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Abstract Metal–support interaction (MSI) is witnessed as an essential manner to stabilize active metals and tune catalytic activity for heterogonous water splitting. Kinetically driving the water electrolysis (WE) appeals for a rational MSI system with the coupled electron‐donating/accepting (e‐D/A) characters for hydrogen/oxygen evolution reactions (HER/OER). However, the metal stabilization effect by MSI will in turn restrict the deblocking of e‐D/A properties and challenge the full electrocatalytic optimization. This study profiles a heterostructure featuring metastable Ru clusters on defective NiFe hydroxide (Ru/d‐NiFe LDH) support as a low‐precious (≈2 wt%) catalytic platform for efficient WE. It is indicated that the interfacial oxygen vacancies can deviate the stable Ru 4d 5 orbit to a metastable Ru 2+δ state, and regulate the metal d‐band center levels toward the facilitated HER/OER processes. Resultantly, the Ru/d‐NiFe LDH heterostructure attains the ultralow overpotentials at 10 mA cm −2 for Pt‐beyond alkaline HER (18 mV) and OER (220 mV) with fast kinetics and durability. The symmetrical water electrolyzer delivers a promising voltage of 1.49 V at 10 mA cm −2 in 1 m KOH and efficient seawater splitting performance. This work carries interesting opportunities in rationalizing sophisticated metal‐support electrocatalysts through metal‐site metastabilization engineering.
Chen et al. (Fri,) studied this question.