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Electrocatalytic 2e− oxygen reduction reaction (2e− ORR) is a promising approach to producing H2O2 at ambient temperature and pressure especially in acidic media, which, however, is hindered by the high cost of precious metal-based electrocatalysts. Hence, the development of efficient earth-abundant electrocatalysts and reaction mechanism exploration for H2O2 production by 2e− ORR in acidic solution are critically important but remain challenging at present. In this work, NiSe2 has been developed as a novel and high-performance 2e− ORR electrocatalyst in acidic media, moreover, using nickel chalcogenides as the models, the influence of different anion species (Se22−, S22−, and O2−) on 2e− ORR electrocatalytic performance of the catalysts has been investigated. The synthesized NiSe2 exhibits outstanding 2e− ORR performance of high selectivity (90%) and long-term durability (12 h). The maximum H2O2 concentration of NiSe2 reaches 988 ppm, which is the highest among all the reported transition metal chalcogenides. This work demonstrates a novel point of view in anion tuning for designing high-efficiency transition-metal-based electrocatalysts for 2e− ORR.
This work was supported by Shanghai Science and Technology Committee Rising-Star Program (No. 22QA1403400), the Natural Science Foundation of Shanghai (No. 21ZR1418700), and the National Natural Science Foundation of China (No. 52201271). The authors would like to thank ECNU Multifunctional Platform for Innovation for support of SEM and TEM characterizations (004).