The Secret of Nanoarrays toward Efficient Electrochemical Water Splitting: A Vision of Self‐Dynamic Electrolyte

Abstract Nanoarray electrocatalysts with unique advantage of facilitating gas bubble detachment have garnered significant interest in gas evolution reactions (GERs). Existing research is largely based on a static hypothesis, assuming that buoyancy is the only driving force for the release of bubbles during GERs. However, this hypothesis overlooks the effect of the self‐dynamic electrolyte flow, which is induced by the release of mature bubbles and helps destabilize and release the smaller, immature bubbles nearby. Herein, the enhancing effect of self‐dynamic electrolyte flow on nanoarray structures is examined. Phase‐field simulations demonstrate that the flow field of electrode with arrayed surface focuses shear force directly onto the gas bubble for efficient detachment, due to the flow could pass through voids and channels to bypass the shielding effect. The flow field therefore has a more substantial impact on the arrayed surface than the nanoscale smooth surface in terms of reducing the critical bubble size. To validate this, superaerophobic ferrous‐nickel sulfide nanoarrays are fabricated and employed for water splitting, which display improved efficiency for GERs. This study contributes to understanding the influence of self‐dynamic electrolyte on GERs and emphasizes that it should be considered when designing and evaluating nanoarray electrocatalysts.