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铈钴复合氧化物催化剂催化CO-SCR反应机理研究
引用本文:付玉秀,仲雪梅,常化振,李俊华. 铈钴复合氧化物催化剂催化CO-SCR反应机理研究[J]. 中国环境科学, 2018, 38(8): 2934-2940
作者姓名:付玉秀  仲雪梅  常化振  李俊华
作者单位:1. 中国人民大学环境学院, 北京 100872;2. 清华大学环境学院, 北京 100084
基金项目:国家重点研发计划项目(2016YFC0203900,2016YFC0203901);国家自然科学基金项目(51778619,21577173)
摘    要:利用共沉淀法制备了一系列Ce-Co-Ox复合氧化物催化剂,并对其CO-SCR反应性能进行了研究.考察了Co和Ce比例对CO-SCR反应活性的影响,确定最佳的Ce和Co复合比例为3:7,最高转化率为84%(250℃).经表征分析发现,Ce(0.3)-Co(0.7)-Ox上发生CO-SCR的主活性位点是Co.掺杂Ce提升催化性能主要有两方面原因:一是催化剂比表面积增大,提高了表面的吸附位数量;二是Ce-Co-Ox催化剂形成的固溶体提升了氧迁移率.反应机理可能是气态或者弱吸附状态的CO与NO的吸附物种(主要是桥接二齿亚硝酸盐物种和螯合式双齿硝酸盐物种)反应.

关 键 词:氧化铈  氧化钴  CO-SCR  弱吸附态CO  桥接二齿亚硝酸盐物种  
收稿时间:2018-01-14

Mechanism study on CO-SCR over Ce-Co-Ox mixed oxides catalysts
FU Yu-xiu,ZHONG Xue-mei,CHANG Hua-zhen,LI Jun-hua. Mechanism study on CO-SCR over Ce-Co-Ox mixed oxides catalysts[J]. China Environmental Science, 2018, 38(8): 2934-2940
Authors:FU Yu-xiu  ZHONG Xue-mei  CHANG Hua-zhen  LI Jun-hua
Affiliation:1. School of Environment & Natural Resource, Renmin University of China, Beijing 100872, China;2. School of Environment, Tsinghua University, Beijing 100084, China
Abstract:In this paper, a series of Ce-Co-Ox catalysts were prepared by co-precipitation method and the CO-SCR performance was studied. The influence of Co and Ce ratio on the activity of CO-SCR was investigated and the Ce(0.3)-Co(0.7)-Ox sample showed the highest NO conversion efficiency of 84% at 250℃. According to characterization results, it was proposed that the active sites for CO-SCR is Co in Ce(0.3)-Co(0.7)-Ox. There were two reasons responsible for the enhanced catalytic performance by Ce doping into the Ce-Co-Ox catalyst. Firstly, the specific surface area and adsorption capacity were increased with Ce doping. Secondly, a solid solution was formed in Ce-Co-Ox catalyst, resulting in the enhanced oxygen migration rate. In situ DRIFTs results suggested that the CO-SCR is likely to follow a mechanism that gaseous or weakly-adsorbed CO reacts with adsorbed NO species in the forms of bridging bidenate nitrite and chelate nitrate.
Keywords:cerium oxide  cobalt oxide  CO-SCR  weak adsorbed CO  bridging bidentate nitrite species  
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