Zhang Peipei, Tan Li, Yang Guohui, Tsubaki Noritatsu
Department of Applied Chemistry , School of Engineering , University of Toyama , Gofuku 3190 , Toyama 930-8555 , Japan . Email:
Chem Sci. 2017 Dec 1;8(12):7941-7946. doi: 10.1039/c7sc03427j. Epub 2017 Oct 16.
The finite petroleum resources and environmental crisis compel the development of non-petroleum carbon resources by chemical transformation routes. Syngas (CO + H) is a crucial junction point that exclusively bridges the non-petroleum carbon resources and other basic chemicals like alcohols, alkane/alkenes, However, the one-pass conversion of syngas to value-added aromatics, especially -xylene, is still a big challenge. Here we presented a promising hybrid catalyst, named Cr/Zn-Zn/Z5@S1, to effectively realize the one-pass conversion of syngas to -xylene. This hybrid catalyst exhibited enhanced activity on syngas conversion (CO conversion of 55.0%), good stability of catalyst lifetime and considerable selectivity of -xylene (27.6% in the total products and 77.3% in xylene). The characterization and catalytic performance evaluation revealed that the well-designed core-shell Zn/Z5@S1 zeolite, as a vital part of this Cr/Zn-Zn/Z5@S1 hybrid catalyst, substantially contributed to its extreme performance for the -xylene one-pass precise synthesis from syngas. The concerted combination of two components in this hybrid catalyst can effectively depress the formation of unwanted by-products and facilitate the oriented synthesis of -xylene from syngas with unprecedented efficiency at the same time.
有限的石油资源和环境危机促使通过化学转化途径开发非石油碳资源。合成气（CO + H）是一个关键的交汇点，它唯一地连接了非石油碳资源和其他基础化学品，如醇类、烷烃/烯烃。然而，将合成气一步转化为增值芳烃，尤其是对二甲苯，仍然是一个巨大的挑战。在此，我们提出了一种有前景的混合催化剂，名为Cr/Zn-Zn/Z5@S1，以有效实现合成气一步转化为对二甲苯。这种混合催化剂在合成气转化方面表现出增强的活性（CO转化率为55.0%），具有良好的催化剂寿命稳定性以及对二甲苯可观的选择性（在总产物中为27.6%，在二甲苯中为77.3%）。表征和催化性能评估表明，精心设计的核壳结构Zn/Z5@S1沸石作为这种Cr/Zn-Zn/Z5@S1混合催化剂的重要组成部分，对其从合成气一步精确合成对二甲苯的卓越性能有很大贡献。这种混合催化剂中两种组分的协同组合可以有效抑制不需要的副产物的形成，同时以前所未有的效率促进从合成气定向合成对二甲苯。
