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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
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-07-11 , DOI: 10.1021/acscatal.3c01527 Yuxue Yue 1, 2 , Saisai Wang 1 , Qi Zhou 1 , Bolin Wang 3 , Chunxiao Jin 1 , Renqin Chang 4 , Liqi Wan 1 , Zhiyan Pan 2 , Yihan Zhu 1, 4 , Jia Zhao 1 , Xiaonian Li 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-07-11 , DOI: 10.1021/acscatal.3c01527 Yuxue Yue 1, 2 , Saisai Wang 1 , Qi Zhou 1 , Bolin Wang 3 , Chunxiao Jin 1 , Renqin Chang 4 , Liqi Wan 1 , Zhiyan Pan 2 , Yihan Zhu 1, 4 , Jia Zhao 1 , Xiaonian Li 1
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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.
中文翻译：
通过碳热冲击法定制不对称 Cu-OP 偶联位点，在碳负载 Cu 催化剂上高效合成氯乙烯
尽管已经开发了多种方法来合成碳载纳米结构催化剂，但获得具有均匀尺寸和分散性的纳米颗粒或具有相同配位结构的单个原子仍然具有挑战性。通常，在乙炔氢氯化法合成氯乙烯（VCM）中，对纳米级碳载铜催化剂的最佳结构了解有限，极大地限制了其进一步的开发和应用。为了实现这一点，具有相同配位环境的 Cu 单原子 (Cu-O 3 P) 和 Cu/Cu 3通过先进的碳热激法制备了尺寸均匀的P纳米颗粒，并探讨了它们在乙炔氢氯化反应中的催化构效关系。具体而言，通过前驱体辅助碳热激法构建了纳米结构铜催化剂平台，并研究了铜位点的耦合结构和电子性质与其催化性能之间的关系。最后，我们得出了定量活性和稳定性描述符，解释了乙炔氢氯化中观察到的 d 轨道耦合和竞争吸附效应。这项工作为设计明确的碳负载金属纳米催化剂并调节其催化性能提供了一种精确且通用的方法。
更新日期：2023-07-11
中文翻译：
通过碳热冲击法定制不对称 Cu-OP 偶联位点，在碳负载 Cu 催化剂上高效合成氯乙烯
尽管已经开发了多种方法来合成碳载纳米结构催化剂，但获得具有均匀尺寸和分散性的纳米颗粒或具有相同配位结构的单个原子仍然具有挑战性。通常，在乙炔氢氯化法合成氯乙烯（VCM）中，对纳米级碳载铜催化剂的最佳结构了解有限，极大地限制了其进一步的开发和应用。为了实现这一点，具有相同配位环境的 Cu 单原子 (Cu-O 3 P) 和 Cu/Cu 3通过先进的碳热激法制备了尺寸均匀的P纳米颗粒，并探讨了它们在乙炔氢氯化反应中的催化构效关系。具体而言，通过前驱体辅助碳热激法构建了纳米结构铜催化剂平台，并研究了铜位点的耦合结构和电子性质与其催化性能之间的关系。最后，我们得出了定量活性和稳定性描述符，解释了乙炔氢氯化中观察到的 d 轨道耦合和竞争吸附效应。这项工作为设计明确的碳负载金属纳米催化剂并调节其催化性能提供了一种精确且通用的方法。
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