power generation, including the Integrated-Gasification Combined Cycle (IGCC) system. If IGCC is to be used successfully for power generation, an economic and efficient way must be found to remove the contaminants, particularly sulfur species, found in coal gas. Except for the hot gas desulfurization system, all major components of IGCC are commercially available or have been shown to meet system requirements. Over the last two decades, the U.S. Department of Energy/Morgantown Energy Technology Center (DOE/METC) has sponsored development of various configurations of high-temperature desulfurization systems including fixed-bed, moving-bed, transport-bed, and fluidized-bed systems. Because of their mode of operation and requirements for sorbent manufacturing, the fixed-bed systems can generally use the same materials as moving-bed configurations, i.e., pelletized or extruded sorbents, while fluidized-bed (circulating or bubbling configurations) and transport reactor configurations use materials generally described as agglomerated or granulated.The objective of this program is to remove hydrogen sulfides from coal gas using sorbent materials.

  9. CURRENT STATUS OF ADVACATE PROCESS FOR FLUE GAS DESULFURIZATION

    EPA Science Inventory

    The following report discusses current bench- and pilot-plant advances in preparation of ADVAnced siliCATE (ADVACATE) calcium silicate sorbentsfor flue gas desulfurization. It also discusses current bench- and pilot-plant advances in sorbent preparation. Fly ash was ground in a l...

  10. ADVANCED SULFUR CONTROL CONCEPTS FOR HOT-GAS DESULFURIZATION TECHNOLOGY

    SciTech Connect

    A. LOPEZ ORTIZ; D.P. HARRISON; F.R. GROVES; J.D. WHITE; S. ZHANG; W.-N. HUANG; Y. ZENG

    1998-10-31

    This research project examined the feasibility of a second generation high-temperature coal gas desulfurization process in which elemental sulfur is produced directly during the sorbent regeneration phase. Two concepts were evaluated experimentally. In the first, FeS was regenerated in a H2O-O2 mixture. Large fractions of the sulfur were liberated in elemental form when the H2O-O2 ratio was large. However, the mole percent of elemental sulfur in the product was always quite small (<<1%) and a process based on this concept was judged to be impractical because of the low temperature and high energy requirements associated with condensing the sulfur. The second concept involved desulfurization using CeO2 and regeneration of the sulfided sorbent, Ce2O2S, using SO2 to produce elemental sulfur directly. No significant side reactions were observed and the reaction was found to be quite rapid over the temperature range of 500°C to 700°C. Elemental sulfur concentrations (as S2) as large as 20 mol% were produced. Limitations associated with the cerium sorbent process are concentrated in the desulfurization phase. High temperature and highly reducing coal gas such as produced in the Shell gasification process are required if high sulfur removal efficiencies are to be achieved. For example, the equilibrium H2S concentration at 800°C from a Shell gas in contact with CeO2 is about 300 ppmv, well above the allowable IGCC specification. In this case, a two-stage desulfurization process using CeO2 for bulk H2S removal following by a zinc sorbent polishing step would be required. Under appropriate conditions, however, CeO2 can be reduced to non-stoichiometric CeOn (n<2) which has significantly greater affinity for H2S. Pre-breakthrough H2S concentrations in the range of 1 ppmv to 5 ppmv were measured in sulfidation tests using CeOn at 700°C in highly reducing gases, as measured by equilibrium O2 concentration, comparable to the Shell gas. Good sorbent durability was indicated in

  11. High-volume, high-value usage of Flue Gas Desulfurization (FGD) by-products in underground mines Phase 1: Laboratory investigations. Quarterly report, July 1994--September 1994

    SciTech Connect

    1994-12-01

    During the quarter a second series of samples were collected and partially characterized chemically and mineralogically. The samples were collected at the disposal site operated by Freeman United Coal Co. The second collection was necessary because of deterioration due to hydration of the original samples. A study of the hydration characteristics was completed during the quarter. Important reactions included the immediate formation of ettringite and portlandite. The hydration and transformation was found to be a slow process. A second phase of gypsum formation from ettringite deterioration was identified. The slow hydration of anhydrite with its resultant swell is a potential problem which will be addressed further. Geotechnical characterization, during the quarter included completion of the preliminary characterization, analysis of the findings, experimentation with sample preparation for the final characterization/mix design, and design of the final experimental program. The analysis of the coals collected during the core drilling and hydrologic planning were completed. Also during the quarter a meeting was held with representatives of the shotcrete industry to discuss transport systems for emplacement. The pros and cons of pneumatic and hydraulic systems were discussed and plans formulated for further investigations.

  12. Enhancing the use of coals by gas reburning-sorbent injection. Environmental monitoring quarterly report No. 9, July 1--September 30, 1992

    SciTech Connect

    Not Available

    1992-11-16

    This Clean Coal Technology project will demonstrate a combination of two developed technologies to reduce both NO{sub x} and SO{sub x} emissions: gas reburning and calcium based dry sorbent injection. The demonstrations will be conducted on two pre-NSPS utility boilers representative of the US boilers which contribute significantly to the inventory of acid rain precursor emissions: tangentially and cyclone fired units. Gas reburning is a combustion modification technique that consists of firing 80--85 percent of the fuel (corresponding to the total heat release) in the lower furnace. Reduction of NO{sub x} to molecular nitrogen (N{sub 2}) is accomplished via the downstream injection of the remaining fuel requirement in the form of natural gas (which also reduces the total SO{sub x} emissions). In a third stage, burnout air is injected at lower temperatures in the upper furnace to complete the combustion process without generating significant additional NO{sub x}. Dry sorbent injection consists of injecting calcium based sorbents (such as limestone, dolomite, or hydrated lime) into the combustion products. For sulfation of the sorbent to CaSO{sub 4}, an injection temperature of about 1230{degrees}C is optimum, but calcium-sulfur reactions can also take place at lower temperatures. Thus, the sorbent may be injected at different locations, such as with the burnout air, at the exit from the superheater, or into the ducting downstream of the air heater with H{sub 2}0 added for humidification. The calcium sulfate or sulfite products are collected together with unreacted sorbent fly ash by the electrostatic precipitator. The specific goal of this project is to demonstrate NO{sub x} and SO{sub x} emission reductions of 60 percent and 50 percent, respectively, on two coal fired utility boilers having the design characteristics mentioned above.

  13. High-volume, high-value usage of flue gas desulfurization (FGD) by-products in underground mines - Phase I: Laboratory investigations. Quarterly report, October 1993--December 1993

    SciTech Connect

    Not Available

    1994-03-01

    This project proposes to use pneumatically or hydraulically emplaced dry-flue gas desulfurization (FGD) by-products to backfill the adits left by highwall mining. Backfilling highwall mine adits with dry-FGD materials is technically attractive. The use of an active highwall mine would allow the dry-FGD material to be brought in using the same transportation network used to move the coal out, eliminating the need to recreated the transportation infrastructure, thereby saving costs. Activities during the period included the negotiations leading to the final cooperative agreement for the project and the implementation of the necessary instruments at the University of Kentucky to administer the project. Early in the negotiations, a final agreement on a task structure was reached and a milestone plan was filed. A review was initiated of the original laboratory plan as presented in the proposal, and tentative modifications were developed. Selection of a mine site was made early; the Pleasant Valley mine in Greenup County was chosen. Several visits were made to the mine site to begin work on the hydrologic monitoring plan. The investigation of the types of permits needed to conduct the project was initiated. Considerations concerning the acceptance and implementation of technologies led to the choice of circulating fluidized bed ash as the primary material for the study. Finally, the membership of a Technical Advisory Committee for the study was assembled.

  14. Molecular biological enhancement of coal desulfurization: Cloning and expression of the sulfoxide/sulfone/sulfonate/sulfate genes in Pseudomonads and Thiobacillae. [Rhodococcus erythropolis, Thiobacillus acidophilus, Thiobacillus novellus

    SciTech Connect

    Krawiec, S.

    1992-01-01

    Research continues on desulfurization of coal using microorganisms. Topics reported on this quarter include: desulfurization with N1-36 (presumptively identified as Rhodochrous erythropolis), pulsed-field gel electrophoresis of chromosomal DNA's of Thiobacillus spp., and fresh isolates with the presumptive capacity to desulfurize dibenzothiophenes.

  15. High-volume, high-value usage of Flue Gas Desulfurization (FGD) by-products in underground mines. Phase 1 -- Laboratory Investigations. Quarterly report, January 1995--March 1995

    SciTech Connect

    1995-06-01

    The study of the kinetics of the mineral transformations which take place after the FGD materials are hydrated was continued this quarter (Task 2, Subtask 2.2). Based on X-ray diffraction data, the anhydrite was found to have essentially disappeared by the fifth day of the study, while gypsum was found to maximize in the first 14 days of the study. The relative abundance of ettringite increased throughout the period of observation (40 days). Ettringite was found to nucleate primarily on or near fly ash particles, while gypsum was found to be more mobile, readily filling in cracks and fractures. A second kinetic study was initiated during the period with an experimental setup which is similar to the current effort. The focus of this study will be to determine the effect of moisture conditions on the rate and types of mineralogical reactions which occur. Column leaching studies (Task 2, Subtask 2.4) on the ADM material were initiated during the quarter. Two columns were packed with fly ash and one with bottom ash. One of the columns was blanketed with CO{sub 2} (2.5%) to model the effects of soil gas on the leachate. The samples are being moisturized to model field conditions. Leachate analysis will be available during the next quarter. Work on the field site (Task 6) to establish background data for the demonstration continued. The proposed demonstration site at the Pleasant Valley mine was found to be displaying the effects of severe weathering. An alternate mine site will be explored.

