Abstract
Heteroatomic substitution of spinel oxides can theoretically optimize oxygen evolution reaction (OER) via redistribution of charges and modification of d-band center. However, the wide pH range of electrocatalysis and catalytic mechanism are still great challenges. Herein, we successfully construct heteroatom Mn-substituted spinel Co3O4 (Mn-Co3O4) with porous hollow sphere structure for highly efficient and wide pH range OER. Benefiting from the atomic Mn-substitution and charge transfer, the Co site in Mn-Co3O4 displays an increased ratio of Co3+/Co2+. Electrochemical measurements demonstrate that Mn-Co3O4 exhibited superior OER activities with small overpotentials of only 305, 520 and 460 mV to afford a current density of 10 mA cm−2 in alkaline, neutral and acidic media, respectively. Meanwhile, Mn-Co3O4 also possesses favorable long-term stability in wide-pH electrolyte. The improved reaction kinetics of Mn-Co3O4 are mainly attributed to the unique hollow sphere structure with high specific surface area, and the increased high valency of Co, which can introduce the d-band center modification of Mn-Co3O4, and reduce the adsorption energy of oxygen intermediates in rate-determining step (RDS).
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