Strategic roles of surface and interface engineering in layered double hydroxides: Transforming photocatalytic hydrogen production efficiency

Abstract

Current research is increasingly focusing on converting renewable chemical and electrical energies into sustainable hydrogen fuel using advanced catalyst mediators. In this context, photocatalysis has emerged as a promising approach, with efficient photocatalysts requiring strong visible-light absorption, prolonged inhibition of charge recombination, abundant active surface sites, and effective charge transport. Layered double hydroxides (LDH) have gained attention due to their inherent structural and compositional versatility, which can be tailored through surface and interface engineering with semiconductors, metals, non-metals, noble metals, and carbon materials. This review aims to provide a comprehensive analysis of the fundamental roles of surface and interface engineering in enhancing photocatalytic H₂ production using LDH-based systems. We highlight innovative strategies such as tuning nanoscale morphology, inducing defects, optimizing band bending, and constructing heterojunctions that effectively promote charge transformation and suppress recombination. Despite these advances, our analysis also reveals current shortcomings in achieving full utilization of the solar spectrum and maintaining long-term stability under operational conditions. Our review concludes with a critical discussion of these challenges, along with opportunities and recommendations for future research to further advance the design, understanding, and practical implementation of LDH-based photocatalysts.