甲酰胺
电化学
法拉第效率
胺气处理
联轴节(管道)
材料科学
组合化学
化学
有机化学
物理化学
冶金
电极
作者
Yun Fan,Tianyang Liu,Yunhui Yan,Zhongcheng Xia,Yuxuan Lu,Yuping Pan,Ruiqi Wang,Dianke Xie,Zhonghuan Zhu,Ta Thi Thuy Nga,Chung‐Li Dong,Yu Jing,Yafei Li,Shuangyin Wang,Yuqin Zou
出处
期刊:Chem
[Elsevier]
日期:2024-04-01
被引量:2
标识
DOI:10.1016/j.chempr.2024.03.024
摘要
N,N-Dimethylformamide (DMF) is a versatile chemical and universal solvent that is commonly synthesized from carbon monoxide and dimethylamine (DMA) under high temperature and pressure. However, this process leads to a large amount of carbon emissions. Herein, we propose an electrochemical strategy to directly convert carbon dioxide (CO2) and DMA to DMF under ambient conditions. Loading palladium (Pd) onto copper (Cu) nanosheet catalysts with Cu vacancies (Pd/Cu-VCu) enabled the efficient synthesis of DMF, and the maximum yield and faradaic efficiency reached 385 mmol·h−1·gcat. −1 and 37.5%, respectively. In situ spectroscopy and density functional theory calculations indicated that Cu vacancies (Cu-VCu) promoted the adsorption of CO2 on the catalyst surface, followed by its spontaneous coupling with DMA to form the C–N bond. Pd nanoparticles accelerated the electrochemical reduction of the intermediate ∗OCN(CH3)2OH to ∗OCHN(CH3)2OH, leading to highly efficient DMF electrosynthesis. This work paves the way for the synthesis of sustainable high-value organic nitrogen compounds from CO2.
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