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在电催化还原二氧化碳过程中通过C-N偶联获得有机氮化合物的进展
作者:小柯机器人 发布时间:2021/11/20 22:13:46

美国耶鲁大学Hailiang Wang小组总结在电催化还原二氧化碳过程中通过C-N偶联获得有机氮化合物的进展。2021年11月17日,国际知名学术期刊《美国化学会杂志》在线发表了这一成果。

研究人员表示,鉴于电催化CO2还原反应仅以CO2和H2O为反应物的产物种类有限,人们希望通过引入提供元素多样性的额外反应物来扩大产物范围。原则上,将含无机杂原子的反应物整合到电催化二氧化碳还原反应中,可以实现有价值产物的可持续合成,如有机氮化合物,这些产品具有广泛的应用,但通常依赖于从能源密集型和依赖化石燃料的哈伯-波斯工艺中提取的NH3进行工业规模生产。
 
研究人员强调了在N-整合电催化二氧化碳还原中建立C-N键的研究进展,并从反应性、催化剂结构和最基本的机制的角度研究了尿素、乙酰胺和胺的电合成。研究人员对这些进展中C-N耦合的机理讨论进行了强调和批判性评价,目的是指导未来的研究,以提高产物产量和扩大N-整合电催化CO2还原的产物范围。
 
附:英文原文

Title: Accessing Organonitrogen Compounds via C–N Coupling in Electrocatalytic CO2 Reduction

Author: Zixu Tao, Conor L. Rooney, Yongye Liang, Hailiang Wang

Issue&Volume: November 17, 2021

Abstract: Given the limited product variety of electrocatalytic CO2 reduction reactions solely from CO2 and H2O as the reactants, it is desirable to expand the product scope by introducing additional reactants that provide elemental diversity. The integration of inorganic heteroatom-containing reactants into electrocatalytic CO2 reduction could, in principle, enable the sustainable synthesis of valuable products, such as organonitrogen compounds, which have widespread applications but typically rely on NH3 derived from the energy-intensive and fossil-fuel-dependent Haber–Bosch process for their industrial-scale production. In this Perspective, research progress toward building C–N bonds in N-integrated electrocatalytic CO2 reduction is highlighted, and the electrosyntheses of urea, acetamides, and amines are examined from the standpoints of reactivity, catalyst structure, and, most fundamentally, mechanism. Mechanistic discussions of C–N coupling in these advances are emphasized and critically evaluated, with the aim of directing future investigations on improving the product yield and broadening the product scope of N-integrated electrocatalytic CO2 reduction.

DOI: 10.1021/jacs.1c10714

Source: https://pubs.acs.org/doi/10.1021/jacs.1c10714

 

期刊信息

JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:14.612
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000