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Synergistic Visible-Light-Driven CO2 Reduction and H2O Oxidation over Ti3C2 Quantum Dot-Modified Cu/g-C3N4
Xiangyin Ji1,2, Jinqi Chen1, Mingyuan Li3
1School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China.
Abstract:
Photocatalytic CO2 reduction into value-added fuels using water as the electron donor represents a sustainable route for artificial photosynthesis, yet it is often hindered by rapid charge recombination and insufficient thermodynamic driving force. Herein, we report a ternary heterojunction photocatalyst composed of zero-dimensional Ti3C2 quantum dots (QDs) and metallic Cu comodified on two-dimensional g-C3N4 (denoted as CCNT). The Cu nanoparticles broaden the visible-light absorption and negatively shift the conduction band of g-C3N4, providing a strong driving force for CO2 reduction. Meanwhile, the highly conductive Ti3C2 QDs act as efficient electron reservoirs, rapidly extracting photogenerated electrons from Cu/g-C3N4 and redistribute photogenerated electrons. This prevents charge accumulation at Cu sites, stabilizes the reduction centers, and maintains electron-hole balance. The optimized CCNT-5 composite achieves CO and CH4 production rates of 24.59 and 20.24 μmol g-1 h-1 under visible light, resulting an electron selectivity toward CO2 reduction as high as 94.90%. Moreover, the catalyst enables simultaneous water oxidation with a nearly 1:1 electron-to-hole consumption ratio and excellent long-term stability. This work demonstrates a rational 0D/metal/two-dimensional (2D) architecture for efficient and stable solar-driven CO2 reduction.
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