Affiliation: | 1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190 China;2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049 China
Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001 China
National Energy Center for Coal to Clean Fuels, Synfuels China Co., Ltd, Huairou District, Beijing, 101400 China
College of Chemistry and Environmental Science, Inner Mongolia Key Laboratory of Green Catalysis, Inner Mongolia Normal University, Hohhot, 010022 China;3. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190 China
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049 China;4. School of Chemical Sciences, The University of Auckland, Auckland, 1142 New Zealand;5. Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001 China
National Energy Center for Coal to Clean Fuels, Synfuels China Co., Ltd, Huairou District, Beijing, 101400 China |
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 gcat−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. |