Polarization-Selective Efficient Hydrogen Evolution Reactions via Chiral Photocatalysis

The growing demand for sustainable energy solutions has stimulated the development of advanced photocatalysts with enhanced efficiency of solar-driven hydrogen production. However, the intrinsic challenges of hydrogen evolution reaction (HER), including rapid electron–hole recombination, and insufficient light absorption of conventional semiconductors, underscore the need for innovative catalytic strategies beyond conventional semiconductors. Here, a chirality-integrated plasmonic photocatalyst synthesized via circularly polarized light (CPL)-guided growth of Au nanoparticles on g-C₃N₄, yielding R-Au/C₃N₄ and L-Au/C₃N₄ with opposite optical chirality is presented. R-Au/C₃N₄ under right-handed CPL (RCP) illumination exhibits a 2.10-fold increase in hydrogen evolution rate compared to under left-handed CPL (LCP), and a 1.71-fold improvement over achiral A-Au/C₃N₄. In-situ Fourier transform infrared spectroscopy (FTIR) and time-resolved photoluminescence (TRPL) analyses revealed that chirality-matched light–catalyst pairs (i.e., RCP irradiation on R-Au/C₃N₄ and LCP irradiation on L-Au/C₃N₄) effectively suppress energy transfer pathway, thereby enriching the excited electron population in g-C₃N₄ and subsequently accelerating HER. Ex-situ EXAFS measurements demonstrated that chiral matching conditions contribute to reinforcing the structural durability of the resulting chiral catalyst. This CPL-responsive platform establishes a new paradigm in photocatalyst design by coupling chirality with light–matter interaction toward efficient solar-to-hydrogen conversion.