Abstract

Realizing rapid electron transfer and mass diffusion in virtue of interface regulation and nanostructure design is an effective strategy to augment the catalytic activity of carbon materials but still a significant challenge. Herein, a novel frontier 1D/3D rambutan-like Mott-Schottky-type nitrogen-doped carbon polyhedron (NiCo-NCP/CNT) consisting of nickel/cobalt species and a 3D porous carbon skeleton intertwined with 1D carbon nanotubes (CNT) is controllably fabricated by rationally utilizing Co/Zn bimetallic-organic frameworks and nickel ions. The photovoltaic device fabricated with NiCo-NCP/CNT electrocatalyst achieves a power conversion efficiency of 8.75%, which is superior to that of conventional Pt electrodes (7.25%). When the NiCo-NCP/CNT electrocatalyst is employed as the cathode for water splitting under alkaline conditions, an overpotential as low as 63 mV is demonstrated at a current density of 10 mA·cm−2. The improved work function (from 4.65 to 4.59 eV) proves that introducing NiCo favors regulating electronic states and optimizing energy level, which could induce more robust self-driven electron transfer at the Mott-Schottky interface. The proposed nickel adsorption-sintering strategy effectively promotes electron/mass transfer capability simultaneously in carbon-based Mott-Schottky catalysts and paves the way for developing low-cost and high-performance electrocatalysts in electrocatalytic fields.

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