理想与还原Fe2O3[001]表面上汞吸附协同催化CO分解作用

doi:10.3866/PKU.WHXB201607271

物理化学学报 >> 2016, Vol. 32 >> Issue (11): 2717-2723.doi: 10.3866/PKU.WHXB201607271

理想与还原Fe₂O₃[001]表面上汞吸附协同催化CO分解作用

李继红¹,林常枫¹,覃吴^1,*(),肖显斌¹,魏利^2,*()

¹ 华北电力大学可再生能源学院,生物质发电成套设备国家工程实验室,北京102206
² 哈尔滨工业大学,城市水资源与水环境国家重点实验室,哈尔滨150090

收稿日期:2016-05-03 发布日期:2016-11-08
通讯作者: 覃吴,魏利 E-mail:qinwugx@126.com;weilihit@126.com
基金资助:
国家自然科学基金(51346001);国家自然科学基金(51106051);中央高校基本科研专项资金(2016YQ07);中央高校基本科研专项资金(2014ZD14)

Synergetic Effect of Mercury Adsorption on the Catalytic Decomposition of CO over Perfect and Reduced Fe₂O₃[001] Surface

Ji-Hong LI¹,Chang-Feng LIN¹,Wu QIN^1,*(),Xian-Bin XIAO¹,Li WEI^2,*()

¹ National Engineering Laboratory for Biomass Power Generation Equipment, School of Renewable Energy Engineering, North China Electric Power University, Beijing 102206, P. R. China
² State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, P. R. China

Received:2016-05-03 Published:2016-11-08
Contact: Wu QIN,Li WEI E-mail:qinwugx@126.com;weilihit@126.com
Supported by:
the National Natural Science Foundation of China(51346001);the National Natural Science Foundation of China(51106051);Fundamental Research Funds for the Central Universities, China(2016YQ07);Fundamental Research Funds for the Central Universities, China(2014ZD14)

摘要/Abstract

摘要：

煤化学链燃烧必然释放汞，汞与载氧体表面相互作用，影响表界面的氧化还原反应。本文采用密度泛函理论计算，研究汞（Hg⁰）在理想表面（Fe₂O₃[001]）和一系列被还原表面（Fe₂O_2.75、Fe₂O_2.5、Fe₂O_2.25、Fe₂O_1.625、Fe₂O_0.875、Fe₂O_0.375和Fe）的吸附，以及Hg⁰对Fe₂O_1.625、Fe₂O_0.875、Fe₂O_0.375和Fe等表面催化CO分解反应的协同作用机理。Hg⁰物理吸附在理想Fe₂O₃[001]表面。随着Fe₂O₃[001]表面不断被还原，Hg⁰发生化学吸附。Hg⁰吸附降低了CO与Fe₂O₃、Fe₂O_2.75、Fe₂O_2.5和Fe₂O_2.25等表面之间的相互作用，抑制O传递氧化CO为CO₂的反应；载氧体进一步还原过程中，Hg⁰吸附促进了CO与Fe₂O_1.625、Fe₂O_0.875、Fe₂O_0.375及Fe等表面之间的相互作用，进而促进了表面对CO的催化分解反应，加速了载氧体表面的积碳，降低了化学链燃烧效率。因此，合理控制载氧体的还原程度既可以减弱Hg⁰的吸附，也可以抑制积碳的形成，这对化学链燃烧的操作优化至关重要。

关键词: 化学链燃烧, 载氧体, 汞, CO₂捕集, 密度泛函理论

Abstract:

Mercury emission from coal during chemical-looping combustion (CLC) is an inevitable process, which can lead to adverse interactions with the surface of the oxygen carrier, thereby affecting the interfacial redox reactions. Density functional theory calculations were performed to investigate the mechanism of elemental mercury (Hg⁰) adsorption and the synergetic effect of Hg⁰ on the catalytic decomposition of CO over a perfect surface (Fe₂O₃[001]), as well as a series of reduced surfaces (Fe₂O_2.75, Fe₂O_2.5, Fe₂O_2.25, Fe₂O_1.625, Fe₂O_0.875, Fe₂O_0.375 and Fe) during a deep CLC process. In this study, Hg⁰ was physically adsorbed on to a perfect Fe₂O₃ surface, and then chemically adsorbed on to a series of reduced surfaces. The adsorption of Hg⁰ inhibited the formation of meaningful interactions between CO and Fe₂O₃[Fe₂O_2.75, Fe₂O_2.5 and Fe₂O_2.25] and hindered the efficient transport of oxygen to oxidize CO into CO₂. In contrast, this process promoted the interactions between CO and Fe₂O_1.625[Fe₂O_0.875, Fe₂O_0.375, and Fe], favoring the catalytic decomposition of CO on these surfaces, which accelerated the carbon deposit reducing CLC efficiency. Rationally controlling the reduction degree of the oxygen carrier could therefore be used to either decrease the adsorption of Hg⁰ or depress the deposition of carbon, which are both crucial for the optimization of CLC processes.

Key words: Chemical looping combustion, Oxygen carrier, Mercury, CO₂ capture, Density functional theory

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李继红,林常枫,覃吴,肖显斌,魏利. 理想与还原Fe₂O₃[001]表面上汞吸附协同催化CO分解作用[J]. 物理化学学报, 2016, 32(11), 2717-2723. doi: 10.3866/PKU.WHXB201607271

Ji-Hong LI,Chang-Feng LIN,Wu QIN,Xian-Bin XIAO,Li WEI. Synergetic Effect of Mercury Adsorption on the Catalytic Decomposition of CO over Perfect and Reduced Fe₂O₃[001] Surface[J]. Acta Phys. -Chim. Sin. 2016, 32(11), 2717-2723. doi: 10.3866/PKU.WHXB201607271

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201607271

https://www.whxb.pku.edu.cn/CN/Y2016/V32/I11/2717

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理想与还原Fe₂O₃[001]表面上汞吸附协同催化CO分解作用

Synergetic Effect of Mercury Adsorption on the Catalytic Decomposition of CO over Perfect and Reduced Fe₂O₃[001] Surface

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