文献类型：期刊文献

英文题名：Molecular-Level Insight into Selective Catalytic Reduction of NOx with NH3 to N2 over a Highly Efficient Bifunctional Vα-MnOx Catalyst at Low Temperature

作者：Xin, Ying[1];Li, Hao[1];Zhang, Nana[1];Li, Qian[1];Zhang, Zhaoliang[1];Cao, Xiaoming[2,3];Hu, P.[2,3];Zheng, Lirong[4];Anderson, James A.[5]

机构：[1]Univ Jinan, Shandong Prov Key Lab Fluorine Chem & Chem Mat, Sch Chem & Chem Engn, Jinan 250022, Shandong, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Ctr Computat Chem, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China;[5]Univ Aberdeen, Surface Chem & Catalysis Grp, Mat & Chem Engn, Aberdeen AB24 3UE, Scotland

年份：2018

卷号：8

期号：6

起止页码：4937

外文期刊名：ACS CATALYSIS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000434369600020)】；

基金：This work was supported by the National Natural Science Foundation of China (Nos. 21477046, 21333003, and 21673072) and Key Technology R&D Program of Shandong Province (No. 2016ZDJS11A03). The authors also acknowledge computing time support from the Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) under Grant No. U1501501.

语种：英文

外文关键词：nitrogen oxides; selective catalytic reduction; bifunctional catalyst; density functional theory; mechanism

摘要：Selective catalytic reduction of NOx with ammonia (SCR) is not only an important model catalytic reaction but is also significant in terms of improving environmental air quality and human health. However, SCR catalysts suffer from low activity and selectivity to N-2 at low temperature, which in part may be attributed to our limited understanding of the reaction mechanism. Here, an unambiguous molecular-level mechanism is presented for an improved low-temperature SCR activity using bifunctional catalysts composed of highly active oxides (Mn2O3) for NH3 activation and highly selective vanadates (Mn2V2O7) that promote N-2 formation. NH3 is initially activated by Mn2O3 to form an NH2 intermediate. Transfer of NH2 to Mn2V2P7 then takes place, which facilitates the capture of gaseous NO leading to the formation of NH2NO over Mn2V2O7, whereafter NH2NO is efficiently converted to the preferred N-2 rather than the undesired byproduct, N2O. The proximity of the two components achieved via sol gel preparation plays a crucial role in the transfer of active intermediates.