Wu Xuemei, Wang Chengwei, Zhao Shengying, Wang Yang, Zhang Tao, Yao Jie, Gao Weizhe, Zhang Baizhang, Arakawa Taiki, He Yingluo, Chen Fei, Tan Minghui, Yang Guohui, Tsubaki Noritatsu
Department of Applied Chemistry, School of Engineering, University of Toyama, Gofuku 3190, Toyama, Japan.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, China.
Nat Commun. 2024 Sep 14;15(1):8064. doi: 10.1038/s41467-024-52482-4.
The direct synthesis of light aromatics, especially para-xylene (p-X), from syngas/CO is drawing strong interest, but improving the space-time yield (STY) of p-X is a significant challenge. Here, a dynamic "dual-engine-driven" (DED) catalytic system is designed by combining two partners of ZnCr and FeMn (named "dual-engine") with Z5@SiO capsule zeolite. The DED catalyst of 1.0%FeMn&[ZnCr&Z5@SiO] shows an extremely higher p-X STY of 36.1 g·k·h, about eight times higher than that of [ZnCr&Z5]. DED manipulates ZnCr engine for methanol formation and drives FeMn engine for light olefins generation together, and then the formed methanol and light olefins are coordinately converted in situ into p-X-rich aromatics over Z5@SiO. The DED model boosts the driving force for syngas/CO conversion, simultaneously concerting the cooperation of "dual-engine" for p-X generation, resulting in extremely high STY of p-X. This study achieves non-petroleum p-X production at industrial-relevant level and advances knowledge in designing innovative heterogeneous catalysts.
由合成气/一氧化碳直接合成轻质芳烃,尤其是对二甲苯(p-X),正引起人们浓厚的兴趣,但提高对二甲苯的时空产率(STY)是一项重大挑战。在此,通过将ZnCr和FeMn这两个伙伴(称为“双引擎”)与Z5@SiO胶囊沸石相结合,设计了一种动态的“双引擎驱动”(DED)催化体系。1.0%FeMn&[ZnCr&Z5@SiO]的DED催化剂显示出极高的对二甲苯时空产率,为36.1 g·k·h,约为[ZnCr&Z5]的八倍。DED操纵ZnCr引擎用于甲醇生成,并共同驱动FeMn引擎用于轻质烯烃生成,然后生成的甲醇和轻质烯烃在Z5@SiO上原位协同转化为富含对二甲苯的芳烃。DED模型增强了合成气/一氧化碳转化的驱动力,同时协调了“双引擎”生成对二甲苯的协同作用,从而实现了极高的对二甲苯时空产率。本研究实现了工业相关水平的非石油对二甲苯生产,并推进了创新多相催化剂设计方面的知识。