Tailoring the Surface Structure of Silicon Carbide Support for Copper Catalyzed Ethanol Dehydrogenation
Tailoring the Surface Structure of Silicon Carbide Support for Copper Catalyzed Ethanol Dehydrogenation
复制标题
铜催化乙醇脱氢碳化硅载体表面结构的定制
DOI：
10.1002/cctc.201801742
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发表时间：
2019-01-09
期刊：
影响因子：
4.5
通讯作者：
Lu, An-Hui
中科院分区：
文献类型：
--
作者：
Li, Meng-Yue;Lu, Wen-Duo;Lu, An-Hui
与化石原料相比，生物质乙醇脱氢生产乙醛是一种可持续的替代方案，铜基催化剂被认为是最有效的工艺。为此，我们对碳化硅进行了表面改性，使其界面性质由富SiO_2变为富C，并制备了一系列铜负载催化剂(Cu/SiO_2、Cu/SiO_2/SiC、Cu/C/SiC)，以考察界面结构和组成对乙醇催化脱氢的影响。在280℃时，由于富SiO_2界面促进了铜纳米粒子的良好分散性，使得催化剂表现出较高的乙醇转化率。相反，在相同的反应条件下，分散在C/SiC上的铜纳米颗粒表现出较低的活性，但具有很好的乙醛选择性和微量的副产物。这种差异归因于乙醛的快速去除，因为它对相对惰性的富C界面(C/SiC)的亲和力较低。这项工作为深入了解Cu-Si-C多界面结构和乙醇脱氢行为提供了理论依据，为设计具有可定制界面结构的新型催化剂提供了理论依据。
The production of acetaldehyde through biomass-derived ethanol dehydrogenation is a sustainable alternative compared to the fossil-feedstock based process, for which Cu-based catalysts are considered to be the most efficient. Herein, we modified the surface of silicon carbide (SiC) to alter the properties of the interface from SiO2-rich to C-rich, and we prepared a series of Cu-supported catalysts (Cu/SiC, Cu/SiO2/SiC, and Cu/C/SiC) with the aim of insight into the effect of the interface structure and composition on catalytic dehydrogenation of ethanol. At 280 degrees C, the Cu/SiO2/SiC catalyst exhibits high ethanol conversion due to the excellent dispersion of Cu nanoparticles promoted by SiO2-rich interface. In contrast, Cu nanoparticles dispersed on C/SiC shows somewhat lower activity but excellent acetaldehyde selectivity with trace amounts of by-products under identical reaction conditions. This difference is attributed to the fast removal of acetaldehyde because of its low affinity for the relatively inert C-rich interface (C/SiC). This work provides an in-depth understanding of Cu-Si-C multi-interfacial structure and the ethanol dehydrogenation behavior, which may shed light on the design of novel catalysts with tailored interfacial structures.