Yang Zhibin, Kang Ting, Ji Yongjun, Li Jing, Zhu Yongxia, Liu Hezhi, Jiang Xingyu, Zhong Ziyi, Su Fabing
School of Metallurgy and Materials Engineering, Jiangsu University of Science and Technology, Zhangjiagang, Changxinzhong Road 8, Zhangjiagang 215600, China.
School of Metallurgy and Materials Engineering, Jiangsu University of Science and Technology, Zhangjiagang, Changxinzhong Road 8, Zhangjiagang 215600, China; State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.
J Colloid Interface Sci. 2021 May;589:198-207. doi: 10.1016/j.jcis.2020.12.069. Epub 2020 Dec 24.
As compared with conventional nanocrystal systems, Cu-based mesocrystals have demonstrated distinct advantages in catalytic applications. Here, we report the preparation of a novel architectural CuO@CuO catalyst system integrated with the core/shell and mesocrystal structures (CuO@CuO MC) via a facile solvothermal process followed by calcination. The formation mechanism of the CuO@CuO MC with hexapod morphology was deciphered based on a series of time-dependent experiments and characterizations. When applied as a Cu-based catalyst to produce trichlorosilane (TCS) via Si hydrochlorination reaction, the CuO@CuO MC exhibited a much higher Si conversion, TCS selectivity, and stability than the catalyst-free industrial process and the CuO@CuO catalyst with a core-shell nanostructure. The enhanced catalytic efficiency of the former is attributed to the collective effects from its quite rough surface for providing abundant adsorption sites, the ordered nanoparticle arrangement in the core and shell for generating strong synergistic effects, and the micrometer size for the improved structural stability. This work demonstrates a practical route for designing sophisticated architectural structures that combine several structural functions within one catalyst system and their catalysis applications.
与传统纳米晶体系统相比，铜基金属中晶在催化应用中展现出显著优势。在此，我们报道了一种通过简便的溶剂热法随后煅烧制备的新型结构的CuO@CuO催化剂体系，该体系兼具核壳结构和中晶结构（CuO@CuO MC）。基于一系列随时间变化的实验和表征，解析了具有六足形态的CuO@CuO MC的形成机理。当用作铜基催化剂通过硅氢氯化反应生产三氯硅烷（TCS）时，CuO@CuO MC表现出比无催化剂的工业过程以及具有核壳纳米结构的CuO@CuO催化剂更高的硅转化率、TCS选择性和稳定性。前者催化效率的提高归因于其非常粗糙的表面提供丰富吸附位点的集体效应、核壳中有序的纳米颗粒排列产生的强协同效应以及微米尺寸带来的结构稳定性提升。这项工作展示了一条设计复杂结构的实用途径，该结构在一个催化剂体系中结合了多种结构功能及其催化应用。