  16. ADVANCED SORBENT DEVELOPMENT PROGRAM; DEVELOPMENT OF SORBENTS FOR MOVING-BED AND FLUIDIZED-BED APPLICATIONS

    SciTech Connect

    AYALA, R E; VENKATARAMANI, V S

    1998-09-30

    The integrated gasification combined cycle (IGCC) power system using high-temperature coal gas cleanup is one of the most promising advanced technologies for the production of electric power from coal in an environmentally acceptable manner. Unlike conventional low-temperature cleanup systems that require costly heat exchangers, high-temperature coal gas cleanup systems can be operated near 482-538 °C (900-1000 °F) or higher, conditions that are a closer match with the gasifier and turbine components in the IGCC system, thus resulting is a more efficient overall system. GE is developing a moving-bed, high-temperature desulfurization system for the IGCC power cycle in which zinc-based regenerable sorbents are currently being used as desulfurization sorbents. Zinc titanate and other proprietary zinc-based oxides are being considered as sorbents for use in the Clean Coal Technology Demonstration Program at Tampa Electric Co.'s (TECo) Polk Power Station. Under cold startup conditions at TECo, desulfurization and regeneration may be carried out at temperatures as low as 343 °C (650 °F), hence a versatile sorbent is desirable to perform over this wide temperature range. A key to success in the development of high-temperature desulfurization systems is the matching of sorbent properties for the selected process operating conditions, namely, sustainable desulfurization kinetics, high sulfur capacity, and mechanical durability over multiple cycles. Additionally, the sulfur species produced during regeneration of the sorbent must be in a form compatible with sulfur recovery systems, such as sulfuric acid or elemental sulfur processes. The overall objective of this program is to develop regenerable sorbents for hydrogen sulfide removal from coal-derived fuel gases in the temperature range 343-538 °C (650-1000 °F). Two categories of reactor configurations are being considered: moving-bed reactors and fluidized-bed (bubbling and circulating) reactors. In addition, a cost

  17. ADVANCED SORBENT DEVELOPMENT PROGRAM DEVELOPMENT OF SORBENTS FOR MOVING-BED AND FLUIDIZED-BED APPLICATIONS

    SciTech Connect

    R.E Ayala; V.S. Venkataramani; Javad Abbasian; Rachid B. Slimane; Brett E. Williams; Minoo K. Zarnegar; James R. Wangerow; Andy H. Hill

    2000-03-31

    The integrated gasification combined cycle (IGCC) power system using high-temperature coal gas cleanup is one of the most promising advanced technologies for the production of electric power from coal in an environmentally acceptable manner. Unlike conventional low-temperature cleanup systems that require costly heat exchangers, high-temperature coal gas cleanup systems can be operated near 482-538 C (900-1000 F) or higher, conditions that are a closer match with the gasifier and turbine components in the IGCC system, thus resulting is a more efficient overall system. GE is developing a moving-bed, high-temperature desulfurization system for the IGCC power cycle in which zinc-based regenerable sorbents are currently being used as desulfurization sorbents. Zinc titanate and other proprietary zinc-based oxides are being considered as sorbents for use in the Clean Coal Technology Demonstration Program at Tampa Electric Co.'s (TECo) Polk Power Station. Under cold startup conditions at TECo, desulfurization and regeneration may be carried out at temperatures as low as 343 C (650 F), hence a versatile sorbent is desirable to perform over this wide temperature range. A key to success in the development of high-temperature desulfurization systems is the matching of sorbent properties for the selected process operating conditions, namely, sustainable desulfurization kinetics, high sulfur capacity, and mechanical durability over multiple cycles. Additionally, the sulfur species produced during regeneration of the sorbent must be in a form compatible with sulfur recovery systems, such as sulfuric acid or elemental sulfur processes. The overall objective of this program is to develop regenerable sorbents for hydrogen sulfide removal from coal-derived fuel gases in the temperature range 343-538 C (650-1000 F). Two categories of reactor configurations are being considered: moving-bed reactors and fluidized-bed (bubbling and circulating) reactors. In addition, a cost assessment

  18. THE BIOCATALYTIC DESULFURIZATION PROJECT

    SciTech Connect

    Steven E. Bonde; David Nunn

    2003-01-01

    During the first quarter of the Biological Desulfurization project several activities were pursued. A project kickoff meeting was held at the Diversa facility in San Diego, CA. Activities that were in process before the meeting and begun afterwards by Diversa Corporation and Petro Star Inc. include: Technology transfer in the form of information generated by Enchira to Diversa, the purchase and installation of equipment by Diversa, development of synthetic methods and preparation of organo-sulfur substrates for use in determining enzyme activities, production of extract via Petro Star's CED process, detailed analysis of Petro Star Inc. diesel and CED extract, and several activities in molecular biology. Diversa Corporation, in the area of molecular biology, engaged in several activities in support of the task list of the contract. These included: construction of a genomic library; development and utilization of a sequence-based gene discovery effort; a parallel discovery approach based on functional expression of enzymes with the ability to oxidize organosulfur compounds. Biodesulfurization genes have already been identified and are being sequenced and subcloned for expression in heterologous biological hosts. Diversa has evaluated and adapted assays developed by Enchira used to assess the activities of DBT and DBTO{sub 2} monooxygenases. Finally, Diversa personnel have developed two novel selection/screen strategies for the improvement of biocatalyst strains by directed evolution.

  19. Enhancing the use of coals by gas reburning-sorbent injection. Quarterly report no. 6, September 1, 1988--November 30, 1988

    SciTech Connect

    Not Available

    1988-12-22

    The objective of this project is to evaluate and demonstrate a cost effective emission control technology for acid rain precursors, oxides of nitrogen (NO{sub x}) and sulfur (SO{sub x}), on three coal fired utility boilers in Illinois. The units selected are representative of pre-NSPS design practices; tangential, wall, and cyclone fired. The specific objectives are to demonstrate reductions of 60 percent in NO{sub x} and 50 percent in SO{sub x} emissions, by a combination of two developed technologies, gas reburning (GR) and sorbent injection (SI). With GR, about 80--85 percent of the coal fuel is fired in the primary combustion zone. The balance of the fuel is added downstream as natural gas to create a slightly fuel rich environment in which NO{sub x} is converted to N{sub 2}. The combustion process is completed by overfire air addition. SO{sub x} emissions are reduced by injecting dry sorbents (usually calcium based) into the upper furnace, at the superheater exit or into the ducting following the air heater. The sorbents trap SO{sub x} as solid sulfates and sulfites, which are collected in the particulate control device.

  20. High-volume, high-value usage of flue gas desulfurization (FGD) by- products in underground mines: Phase 1, Laboratory investigations. Quarterly report, April--June 1995

    SciTech Connect

    1995-09-01

    The kinetics study which is investigating hydration reactions of the ADM by-product (Subtask 2.2) was continued this quarter. This study further aided in gaining information on mineral precipitation and dissolution reactions during hydration of the ADM materials. The information is of importance for a comprehensive understanding of the factors that control strength and long-term stability during aging of FGD materials. The decision was made by Addington, Inc., DOE, and the University of Kentucky that the originally selected mine site for the emplacement demonstration must be changed, mainly for safety reasons. Mine selection will be a priority for the next quarter (Jul--Sep, 1995). Another activity during this reporting period was related to Subtask 4.3, the selection and testing of the transport system for the FGD material. A laboratory-scale pneumatic emplacement test unit (ETU) for dry FGD materials was built at the CAER to generate data so that a final selection of the field demonstration technology can be made. A dry pneumatic system was chosen for laboratory testing because the equipment and expertise available at the CAER matched this sort of technology best. While the design of the laboratory system was based on shotcrete technology, the physical properties of the emplaced FGD material is expected to be similar for other transport techniques, either pneumatic or hydraulic. In other words, the selection of a dry pneumatic transport system for laboratory testing does not necessarily imply that a scaled-up version will be used for the field demonstration. The ETU is a convenient means of producing samples for subsequent chemical and physical testing by a representative emplacement technology. Ultimately, the field demonstration technology will be chosen based on the laboratory data and the suitability of locally available equipment.

  1. Flue gas desulfurization wastewater treatment primer

    SciTech Connect

    Higgins, T.E.; Sandy, A.T.; Givens, S.W.

