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

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.