文献类型：期刊文献

英文题名：Activity Self-Optimization Steered by Dynamically Evolved Fe3+@Fe2+ Double-Center on Fe2O3 Catalyst for NH3-SCR

作者：Yuan, Hai Yang[1,2,3,4];Sun, Ningning[1,2,3];Chen, Jianfu[1,2,3];Yang, Hua Gui[4];Hu, P.[1,2,3,5];Wang, Haifeng[1,2,3]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Res Inst Ind Catalysis, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Ctr Computat Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, Shanghai 200237, Peoples R China;[5]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9, North Ireland

年份：2022

卷号：2

期号：10

起止页码：2352

外文期刊名：JACS AU

收录：EI(收录号：20224212897767);WOS:【ESCI(收录号:WOS:000861774100001)】；

基金：? ACKNOWLEDGMENTS This project was supported by the National Key Research and Development Program of China (2021YFA1500700) , the National Natural Science Foundation of China (91945302, 92045303, 21902048, 21873028) , the National Ten Thousand Talent Program for Young Top-notch Talents in China, and the Fundamental Research Funds for the Central Universities.

语种：英文

外文关键词：dynamically active center; activity self-optimization; reaction mechanism; NH3-SCR; Fe2O3 catalyst

摘要：Identification of the active centers dynamically stable under the reaction condition is of paramount importance but challenging because of the limited knowledge of steady-state chemistry on catalysts at the atomic level. Herein, focusing on the Fe2O3 catalyst for the selective catalytic reduction of NO with NH3 (NH3-SCR) as a model system, we reveal quantitatively the self-evolving Fe3+@Fe2+ (similar to 1:1) double-centers under the in-situ condition by the first-principles microkinetic simulations, which enables the accurate prediction of the optimal industry operating temperature (590 K). The cooperation of this double-center achieves the self-optimization of catalytic activity and rationalizes the intrinsic origin of Fe2O3 catalyzing NH3-SCR at middle-high temperatures instead of high temperatures. Our findings demonstrate the atomic-level self-evolution of active sites and the dynamically adjusted activity variation of the catalyst under the in-situ condition during the reaction process and provide insights into the reaction mechanism and catalyst optimization.