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Developing low-cost, environmentally friendly and efficient non-precious metal electrocatalysts as alternatives to noble metals for the hydrogen evolution reaction (HER) is highly essential for the sustainable advancement of green hydrogen energy. Herein, a novel heterostructured Ni 3 P/Ni nanoparticle anchored in nitrogen-doped mesoporous carbon nanofibers (Ni 3 P/Ni@N-CNFs) is prepared by a facile solid-phase calcination protocol. The results demonstrated that benefiting from the intensive electronic coupling effect at the interface of the Ni 3 P/Ni heterostructure, the electron configuration of the Ni active site is optimized and thus the favorable HER activity. Furthermore, the N-doped carbon nanofiber scaffold with an extensive mesoporous structure endows Ni 3 P/Ni@N-CNFs with abundant electrochemically active sites together with excellent conductivity and stability, contributing to fast electron/mass transport. As expected, the resultant Ni 3 P/Ni@N-CNF electrocatalyst exhibited exceptional HER catalytic properties under universal pH conditions, driving a current density of 10 mA cm -2 at pretty low overpotentials of 121 mV, 145 mV and 187 mV in acidic, basic and neutral solutions, respectively, and retaining the catalytic stability for over 60 h. This intriguing work represents a fresh perspective for designing and exploiting highly advanced phosphide electrocatalysts for green hydrogen fuel production.

Tuning the coupling interface of a heterostructured catalyst is an effective approach to achieve abundant surface catalytic active sites and strong electronic interactions among active materials for improving electrocatalytic water splitting performance. Herein, we report a novel heterogeneous catalyst comprising Ni3S2 nanoparticles embedded in ultrathin NiV-layered double hydroxide nanosheet arrays supported on nickel foam, denoted as Ni3S2@NiV-LDH/NF. We demonstrate that the active edge-state length and the surface chemical state of such NiV-LDH-based heterostructures are well modulated by tailoring the coupling interfaces, resulting in the exposure of more catalytic reaction sites and enhancement of the electronic interactions between NiV-LDH and Ni3S2, thus greatly promoting the water dissociation kinetics. As expected, the optimized Ni3S2@NiV-LDH/NF heterostructures exhibit outstanding electrocatalytic activity for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), with an extremely low overpotential of 126 mV and 190 mV to deliver 10 mA cm-2 for the HER and OER without iR compensation in alkaline media, respectively. More importantly, Ni3S2@NiV-LDH/NF simultaneously functioned as both the anode and cathode for water splitting to yield a current density of 10 mA cm-2 at a cell voltage of only 1.53 V with an outstanding durability for 160 h. This work provides a new insight into the regulation of the coupling interface for obtaining highly active heterostructured catalysts for overall water splitting.