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在强酸性介质中,以800 mA/cm²的电流密度将稀释的CO电还原为具有高碳利用率的多碳产物。

Electroreduction of diluted CO to multicarbon products with high carbon utilization at 800 mA cm in strongly acidic media.

作者信息

Qin Xue-Rong, Li Jing-Jing, Wang Lin-Lin, Liu Huan, Yang Zuo-Tao, Feng Guo-Jin, Wang Xiao-Ran, Cheng Xuan-Xuan, Zhang Chao, Yu Zi-You, Lu Tong-Bu

机构信息

MOE International Joint Laboratory of Materials Microstructure, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science & Engineering, Tianjin University of Technology, Tianjin, China.

出版信息

Nat Commun. 2025 May 13;16(1):4447. doi: 10.1038/s41467-025-59783-2.

DOI:10.1038/s41467-025-59783-2
PMID:40360538
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12075586/
Abstract

Acidic CO electroreduction using diluted CO (as in flue gas) as the feedstock can simultaneously circumvent the CO purification step and lower the carbon loss in conventional alkaline or neutral electrolyte, and thus is highly desired but has rarely been achieved thus far. Herein, we report a simple and general strategy using an imidazolium-based anion-exchange ionomer as the coating layer, which could enrich the diluted CO to generate a high local CO concentration, and simultaneously block the proton transport to the cathode surface to suppress the competing hydrogen evolution reaction. As a result, the ionomer-modified Cu catalyst can achieve an efficient electroreduction of diluted CO (15 vol% CO) to multicarbon (C) products in strong acid (pH 0.8), with a high C Faradaic efficiency of 70.5% and a high single-pass carbon efficiency of 73.6% at a current density of 800 mA cm, competitive with that obtained with pure CO. These findings provide opportunity for the direct electrochemical conversion of flue gas into valuable products with high efficiency.

摘要

使用稀释的一氧化碳(如烟道气中的一氧化碳)作为原料进行酸性一氧化碳电还原,可同时规避一氧化碳纯化步骤,并降低传统碱性或中性电解质中的碳损失,因此备受期待,但迄今为止很少实现。在此,我们报告了一种简单通用的策略,即使用基于咪唑鎓的阴离子交换离聚物作为涂层,该涂层可富集稀释的一氧化碳以产生高局部一氧化碳浓度,同时阻断质子向阴极表面的传输,从而抑制竞争性析氢反应。结果,离聚物修饰的铜催化剂能够在强酸(pH 0.8)中将稀释的一氧化碳(15体积%一氧化碳)高效电还原为多碳产物,在电流密度为800 mA/cm²时,具有70.5%的高碳法拉第效率和73.6%的高单程碳效率,与使用纯一氧化碳时的效率相当。这些发现为将烟道气直接高效电化学转化为有价值的产品提供了机会。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/78c1/12075586/b3a2a9ed860d/41467_2025_59783_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/78c1/12075586/12245285b0a4/41467_2025_59783_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/78c1/12075586/7d9b07d1b1d9/41467_2025_59783_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/78c1/12075586/78ddadb5a096/41467_2025_59783_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/78c1/12075586/6539b8b01c20/41467_2025_59783_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/78c1/12075586/b3a2a9ed860d/41467_2025_59783_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/78c1/12075586/12245285b0a4/41467_2025_59783_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/78c1/12075586/7d9b07d1b1d9/41467_2025_59783_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/78c1/12075586/78ddadb5a096/41467_2025_59783_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/78c1/12075586/6539b8b01c20/41467_2025_59783_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/78c1/12075586/b3a2a9ed860d/41467_2025_59783_Fig5_HTML.jpg

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本文引用的文献

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CO electrolysis to multi-carbon products in strong acid at ampere-current levels on La-Cu spheres with channels.在具有通道的镧 - 铜球体上,于强酸性环境中在安培电流水平下将一氧化碳电解为多碳产物。
Nat Commun. 2024 Jun 6;15(1):4821. doi: 10.1038/s41467-024-49308-8.
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Efficient Capture and Electroreduction of Dilute CO into Highly Pure and Concentrated Formic Acid Aqueous Solution.将稀一氧化碳高效捕获并电还原为高纯度浓缩甲酸水溶液
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Addressing the Carbonate Issue: Electrocatalysts for Acidic CO Reduction Reaction.
解决碳酸盐问题:用于酸性CO还原反应的电催化剂。
Adv Mater. 2025 Jan;37(2):e2312894. doi: 10.1002/adma.202312894. Epub 2024 May 17.
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Local CO reservoir layer promotes rapid and selective electrochemical CO reduction.局部一氧化碳储存层促进快速且选择性的电化学一氧化碳还原。
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Reaction Environment Regulation for Electrocatalytic CO Reduction in Acids.酸性环境中电催化CO还原的反应环境调控
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Efficient multicarbon formation in acidic CO reduction via tandem electrocatalysis.通过串联电催化在酸性CO还原中高效形成多碳产物
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