双引擎驱动实现直接从含二氧化碳合成气中高产合成对二甲苯

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Nature Communications Pub Date : 2024-09-14 DOI:10.1038/s41467-024-52482-4
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
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引用次数: 0

摘要

从合成气/二氧化碳中直接合成轻芳烃,特别是对二甲苯(p-X)的技术正在引起人们的强烈兴趣,但提高对二甲苯的时空产率(STY)是一项重大挑战。本文设计了一种动态 "双引擎驱动"(DED)催化系统,将 ZnCr 和 FeMn 两种伙伴(命名为 "双引擎")与 Z5@SiO2 胶囊沸石相结合。1.0%FeMn&[ZnCr&Z5@SiO2] 的 DED 催化剂显示出极高的 p-X STY,达到 36.1 gp-x-kgcat-1-h-1,是 [ZnCr&Z5] 催化剂的八倍。DED 操纵 ZnCr 引擎生成甲醇,同时驱动 FeMn 引擎生成轻烯烃,然后形成的甲醇和轻烯烃在 Z5@SiO2 上原位协同转化为富含 p-X 的芳烃。DED 模型增强了合成气/CO2 转化的驱动力,同时协调了 p-X 生成的 "双引擎 "合作,从而实现了极高的 p-X STY。这项研究实现了工业相关水平的非石油 p-X 生产,并推动了创新型异质催化剂设计知识的发展。
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Dual-engine-driven realizing high-yield synthesis of Para-Xylene directly from CO2-containing syngas

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.

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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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