Photo‐Driven Hydrogen Production from Methanol and Water using Plasmonic Cu Nanoparticles Derived from Layered Double Hydroxides

Abstract Methanol steam reforming (MSR) is viewed as an important technology in the growth of a future hydrogen economy, with methanol serving as an easily transportable and storable liquid hydrogen carrier. However, the thermocatalytic MSR reaction is energy intensive as it requires high temperatures. Herein, a novel L‐Cu catalyst is successfully fabricated for photo‐driven MSR through reduction of CuAl layered double hydroxide (CuAl‐LDH) nanosheets. L‐Cu offers outstanding activity for the photothermal conversion of methanol and water to hydrogen (160.5 µmol g_cat⁻¹ s⁻¹) under ultraviolet‐visible irradiation, with this rate being much higher than that achieved for L‐Cu at the same temperature in the dark. Characterization studies using X‐ray diffraction, X‐ray photoelectron spectroscopy, X‐ray absorption spectroscopy, and high‐resolution transmission electron microscopy determine that L‐Cu catalyst comprise Cu nanoparticles on an amorphous alumina support. Computational calculations reveale that Cu localized surface plasmon resonance effects promote the activation of H₂O, thereby underpinning the remarkable hydrogen production rates achieved during photo‐driven MSR. This study introduces a novel photothermal strategy for hydrogen generation from methanol, demonstrating the enormous potential of photothermal catalysis in the chemical and energy sectors.