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Electrochemical reduction of acetonitrile to ethylamine
Nature Communications ( IF 14.7 ) Pub Date : 2021-03-29 , DOI: 10.1038/s41467-021-22291-0
Rong Xia , Dong Tian , Shyam Kattel , Bjorn Hasa , Haeun Shin , Xinbin Ma , Jingguang G. Chen , Feng Jiao

Electrifying chemical manufacturing using renewable energy is an attractive approach to reduce the dependence on fossil energy sources in chemical industries. Primary amines are important organic building blocks; however, the synthesis is often hindered by the poor selectivity because of the formation of secondary and tertiary amine byproducts. Herein, we report an electrocatalytic route to produce ethylamine selectively through an electroreduction of acetonitrile at ambient temperature and pressure. Among all the electrocatalysts, Cu nanoparticles exhibit the highest ethylamine Faradaic efficiency (~96%) at −0.29 V versus reversible hydrogen electrode. Under optimal conditions, we achieve an ethylamine partial current density of 846 mA cm−2. A 20-hour stable performance is demonstrated on Cu at 100 mA cm−2 with an 86% ethylamine Faradaic efficiency. Moreover, the reaction mechanism is investigated by computational study, which suggests the high ethylamine selectivity on Cu is due to the moderate binding affinity for the reaction intermediates.



中文翻译:

乙腈电化学还原成乙胺

使用可再生能源使化学制造电气化是减少化学工业对化石能源的依赖的一种有吸引力的方法。伯胺是重要的有机结构单元;然而,由于仲胺和叔胺副产物的形成,选择性通常很差,阻碍了合成。在本文中,我们报道了在环境温度和压力下通过乙腈的电还原选择性地产生乙胺的电催化途径。在所有电催化剂中,与可逆氢电极相比,Cu纳米粒子在-0.29 V时表现出最高的乙胺法拉第效率(〜96%)。在最佳条件下,我们实现了846 mA cm -2的乙胺分电流密度。在100 mA cm的铜上显示了20小时的稳定性能-2,具有86%的乙胺法拉第效率。此外,通过计算研究研究了反应机理,这表明对铜的高乙胺选择性是由于对反应中间体的中等结合亲和力。

更新日期:2021-03-29
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