Jing Xu , Junfeng Lu , Yongjun Ji , Baofang Jin , Yongxia Zhu , Jianbo Geng , Yanlei Wang , Wenxing Chen , Ziyi Zhong , Guangwen Xu , Peng Wu , Fabing Su
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引用次数: 0
摘要
研究新型促进剂并理解其作用是一项重要而艰巨的任务。在本研究中,我们通过水热法直接合成 CuO,然后进行浸渍,在 CuO 表面晶格中引入了双主基团单原子 In 和 P 作为协同促进剂(In-P/CuO)。在重要的工业 Rochow-Müller 反应中,In-P/CuO 催化剂在二甲基二氯硅烷选择性和产率方面的催化性能优于原始 CuO 和含单一促进剂的 CuO。结合全面的实验表征和密度泛函理论计算发现,In 和 P 双促进剂之间的电子相互作用可以优化 CuO 的局部电子结构,促进 MeCl 在 CuO 表面解离,加速 CuO 向 Cu2O、CuCl 以及最终活性相 Cu3Si 的转化,从而提高整体活性。这项研究探讨了催化剂中双主基团单原子促进剂之间的协同作用,为设计高效催化剂提供了一种行之有效的方法。
The dual single-atom In and P co-promoters boost dimethyldichlorosilane production in the Rochow-Müller reaction
Investigating novel promoters and comprehending their roles is an important yet difficult task. In this study, we have introduced dual main-group single-atom In and P as co-promoters into the CuO surface lattice (In-P/CuO) via a straightforward hydrothermal CuO synthesis followed by impregnation. The In-P/CuO catalyst showed superior catalytic performance in dimethyldichlorosilane selectivity and yield to that of the pristine CuO and CuO with a single promoter in the important industrial Rochow-Müller reaction. The combination of thorough experimental characterization and density functional theory calculations reveals that the electron interaction between dual In and P promoters could optimize the local electronic structure of CuO and facilitate MeCl dissociation on the CuO surface, accelerating the transformation of CuO to Cu2O, then CuCl, and eventually the active phase Cu3Si and thereby enhancing overall activity. This work examines the synergistic interactions between dual main-group single-atom promoters in catalysts, offering a proven method for designing highly efficient catalysts.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.