Electrochemical coupling of carbon monoxide and amine on iodide coordination stabilized Cuδ+ site

Yun Fan, Yunhui Yan, Qizheng An, Zhongcheng Xia, Yuping Pan, Yuxuan Lu, Zhonghuan Zhu, Ruiqi Wang, Qinghua Liu, Yuqin Zou (), Yongjun Li () and Shuangyin Wang ()
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Yun Fan: Hunan University
Yunhui Yan: Hunan University
Qizheng An: University of Science and Technology of China
Zhongcheng Xia: Hunan University
Yuping Pan: Hunan University
Yuxuan Lu: Hunan University
Zhonghuan Zhu: Hunan University
Ruiqi Wang: Hunan University
Qinghua Liu: University of Science and Technology of China
Yuqin Zou: Hunan University
Yongjun Li: Hunan University
Shuangyin Wang: Hunan University

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract The use of renewable electricity to drive the electrocatalytic coupling of CO with nitrogen-containing organics offers a promising strategy for producing high-value chemicals. In this work, we conduct a systematic investigation of the coordination effect between iodide and copper oxide to generate Cuδ+ active sites. These Cuδ+ sites enable the electrosynthesis of dimethylacetamide from CO and dimethylamine. Through precise regulation of the electrode surface microenvironment, a dimethylacetamide Faradaic efficiency of 45.6% is achieved at a partial current density of 182.4 mA·cm-2, with a production rate of 435.9 mmol·gcat.−1·h-1 and selectivity approaching 70%. Mechanistic studies reveal that specific adsorption of I- forms an iodide-enriched Cu0/Cu+ interface that synergistically promotes dimethylacetamide formation by enhancing adsorption of ketene intermediates (*CCO) and facilitating C–N bonds formation. This anion-coordination interfacial engineering strategy demonstrates broad applicability for synthesizing various acetamide derivatives from CO2/CO and amine, providing a foundational framework for electrocatalytic C-N coupling in acetamide synthesis.

Date: 2025
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DOI: 10.1038/s41467-025-62291-y

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