Exploring highly active earth-abundant bifunctional electrocatalysts for water splitting at a high output is essential for the forthcoming hydrogen economy.Non-noble Fe3O4 catalyst owns outstanding conductiv-ity and its octahedral Fe sites can markedly promote water dissociation.However,it lacks active centers on the surface,resulting in its poor activity when used as a catalyst for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Herein,an electron redistribution strategy is proposed by introduc-ing Ni sites onto the surface of Fe3O4(Ni/Fe3O4).The abundant delocalized electrons,derived from the electronic interaction of Ni and Fe3O4 species,significantly optimize the electronic structure of the Ni/Fe3O4 catalyst,leading to its improved adsorption behavior.This Ni/Fe3O4 catalyst exhibits remarkable bifunctional activity,steadily outputting 1000 mA cm-2 at the low overpotential of 387 mV for HER and 338 mV for OER,respectively.Using Ni/Fe3O4 as a bifunctional catalyst for overall water splitting reaction exhibits the optimal performance with outstanding stability,obtaining a current density of 1000 mA cm-2 at 1.98 V,much superior to a Pt/C‖IrO2 cell.Experimental analysis and theoretical calcu-lations collectively corroborate that the electron redistribution of Fe3O4 is activated by coupling Ni spe-cies,leading to the promoted HER and OER kinetics.This electron redistribution strategy provides an effective method to activate transition metal-based catalysts which are promising to be utilized as supe-rior electrocatalysts for the industrial overall water splitting reaction.

Wenli Xu;Wenda Zhong;Chenfan Yang;Rong Zhao;Jing Wu;Xuanke Li;Nianjun Yang

Hubei Province Key Laboratory of Coal Conversion and New Carbon Materials,Wuhan University of Science and Technology,Wuhan 430081,Hubei,China;Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology,Hunan University,Changsha 410082,Hunan,China;Institute of Materials Engineering,University of Siegen,Siegen 57076,Germany

能源化学

[1]Wenli Xu;Wenda Zhong;Chenfan Yang;Rong Zhao;Jing Wu;Xuanke Li;Nianjun Yang-.Tailoring interfacial electron redistribution of Ni/Fe3O4 electrocatalysts for superior overall water splitting)[J].能源化学,2022(10):330-338

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