Wang Lingxiang, Guan Erjia, Wang Yeqing, Wang Liang, Gong Zhongmiao, Cui Yi, Meng Xiangju, Gates Bruce C, Xiao Feng-Shou
Key Lab of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, 310027, Hangzhou, China.
Key Laboratory of Applied Chemistry of Zhejiang Province, Department of Chemistry, Zhejiang University, 310028, Hangzhou, China.
Nat Commun. 2020 Feb 25;11(1):1033. doi: 10.1038/s41467-020-14817-9.
The reaction pathways on supported catalysts can be tuned by optimizing the catalyst structures, which helps the development of efficient catalysts. Such design is particularly desired for CO hydrogenation, which is characterized by complex pathways and multiple products. Here, we report an investigation of supported cobalt, which is known for its hydrocarbon production and ability to turn into a selective catalyst for methanol synthesis in CO hydrogenation which exhibits good activity and stability. The crucial technique is to use the silica, acting as a support and ligand, to modify the cobalt species via Co‒O‒SiO linkages, which favor the reactivity of spectroscopically identified *CHO intermediates, that more readily undergo hydrogenation to methanol than the C‒O dissociation associated with hydrocarbon formation. Cobalt catalysts in this class offer appealing opportunities for optimizing selectivity in CO hydrogenation and producing high-grade methanol. By identifying this function of silica, we provide support for rationally controlling these reaction pathways.
通过优化催化剂结构可以调控负载型催化剂上的反应路径，这有助于开发高效催化剂。对于具有复杂反应路径和多种产物的CO加氢反应而言，这种设计尤为必要。在此，我们报道了对负载型钴的研究，钴以其在CO加氢反应中生成烃类以及转化为甲醇合成选择性催化剂的能力而闻名，该催化剂表现出良好的活性和稳定性。关键技术是使用作为载体和配体的二氧化硅，通过Co‒O‒SiO键修饰钴物种，这有利于光谱鉴定的*CHO中间体的反应活性，该中间体比与烃类形成相关的C‒O解离更容易加氢生成甲醇。这类钴催化剂为优化CO加氢反应的选择性和生产高纯度甲醇提供了有吸引力的机会。通过确定二氧化硅的这一功能，我们为合理控制这些反应路径提供了支持。
