Dual-engine-driven realizing high-yield synthesis of Para-Xylene directly from CO2-containing syngas

作者：Xuemei Wu, Chengwei Wang, Shengying Zhao, Yang Wang, Tao Zhang, Jie Yao, Weizhe Gao, Baizhang Zhang, Taiki Arakawa, Yingluo He, Fei Chen, Minghui Tan, Guohui Yang, Noritatsu Tsubaki · 发表于：Nature Communications · 年份：2024 · DOI：10.1038/s41467-024-52482-4 · 被引用次数：28 · 研究领域：Catalytic Processes in Materials Science、Catalysts for Methane Reforming、Catalysis and Oxidation Reactions

The direct synthesis of light aromatics, especially para-xylene (p-X), from syngas/CO2 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@SiO2 capsule zeolite. The DED catalyst of 1.0%FeMn&[ZnCr&Z5@SiO2] shows an extremely higher p-X STY of 36.1 gp-x·kgcat-1·h-1, 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@SiO2. The DED model boosts the driving force for syngas/CO2 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. The direct synthesis of light aromatics, particularly para-xylene (p-X), from syngas/CO2 is gaining considerable attention, though enhancing the space-time yield (STY) of p-X remains a significant challenge. Here, the authors develop a dynamic ‘dual-engine-driven’ catalytic system that achieves a remarkably higher p-X STY by integrating ZnCr and FeMn with Z5@SiO2 capsule zeolite.