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通过铁基串联催化剂调整氧键合将一氧化碳转化为C醇

Transformation of CO to C alcohols by tailoring the oxygen bonding via Fe-based tandem catalyst.

作者信息

Wang Wenhang, Guo Xiangyu, Wang Yang, Lin Simin, Gao Xinhua, Liang Jie, Zhang Jinqiang, Xie Jinghao, Jiang Hu, Cao Fengliang, Chen Yongjie, Yang Guohui, Frauenheim Thomas, Wang Mingqing, Xing Tao, Lu Yiwu, Liu Qiang, Novoselov Kostya S, Tsubaki Noritatsu, Wu Mingbo

机构信息

State Key Laboratory of Heavy Oil Processing, College of New Energy, China University of Petroleum (East China), Qingdao, China.

Department of Applied Chemistry, Graduate School of Engineering, University of Toyama, Toyama, Japan.

出版信息

Nat Commun. 2025 Aug 6;16(1):7265. doi: 10.1038/s41467-025-62727-5.

DOI:10.1038/s41467-025-62727-5
PMID:40770265
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12328738/
Abstract

Direct conversion of CO into valuable organic products is probably the most important but challenging issue for global sustainability efforts. Metal carbides are promising as vital catalytic components in achieving this goal. Understanding the evolution of chemical orbitals and the corresponding energy levels on their interfaces are essential for targeted product synthesis. In this study, we discover that a highly active FeCo alloy carbide has a distinctive oxygen-bonding ability to regulate the evolution of oxygen-containing reaction intermediates. Combining with the copper/zinc/aluminum catalytic component, the designed tandem catalyst allows for the extremely high C alcohols selectivity (49.1 percent) and space-time yield (245.7 milligram per gram catalyst per hour) at a CO conversion of 51.1 percent. The excellent catalyst stability (>1000 hours) and potential economic viability make this process promising in eliminating carbon emissions at industrial application scale.

摘要

将一氧化碳直接转化为有价值的有机产品可能是全球可持续发展努力中最重要但也最具挑战性的问题。金属碳化物有望成为实现这一目标的关键催化成分。了解其界面上化学轨道的演化以及相应的能级对于有针对性的产品合成至关重要。在本研究中,我们发现一种高活性的铁钴合金碳化物具有独特的氧键合能力,可调节含氧化合物反应中间体的演化。与铜/锌/铝催化成分相结合,所设计的串联催化剂在一氧化碳转化率为51.1%时,可实现极高的C醇选择性(49.1%)和时空产率(每克催化剂每小时245.7毫克)。优异的催化剂稳定性(>1000小时)和潜在的经济可行性使该过程在工业应用规模上消除碳排放方面具有前景。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/4491cffe2be5/41467_2025_62727_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/eeb95c3bdeeb/41467_2025_62727_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/ad76fa71c501/41467_2025_62727_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/01a2e2da6961/41467_2025_62727_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/25c154a3f204/41467_2025_62727_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/426003063d58/41467_2025_62727_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/4491cffe2be5/41467_2025_62727_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/eeb95c3bdeeb/41467_2025_62727_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/ad76fa71c501/41467_2025_62727_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/01a2e2da6961/41467_2025_62727_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/25c154a3f204/41467_2025_62727_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/426003063d58/41467_2025_62727_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0407/12328738/4491cffe2be5/41467_2025_62727_Fig6_HTML.jpg

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