Abstract

Structural and interface engineering enable the optimization of electrocatalysts in terms of both activity and durability. Herein, the three-dimensional (3D) architecture graphdiyne nanowall (GDY) serving as scaffolds anchor metal cations to form the NiFe layered double hydroxide (LDH) nanodots/graphdiyne (NiFe ND/GDY) heterojunction electrocatalysts for water oxidation in alkaline solution. After tuning the loading amount of NiFe-LDH carefully, the NiFe ND displays ultrasmall nanometer size of 2.7 nm and intimate interfacial coupling with GDY. Owing to the optimized 0D/3D structure, strong interfacial forces and the unique properties of GDY, the resulting NiFe ND/GDY requires an overpotential of only 252 mV to deliver current density of 10 mA cm−2 and shows favorable kinetics with a small Tafel slope of 39.70 mV dec−1. Notably, the mass activity of NiFe ND/GDY heterojunction is 70 times higher than that of the commercial RuO2 (631 A g−1 vs. 9 A g−1 to RuO2, at η = 300 mV), and it exhibits a superior long-term stability (only 10% degradation during continuous electrolysis of 100 h). This work indicates that GDY can serve as a promising substrate to anchor the ultrafine nanoparticle catalysts for water oxidation or beyond.

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