    2009-03-15

    Purge water from a typical wet flue gas desulfurization system contains myriad chemical constituents and heavy metals whose mixture is determined by the fuel source and combustion products as well as the stack gas treatment process. A well-designed water treatment system can tolerate upstream fuel and sorbent arranged in just the right order to produce wastewater acceptable for discharge. This article presents state-of-the-art technologies for treating the waste water that is generated by wet FGD systems. 11 figs., 3 tabs.

  2. High volume-high value usage of flue gas desulfurization (FGD) by-products in underground mines: Phase 2 -- Field investigations. Quarterly report, January 1--March 31, 1998

    SciTech Connect

    1998-09-01

    The factors that control the strength of FBC ash grout were the focus of work during this quarter. Samples were prepared at different water contents and placed into cylindrical PVC molds. At specified curing intervals, the grout cylinders were subjected to unconfined compressive strength testing as per procedures described in previous reports. Chemical, mineralogical, and microscopical analyses were also conducted on the samples. It was found that higher curing temperatures significantly increase the strength gain rate of the FBC ash grout, in agreement with earlier results. As expected, water content also exerts a strong influence on the strength of the grout. The compressive strength data obtained for the laboratory-prepared samples are in excellent agreement with strength data obtained on grout placed in auger holes during the field demonstrations. The data also indicate that the field samples suffered negligible deterioration over the course of the curing period in the auger holes. Analysis of the laboratory prepared grout samples using XRD revealed a mineralogy similar to the field samples. A correspondence between ettringite abundance and compressive strength was observed only during grout curing. The formation of minerals such as ettringite is apparently a good indication that curing reactions are progressing and that the grout strength is increasing, but mineral distribution by itself does not explain or predict final strength. The microscopy data, in combination with geotechnical and XRD data, suggest that the strength of the grout is largely a function of the density of an amorphous (or finely crystalline) material that comprises the majority of the cured grout. Therefore, an increase in density of this material results in an increase in grout strength.

  3. Flue gas desulfurization: Physicochemical and biotechnological approaches

    SciTech Connect

    Pandey, R.A.; Biswas, R.; Chakrabarti, T.; Devotta, S.

    2005-07-01

    Various flue gas desulfurization processes - physicochemical, biological, and chemobiological - for the reduction of emission of SO{sub 2} with recovery of an economic by-product have been reviewed. The physicochemical processes have been categorized as 'once-through' and 'regenerable.' The prominent once-through technologies include wet and dry scrubbing. The wet scrubbing technologies include wet limestone, lime-inhibited oxidation, limestone forced oxidation, and magnesium-enhanced lime and sodium scrubbing. The dry scrubbing constitutes lime spray drying, furnace sorbent injection, economizer sorbent injection, duct sorbent injection, HYPAS sorbent injection, and circulating fluidized bed treatment process. The regenerable wet and dry processes include the Wellman Lord's process, citrate process, sodium carbonate eutectic process, magnesium oxide process, amine process, aqueous ammonia process, Berglau Forchung's process, and Shell's process. Besides these, the recently developed technologies such as the COBRA process, the OSCAR process, and the emerging biotechnological and chemobiological processes are also discussed. A detailed outline of the chemistry, the advantages and disadvantages, and the future research and development needs for each of these commercially viable processes is also discussed.

  4. HIGH EFFICIENCY DESULFURIZATION OF SYNTHESIS GAS

    SciTech Connect

    Kwang-Bok Yi; Anirban Mukherjee; Elizabeth J. Podlaha; Douglas P. Harrison

    2004-03-01

    Mixed metal oxides containing ceria and zirconia have been studied as high temperature desulfurization sorbents with the objective of achieving the DOE Vision 21 target of 1 ppmv or less H{sub 2}S in the product gas. The research was justified by recent results in this laboratory that showed that reduced CeO{sub 2}, designated CeOn (1.5 < n < 2.0), is capable of achieving the 1 ppmv target in highly reducing gas atmospheres. The addition of ZrO{sub 2} has improved the performance of oxidation catalysts and three-way automotive catalysts containing CeO{sub 2}, and was postulated to have similar beneficial effects on CeO{sub 2} desulfurization sorbents. An electrochemical method for synthesizing CeO{sub 2}-ZrO{sub 2} mixtures was developed and the products were characterized by XRD and TEM during year 01. Nanocrystalline particles having a diameter of about 5 nm and containing from approximately 10 mol% to 80 mol% ZrO{sub 2} were prepared. XRD analysis showed the product to be a solid solution at low ZrO{sub 2} contents with a separate ZrO{sub 2} phase emerging at higher ZrO{sub 2} levels. Unfortunately, the quantity of CeO{sub 2}-ZrO{sub 2} that could be prepared electrochemically was too small to permit desulfurization testing. Also during year 01 a laboratory-scale fixed-bed reactor was constructed for desulfurization testing. All components of the reactor and analytical systems that were exposed to low concentrations of H{sub 2}S were constructed of quartz, Teflon, or silcosteel. Reactor product gas composition as a function of time was determined using a Varian 3800 gas chromatograph equipped with a pulsed flame photometric detector (PFPD) for measuring low H{sub 2}S concentrations from approximately 0.1 to 10 ppmv, and a thermal conductivity detector (TCD) for higher concentrations of H{sub 2}S. Larger quantities of CeO{sub 2}-ZrO{sub 2} mixtures from other sources, including mixtures prepared in this laboratory using a coprecipitation procedure, were obtained

  5. FLUE GAS DESULFURIZATION INFORMATION SYSTEM (FGDIS) DATA BASE USER'S MANUAL

    EPA Science Inventory

    The document is a user's manual and reference book/primer for Flue Gas Desulfurization Information System (FGDIS) users and recipients of the quarterly Utility FGD Survey. Part I, interactive computer procedures for the FGDIS, addresses the use of and terminology related to the u...

  6. Study on the stability of sorbents removing H{sub 2}S from hot coal gas

    SciTech Connect

    Li-Ping Chang; Zong-You Zhang; Xiu-Rong Ren; Fan Li; Ke-Chang Xie

    2009-01-15

    Mixed metal oxide containing iron with the high-sulfur capacity and reactivity is considered as one of the most favorable sorbents for desulfurization in hot gas. The stability and life of iron-based sorbents are the main challenges for the hot gas cleanup techniques. Not only the effect of gas atmosphere but also the effect of ZnO and MgO on the stability of iron-based sorbent was studied in this work. The mechanism and factors influencing sorbent stability are discussed. The results showed that the coexistence of CO and H{sub 2} result in the instability of the zinc-iron-based sorbents. The reaction of carbon deposit is the crucial step affecting the stability of sorbent for hot gas desulfurization. ZnO in the sorbent is adverse to the physical stability of the iron-based sorbents. MgO in the sorbent hardly affects the physical stability of the iron-based sorbents but improves the capacity of removing the hydrogen sulfide from hot coal gas at 773 K. 12 refs., 8 figs., 5 tabs.

  7. Laboratory evaluation of high-temperature sulfur removal sorbents for direct coal-fired turbines: Final report

    SciTech Connect

    Newby, R.A.; DeZubay, E.A.; Chamberlin, R.M.

    1987-06-01

    Direct coal-fired turbine concepts currently being developed require substantial levels of sulfur removal from high-temperature gas streams. Calcium-based sorbents, limestones, dolomites, limes and lime hydrates, are capable of sulfur removal in direct coal-fired turbine combustor environments at temperature up to 1200/degree/C. Two types of desulfurizer processes are considered in this report using calcium- based sorbents: fluidized bed desulfurizer using coarse sorbent particles (300-1000 ..mu..m), and entrained desulfurizer using fine sorbent particles (1-40 ..mu..m). Small-scale laboratory tests were performed on a variety of calcium-based sorbents to determine the kinetics of sulfation and sulfidation over ranges of conditions applicable to both types of desulfurizer processes. Correlations are developed in the report for the effect of pressure; temperature, and particle size. Engineering models are also developed for both desulfurizer types that incorporate the laboratory reaction kinetics and predict potential commercial performance and performance trends. It is concluded that both desulfurizer concepts can be effective in direct coal-fired turbines, with calcium-to-sulfur molar feed ratios ranging from 1.5 to 3.0, if the correct calcium-based sorbent is selected, and if applicable design and operating conditions are identified. Both desulfurizer concepts have limitations and key development requirements, and site and fuel specific engineering assessment is required to select the best concept for a given combustor system. The influence of the desulfurizer concepts on turbine protection, through their influence on particle loading and alkali release must also be assessed. 51 refs., 73 figs., 9 tabs.

  8. Development of regenerable copper-based sorbents for hot gas cleanup: Final technical report, September 1, 1995--August 31, 1996

    SciTech Connect

    Abbasian, J.; Slimane, R.B.; Wangerow, J.R.

