Abstract
The conversion of CO2 into solar fuels via photo-driven catalytic reduction presents a promising avenue toward achieving carbon neutrality. Herein, copper-based catalysts are prepared and explored for photo-driven photothermal CO2 reduction reaction. The optimized catalyst exhibits a consistent CO production rate of 165.9 mmol g−1 h−1 and 100% CO selectivity at ambient pressure. We unveil the intricate adsorption dynamics at play: H2 molecules predominantly interact with and activate at Cu sites, while CO2 molecules preferentially adsorb and activate at interfacial sites within the composites. Furthermore, we elucidate how the positive shift of the d-band center (εd) for Cu 3d orbitals significantly enhances H2 adsorption and activation. Crucially, the subsequent dissociation of H2 molecules at Cu sites drives the efficient conversion of adsorbed CO2 molecules at interfacial sites into CO. Overall, our findings not only advance the theoretical understanding but also offer practical insights for realizing photothermal catalytic CO2 reduction reactions.
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