A review on research and development of iron-based sorbents for removal of hydrogen sulfide from hot coal gases

Frontiers of Chemical Engineering in China - Tập 4 - Trang 529-535 - 2010
Jianglong Yu1,2, Liping Chang3, Fan Li3, Kechang Xie3
1Key Laboratory of Coal-Based Fuels for Aviation, Shenyang Aerospace University, Shenyang, China
2School of Chemical Engineering, University of Science and Technology Liaoning, Anshan, China
3Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan, China

Tóm tắt

In poly-generation and integrated gasification-combined cycle (IGCC) systems for clean energy conversion, it is essential to remove impurities such as sulfur species from hot coal gases prior to entering the subsequent units. This paper provides a comprehensive review on previous studies on high temperature removal of hydrogen sulfide from high temperature coal gases using iron-based sorbents. A two-step desulphurization process for hot coal gas cleanup is highlighted, which is integrated with direct production of elemental sulfur during regeneration of iron-based sorbents in the primary desulphurization step. Different kinetic modeling approaches for sulfidation and regeneration were compared. Limited research on activated carbon supported sorbents was also briefly summarized.

Tài liệu tham khảo

Fan H L, Li C H, Xie K C. Sorbents for high-temperature removal of hydrogen sulfide from coal-derived fuel gas. Journal of Natural Gas Chemistry, 2001, 10: 256–270 (in Chinese) Xie W, Chang L P, Yu J L, Xie K C. Research progress of the removal of H2S from coal gas by dry method. J Chem Industry Eng, 2006, 57: 2012–2020 (in Chinese) Ohtsuka Y, Mori H, Nonaka K, Watanabe T, Asami K. Selective conversion of coal nitrogen to N2 with iron. Energy & Fuels, 1993, 7(6): 1095–1096 Yu J L, Tian F J, McKenzie L J, Li C Z. Char-supported nano iron catayst for water-gas-shift reaction: hydrogen production from coal/biomass gasification. Process Safety and Environmental Protection, 2006, 84(2): 125–130 Kobayashi M, Shirai H, Nunokawa M. Elucidation of sulfidation mechanisms of zinc ferrite in a reductive gas environment by in situ X-ray diffraction analysis and Mo1ssbauer spectroscopy. Industrial & Engineering Chemistry Research, 2000, 39(6): 1934–1943 Lu Z, Sha X, Lu J, Wu Y, Pen Z. Coal gas desulphurization at high temperature: I. Sulfidation and kinetics of Fe/Zn based sorbents. Journal of Fuel Chemistry and Technology, 1996, 24: 492–497 (in Chinese) Ying Y, Song W, Yu J, Xie E. Hot gas desulphurization sorbent preparation. Clean Coal Technology, 1997, 3: 38–43 (in Chinese) Piao L, Li C, Li Y. Study on reduction and sulfidation of ZnFe2O4 desulfurizer at high temperature. Journal of Chemical Engineering of Chinese Universities, 2001, 15: 546–551 (in Chinese) Lu Z, Sha X, Li S, Tian A, Wang Y. Coal gas desulphurization at high temperature: II. Regeneration conditions of Fe/Zn based sorbents. Journal of Fuel Chemistry and Technology, 1997, 25: 55–59 (in Chinese) Xu H, Li C, Liang M, Wang Y. Reactivity evaluation and characterization of zinc ferrite as high temperature desulfurizer. Environmental Protection of Chemical Industry, 1997, 24: 165–168 Ahmed M A, Alonso L, Palacios J M, Cilleruelo C, Abanades J C. Structure changes in zinc ferrites as regenerable sorbents for hot coal gas desulphurization. Solid State Ionics, 2000, 138(1–2): 51–62 Gupta R, Gangwal S K, Jain S C. Development of Zinc ferrite sorbents