    1997-05-01

    The overall objective of this study was to determine the effectiveness of the copper-chromite sorbent (developed in previous ICCI-funded projects) for longer duration application under optimum conditions in the temperature range of 550{degrees}-650{degrees}C to minimize sorbent reduction and degradation during the cyclic process. Three (3) formulations of attrition resistant granules of the copper chromite sorbent (i.e., CuCr-10, CuCr-21, and CuCr-29) as well as one (1) copper chromite sorbent in pellet form (i.e., CuCr-36) were selected for cyclic desulfurization tests. The desulfurization and regeneration capabilities of the selected formulations as well as the effects of operating parameters were determined, to identify the {open_quotes}best{close_quotes} sorbent formulation and the optimum operating conditions. The durability of the {open_quotes}best{close_quotes} sorbent formulation was determined in {open_quotes}long-term{close_quotes} multicycle tests conducted at the optimum operating conditions. The attrition resistance of the selected formulations were determined and compared with those of other sorbents, including a limestone, a dolomite, and a commercial zinc titanate sorbent. The results obtained in this study indicate that, the CuCr-29 sorbent has excellent attrition resistance and desulfurization performance, which are far superior to the commercial zinc titanate sorbents. The optimum desulfurization temperature in terms of sorbent efficiency and utilization appears to be about 600{degrees}C. Sorbent regeneration at 750{degrees}C ensured complete conversion of the copper sulfide to oxide without sulfate formation or reactivity deterioration in subsequent cycles.

  9. Theoretical approach for enhanced mass transfer effects in-duct flue gas desulfurization processes

    SciTech Connect

    Not Available

    1990-08-22

    While developing dry sorbent duct injection flue gas desulfurization processes may offer significant improvement in capital cost and process simplicity compared to wet scrubbing systems, the economics of this technology can be improved significantly by an improvement in sorbent utilization. While a general understanding of the mechanism by which the sorbents operate is known, a much more detailed knowledge of reaction rate-controlling phenomena, the role of inherent reactivity, and mass transfer effects and their interaction in needed. Objectives of this project are threefold: 1. Mass transfer investigation--determine the controlling physical and chemical processes that limit sorbent utilization. In particular, determine whether mass transfer is a controlling factor in in-duct flue gas desulfurization and establish the relative contributions of gas- and liquid-phase mass transfer and inherent sorbent reactivity. 2. Field test support--evaluate various sorbents, operating conditions and process schemes to support large-scale field testings at Meredosia and Beverly. 3. Mass transfer enhancement--examine various techniques that will enable sorbent utilization rates of at least 75 percent to be achieved. Sorbents investigated were Ca(OH){sub 2}, Mississippi hydrate and Mississippi slaked lime. Epsom Salt was investigated as an additive. Agglomeration of Ca(OH){sub 2} solids was also investigated. 3 refs., 92 figs., 23 tabs.

  10. HIGH EFFICIENCY DESULFURIZATION OF SYNTHESIS GAS

    SciTech Connect

    Kwang-Bok Yi; Elizabeth J. Podlaha; Douglas P. Harrison

    2002-11-01

    Mixed metal oxides containing CeO{sub 2} and ZrO{sub 2} are being studied as high temperature desulfurization sorbents capable of achieving the DOE Vision 21 target of 1 ppmv or less H{sub 2}S. The research is justified by recent results in this laboratory that showed that reduced CeO{sub 2}, designated CeO{sub n} (1.5 < n < 2.0), is capable of achieving the 1 ppmv target in highly reducing gas atmospheres. The addition of ZrO{sub 2} has improved the performance of oxidation catalysts and three-way automotive catalysts containing CeO{sub 2}, and should have similar beneficial effects on CeO{sub 2} desulfurization sorbents. An electrochemical method for synthesizing CeO{sub 2}-ZrO{sub 2} was developed and the products were characterized by XRD and TEM during year 01. Nanocrystalline particles having a diameter of about 5 nm and containing from approximately 10 mol% to 80 mol% ZrO{sub 2} were prepared. XRD showed the product to be a solid solution at low ZrO{sub 2} contents with a separate ZrO{sub 2} phase emerging at higher ZrO{sub 2} levels. Unfortunately, the quantity of CeO{sub 2}-ZrO{sub 2} that could be prepared electrochemically was too small to permit full testing in our desulfurization reactor. Also during year 01 a laboratory-scale fixed-bed reactor was constructed for desulfurization testing. All components of the reactor and analytical systems that may be exposed to low concentrations of H{sub 2}S are constructed of quartz, Teflon, or silcosteel. Reactor product gas composition as a function of time is determined using a Varian 3800 gas chromatograph equipped with a pulsed flame photometric detector (PFPD) for measuring low H{sub 2}S concentrations ({approx}< 10 ppmv) and a thermal conductivity detector (TCD) for higher concentrations of H{sub 2}S. Larger quantities of CeO{sub 2}-ZrO{sub 2} mixtures from other sources, including mixtures prepared in this laboratory using a coprecipitation procedure, have been obtained. Characterization and desulfurization

  11. Low temperature SO{sub 2} removal with solid sorbents in a circulating fluidized bed absorber. Quarterly report, May 1--July 31, 1992

    SciTech Connect

    Lee, S.K.; Keener, T.C.

    1992-08-12

    The nozzle installed in the circulating fluidized bed absorber (CFBA) was slightly modified because of a technical difficulty in making the small holes less than 100 {mu}m. The holes were punctured with a very tiny drill bits in diameter of 275 {mu}m, and the number of holes were adjusted. The 951 TGA (Du Pont Co.) was also modified for the kinetic information on the hydration and sulfation of limes under low temperatures. The modified thermalgravimetric analyzer (TGA) includes a syringe in order to simulate the water sprayings in a CFBA. Water droplets through the needle attached to the syringe are added onto the lime sample in a TGA. Two discrete ranges of Dravo limes were prepared as solid sorbents for sulfation tests. One ranged between 1095 {mu}m (16 mesh) and 2380 {mu}m (8 mesh) in diameter and the other ranged between 595 {mu}m (30 mesh) and 1095 {mu}m (16 mesh). The experimental methods for kinetic studies with TGA and for CFBA operation were established through the pre-operation of CFBA.

  12. Anion-exchange resin-based desulfurization process

    SciTech Connect

    Sheth, A.C.; Dharmapurikar, R.

    1992-01-01

    Under DOE Grant No. DE-FG22-90PC90309, the University of Tennessee Space Institute (UTSI) is contracted to further develop its anion-exchange, resin-based desulfurization concept to desulfurize alkali metal sulfates. From environmental as well as economic viewpoints, it is necessary to remove soluble sulfates from the wastes created by flue gas desulfurization systems. In order to do this economically, a low-cost desulfurization process for spent sorbents is necessary. UTSI's anion-exchange resin-based desulfurization concept is believed to satisfy these requirements. During the reporting period, October 1, 1992--December 31, 1992, UTSI has completed the batch mode experiments to evaluate the performance enhancement effect caused by organic acids on the resin's exhaustion efficiency. At present, batch mode experiments are being conducted to locate the position of the CO[sub 3]= and SO[sub 4]= ions in the affinity chart, and also reviewing/assessing the ASPEN Code's capabilities for use in the development of the Best Process Schematic and related economics.

  13. MODELING OF SO2 REMOVAL IN SPRAY-DRYER FLUE-GAS DESULFURIZATION SYSTEM

    EPA Science Inventory

    The report presents a comprehensive mathematical model of the SO2 removal process in a spray-dryer flue-gas desulfurization system. Simultaneous evaporation of a sorbent droplet and absorption/reaction of SO2 in the droplet are described by the corresponding heat- and mass-transf...

  14. Integration and testing of hot desulfurization and entrained-flow gasification for power generation systems

    SciTech Connect

    Robin, A.M.; Kassman, J.S.; Leininger, T.F.; Wolfenbarger, J.K.; Wu, C.M.; Yang, P.P.

    1991-09-01

    This second Topical Report describes the work that was completed between January 1, 1989 and December 31, 1990 in a Cooperative Agreement between Texaco and the US Department of Energy that began on September 30, 1987. During the period that is covered in this report, the development and optimization of in-situ and external desulfurization processes were pursued. The research effort included bench scale testing, PDU scoping tests, process economic studies and advanced instrument testing. Two bench scale studies were performed at the Research Triangle Institute with zinc titanate sorbent to obtain data on its cycle life, sulfur capacity, durability and the effect of chlorides. These studies quantify sulfur capture during simulated air and oxygen-blown gasification for two zinc titanate formulations. Eight PDU runs for a total of 20 days of operation were conducted to evaluate the performance of candidate sorbents for both in-situ and external desulfurization. A total of 47 tests were completed with oxygen and air-blown gasification. Candidate sorbents included iron oxide for in-situ desulfurization and calcium based and mixed metal oxides for external desulfurization. Gasifier performance and sorbent sulfur capture are compared for both air-blown and oxygen-blown operation.

  15. Crude oil desulfurization

    NASA Technical Reports Server (NTRS)

    Kalvinskas, J. J.; Hsu, G. C.; Ernest, J. B. (Inventor)

    1982-01-01

    High sulfur crude oil is desulfurized by a low temperature (25-80 C.) chlorinolysis at ambient pressure in the absence of organic solvent or diluent but in the presence of water (water/oil=0.3) followed by a water and caustic wash to remove sulfur and chlorine containing reaction products. The process described can be practiced at a well site for the recovery of desulfurized oil used to generate steam for injection into the well for enhanced oil recovery.

