文献类型：期刊文献

英文题名：An Atom-Pair Design Strategy for Optimizing the Synergistic Electron Effects of Catalytic Sites in NO Selective Reduction

作者：Qu, Weiye[1];Yuan, Haiyang[2,3,6];Ren, Zhouhong[4];Qi, Jizhen[5];Xu, Dongrun[1];Chen, Junxiao[1];Chen, Liwei[4,5,7];Yang, Huagui[6];Ma, Zhen[1,8];Liu, Xi[4];Wang, Haifeng[2,3];Tang, Xingfu[1,8]

机构：[1]Fudan Univ, Dept Environm Sci & Engn, Shanghai 200438, Peoples R China;[2]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Ctr Computat Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]Shanghai Jiao Tong Univ, In Situ Ctr Phys Sci, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China;[5]Chinese Acad Sci, CAS Ctr Excellence Nanosci, i Lab, Suzhou Inst Nanotech & Nanob SINANO, Suzhou 215123, Peoples R China;[6]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;[7]Shanghai Jiao Tong Univ, Frontiers Sci Ctr Transformat Mol, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China;[8]Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China

年份：2022

卷号：61

期号：12

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20224913213700);WOS:【SCI-EXPANDED(收录号:WOS:000890471300001)】；

基金：Acknowledgements We thank Prof. Jianjun Chen from Tsinghua University for the help in the Raman and DRIFTS measurements. The XAS were carried out with the support of BL14W1 beamline at Shanghai Synchrotron Radiation Facility (SSRF) and 4B9B beamline at Beijing Synchrotron Radiation Facility (BSRF). This work was supported financially by the National Natural Science Foundation of China (21976037, 22072090, 21991153, 21873028, and 91945302) and National Key R&D Program of China (2021YFB3500600, 2021YFA1500300, 2021YFA1500700).

语种：英文

外文关键词：Atom-Pair Catalytic Sites; Reaction Mechanisms; Selective Catalytic Reduction; Surface Reactions; Synergistic Electron Effects

摘要：Effective adsorption and speedy surface reactions are vital requirements for efficient active sites in catalysis, but it remains challenging to maximize these two functions simultaneously. We present a solution to this issue by designing a series of atom-pair catalytic sites with tunable electronic interactions. As a case study, NO selective reduction occurring on V-1-W-1/TiO2 is chosen. Experimental and theoretical results reveal that the synergistic electron effect present between the paired atoms enriches high-energy spin charge around the Fermi level, simultaneously rendering reactant (NH3 or O-2) adsorption more effective and subsequent surface reactions speedier as compared with single V or W atom alone, and hence higher reaction rates. This strategy enables us to rationally design a high-performance V-1-Mo-1/TiO2 catalyst with optimized vanadium(IV)-molybdenum(V) electronic interactions, which has exceptional activity significantly higher than the commercial or reported catalysts.