Corresponding Author

Dong-Xu Tian(tiandx@dlut.edu.cn);
Xi-Qiang Yan(965664856@qq.com)


The slow kinetics of oxygen reduction reaction (ORR) limits the performance of low temperature fuel cells. Thus, it needs to design effective catalysts with low cost. Core-shell clusters (CSNCs) show promising activity because of their size-dependent geometric and electronic effects. The ORR activity trend of Nim@Pt1Aun-m-1(n = 19, 38, 55, 79; m = 1, 6, 13, 19) was studied using the GGA-PBE-PAW methods. The adsorption configurations of *O, *OH and *OOH were optimized and the reaction free energies of four proton electron (H+ + e-) transfer steps were calculated. Using overpotential as a descriptor for the catalytic activity, Ni6@Pt1Au31 was found to be the most active ORR catalyst. Ni1@Pt1Au17, Ni13@Pt1Au41, and Ni19@Pt1Au59 had better activity than pure Pt clusters and Pt(111). Bader charge and DOS data indicate that the single Pt atom embedded on Nim@Aun-m can tune the electronic property of active site, and thus, significantly improve the activity. The present study showed that the single Pt atom embedded on Nim@Aun-m is a rational strategy to design effective core-shell ORR catalysts.

Graphical Abstract


core-shell metal clusters, oxygen reduction reaction, density functional theory, overpotential, single atom catalysis

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