  16. Metal sulfide initiators for metal oxide sorbent regeneration

    DOEpatents

    Turk, Brian S.; Gupta, Raghubir P.

    1999-01-01

    A process of regenerating a sulfided sorbent is provided. According to the process of the invention, a substantial portion of the energy necessary to initiate the regeneration reaction is provided by the combustion of a particulate metal sulfide additive. In using the particulate metal sulfide additive, the oxygen-containing gas used to regenerate the sulfided sorbent can be fed to the regeneration zone without heating or at a lower temperature than used in conventional processes wherein the regeneration reaction is initiated only by heating the oxygen-containing. The particulate metal sulfide additive is preferably an inexpensive mineral ore such as iron pyrite which does not adversely affect the regeneration or corresponding desulfurization reactions. The invention further includes a sorbent composition comprising the particulate metal sulfide additive in admixture with an active metal oxide sorbent capable of removing one or more sulfur compounds from a sulfur-containing gas stream.

  17. Metal sulfide initiators for metal oxide sorbent regeneration

    DOEpatents

    Turk, Brian S.; Gupta, Raghubir P.

    2001-01-01

    A process of regenerating a sulfided sorbent is provided. According to the process of the invention, a substantial portion of the energy necessary to initiate the regeneration reaction is provided by the combustion of a particulate metal sulfide additive. In using the particulate metal sulfide additive, the oxygen-containing gas used to regenerate the sulfided sorbent can be fed to the regeneration zone without heating or at a lower temperature than used in conventional processes wherein the regeneration reaction is initiated only by heating the oxygen-containing gas. The particulate metal sulfide additive is preferably an inexpensive mineral ore such as iron pyrite which does not adversely affect the regeneration or corresponding desulfurization reactions. The invention further includes a sorbent composition comprising the particulate metal sulfide additive in admixture with an active metal oxide sorbent capable of removing one or more sulfur compounds from a sulfur-containing gas stream.

  18. Novel Sorbent to Clean Up Biogas for CHPs

    SciTech Connect

    Alptekin, Gökhan O.; Jayataman, Ambalavanan; Schaefer, Matthew; Ware, Michael; Hunt, Jennifer; Dobek, Frank

    2015-05-30

    In this project, TDA Research Inc. (TDA) has developed low-cost (on a per unit volume of gas processed basis), high-capacity expendable sorbents that can remove both the H2S and organic sulfur species in biogas to the ppb levels. The proposed sorbents will operate downstream of a bulk desulfurization system as a polishing bed to provide an essentially sulfur-free gas to a fuel cell (or any other application that needs a completely sulfur-free feed). Our sorbents use a highly dispersed mixed metal oxides active phase with desired modifiers prepared over on a mesoporous support. The support structure allows the large organic sulfur compounds (such as the diethyl sulfide and dipropyl sulfide phases with a large kinetic diameter) to enter the sorbent pores so that they can be adsorbed and removed from the gas stream.

  19. Metal sulfide initiators for metal oxide sorbent regeneration

    DOEpatents

    Turk, B.S.; Gupta, R.P.

    1999-06-22

    A process of regenerating a sulfided sorbent is provided. According to the process of the invention, a substantial portion of the energy necessary to initiate the regeneration reaction is provided by the combustion of a particulate metal sulfide additive. In using the particulate metal sulfide additive, the oxygen-containing gas used to regenerate the sulfided sorbent can be fed to the regeneration zone without heating or at a lower temperature than used in conventional processes wherein the regeneration reaction is initiated only by heating the oxygen-containing gas. The particulate metal sulfide additive is preferably an inexpensive mineral ore such as iron pyrite which does not adversely affect the regeneration or corresponding desulfurization reactions. The invention further includes a sorbent composition comprising the particulate metal sulfide additive in admixture with an active metal oxide sorbent capable of removing one or more sulfur compounds from a sulfur-containing gas stream. 1 fig.

  20. HIGH EFFICIENCY DESULFURIZATION OF SYNTHESIS GAS

    SciTech Connect

    Kwang-Bok Yi; Elizabeth J. Podlaha; Douglas P. Harrison

    2003-11-01

    Mixed metal oxides containing CeO{sub 2} and ZrO{sub 2} are being studied as high temperature desulfurization sorbents capable of achieving the DOE Vision 21 target of 1 ppmv or less H{sub 2}S. The research is justified by recent results in this laboratory that showed that reduced CeO{sub 2}, designated CeOn (1.5 < n < 2.0), is capable of achieving the 1 ppmv target in highly reducing gas atmospheres. The addition of ZrO{sub 2} has improved the performance of oxidation catalysts and three-way automotive catalysts containing CeO{sub 2}, and should have similar beneficial effects on CeO{sub 2} desulfurization sorbents. An electrochemical method for synthesizing CeO{sub 2}-ZrO{sub 2} was developed and the products were characterized by XRD and TEM during year 01. Nanocrystalline particles having a diameter of about 5 nm and containing from approximately 10 mol% to 80 mol% ZrO{sub 2} were prepared. XRD analysis showed the product to be a solid solution at low ZrO{sub 2} contents with a separate ZrO{sub 2} phase emerging at higher ZrO{sub 2} levels. Unfortunately, the quantity of CeO{sub 2}-ZrO{sub 2} that could be prepared electrochemically was too small to permit full desulfurization testing. Also during year 01 a laboratory-scale fixed-bed reactor was constructed for desulfurization testing. All components of the reactor and analytical systems that may be exposed to low concentrations of H{sub 2}S are constructed of quartz, Teflon, or silcosteel. Reactor product gas composition as a function of time is determined using a Varian 3800 gas chromatograph equipped with a pulsed flame photometric detector (PFPD) for measuring low H{sub 2}S concentrations (<{approx}10 ppmv) and a thermal conductivity detector (TCD) for higher concentrations of H{sub 2}S. Larger quantities of CeO{sub 2}-ZrO{sub 2} mixtures from other sources, including mixtures prepared in this laboratory using a coprecipitation procedure, have been obtained. Much of the work during year 02 consisted of

  1. HIGH EFFICIENCY DESULFURIZATION OF SYNTHESIS GAS

    SciTech Connect

    Anirban Mukherjee; Kwang-Bok Yi; Elizabeth J. Podlaha; Douglas P. Harrison

    2001-11-01

    Mixed metal oxides containing CeO{sub 2} and ZrO{sub 2} are being studied as high temperature desulfurization sorbents capable of achieving the DOE Vision 21 target of 1 ppmv of less H{sub 2}S. The research is justified by recent results in this laboratory that showed that reduced CeO{sub 2}, designated CeO{sub n} (1.5 < n < 2.0), is capable of achieving the 1 ppmv target in highly reducing gas atmospheres. The addition of ZrO{sub 2} has improved the performance of oxidation catalysts and three-way automotive catalysts containing CeO{sub 2}, and should have similar beneficial effects on CeO{sub 2} desulfurization sorbents. An electrochemical method for synthesizing CeO{sub 2}-ZrO{sub 2} has been developed and the products have been characterized by XRD and TEM during year 01. Nanocrystalline particles having a diameter of about 5 nm and containing from approximately 10 mol% to 80 mol% ZrO{sub 2} have been prepared. XRD showed the product to be a solid solution at low ZrO{sub 2} contents with a separate ZrO{sub 2} phase emerging at higher ZrO{sub 2} levels. Phase separation did not occur when the solid solutions were heat treated at 700 C. A flow reactor system constructed of quartz and teflon has been constructed, and a gas chromatograph equipped with a pulsed flame photometric detector (PFPD) suitable for measuring sub-ppmv levels of H{sub 2}S has been purchased with LSU matching funds. Preliminary desulfurization tests using commercial CeO{sub 2} and CeO{sub 2}-ZrO{sub 2} in highly reducing gas compositions has confirmed that CeO{sub 2}-ZrO{sub 2} is more effective than CeO{sub 2} in removing H{sub 2}S. At 700 C the product H{sub 2}S concentration using CeO{sub 2}-ZrO{sub 2} sorbent was near the 0.1 ppmv PFPD detection limit during the prebreakthrough period.

  2. Pilot plant tests of Z-Sorb{trademark} sorbent

    SciTech Connect

    Greenwood, G.J.; Khare, G.P.; Kubicek, D.H.; Delzer, G.A.; Kinsinger, D.L.

    1995-06-01

    The objective of this work is to determine the long-term chemical reactivity and mechanical durability of Phillips Petroleum Company`s (PPCo`s) proprietary Z-Sorb{trademark} sorbent. Materials developed for fixed-, moving- and fluid bed desulfurization of coal derived gases at high pressure (5-20 atm) and moderate operating temperatures (600-1000{degrees}F) will be discussed.

