Lai, F; Feng, J; Ye, X; Zong, W; He, G; Miao, Y-E; Han, X; ... Liu, T; + view all Lai, F; Feng, J; Ye, X; Zong, W; He, G; Miao, Y-E; Han, X; Ling, XY; Parkin, IP; Pan, B; Sun, Y; Liu, T; - view fewer (2019) Energy level engineering in transition-metal doped spinel-structured nanosheets for efficient overall water splitting. Journal of Materials Chemistry A , 7 (2) pp. 827-833. 10.1039/c8ta10162k.

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Abstract

Unraveling the role of transition-metal doping in affecting the native spinel-structured nanosheets' water splitting remains a grand challenge. In this work, a series of spinel-structured nanosheets wrapped hollow nitrogen-doped carbon polyhedrons were constructed, and doped transition-metal domains were deliberately introduced on the surface. Theoretical investigations show that their energy level can be finely tuned via direct transition-metal doping engineering. As a prototype, an Fe-doped NiCo2O4 nanosheets wrapped hollow nitrogen-doped carbon polyhedron (Fe–NiCo2O4@HNCP) exhibits outstanding bifunctional electrocatalytic performances with low overpotentials (η = 270 mV for OER, η = 84 mV for HER), low Tafel slopes (b = 42 mV dec−1 for OER, b = 47 mV dec−1 for HER), and high durability. The enhanced performance is attributed to the synergistic effects of energy level matching for electron transfer, and partial charge delocalization-induced rich active sites for reactant adsorption via thermodynamic and kinetic acceleration. This work may open a new pathway to design highly active and stable transition-metal doped electrocatalysts by manipulated energy levels for efficient overall water splitting.

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