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Pd/activated carbon sorbents for mid-temperature capture of mercury from coal-derived fuel gas
作者姓名:Dekui Li  Jieru Han  Lina Han  Jiancheng Wang  Liping Chang
作者单位:Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China;Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China;College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China;Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China;Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China
基金项目:This work was supported by the National Natural Science Foundation of China (Nos. 21006067, 21276170), the Shanxi Province Natural Science Foundation (Nos. 2010021008-1, 201101008-4) and the National High-Tech Research and Development Program (863) of China (No. 2013AA065404E).
摘    要:Higher concentrations of Hg can be emitted from coal pyrolysis or gasification than from coal combustion, especially elemental Hg. Highly efficient Hg removal technology from coal-derived fuel gas is thus of great importance. Based on the very excellent Hg removal ability of Pd and the high adsorption abilities of activated carbon(AC) for H2 S and Hg, a series of Pd/AC sorbents was prepared by using pore volume impregnation, and their performance in capturing Hg and H2 S from coal-derived fuel gas was investigated using a laboratory-scale fixed-bed reactor. The effects of loading amount, reaction temperature and reaction atmosphere on Hg removal from coal-derived fuel gas were studied. The sorbents were characterized by N2 adsorption, X-ray diffraction(XRD) and X-ray photoelectron spectroscopy(XPS). The results indicated that the efficiency of Hg removal increased with the increasing of Pd loading amount, but the effective utilization rate of the active component Pd decreased significantly at the same time. High temperature had a negative influence on the Hg removal. The efficiency of Hg removal in the N2-H2S-H2-CO-Hg atmosphere(simulated coal gas) was higher than that in N2-H2S-Hg and N2-Hg atmospheres, which showed that H2 and CO, with their reducing capacity, could benefit promote the removal of Hg. The XPS results suggested that there were two different ways of capturing Hg over sorbents in N2-H2S-Hg and N2-Hg atmospheres.

关 键 词:碳吸附剂  燃料气体  煤燃烧  活性炭  除汞  衍生  捕获  X射线光电子能谱
收稿时间:8/6/2013 12:00:00 AM
修稿时间:20 November 2013

Pd/activated carbon sorbents for mid-temperature capture of mercury from coal-derived fuel gas
Dekui Li,Jieru Han,Lina Han,Jiancheng Wang,Liping Chang.Pd/activated carbon sorbents for mid-temperature capture of mercury from coal-derived fuel gas[J].Journal of Environmental Sciences,2014,26(7):1497-1504.
Authors:Dekui Li  Jieru Han  Lina Han  Jiancheng Wang and Liping Chang
Institution:Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China;Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China;College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China;Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China;Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China
Abstract:Higher concentrations of Hg can be emitted from coal pyrolysis or gasification than from coal combustion, especially elemental Hg. Highly efficient Hg removal technology from coal-derived fuel gas is thus of great importance. Based on the very excellent Hg removal ability of Pd and the high adsorption abilities of activated carbon (AC) for H2S and Hg, a series of Pd/AC sorbents was prepared by using pore volume impregnation, and their performance in capturing Hg and H2S from coal-derived fuel gas was investigated using a laboratory-scale fixed-bed reactor. The effects of loading amount, reaction temperature and reaction atmosphere on Hg removal from coal-derived fuel gas were studied. The sorbents were characterized by N2 adsorption, X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The results indicated that the efficiency of Hg removal increased with the increasing of Pd loading amount, but the effective utilization rate of the active component Pd decreased significantly at the same time. High temperature had a negative influence on the Hg removal. The efficiency of Hg removal in the N2-H2S-H2-CO-Hg atmosphere (simulated coal gas) was higher than that in N2-H2S-Hg and N2-Hg atmospheres, which showed that H2 and CO, with their reducing capacity, could benefit promote the removal of Hg. The XPS results suggested that there were two different ways of capturing Hg over sorbents in N2-H2S-Hg and N2-Hg atmospheres.
Keywords:Coal-derived fuel gas  Hg removal  Pd/AC sorbents  H2S removal
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