• • Achieved hydrogen evolution rate of 84.3 mmol g-1 h-1 and benzaldehyde evolution rate of 75.1 mmol g-1 h-1, representing a significant advancement over conventional heterojunction systems; this performance is critical for industrial-scale solar fuel production where high throughput is essential for economic viability.
• • Demonstrated 94.8% selectivity for benzyl alcohol oxidation to benzaldehyde, minimizing overoxidation to CO2; this high selectivity is industrially crucial for producing high-value fine chemicals while maintaining high atom economy and reducing downstream separation costs.
• • Engineered an atomically coherent interface with ultralow lattice mismatch of 2.5%, which suppresses structural defects and enhances charge transfer; this structural precision is vital for long-term operational stability and consistent performance in photocatalytic reactors.
• • Validated the proton spillover pathway via kinetic isotope effect and in situ infrared spectroscopy, confirming that electrons and protons converge at cobalt sites; this mechanistic insight enables rational design of next-generation photocatalysts with optimized reaction kinetics.