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

Journal 2023 · IF 12.9 · 发表于 2023 年 7 月 11 日
作者: Yuxue Yue,Saisai Wang,Qi Zhou,Bolin Wang,Chunxiao Jin,Renqin Chang,Liqi Wan,Zhiyan Pan,Yihan Zhu,Jia Zhao,Xiaonian Li
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摘要

It remains challenging to achieve nanoparticles with uniform size and dispersion or single atoms with identical coordination structure, although various methods have been developed to synthesize carbon-supported nanostructured catalysts. Typically, in the synthesis of vinyl chloride (VCM) by acetylene hydrochlorination, a limited understanding of the optimal architecture for carbon-supported Cu catalysts at the nanoscale greatly restrains their further development and application. To achieve this, Cu single-atom (Cu-O3P) with identical coordination environments and Cu/Cu3P nanoparticles with uniform size were tailored via advanced carbothermal shock method, and their catalytic structure–activity relationships were explored in the acetylene hydrochlorination reaction. In detail, a platform of nanostructured copper catalysts was constructed by the precursor-assisted carbothermal shock method, and the relationship between the coupling structure and electron properties of copper sites and their catalytic performance is correlated. Finally, we derived quantitative activity and stability descriptors that account for the d-orbital coupling and competitive adsorption effects observed in acetylene hydrochlorination. This work provides a precise and versatile approach for designing well-defined carbon-supported metal nanocatalysts and regulating their catalytic performance.

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