  3. Flue gas desulfurization method and apparatus

    DOEpatents

    Madden, Deborah A.; Farthing, George A.

    1998-08-18

    A combined furnace limestone injection and dry scrubber flue gas desulfurization (FGD) system collects solids from the flue gas stream in first particulate collection device located downstream of an outlet of a convection pass of the furnace and upstream of the dry scrubber. The collected solids are diverted to the dry scrubber feed slurry preparation system to increase sulfur oxide species removal efficiency and sorbent utilization. The level of lime in the feed slurry provided to the dry scrubber is thus increased, which enhances removal of sulfur oxide species in the dry scrubber. The decreased particulate loading to the dry scrubber helps maintain a desired degree of free moisture in the flue gas stream entering the dry scrubber, which enhances sulfur oxide species removal both in the dry scrubber and downstream particulate collector, normally a baghouse.

  4. Flue gas desulfurization method and apparatus

    DOEpatents

    Madden, D.A.; Farthing, G.A.

    1998-08-18

    A combined furnace limestone injection and dry scrubber flue gas desulfurization (FGD) system collects solids from the flue gas stream in first particulate collection device located downstream of an outlet of a convection pass of the furnace and upstream of the dry scrubber. The collected solids are diverted to the dry scrubber feed slurry preparation system to increase sulfur oxide species removal efficiency and sorbent utilization. The level of lime in the feed slurry provided to the dry scrubber is thus increased, which enhances removal of sulfur oxide species in the dry scrubber. The decreased particulate loading to the dry scrubber helps maintain a desired degree of free moisture in the flue gas stream entering the dry scrubber, which enhances sulfur oxide species removal both in the dry scrubber and downstream particulate collector, normally a baghouse. 5 figs.

  5. Flue gas desulfurization method and apparatus

    DOEpatents

    Madden, Deborah A.; Farthing, George A.

    1998-09-29

    A combined furnace limestone injection and dry scrubber flue gas desulfurization (FGD) system collects solids from the flue gas stream in first particulate collection device located downstream of an outlet of a convection pass of the furnace and upstream of the dry scrubber. The collected solids are diverted to the dry scrubber feed slurry preparation system to increase sulfur oxide species removal efficiency and sorbent utilization. The level of lime in the feed slurry provided to the dry scrubber is thus increased, which enhances removal of sulfur oxide species in the dry scrubber. The decreased particulate loading to the dry scrubber helps maintain a desired degree of free moisture in the flue gas stream entering the dry scrubber, which enhances sulfur oxide species removal both in the dry scrubber and downstream particulate collector, normally a baghouse.

  6. Flue gas desulfurization method and apparatus

    DOEpatents

    Madden, D.A.; Farthing, G.A.

    1998-09-29

    A combined furnace limestone injection and dry scrubber flue gas desulfurization (FGD) system collects solids from the flue gas stream in first particulate collection device located downstream of an outlet of a convection pass of the furnace and upstream of the dry scrubber. The collected solids are diverted to the dry scrubber feed slurry preparation system to increase sulfur oxide species removal efficiency and sorbent utilization. The level of lime in the feed slurry provided to the dry scrubber is thus increased, which enhances removal of sulfur oxide species in the dry scrubber. The decreased particulate loading to the dry scrubber helps maintain a desired degree of free moisture in the flue gas stream entering the dry scrubber, which enhances sulfur oxide species removal both in the dry scrubber and downstream particulate collector, normally a baghouse. 5 figs.

  7. Recent advances in flue gas desulfurization technologies

    SciTech Connect

    Pan, Y.S.

    1991-01-01

    Recent advances in flue gas desulfurization (FGD) technologies are reported. The technological advances include conventional wet FGD system improvements, advanced wet FGD system development, spray dryer system operations, technologies for furnace sorbent injections, post-combustion dry technologies, combined SO{sub 2}/NO{sub x} technologies, and several emerging FGD technologies. In addition, progress of by-product utilization that affects the operating cost of FGD systems is described. Economics of some commercially available and nearly maturing FGD technologies is also discussed. The materials included in this report are obtained from technical presentations made through September 1990, at several national and international conferences. This report is intended to document current advances and status of various FGD technologies. 101 refs., 16 figs.

  8. Effect of sorbent attrition on utilization. Final report

    SciTech Connect

    Keener, T.C.; Khang, S.J.; Li, G.

    1993-09-30

    The overall objective for 1992-1993 was to investigate ways of using chemical attrition to improve dolomitic sorbent utilization for duct injection processes. It is known that one of the primary mechanisms for poor sorbent utilization lies in the fact that the products of SO{sub 2}-sorbent reactions have such large molar volumes that they plug the pores necessary for SO{sub 2} to diffuse into the particle interior. Any method that may cause the fracture of used sorbent particles will thus expose fresh un-reacted surface of sorbent and result in available sorbent recovery. There are several mechanisms that may cause the breakage of particles. External mechanical stress may be exerted on a particle and cause particle fracture when it exceeds the cohesive forces to prevent the breakage. Heat and pressure can also induce particle fracture. In addition, chemical reaction is also a very important factor in leading to particle fracture. Among many sorbents currently used in desulfurization processes, dolomitic lime may be a good candidate for use in medium temperature duct injection. Dolomites are characterized by a large portion of magnesium (instead of high calcium) in the crystal structure of common limestones. Because of the special composition of dolomitic lime and its reactions with flue gas constituents under medium temperature duct injection conditions, a unique structure is formed for spent dolomitic particles that provides for the potential of recovering available sorbent just by hydration-induced particle fracture. By re-injecting the recovered sorbent, it is expected that a high sorbent utilization can be obtained.

  9. Fluidized bed coal desulfurization

    NASA Technical Reports Server (NTRS)

    Ravindram, M.

    1983-01-01

    Laboratory scale experiments were conducted on two high volatile bituminous coals in a bench scale batch fluidized bed reactor. Chemical pretreatment and posttreatment of coals were tried as a means of enhancing desulfurization. Sequential chlorination and dechlorination cum hydrodesulfurization under modest conditions relative to the water slurry process were found to result in substantial sulfur reductions of about 80%. Sulfur forms as well as proximate and ultimate analyses of the processed coals are included. These studies indicate that a fluidized bed reactor process has considerable potential for being developed into a simple and economic process for coal desulfurization.

  10. High-Temperature Desulfurization of Heavy Fuel-Derived Reformate Gas Streams for SOFC Applications

    NASA Technical Reports Server (NTRS)

    Flytzani-Stephanopoulos, Maria; Surgenor, Angela D.

    2007-01-01

    Desulfurization of the hot reformate gas produced by catalytic partial oxidation or autothermal reforming of heavy fuels, such as JP-8 and jet fuels, is required prior to using the gas in a solid oxide fuel cell (SOFC). Development of suitable sorbent materials involves the identification of sorbents with favorable sulfidation equilibria, good kinetics, and high structural stability and regenerability at the SOFC operating temperatures (650 to 800 C). Over the last two decades, a major barrier to the development of regenerable desulfurization sorbents has been the gradual loss of sorbent performance in cyclic sulfidation and regeneration at such high temperatures. Mixed oxide compositions based on ceria were examined in this work as regenerable sorbents in simulated reformate gas mixtures and temperatures greater than 650 C. Regeneration was carried out with dilute oxygen streams. We have shown that under oxidative regeneration conditions, high regeneration space velocities (greater than 80,000 h(sup -1)) can be used to suppress sulfate formation and shorten the total time required for sorbent regeneration. A major finding of this work is that the surface of ceria and lanthanan sorbents can be sulfided and regenerated completely, independent of the underlying bulk sorbent. This is due to reversible adsorption of H2S on the surface of these sorbents even at temperatures as high as 800 C. La-rich cerium oxide formulations are excellent for application to regenerative H2S removal from reformate gas streams at 650 to 800 C. These results create new opportunities for compact sorber/regenerator reactor designs to meet the requirements of solid oxide fuel cell systems at any scale.

  11. Development of advanced hot-gas desulfurization processes

    SciTech Connect

    Jothimurugesan, K.

