Synergistic Entropy-Rich Alloy Effect and Metal–Support Interaction Fine-Tune the Electronic Structure for Augmented Oxygen Evolution Electrocatalysis

Developing multicomponent materials with high activity and establishing the precise regulation tactics of electronic structures at active sites, as well as their underlying mechanism of catalytic activity, are of great significance for oxygen evolution reaction (OER) electrocatalysis. In this study, we utilize the NaCl-templated assisted pyrolysis tactics to prepare a quinary NiCoFeMoZn catalyst, one heterostructure formed between a Zn-doped NiCoFe alloy and Mo_<i>x</i>C-based phases within a carbon sponge. This smart design enables an effective dual-mode electronic structure fine-tuning strategy, incorporating entropy-induced modulation and metal-support interactions to precisely regulate the electronic structure of Ni active sites and enhance electrocatalytic activity. As a result, the quinary NiCoFeMoZn electrocatalyst exhibits a low overpotential of 286 mV at 10 mA cm^-2, which is superior to those of quaternary and ternary counterparts. Furthermore, systematic experimental and theoretical studies confirm the universality of this dual-modality approach, providing an innovative avenue for modulating electronic structure precisely to obtain advanced OER electrocatalysts.