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Promoting effect of Cu-doping on catalytic activity and SO2 resistance of porous CeO2 nanorods for H2S selective oxidation
Journal of Catalysis ( IF 7.3 ) Pub Date : 2020-06-20 , DOI: 10.1016/j.jcat.2020.06.010
Xiaohai Zheng , Yanli Li , Shijing Liang , Zheng Yao , Yong Zheng , Lijuan Shen , Yihong Xiao , Yongfan Zhang , Chaktong Au , Lilong Jiang

A facile procedure for doping copper species into CeO2 lattices to prevent ceria from being deactivated and to offer additional active sites for selective H2S oxidation is reported here. Among the prepared catalysts, porous 10Cu/Ce nanorods with well-defined (100) and (110) reactive planes display excellent catalytic performance, exhibiting H2S conversion and sulfur selectivity of 100% at 220 °C, which is higher than those of most reported Ce-based catalysts. More importantly, electron transfer from Cu+ to Ce4+ suppresses the transfer of electrons from SO2 to Ce4+, leading to inhibition of SO2 oxidation to surface sulfate , which could deactivate the catalyst. Overall, the results of systematic experimental and theoretical studies prove that copper doping effectively promotes the formation of oxygen vacancies and resistance against SO2 poisoning. Furthermore, through in situ diffuse reflection infrared Fourier transform spectroscopy investigation and density functional theory calculations, the reaction intermediates in selective H2S oxidation and mechanism of SO2 resistance over the Cu-doped CeO2 catalysts are revealed.



中文翻译:

铜掺杂对多孔CeO 2纳米棒对H 2 S选择氧化的催化活性和抗SO 2的促进作用

这里报道了一种将铜物质掺杂到CeO 2晶格中的简便方法,以防止二氧化铈失活并为选择性H 2 S氧化提供额外的活性位点。在制备的催化剂中,具有明确的(100)和(110)反应面的多孔10Cu / Ce纳米棒显示出优异的催化性能,在220°C下具有H 2 S转化率和100%的硫选择性,高于大多数报道的铈基催化剂。更重要的是,电子从Cu +转移到Ce 4+抑制了电子从SO 2转移到Ce 4+,从而抑制了SO 2氧化成表面硫酸盐,可能会使催化剂失活。总体而言,系统的实验和理论研究结果证明,铜掺杂有效地促进了氧空位的形成和对SO 2中毒的抵抗力。此外,通过原位漫反射红外傅里叶变换光谱研究和密度泛函理论计算,揭示了在选择性H 2 S氧化反应中的反应中间体和对Cu掺杂的CeO 2催化剂抗SO 2的机理。

更新日期:2020-07-08
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