    1999-04-26

    Advanced integrated gasification combined cycle (IGCC) power plants nearing completion, such as Sierra-Pacific, employ a circulating fluidized-bed (transport) reactor hot-gas desulfurization (HGD) process that uses 70-180 {micro}m average particle size (aps) zinc-based mixed-metal oxide sorbent for removing H{sub 2}S from coal gas down to less than 20 ppmv. The sorbent undergoes cycles of absorption (sulfidation) and air regeneration. The key barrier issues associated with a fluidized-bed HGD process are chemical degradation, physical attrition, high regeneration light-off (initiation) temperature, and high cost of the sorbent. Another inherent complication in all air-regeneration-based HGD processes is the disposal of the problematic dilute SO{sub 2} containing regeneration tail-gas. Direct Sulfur Recovery Process (DSRP), a leading first generation technology, efficiently reduces this SO{sub 2} to desirable elemental sulfur, but requires the use of 1-3% of the coal gas, thus resulting in an energy penalty to the plant. Advanced second-generation processes are under development that can reduce this energy penalty by modifying the sorbent so that it could be directly regenerated to elemental sulfur. The objective of this research is to support the near and long term DOE efforts to commercialize the IGCC-HGD process technology. Specifically we aim to develop: optimized low-cost sorbent materials with 70-80 {micro}m average aps meeting all Sierra specs; attrition resistant sorbents with 170 {micro}m aps that allow greater flexibility in the choice of the type of fluidized-bed reactor e.g. they allow increased throughput in a bubbling-bed reactor; and modified fluidizable sorbent materials that can be regenerated to produce elemental sulfur directly with minimal or no use of coal gas. The effort during the reporting period has been devoted to development of optimized low-cost zinc-oxide-based sorbents for Sierra-Pacific. The sorbent surface were modified to prevent

  12. Handling, transport and dispersion of sorbent powder for in-furnace injection. Final report

    SciTech Connect

    Fan, Liang-Shih; Abou-Zeida, E.; Liang, Shu-Chien; Luo, Xukun

    1996-02-01

    The focus of this project is on sorbent injection technologies using dry, calcium-based sorbents for high-sulfur coal flue gas desulfurization. The goal is to provide research findings on handling, transport and dispersion of sorbent powder, aimed at improving SO{sub 2} (to at least 90%) removal and increasing sorbent utilization in a cost-effective fashion. With this goal, the purpose of this project is to investigate the fundamental aspects of powder technology relevant to the fine sorbent powders, and to provide means of improving sorbent performance through superior dispersion and reduced dispersed particle size. The fifth year`s project contains three phases, Phase I ``Characterization of Electrostatic Properties``, Phase II ``Cohesive Strength of Modified Sorbents``. and Phase III ``Modeling of Powder Dispersion``. Work under Phase I involves characterization of the sorbents in terms of their electrostatic properties. Phase II investigates the flow properties of several calcium-based sorbents under different handling and transporting conditions. In Phase III, experimental studies are performed to measure the sorbent powder size distribution in different apparatuses and under different conditions. The population balance model proposed in previous studies can reasonably simulate these experiment results. These three areas of investigations are discussed in this report.

  13. Desulfurization with a modified limestone formulation in an industrial CFBC boiler

    SciTech Connect

    Young Goo Park; Seung Ho Kim

    2006-02-01

    This work presents a practical result of experimental investigation of the limestone particle size effect on de-SOx from a circulating fluidized bed combustion (CFBC) boiler that burns domestic anthracite and is the first industrial scale in Korea. Because of combustion problems such as clinker formation, fine limestone has not been used as a desulfurization agent. The present test, however, showed that higher content (up to 50%) of the particles under 0.1 mm did not entail any malfunction in a modern CFBC system. In addition, the desulfurization efficiency was found to be comparable to the old mode of limestone sorbents. 17 refs., 4 figs., 3 tabs.

  14. Pressurized fluidized-bed hydroretorting of Eastern oil shales -- Sulfur control. Topical report for Subtask 3.1, In-bed sulfur capture tests; Subtask 3.2, Electrostatic desulfurization; Subtask 3.3, Microbial desulfurization and denitrification

    SciTech Connect

    Roberts, M.J.; Abbasian, J.; Akin, C.; Lau, F.S.; Maka, A.; Mensinger, M.C.; Punwani, D.V.; Rue, D.M.; Gidaspow, D.; Gupta, R.; Wasan, D.T.; Pfister, R.M.: Krieger, E.J.

    1992-05-01

    This topical report on ``Sulfur Control`` presents the results of work conducted by the Institute of Gas Technology (IGT), the Illinois Institute of Technology (IIT), and the Ohio State University (OSU) to develop three novel approaches for desulfurization that have shown good potential with coal and could be cost-effective for oil shales. These are (1) In-Bed Sulfur Capture using different sorbents (IGT), (2) Electrostatic Desulfurization (IIT), and (3) Microbial Desulfurization and Denitrification (OSU and IGT). The objective of the task on In-Bed Sulfur Capture was to determine the effectiveness of different sorbents (that is, limestone, calcined limestone, dolomite, and siderite) for capturing sulfur (as H{sub 2}S) in the reactor during hydroretorting. The objective of the task on Electrostatic Desulfurization was to determine the operating conditions necessary to achieve a high degree of sulfur removal and kerogen recovery in IIT`s electrostatic separator. The objectives of the task on Microbial Desulfurization and Denitrification were to (1) isolate microbial cultures and evaluate their ability to desulfurize and denitrify shale, (2) conduct laboratory-scale batch and continuous tests to improve and enhance microbial removal of these components, and (3) determine the effects of processing parameters, such as shale slurry concentration, solids settling characteristics, agitation rate, and pH on the process.

  15. Methods, systems, and devices for deep desulfurization of fuel gases

    DOEpatents

    Li, Liyu; King, David L.; Liu, Jun; Huo, Qisheng

    2012-04-17

    A highly effective and regenerable method, system and device that enables the desulfurization of warm fuel gases by passing these warm gasses over metal-based sorbents arranged in a mesoporous substrate. This technology will protect Fischer-Tropsch synthesis catalysts and other sulfur sensitive catalysts, without drastic cooling of the fuel gases. This invention can be utilized in a process either alone or alongside other separation processes, and allows the total sulfur in such a gas to be reduced to less than 500 ppb and in some instances as low as 50 ppb.

  16. A novel semidry flue gas desulfurization process with the magnetically fluidized bed reactor.

    PubMed

    Zhang, Qi; Gui, Keting

    2009-09-15

    The magnetically fluidized bed (MFB) was used as the reactor in a novel semidry flue gas desulfurization (FGD) process to achieve high desulfurization efficiency. Experiments in a laboratory-scale apparatus were conducted to reveal the effects of approach to adiabatic saturation temperature, Ca/S molar ratio and applied magnetic field intensity on SO(2) removal. Results showed that SO(2) removal efficiency can be obviously enhanced by decreasing approach to adiabatic saturation temperature, increasing Ca/S molar ratio, or increasing applied magnetic field intensity. At a magnetic field intensity of 300Oe and a Ca/S molar ratio of 1.0, the desulfurization efficiency (excluding desulfurization efficiency in the fabric filter) was over 80%, while spent sorbent appeared in the form of dry powder. With the SEM, XRD and EDX research, it can be found that the increase of DC magnetic field intensity can make the surface morphology on the surface of the ferromagnetic particles loose and enhance the oxidation of S(IV), hence reducing the liquid phase mass transfer resistance of the slurry droplets and increasing desulfurization reaction rate, respectively. Therefore, the desulfurization efficiency increased obviously with the increase of DC field intensity. PMID:19369002

  17. Adsorption and desorption of sulfur dioxide on novel adsorbents for flue gas desulfurization. Final report, September 1, 1994--February 29, 1996

    SciTech Connect

    Lin, Y.S.; Deng, S.G.

    1996-08-05

    A sol-gel granulation method was developed to prepare spherical {gamma}-alumina granular supports and supported CuO granular sorbents for flue gas desulfurization. The prepared {gamma}-alumina supported CuO sorbents exhibit desirable pore structure and excellent mechanical properties. The sorbents contain higher loading (30-40 wt. %) of CuO dispersed in the monolayer or sub-monolayer form, giving rise to a larger SO{sub 2} sorption capacity ({gt}20 wt.%) and a faster sorption rate as compared to similar sorbents reported in the literature. With these excellent sulfation and mechanical properties, the sol-gel derived {gamma}-alumina supported CuO granular sorbents offer great potential for use in the dry, regenerative flue gas desulfurization process. Research efforts were also made to prepare DAY zeolite supported sorbents with various CuO contents by the microwave and conventional thermal dispersion methods at different conditions. Monolayer or sub-monolayer coating of Cu(NO{sub 3})sub 2 or CuO was achieved on several DAY supported sorbents by the microwave heating method but not by the conventional thermal dispersion method. The DAY zeolite supported CuO sorbents prepared by the microwave heating method can adsorb up to 15 wt.% of SO{sub 2}. The results obtained have demonstrated the feasibility of effective preparation of zeolite supported CuO sorbents by the microwave heating method.

  18. Enzymatic desulfurization of coal

    SciTech Connect

    Boyer, Y.N.; Crooker, S.C.; Kitchell, J.P.; Nochur, S.V.

    1991-05-16

    The overall objective of this program was to investigate the feasibility of an enzymatic desulfurization process specifically intended for organic sulfur removal from coal. Toward that end, a series of specific objectives were defined: (1) establish the feasibility of (bio)oxidative pretreatment followed by biochemical sulfate cleavage for representative sulfur-containing model compounds and coals using commercially-available enzymes; (2) investigate the potential for the isolation and selective use of enzyme preparations from coal-utilizing microbial systems for desulfurization of sulfur-containing model compounds and coals; and (3) develop a conceptual design and economic analysis of a process for enzymatic removal of organic sulfur from coal. Within the scope of this program, it was proposed to carry out a portion of each of these efforts concurrently. (VC)

  19. Coal Liquefaction desulfurization process

    DOEpatents

    Givens, Edwin N.

