Regulating atomic Fe-Rh site distance for efficient oxygen reduction reaction

查看全文 作　　者：Tong [1]Liu;Yudan [1]Chen;Airong [1]Xu;Xiaokang [1]Liu;Dong [1]Liu;Sicheng [1]Li;Hui [1]Huang;Li [1]Xu;Shuaiwei [1]Jiang;Qiquan [3]Luo;Tao [1,2]Ding;Tao [1,2]Yao

机构地区：[1]National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,China;[2]Key Laboratory of Precision and Intelligent Chemistry,Hefei National Research Center for Physical Sciences at the Microscale,University of Science and Technology of China,Hefei 230026,China;[3]Institutes of Physical Science and Information Technology,Anhui University,Hefei 230601,China

出　　处：《Science China Chemistry》索引2024年第67卷第4期,共8页

基　　金：supported by the National Key R&D Program of China(2021YFA1600800 and 2020YFA0710203);the National Natural Science Foundation of China(12025505,22002147,22179125 and 12205304);the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0450200);the University of China Innovation Program of Anhui Province(GXXT-2020-053);the Youth Innovation Promotion Association CAS(2015366 and 2022458);the Fellowship of China Postdoctoral Science Foundation(2021TQ0319)。 摘　　要：Exploring the atomic interaction mechanisms of dense single-atom catalysts(SACs)is of great significance for their application in oxygen reduction reaction(ORR).However,the intrinsic mechanism of the site-distance effect on the catalytic performance has been largely ignored.Here,we demonstrate the site-distance effect of Fe-Rh_(x)@NC catalysts in ORR theoretically and experimentally.Bader charge analysis reveals that the strong interaction between Fe and Rh atoms at a certain atomic distance(dFe-Rh)alters the catalytic electronic structure,facilitating the optimization of catalyst adsorption strength.Motivated by the theoretical calculations,we designed and synthesized the Fe-Rhx@NC catalysts through a spatial confinement strategy.The characterization results prove that the Fe-Rh_(2)@NC has the optimal d_(Fe-Rh),which improves its intrinsic ORR activity,providing a half wave potential of 0.91 V,higher than that of the commercial Pt/C(0.86 V).This study emphasizes the importance of determining the basic mechanism of the site-distance effect in dissimilar metal atoms catalysts,which is conducive to the design of efficient catalyst systems for practical applications. 关键词：Density functional theory single-atom catalyst in-situ encapsulating site-distance effect oxygen reduction reaction

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Regulating atomic Fe-Rh site distance for efficient oxygen reduction reaction

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