for desulphurization of hot coal gas in a fluid-bed reactor. Energy & Fuels, 1992, 6(1): 21–27 Li Y, Li C, Guo H, Zhong B. Preparation of iron-calcium oxide hot coal gas desulfurizer. Journal of Fuel Chemstry and Technology, 1999, 27: 529–532 (in Chinese) Du X R, Huang J R, Fang Y R, Wang Y. Regeneration of Fe-Ca based sorbent for hot gas cleaning. Ranliao Huaxue Xuebao, 2003, 31: 405–410 (in Chinese) Sasaoka E, Ichio T, Kasaoka S. High-temperature H2S removal from coal-derived gas by iron ore. Energy & Fuels, 1992, 6(5): 603–608 Shen F, Li C, Shangguan J, Fan H, Liang S. Study on iron oxide desulfurizer of hot gas desulphurization. Coal Conversion, 2004, 21: 54–57 (in Chinese) Li Y, Tian Q, Guo H. Study of high temperature desulphurization using an iron oxide desulfurizer-Kinetics of reduction and sulfidation. Journal of Fuel Chemistry and Technology, 1998, 26: 131–136 (in Chinese) Najjar M S, Jung D Y. High temperature desulphurization of synthesis gas with iron compound. Fuel Processing Technology, 1995, 44(1-3): 173–180 No I, Ohgaito Y, Matsushima H, Suzuki T. Preparation of zinc ferrites in the presence of carbon material and its application to hot gas cleaning. Fuel, 2004, 83(6): 661–669 Kobayashi M, Shirai H, Nunokawa M. High-temperature sulfidation behavior of reduced Zinc ferrite in simulated coal gas revealed by in situ X-ray diffraction analysis and Mo1ssbauer spectroscopy. Energy & Fuels, 2002, 16(3): 601–607 Kobayashi M, Shirai H, Nunokawa M. Measurements of sulfur capacity proportional to Zinc sulfidation on sorbent containing Zinc ferrite-silica composite powder in pressurized coal gas. Industrial & Engineering Chemistry Research, 2002, 41(12): 2903–2909 Atimtay A T, Gasper-Galvin L D, Poston J A. Novel supported sorbent for hot gas desulphur-ization. Environmental Science & Technology, 1993, 27(7): 1295–1303 Patrick V, Gavalas G R, Sharma P K. Reduction, sulfidation, and regeneration of mixed iron-aluminum oxide sorbents. Industrial & Engineering Chemistry Research, 1993, 32(3): 519–532 Miura K, Mae K, Inoue T, Yoshimi T, Nakagawa H, Hashimoto K. Simultaneous removal of carbonyl sulfide and hydrogen sulfide from coke oven gas at low temperature by iron oxide. Industrial & Engineering Chemistry Research, 1992, 31(1): 415–419 Lizzio A A, Strickler B W, Cal M P, Rood M J, Kelly M A. Activated char from bituminous coal for removal of hydrogen sulfide from hot coal gas. American Carbon Society, 1999, 534–535 Tan X, Li X, Wu D, Yuan Q. Removal of H2S by catalytic oxidation with impregnated activated carbon at ambient temperature. Petroleum Chemical Industry (China), 1995, 10: 716–721 (in Chinese) Zhang X, Chen Q, Xu D, Shi H. Effect of pore structure and loaded metal catalyst on SO2 removal property of porous carbon. Part (I): influence of Ca catalyst on meso-port formation of activated carbon. Coal Conversion (China), 2004. 4: 87–90 (in Chinese) Sakanishi K, Matsumura A, Saito I, Wu Z, Hanaoka T, Minowa T, Tada M, Iwasaki T. Simultaneous removalof H2S and COS using activated-carbons and their supported catalysts. Catalysis Today, 2005, 104(1): 94–100 Palmer A, Heeney P, Furimsky E. Regeneration of iron oxide-containing pellets used for hot gas clean-up. Fuel Processing Technology, 1998, 23(1): 75–85 Van der Waal W J. Desulphurization of process gas by means of iron oxide on silica sorbents. Dissertation for the Doctoral Degree. Utrecht: University of Utrecht, 1987, 36–58