Transforming Adsorbate Surface Dynamics in Aqueous Electrocatalysis: Pathways to Unconstrained Performance

Abstract Developing highly efficient catalysts to accelerate sluggish electrode reactions is critical for the deployment of sustainable aqueous electrochemical technologies, yet remains a great challenge. Rationally integrating functional components to tailor surface adsorption behaviors and adsorbate dynamics would divert reaction pathways and alleviate energy barriers, eliminating conventional thermodynamic constraints and ultimately optimizing energy flow within electrochemical systems. This approach has, therefore, garnered significant interest, presenting substantial potential for developing highly efficient catalysts that simultaneously enhance activity, selectivity, and stability. The immense promise and rapid evolution of this design strategy, however, do not overshadow the substantial challenges and ambiguities that persist, impeding the realization of significant breakthroughs in electrocatalyst development. This review explores the latest insights into the principles guiding the design of catalytic surfaces that enable favorable adsorbate dynamics within the contexts of hydrogen and oxygen electrochemistry. Innovative approaches for tailoring adsorbate‐surface interactions are discussed, delving into underlying principles that govern these dynamics. Additionally, perspectives on the prevailing challenges are presented and future research directions are proposed. By evaluating the core principles and identifying critical research gaps, this review seeks to inspire rational electrocatalyst design, the discovery of novel reaction mechanisms and concepts, and ultimately, advance the large‐scale implementation of electroconversion technologies.