AFM-Quantified Adhesion Energy Describes Bubble-Mediated Mass Transport on Gas-Evolving Electrodes.

Mass transport at three-phase interfaces is a primary bottleneck for industrial gas-evolving electrodes due to severe bubble coverage and suppressed liquid renewal. Here, we establish the interfacial work of adhesion (ΔGad)-quantified via spherical-tip AFM nanoindentation-as a predictive nanoscale descriptor of surface energetics under ambient conditions. ΔGad captures the thermodynamic competition between electrolyte wetting and gas adhesion at the solid surface, thereby governing bubble-mediated mass transport. Using model MoS2 electrodes, we show that vertical structuring and phase engineering (Vhetero-MoS2) significantly increase the AFM-quantified ΔGad. This heightened ΔGad strengthens the solid-electrolyte affinity, effectively suppressing gas adhesion and reducing bubble blockage. In situ Particle Image Velocimetry (PIV) and pseudopotential simulations consistently show that surfaces with higher ΔGad yield smaller bubbles and enhanced interfacial renewal. Accordingly, the apparent aerophobicity follows from stronger electrolyte affinity via interfacial energy competition. Using hydrogen evolution as a representative gas-evolving reaction, the Vhetero-MoS2 electrode sustains stable hydrogen evolution at 1000 mA cm- 2. This work provides a unified energetic framework for three-phase interface engineering, establishing ΔGad as a quantifiable, AFM-accessible metric for the rational design of high-performance gas-evolving electrodes.