Tailoring Asymmetric Cu-O-P Coupling Site by Carbothermal Shock Method for Efficient Vinyl Chloride Synthesis over Carbon Supported Cu Catalysts

ACS CATALYSIS(2023)

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摘要
It remains challenging to achieve nanoparticles withuniform sizeand dispersion or single atoms with identical coordination structure,although various methods have been developed to synthesize carbon-supportednanostructured catalysts. Typically, in the synthesis of vinyl chloride(VCM) by acetylene hydrochlorination, a limited understanding of theoptimal architecture for carbon-supported Cu catalysts at the nanoscalegreatly restrains their further development and application. To achievethis, Cu single-atom (Cu-O3P) with identical coordinationenvironments and Cu/Cu3P nanoparticles with uniform sizewere tailored via advanced carbothermal shock method, and their catalyticstructure-activity relationships were explored in the acetylenehydrochlorination reaction. In detail, a platform of nanostructuredcopper catalysts was constructed by the precursor-assisted carbothermalshock method, and the relationship between the coupling structureand electron properties of copper sites and their catalytic performanceis correlated. Finally, we derived quantitative activity and stabilitydescriptors that account for the d-orbital coupling and competitiveadsorption effects observed in acetylene hydrochlorination. This workprovides a precise and versatile approach for designing well-definedcarbon-supported metal nanocatalysts and regulating their catalyticperformance.
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关键词
copper catalysis,acetylene hydrochlorination,Cu-O-P coupling,carbothermal shock,d-orbitalsplitting,asymmetric coordination
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