Transformation of H2S in In Situ Landfill Gas Deoxygen with Pt/γ-Al2O3 as the Catalyst and Its Impact on Catalyst Activity

被引:0
作者
Lin, Feng [1 ]
Yang, Xinyu [1 ,2 ]
Chen, Zezhi [1 ]
Gong, Huijuan [1 ,3 ]
Wang, Xiaoshu [3 ]
Yang, Ziyi [1 ]
机构
[1] Nanjing Univ, Sch Environm, State Key Lab Pollut Control & Resource Reuse, Nanjing 210023, Peoples R China
[2] Hubei Normal Univ, Coll Urban & Environm Sci, Huangshi 435002, Peoples R China
[3] Nanjing Univ, Ctr Mat Anal, Nanjing 210023, Peoples R China
基金
中国国家自然科学基金;
关键词
METHANE OXIDATION; SO2; REGENERATION; ACTIVATION; OXYGEN;
D O I
10.1021/acs.jpcc.4c02986
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Catalytic deoxygenation is an effective technique for oxygen removal from landfill gas (LFG) in industry, thereby upgrading LFG to biomethane as a viable alternative energy source. However, LFG typically contains trace amounts of H2S, which may potentially exert adverse effects on the catalytic deoxygen reaction. To clarify this issue and provide a theoretical support for industrial practice, we simulated the actual catalytic deoxygen reaction of LFG in the presence of 200 ppm of H2S. Different from the conventional belief that H2S is a catalyst poison in various reactions, the present study has discovered that trace amounts of H2S exhibit a promotional effect on the catalytic deoxygen activity of the Pt/gamma-Al2O3 catalyst. Characterizations and theoretical calculations reveal the transformation behavior of H2S and its promotion mechanism. It is demonstrated that H2S is adsorbed on Pt sites, undergoing multistep oxidation and ultimately forming SO42-. A portion of SO42- adsorbed on Pt sites is transferred to the support, while another portion is reduced to SO2 and enters the gas phase. The SO42- temporarily present on Pt sites significantly promotes the heterolytic cleavage of the C-H bond of methane, thereby enhancing the Pt/gamma-Al2O3 catalyst deoxygen activity.
引用
收藏
页码:13387 / 13394
页数:8
相关论文
共 26 条
  • [1] Higher tolerance to sulfur poisoning in CO2 methanation by the presence of CeO2
    Alarcon, Andreina
    Guilera, Jordi
    Soto, Rodrigo
    Andreu, Teresa
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 263
  • [2] The water gas shift reaction: Catalysts and reaction mechanism
    Baraj, Erlisa
    Ciahotny, Karel
    Hlincik, Tomas
    [J]. FUEL, 2021, 288
  • [3] Methane oxidation over alumina supported platinum investigated by time-resolved in situ XANES spectroscopy
    Becker, Elin
    Carlsson, Per-Anders
    Gronbeck, Henrik
    Skoglundh, Magnus
    [J]. JOURNAL OF CATALYSIS, 2007, 252 (01) : 11 - 17
  • [4] C-H bond activation in hydrocarbon oxidation on solid catalysts
    Burch, R
    Hayes, MJ
    [J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1995, 100 (1-3) : 13 - 33
  • [5] Fe-oxide/Al2O3 for the enhanced activity of H2S decomposition under realistic conditions: Mechanistic studies by in-situ DRIFTS and XPS
    Cha, Byeong Jun
    Choi, Ji Yoon
    Ji, Yujing
    Zhao, Shufang
    Kim, Soong Yeon
    Kim, Soo Hyun
    Kim, Young Dok
    [J]. CHEMICAL ENGINEERING JOURNAL, 2022, 443
  • [6] Engineering Operation Performance of Catalytic Deoxygenation Equipment for Landfill Gas Upgrading
    Chen, Zezhi
    Gong, Huijuan
    Bao, Yanchu
    Wu, Weili
    [J]. ENERGY & FUELS, 2017, 31 (04) : 4565 - 4570
  • [7] Study on the deactivation of the deoxygen catalyst during the landfill gas upgrading process
    Gong, Huijuan
    Chen, Zezhi
    Zhang, Mengqun
    Wu, Weili
    Wang, Weixing
    Wang, Weibing
    [J]. FUEL, 2015, 144 : 43 - 49
  • [8] A study on the feasibility of the catalytic methane oxidation for landfill gas deoxygen treatment
    Gong, Huijuan
    Chen, Zezhi
    Wang, Mengqiu
    Wu, Weili
    Wang, Weixing
    [J]. FUEL, 2014, 120 : 179 - 185
  • [9] Enhancing Thermocatalytic Activities by Upshifting the d-Band Center of Exsolved Co-Ni-Fe Ternary Alloy Nanoparticles for the Dry Reforming of Methane
    Joo, Sangwook
    Kim, Kyeounghak
    Kwon, Ohhun
    Oh, Jinkyung
    Kim, Hyung Jun
    Zhang, Linjuan
    Zhou, Jing
    Wang, Jian-Qiang
    Jeong, Hu Young
    Han, Jeong Woo
    Kim, Guntae
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2021, 60 (29) : 15912 - 15919
  • [10] A study of the regeneration of fresh and aged SOx adsorbers under reducing conditions
    Limousy, L
    Mahzoul, H
    Brilhac, JF
    Garin, E
    Maire, G
    Gilot, P
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2003, 45 (03) : 169 - 179