    1983-01-01

    In a solvent refined coal liquefaction process, more effective desulfurization of the high boiling point components is effected by first stripping the solvent-coal reacted slurry of lower boiling point components, particularly including hydrogen sulfide and low molecular weight sulfur compounds, and then reacting the slurry with a solid sulfur getter material, such as iron. The sulfur getter compound, with reacted sulfur included, is then removed with other solids in the slurry.

  20. Flue gas desulfurization process

    SciTech Connect

    Korosy, L.B.; Senatore, P.J.

    1982-12-28

    A regenerative process for the desulfurization of gas containing from about 100 ppm to about 30 volume percent sulfur dioxide in which the gas is contacted at from about 15/sup 0/ to 80/sup 0/C with an about 0.1 molar to saturated aqueous solution of potassium citrate at a ph of from about 3 to 9 and the contacted solution is then heated to strip sulfur dioxide therefrom.

  1. Enzymatic desulfurization of coal

    SciTech Connect

    Marquis, J.K. . School of Medicine); Kitchell, J.P. )

    1988-10-07

    Our current efforts to develop clean coal technology, emphasize the advantages of enzymatic desulfurization techniques and have specifically addressed the potential of using partially-purified extracellular microbial enzymes or commercially available enzymes. Our work is focused on the treatment of model'' organic sulfur compounds such as dibenzothiophene (DBT) and ethylphenylsulfide (EPS). Furthermore, we are designing experiments to facilitate the enzymatic process by means of a hydrated organic solvent matrix.

  2. Enzymatic desulfurization of coal

    SciTech Connect

    Marquis, J.K. . School of Medicine); Kitchell, J.P. )

    1988-12-15

    Our current efforts to develop clean coal technology emphasize the advantages of enzymatic desulfurization techniques and have specifically addressed the potential of using partially-purified extracellular microbial enzymes or commercially available enzymes. Our work is focused on the treatment of model'' organic sulfur compounds such as dibenzothiophene (DBT) and ethylphenylsulfide (EPS). Furthermore, we are designing experiments to facilitate the enzymatic process by means of a hydrated organic solvent matrix.

  3. Enzymatic desulfurization of coal

    SciTech Connect

    Boyer, Y.N.; Crooker, S.C.; Kitchell, J.P.; Nochur, S.V. ); Marquis, J.K. . School of Medicine)

    1989-06-16

    Our current efforts to develop clean coal technology emphasize the advantages of enzymatic desulfurization techniques and have specifically addressed the potential of using partially-purified extracellular microbial enzymes as well as commercially available enzymes. Our work is focused on the treatment of model'' organic sulfur compounds such as dibenzothiophene (DBT) and ethylphenylsulfide (EPS). Furthermore, we are designing experiments to facilitate the enzymatic process by means of a hydrated organic solvent matrix.

  4. Fluidized bed desulfurization

    NASA Technical Reports Server (NTRS)

    Ravindram, M.; Kallvinskas, J. J. (Inventor)

    1985-01-01

    High sulfur content carbonaceous material, such as coal is desulfurized by continuous fluidized suspension in a reactor with chlorine gas, inert dechlorinating gas and hydrogen gas. A source of chlorine gas, a source of inert gas and a source of hydrogen gas are connected to the bottom inlet through a manifold and a heater. A flow controler operates servos in a manner to continuously and sequentially suspend coal in the three gases. The sulfur content is reduced at least 50% by the treatment.

  5. Microbial desulfurization of coal

    NASA Technical Reports Server (NTRS)

    Dastoor, M. N.; Kalvinskas, J. J.

    1978-01-01

    Experiments indicate that several sulfur-oxidizing bacteria strains have been very efficient in desulfurizing coal. Process occurs at room temperature and does not require large capital investments of high energy inputs. Process may expand use of abundant reserves of high-sulfur bituminous coal, which is currently restricted due to environmental pollution. On practical scale, process may be integrated with modern coal-slurry transportation lines.

  6. Highly Attrition Resistant Zinc Oxide-Based Sorbents for H2S Removal by Spray Drying Technique

    SciTech Connect

    Ryu, C.K.; Lee, J.B.; Ahn, D.H.; Kim, J.J.; Yi, C.K.

    2002-09-19

    Primary issues for the fluidized-bed/transport reactor process are high attrition resistant sorbent, its high sorption capacity and regenerability, durability, and cost. The overall objective of this project is the development of a superior attrition resistant zinc oxide-based sorbent for hot gas cleanup in integrated coal gasification combined cycle (IGCC). Sorbents applicable to a fluidized-bed hot gas desulfurization process must have a high attrition resistance to withstand the fast solid circulation between a desulfurizer and a regenerator, fast kinetic reactions, and high sulfur sorption capacity. The oxidative regeneration of zinc-based sorbent usually initiated at greater than 600 C with highly exothermic nature causing deactivation of sorbent as well as complication of sulfidation process by side reaction. Focusing on solving the sorbent attrition and regenerability of zinc oxide-based sorbent, we have adapted multi-binder matrices and direct incorporation of regeneration promoter. The sorbent forming was done with a spray drying technique that is easily scalable to commercial quantity.

  7. Coal desulfurization by cyclonic whirl

    SciTech Connect

    Jianguo, Y.; Wenjun, Z.; Yuling, W.

    1999-07-01

    The crux of coal desulfurization is how to improve separation efficiency for 3--0.1mm materials. Cyclonic whirl produce centrifugal force and shearing force, heavy medium cyclone uses former, and cyclone flotation column uses both of them. A new system with heavy medium cyclone and cyclone flotation column is provided and testified to be very efficient in commercial desulfurization.

  8. Coal desulfurization with iron pentacarbonyl

    NASA Technical Reports Server (NTRS)

    Hsu, G. C.

    1979-01-01

    Coal desulfurization with iron pentacarbonyl treatment under mild conditions removes up to eighty percent of organic sulfur. Preliminary tests on treatment process suggest it may be economical enough to encourage investigation of use for coal desulfurization. With mild operating conditions, process produces environmentally-acceptable clean coal at reasonable cost.

  9. Evaluation of sulfur-reducing microorganisms for organic desulfurization

    SciTech Connect

    Miller, K.W. . Dept. of Biological Sciences)

    1991-01-01

    Because a substantial portion of the sulfur in Illinois coal is organically bound sulfur, microbial desulfurization of sulfidic and thiophenic functionalities holds great potential for complementing pyritic sulfur removal. The release of H{sub 2}S from anaerobic systems such as the gut, sewage, and marine and freshwater sediments, is a common occurrence and the role of microorganisms in this process has long been recognized. The principal goals of our project are: to obtain anaerobic microbial cultures that produce H{sub 2}S from compounds representative of the organosulfur functionalities in coal; to optimize this activity; to evaluate the effectiveness of using these cultures to remove organic sulfur from Illinois coal. Our immediate objectives for this year are the following: To obtain additional cultures from coal mine waste and municipal sewage sludge, two environments previously unexplored by our laboratory; to continue optimizing activity in cultures that desulfurize model compounds, including identification of individual microbial species; to expand coal desulfurization experiments to include additional coals; and, to address the recently discovered problem of sulfide sorbing to coal. This quarter we report on the following: (1) desulfurization experiments with IBC-101; (2) quantitative experiments dealing with dibenzyldisulfide (DBDS) degradation in mixed cultures derived from petroleum wastes; (3) thiophene, dibenzothiophene (DBT), DBT sulfone, or phenyl sulfone as substrates for pure cultures of sulfate-reducing bacteria. 36 refs., 1 fig. 6 tabs.

  10. Characterization and optimization of sorbents utilized for emission control during coal gasification. Final report

    SciTech Connect

    Huque, Z.; Mei, D.; Zhou, J.

    1998-07-14

    To overcome the shortage of components required for high temperature operation required by current IGCC and PFBC systems, researchers recently have decided that the power systems can be optimized within an operation temperature range of 343 to 538 C. The findings of this research work support the use of iron oxides as an efficient, disposable hot gas desulfurization sorbent candidate to meet the temperature range of 343 to 538 C to further optimize its application for hot gas desulfurization. A parametric study was performed to characterize the controlling parameters dominating the absorption process of hydrogen sulfide by waste iron oxide as a sorbent alternative within a stringent environment with the use of simulated KRW reducing gas. The major parameters studied for hot gas desulfurization with the use of waste iron oxide; mixed in coal ash and reacted with hot sulfurized gas; in hot gas stream include (1) dust cake permeability during heavy dust loading, (2) feasibility of dust cake removal with current back pulse cleaning technology, (3) the reaction temperature, (4) the space velocity of the gas stream. Based on the parametric testing performed on hot gas desulfurization and particulate filtration, the test results of this study indicate that the simultaneous operation of hot gas desulfurization and particulate filtration is feasible. The significant savings of capital investment, system operation and maintenance justify the use of iron oxides as an excellent candidate for hot gas cleanup.