Electronic interactions between neighboring functionalized guest Sb single atoms and Pt clusters enhance CO tolerance  

作　　者：Wenkang Miao Ronghui Hao Lu Gan Wanyin Xu Zihan Wang Wenxin Lin Heguang Liu Yinchun Lyu Qianqian Li Jinyang Xi Anmin Nie Jinsong Wu Hongtao Wang 

机构地区：[1]Materials Genome Institute,Shanghai University,Shanghai 200444,China [2]School of Materials Science and Engineering,Zhejiang Sci-Tech University,Hangzhou 310018,Jiangsu,China [3]School of Materials Science and Engineering,Xi'an University of Technology,Xi'an 710048,Shaanxi,China [4]Center for High Pressure Science,State Key Laboratory of Metastable Materials Science and Technology,Yanshan University,Qinhuangdao 66004,Hebei,China [5]Nanostructure Research Center,Wuhan University of Technology,Wuhan 430070,Hubei,China [6]Center for X-mechanics,Zhejiang University,Hangzhou 310027,Zhejiang,China

出　　处：《Journal of Energy Chemistry》2025年第2期733-743,I0016,共12页能源化学(英文版)

基　　金：financially supported by the Shanghai RisingStar Program(No.23QA1403700);the National Natural Science Foundation of China(NSFC,Grant No.U2230102);the sponsored by National Key Research and Development Program of China(No.2021YFB3502200);the Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University.

摘　　要：Platinum-based(Pt)catalysts are notoriously susceptible to deactivation in industrial chemical processes due to carbon monoxide(CO)poisoning.Overcoming this poisoning deactivation of Pt-based catalysts while enhancing their catalytic activity,selectivity,and durability remains a major challenge.Herein,we propose a strategy to enhance the CO tolerance of Pt clusters(Pt_n)by introducing neighboring functionalized guest single atoms(such as Fe,Co,Ni,Cu,Sb,and Bi).Among them,antimony(Sb)single atoms(SAs)exhibit significant performance enhancement,achieving 99%CO selectivity and 33.6%CO_(2)conversion at 450℃,Experimental results and density functional theory(DFT)calculations indicate the optimization arises from the electronic interaction between neighboring functionalized Sb SAs and Pt clusters,leading to optimal 5d electron redistribution in Pt clusters compared to other functionalized guest single atoms.The redistribution of 5d electrons weaken both theσdonation andπbackdonation interactions,resulting in a weakened bond strength with CO and enhancing catalyst activity and selectivity.In situ environmental transmission electron microscopy(ETEM)further demonstrates the exception thermal stability of the catalyst,even under H_(2)at 700℃.Notably,the functionalized Sb SAs also improve CO tolerance in various heterogenous catalysts,including Co/CeO_(2),Ni/CeO_(2),Pt/Al_(2)O_(3),and Pt/CeO_(2)-C.This finding provides an effective approach to overcome the primary challenge of CO poisoning in Pt-based catalysts,making their broader applications in various industrial catalysts.

关 键 词：Functionalized guest single atoms Pt cluster CO tolerance Electronic effect In-situ TEM 

分 类 号：O64[理学—物理化学]