Abstract

In this study, scalable and facile electroless plating accompanied with phosphorization process is explored for preparation of interconnectednetwork of Ni2P–Co2P on carbon clothes (CC) substrate. The binder-free Ni2P–Co2P/CC electrocatalyst with optimized Ni2P:Co2P ratio displays outstanding HER activity in both alkaline and acidic conditions requiring only 93 mV and 172 mV vs. RHE of overpotential to reach 10 mA cm−2 of current density. The superior HER activity of Ni2P–Co2P/CC could be attributed to (i) the abundantinterfacial contactandlarger electrochemical surface area; (ii) regulated electronic structure and hydrophilic surface of the catalyst, and (iii) interfacial charge redistribution contributing more high-valence Ni active sites, as visualized by off-axis electron holography. Overall, this work directly demonstrates the interfacial charge redistribution in Ni2P–Co2P/CC interconnected network, and suggests a facile strategy for structural design and preparation of highly efficient phosphide electrocatalysts.

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