由一氧化碳和水直接合成超重烯烃。

Direct synthesis of extra-heavy olefins from carbon monoxide and water.

机构信息

Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, 230026, Hefei, Anhui, P. R. China.

School of Chemistry & Chemical Engineering, Anhui University of Technology, 243002, Ma'anshan, Anhui, P. R. China.

出版信息

Nat Commun. 2023 Apr 3;14(1):1857. doi: 10.1038/s41467-023-37599-2.

DOI:10.1038/s41467-023-37599-2

PMID:37012291

原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10070633/

Abstract

Extra-heavy olefins (C), feedstocks to synthesize a wide range of value-added products, are conventionally generated from fossil resources via energy-intensive wax cracking or multi-step processes. Fischer-Tropsch synthesis with sustainably obtained syngas as feed-in provides a potential way to produce C, though there is a trade-off between enhancing C-C coupling and suppressing further hydrogenation of olefins. Herein, we achieve selective production of C via the overall conversion of CO and water, denoted as Kölbel-Engelhardt synthesis (KES), in polyethylene glycol (PEG) over a mixture of Pt/MoN and Ru particles. KES provides a continuously high CO/H ratio, thermodynamically favoring chain propagation and olefin formation. PEG serves as a selective extraction agent to hinder hydrogenation of olefins. Under an optimal condition, the yield ratio of CO to hydrocarbons reaches the theoretical minimum, and the C yield reaches its maximum of 1.79 mmol with a selectivity (among hydrocarbons) of as high as 40.4%.

摘要

额外的重烯烃（C）是合成各种高附加值产品的原料，传统上是通过能源密集型蜡裂解或多步工艺从化石资源中获得的。使用可持续获得的合成气作为进料的费托合成提供了一种生产 C 的潜在方法，但在增强 C-C 偶联和抑制烯烃进一步加氢之间存在权衡。在此，我们通过在 Pt/MoN 和 Ru 颗粒的混合物上的聚乙二醇（PEG）中进行的 CO 和水的总转化，实现了 C 的选择性生产，称为 Kölbel-Engelhardt 合成（KES）。KES 提供了连续高的 CO/H 比，有利于链的增长和烯烃的形成。PEG 作为一种选择性萃取剂，阻止烯烃的加氢。在最佳条件下，CO 与碳氢化合物的产率比达到理论最小值，C 的产率达到 1.79mmol 的最大值，碳氢化合物的选择性（在碳氢化合物中）高达 40.4%。