Insights into H2S-absorption and oxidation-regeneration behavior of Ni-doped ZnO-based sorbents supported on SBA-15 for desulfurization of hot coal gas

被引:24
作者
Wang, Xiaowen [1 ,2 ,3 ]
Zhang, Ran [1 ,2 ,3 ]
Li, Qiaochun [1 ,4 ]
Mi, Jie [1 ,2 ,3 ]
Wu, Mengmeng [1 ,2 ,3 ]
机构
[1] Taiyuan Univ Technol, State Key Lab Clean & Efficient Coal Utilizat, Taiyuan 030024, Peoples R China
[2] Taiyuan Univ Technol, Key Lab Coal Sci & Technol Shanxi Prov, Taiyuan 030024, Peoples R China
[3] Taiyuan Univ Technol, Minist Educ, Taiyuan 030024, Peoples R China
[4] China Shanxi Intellectual Property Protect Ctr, Taiyuan 030006, Peoples R China
基金
中国国家自然科学基金;
关键词
H2S; COS; Desulfurization; Ni doping; Sorbents; Regeneration; HYDROGEN-SULFIDE; TEMPERATURE; OXIDE; ADSORBENTS; NICKEL;
D O I
10.1016/j.fuel.2022.126052
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
Sulfur removal from hot coal gas is one of important technologies for highly efficient coal-based energy system. H2S-absorption and oxidation-regeneration behavior of Ni-doped ZnO-based sorbents supported on SBA-15 (ZnNi/SBA-15) was analyzed in this work. The results indicate that ZnNi/SBA-15 shows highest H2S-uptake capacity (16 g S/100 g sorbent) and lowest amount of produced COS (0.0004 g COS/100 g sorbent) when used for desulfurization at 500 degrees C. Removal of H2S at 700 degrees C leads to lowest breakthrough sulfur capacity of sorbents. It is ascribed to the destruction of typical microscopic morphology of SBA-15. Boltzmann function is suitable for modeling the H2S-absorption behavior of ZnNi/SBA-15. The evolution rate of H2S for sorbents varies from 0.096 to 0.228 min(-1) at 400-700 degrees C. H2S-CO and H2S-CO2 reactions both contribute to the formation of COS at the stage of H2S-absorption saraturation. Increase of temperature from 550 to 600 degrees C results in the disappearance of ZnS in regenerated ZnNi/SBA-15. Moreover, most of plugged pore structure caused by sulfidation reaction could restore after regeneration at 600 degrees C. Further increase of regeneration temperature causes the decline of regeneration efficiency and less porous sorbent. Additionally, the sorbents have stable desulfurization ability and low COS emission during multiple sulfidation-regeneration cycles.
引用
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页数:12
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共 41 条
[1]  
Barrett R. L., 1962, J CHEM EDUC, V39, DOI DOI 10.1021/ED039P251
[2]   A step-by-step guide to non-linear regression analysis of experimental data using a Microsoft Excel spreadsheet [J].
Brown, AM .
COMPUTER METHODS AND PROGRAMS IN BIOMEDICINE, 2001, 65 (03) :191-200
[3]   Low-temperature hydrolysis of carbonyl sulfide in blast furnace gas using Al2O3-based catalysts with high oxidation resistance [J].
Cao, Rui ;
Ning, Ping ;
Wang, Xueqian ;
Wang, Langlang ;
Ma, Yixing ;
Xie, Yibing ;
Zhang, Hui ;
Qu, Jiaxin .
FUEL, 2022, 310
[4]   Review of Mid- to High-Temperature Sulfur Sorbents for Desulfurization of Biomass- and Coal-derived Syngas [J].
Cheah, Singfoong ;
Carpenter, Daniel L. ;
Magrini-Bair, Kimberly A. .
ENERGY & FUELS, 2009, 23 (11) :5291-5307
[5]   Effect of temperature on hydrophobic interaction between proteins and hydrophobic adsorbents: Studies by isothermal titration calorimetry and the van't Hoff equation [J].
Chen, WY ;
Huang, HM ;
Lin, CC ;
Lin, FY ;
Chan, YC .
LANGMUIR, 2003, 19 (22) :9395-9403
[6]   Desulfurization sorbents for green and clean coal utilization and downstream toxics reduction: A review and perspectives [J].
Feng, Yu ;
Lu, Jianjun ;
Wang, Jiancheng ;
Mi, Jie ;
Zhang, Man ;
Ge, Mingzheng ;
Li, Yang ;
Zhang, Zhiyi ;
Wang, Wenyu .
JOURNAL OF CLEANER PRODUCTION, 2020, 273
[7]   Synergistic effects of ZrO2 crystallite islands and high dispersion of active Ni0 nanoparticles on CH4/CO2 reforming reaction [J].
Guo, Shitong ;
Li, Jianfa ;
Xia, Chan ;
Au, Chak-Tong ;
Liu, Bingsi .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2021, 46 (40) :20972-20983
[8]   Gas-solid reaction modeling as applied to the fine desulfurization of gaseous feedstocks [J].
Hartmann, V. L. .
CHEMICAL ENGINEERING JOURNAL, 2007, 134 (1-3) :190-194
[9]   Porous olive-like BiVO4: Alcoho-hydrothermal preparation and excellent visible-light-driven photocatalytic performance for the degradation of phenol [J].
Jiang, Haiyan ;
Dai, Hongxing ;
Meng, Xue ;
Ji, Kemeng ;
Zhang, Lei ;
Deng, Jiguang .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2011, 105 (3-4) :326-334
[10]   Inhibition and elimination of carbon deposition in dry gas desulfurization process under oxy-fuel IGCC derived coal gas environment [J].
Kobayashi, Makoto ;
Nakao, Yoshinobu .
FUEL, 2015, 152 :19-28