文献类型：期刊文献

英文题名：Asymmetric coordinative modulation boosting the activity and thermal stability of Pt1/CeO2 for CO oxidation under harsh condition

作者：Ni, Lijun[1,2];Zhou, Yuwei[1,2];Tan, Wei[3];Li, Hong[4];Wang, Dong[5,6];Zhang, Qi[1,2];Yang, Bing[4];Xu, Jing[7];Zhang, Ying[1,2];Pan, Chengsi[1,2];Zhu, Yongfa[8];Liu, Fudong[9];Lou, Yang[1,2]

机构：[1]Jiangnan Univ, Sch Chem & Mat Engn, Key Lab Synthet & Biol Colloids, Minist Educ, Wuxi 214122, Jiangsu, Peoples R China;[2]Jiangnan Univ, Int Joint Res Ctr Photorespons Mol & Mat, Wuxi 214122, Jiangsu, Peoples R China;[3]Nanjing Univ, Ctr Modern Anal, Key Lab Mesoscop Chem MOE, Sch Chem & Chem Engn,State Key Lab Pollut Control, Nanjing 210023, Jiangsu, Peoples R China;[4]Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian 116023, Liaoning, Peoples R China;[5]East China Univ Sci & Technol, Ctr Computat Chem, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[6]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[7]Jiangnan Univ, Sch Food Sci & Technol, Wuxi 214122, Jiangsu, Peoples R China;[8]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China;[9]Univ Calif Riverside, Ctr Environm Res & Technol CE CERT, Mat Sci & Engn MSE Program, Dept Chem & Environm Engn,Bourns Coll Engn, Riverside, CA 92521 USA

年份：2024

卷号：501

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20244617354754);WOS:【SCI-EXPANDED(收录号:WOS:001357043600001)】；

基金：This project was supported financially by the National Key R & D Program of China (2021YFB3501900), National Natural Science Foundation of China (U21A20326, 22072118, 22273021, 22379054, 22306090), Jiangsu Specially-Appointed Professor (1046010241211400), Natural Science Foundation of Jiangsu Province (BK20211239, BK20230773), and Shanghai Science and Technology Development Funds (22QA1402900). F. L. acknowledges the Startup Fund from the University of California, Riverside (UCR). The authors gratefully acknowledge the use of facilities within the Central Laboratory, School of Chemical and Material Engineering at Jiangnan University.

语种：英文

外文关键词：Single atom catalysts; Surface coating; Coordination configuration; Low-temperature activity; Thermal stability

摘要：Supported metal catalysts play a central role in chemical industry, but it remains a formidable challenge to realize high activity while maintaining atomically dispersed status to maximize atom efficiency under harsh conditions. Herein, a novel strategy of constructing asymmetric coordination Pt active sites via coating N-doped carbon onto ceria supported Pt single atoms (Pt1/CeO2@CN) is proposed, through which superior lowtemperature CO oxidation activity and satisfactory thermal stability are achieved simultaneously. Experimental and density functional theory results confirm that the unique asymmetric N2-Pt1-O2 coordinative configuration on Pt1/CeO2@CN tailors the electronic properties of Pt 5d states, increasing the turnover frequency by 15 times for CO oxidation at 120 degrees C compared with that on Pt1/CeO2 and sustaining the atomically dispersed status of Pt at as high as 400 degrees C under H2-containing atmosphere. This strategy suggests a promising avenue to fabricating highly active and stable supported metal catalysts for practical applications under harsh conditions.