Single-atom catalysts with anionic metal centers: Promising electrocatalysts for the oxygen reduction reaction and beyond

作     者：Jinxing Gu Yinghe Zhao Shiru Lin Jingsong Huang Carlos R.Cabrera Bobby G.Sumpter Zhongfang Chen Jinxing Gu;Yinghe Zhao;Shiru Lin;Jingsong Huang;Carlos R.Cabrera;Bobby G.Sumpter;Zhongfang Chen

作者机构：Department of ChemistryUniversity of Puerto Rico.Rio Piedras Campus.San Juan.Puerto Rico 00931USA Center for Nanophase Materials SciencesOak Ridge National LaboratoryOak RidgeTennessee 37831USA Department of Chemistry and BiochemistryThe University of Texas at El PasoEl PasoTexas 79968USA 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2021年第30卷第12期

页      面：285-293,I0006页

核心收录：

学科分类：0808[工学-电气工程] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 0702[理学-物理学] 

基　　金：financially supported by the National Science Foundation-Centers of Research Excellence in Science and Technology (NSF-CREST Center) for Innovation,Research and Education in Environmental Nanotechnology (CIRE2N) (Grant No.HRD-1736093) the NSF Center for the Advancement of Wearable Technologies (Grant No.1849243) National Energy Research Scientific Computing Center,which is supported by the Office of Science of the U.S.DOE under Contract No.DE-AC02-05CH11231 

主　　题：Single-atom catalysts Anionic metal centers Antimonene Oxygen reduction reaction Nitrogen reduction reaction 

摘      要：Ongoing efforts to develop single-atom catalysts(SACs) for the oxygen reduction reaction(ORR) typically focus on SACs with cationic metal centers,while SACs with anionic metal centers(anionic SACs) have been generally ***,anionic SACs may offer excellent active sites for ORR,since anionic metal centers could facilitate the activation of O_(2) by back donating electrons to the antibonding orbitals of O_(2).In this work,we propose a simple guideline for designing anionic SACs:the metal centers should have larger electronegativity than the surrounding atoms in the substrate on which the metal atoms are *** means of density functional theory(DFT) simulations,we identified 13 anionic metal centers(Co,Ni,Cu,Ru,Rh,Pd,Ag,Re,Os,Ir,Pt,Au,and Hg) dispersed on pristine or defective antimonene substrates as new anionic SACs,among which anionic Au and Co metal centers exhibit limiting potentials comparable to,or even better than,conventional Pt-based catalysts towards *** also found that anionic Os and Re metal centers on the defective antimonene can electrochemically catalyze the nitrogen reduction reaction(NRR) with a limiting potential close to that of stepped Ru(0001).Overall,our work shows promise towards the rational design of anionic SACs and their utility for applications as electrocatalysts for ORR and other important electrochemical reactions.