Optimizing water dissociation dehydrogenation process via Sn single atom incorporation for boosting photocatalytic CO2 methanation
Chem Catalysis(2023)
摘要
The conversion of CO2 into value-added methane (CH4) via light -driven processes represents a promising strategy for mitigating en-ergy scarcity and curtailing CO2 pollution. However, the intricate re-action kinetics of multiple electron-proton coupling processes remain a significant challenge. During the CO2 photoreduction pro-cess, the promotion of proton production from water dissociation for CH4 generation has been overlooked. Herein, Co3O4 is modified by Sn single atoms to realize selective CH4 production from CO2 photoreduction. The introducing of Sn induces generation of oxy-gen vacancy and adjacent low-valence Co (Co2+), which favors CO2 adsorption and activation by virtue of the reduced steric hindrance and enriched electrons at Co2+ sites. Specifically, Sn single atoms serve as H2O dissociation sites, accelerating the production of pro-tons and reducing the energy barrier of the rate-determining step. Our work endows a guideline for controlling CO2 photoreduction products' selectivity through the delicate design of active sites in catalysts and reaction kinetics optimization.
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关键词
photocatalytic co2 methanation,water dissociation dehydrogenation process,single atom incorporation
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