Hydroxyl Surface Enrichment Strategy to Achieve Dual‐Mechanism Pathway for Overcoming the Activity–Stability Trade‐Off of Oxygen Evolution Reaction

ABSTRACT Constructing a coupling pathway between the adsorption evolution (AEM) and lattice oxygen‐mediated mechanisms (LOM) may be a promising solution to break the activity–stability trade‐off in oxygen evolution reaction (OER), which still remains a critical scientific challenge. Herein, we propose a hydroxyl enrichment strategy by introducing a hard Lewis acid (ZrO 2 ) into NiFeP matrix, which not only promotes the formation of key oxygen‐containing intermediates and accelerates AEM reaction kinetics but also induces the rapid generation of a high‐valent Ni active phase, thereby activating lattice oxygen and facilitating the LOM process. The implementation of AEM and LOM dual‐mechanism successfully overcomes the traditional trade‐off between activity and stability in the OER process, because the formation of a dynamic hydrogen‐bond network and the rapid reversible regeneration of lattice oxygen effectively ensure structural stability during the OER process, which have been confirmed by electrochemical probes, in situ spectroscopies and theoretical calculations. Benefiting from optimized interfacial dynamics and dual‐reaction pathways, the as‐synthesized catalyst (ZrO 2 ‐NiFeP) can stably operate over 1100 h @ 1.0 A cm −2 in alkaline water electrolyzer. In summary, the AEM and LOM dual‐mechanism proposed here may provide a novel paradigm to boost both activity and stability of OER electrocatalysts.