Wang Yang, Gao Weizhe, Wang Kangzhou, Gao Xinhua, Zhang Baizhang, Zhao Heng, Ma Qingxiang, Zhang Peipei, Yang Guohui, Wu Mingbo, Tsubaki Noritatsu
College of New Energy, State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China) Qingdao 266580 China
Department of Applied Chemistry, Graduate School of Engineering, University of Toyama Gofuku 3190 Toyama 930-8555 Japan
Chem Sci. 2021 Apr 26;12(22):7786-7792. doi: 10.1039/d1sc01859k.
Even though the transformation of syngas into aromatics has been realized a methanol-mediated tandem process, the low product yield is still the bottleneck, limiting the industrial application of this technology. Herein, a tailor-made zeolite capsule catalyst with Ga doping and SiO coating was combined with the methanol synthesis catalyst CrO to boost the synthesis of value-added aromatics, especially -xylene, from syngas. Multiple characterization studies, control experiments, and density functional theory (DFT) calculation results clarified that Ga doped zeolites with strong CO adsorption capability facilitated the transformation of the reaction intermediate methanol by optimizing the first C-C coupling step under a high-pressure CO atmosphere, thereby driving the reaction forward for aromatics synthesis. This work not only reveals the synergistic catalytic network in the tandem process but also sheds new light on principles for the rational design of a catalyst in terms of oriented conversion of syngas.
尽管通过甲醇介导的串联过程已实现合成气向芳烃的转化,但低产物收率仍是瓶颈,限制了该技术的工业应用。在此,将具有Ga掺杂和SiO涂层的定制沸石胶囊催化剂与甲醇合成催化剂CrO相结合,以促进从合成气中合成增值芳烃,尤其是对二甲苯。多项表征研究、对照实验和密度泛函理论(DFT)计算结果表明,具有强CO吸附能力的Ga掺杂沸石通过在高压CO气氛下优化首个C-C偶联步骤,促进了反应中间体甲醇的转化,从而推动反应朝着芳烃合成方向进行。这项工作不仅揭示了串联过程中的协同催化网络,还为合成气定向转化催化剂的合理设计原则提供了新的思路。