Intensifying uneven charge distribution via geometric distortion engineering in atomically dispersed M-N_(x)/S sites for efficient oxygen electroreduction

查看全文 作　　者：Zhuting [1]Zhang;Simin [1]Yang;Rui [1]Jiang;Tian [2]Sheng;Chunfeng [3]Shi;Yueguang [1]Chen;Leyu [1]Wang

机构地区：[1]State Key Laboratory of Chemical Resource Engineering,College of Chemistry,Beijing University of Chemical Technology,Beijing 100029,China;[2]College of Chemistry and Materials Science,Anhui Normal University,Wuhu 214000,China;[3]Research Institute of Petroleum Processing,SINOPEC,Beijing 100083,China

出　　处：《Nano Research》索引2022年第15卷第10期,共8页

基　　金：supported by the National Natural Science Foundation of China(Nos.21701005 and 21903001);the Fundamental Research Funds for the Central Universities(No.XK2020-02);China Petroleum&Chemical Corporation(SINOPEC)(No.421028)。 摘　　要：Fine regulation of geometric structures has great promise to acquire specific electronic structures and improve the catalytic performance of single-atom catalysts,yet it remains a challenge.Herein,a novel seed encapsulation–decomposition strategy is proposed for the geometric distortion engineering and thermal atomization of a series of Cu-N_(x)/S moieties anchored on carbon supports.During pyrolysis,seeds(Cu^(2+),CuO,or Cu_(7)S_(4) nanoparticles)confined in metal organic framework can accommodate single Cu atoms with Cu–N or Cu–S coordination bonds and simultaneously induce C–S or C–N bond cleavage in the second coordination shell of Cu centers,which are identified to manipulate the distortion degree of Cu-N_(x)/S moieties.The severely distorted Cu-N3S molecular structure endows the resultant catalyst with excellent oxygen reduction reaction activity(E_(1/2)=0.885 V)and zinc-air battery performance(peak power density of 210 mW·cm^(−2)),outperforming the asymmetrical and symmetrical Cu-N4 structures.A combined experimental and theoretical study reveals that the geometric distortion of Cu-N_(x)/S moieties creates uneven charge distribution by a unique topological correlation effect,which increases the metal charge and shifts the d-band center toward the Fermi level,thereby optimizing the inter-mediate adsorption energy. 关键词：single-atomic sites geometric distortion engineering seed encapsulation-decomposition strategy charge distribution oxygen reduction reaction

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Intensifying uneven charge distribution via geometric distortion engineering in atomically dispersed M-N_(x)/S sites for efficient oxygen electroreduction

参考文献(42)

引证文献(3)

耦合文献(118)

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