首页|The photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu2(OH)2CO3 for stable photocatalytic CO2 reduction
The photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu2(OH)2CO3 for stable photocatalytic CO2 reduction
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Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO2 reduc-tion(PCO2R)systems.Herein,monoclinic Cu2(OH)2CO3 is firstly proven to be a new class of photocatalyst,which has excellent catalytic stability and selectivity for PCO2R in the absence of any sacrificial agent and cocatalysts.Based on a Cu2(OH)23CO3 photocatalyst and 13CO2 two-sided 13C isotopic tracer strategy,and combined with in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis and density functional theory(DFT)calculations,two main CO2 transformation routes,and the photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu2(OH)2CO3 are definitely revealed.The PCO2R activity of Cu2(OH)2CO3 is comparable to some of state-of-the-art novel photocata-lysts.Significantly,the PCO2R properties can be further greatly enhanced by simply combining Cu2(OH)2CO3 with typical TiO2 to construct composites photocatalyst.The highest CO and CH4 production rates by 7.5 wt％Cu2(OH)2CO3-TiO2 reach 16.4 μmol g-1h-1 and 116.0 μmol g-1h1,respectively,which are even higher than that of some of PCO2R systems containing sacrificial agents or precious metals mod-ified photocatalysts.This work provides a better understanding for the PCO2R mechanism at the atomic levels,and also indicates that basic carbonate photocatalysts have broad application potential in the future.
CO2 photocatalytic reductionPhotocatalysisBasic copper carbonateSelf-reconstructionPhotocatalyst
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