Efficient Carrier Separation via Ru@TS@C Zeolite: Enabling Photo‐Cathodes for High‐Efficiency Photo‐Assisted Metal−Air Batteries

Abstract Neutral aqueous Zn−air batteries (ZABs), while promising for extended lifespans and recyclability compared to alkaline systems, are hindered by sluggish kinetics that limit energy efficiency and power output. Here, we report an effective approach to construct a photo‐assisted near‐neutral ZAB based on a photo‐responsive titanium silicalite‐1 zeolite (TS‐1). The incorporation of Ru active centers into the 3D porous architecture of TS@C (Ru@TS@C), which exhibits remarkably enhanced electronic conduction, creates interconnected conductive pathways. This unique design facilitates rapid charge transfer across the 3D network, enabling exceptional reaction kinetics, and improved separation efficiency of photogenerated electron–hole pairs. Synergistic experimental and theoretical analyses reveal a photoinduced charge transfer mechanism in the conductive zeolite, where light‐driven Ru‐mediated electron exchange with oxygen adsorbates accelerates 4e − ‐dominant oxygen reduction reaction (ORR) kinetics. Consequently, the Ru@TS@C‐based photo‐assisted ZAB exhibits exceptional 4e − selectivity and reversibility, achieving a low overpotential of 218 mV at 0.2 mA cm −2 under illumination (74% reduction compared to dark conditions). Extended to Li–O 2 batteries, this multifunctional architecture demonstrates superior rate capability and cycling stability (>150 cycles). This work pioneers the use of photoactive zeolites in metal–air batteries and establishes a universal framework for engineering photo‐responsive interfaces to overcome intrinsic kinetic limitations in sustainable energy systems.