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电化学碳-氮偶联的最新进展:金属催化剂策略与应用

Recent progress in electrochemical C-N coupling: metal catalyst strategies and applications.

作者信息

Xu Lekai, Yang Zhuojun, Zhang Chao, Chen Chen

机构信息

Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing 100084, China.

State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, School of Chemistry, Xinjiang University, Urumqi, Xin Jiang, 830017, China.

出版信息

Chem Commun (Camb). 2024 Sep 26;60(78):10822-10837. doi: 10.1039/d4cc03256j.

Abstract

Electrochemical C-N coupling reactions hold significant importance in the fields of organic chemistry and green chemistry. Conventional methods for constructing C-N bonds typically rely on high temperatures, high pressures, and other conditions that are energy-intensive and prone to generating environmental pollutants. In contrast, the electrochemical approaches employ electrical energy as the driving force to achieve C-N bond formation under ambient conditions, representing a more environment-friendly and sustainable alternative. The notable advantages of electrochemical C-N coupling include high efficiency, good selectivity, and mild reaction conditions. Through rational design of corresponding electrocatalysts, it is possible to achieve efficient C-N bond coupling at low potentials. Moreover, the electrochemical methods allow for precise control over reaction conditions, thereby avoiding side reactions and by-products that are common for conventional methods, improving both selectivity and product purity. Despite the extensive research efforts devoted to exploring the potential of electrochemical C-N coupling, the design of efficient and stable metal catalysts remains a significant challenge. In this review, we summarize and evaluate the latest strategies developed for designing metal catalysts, and their application prospects for different nitrogen sources such as N and NO. We delineate how the control over nanoscale structures, morphologies, and electronic properties of metal catalysts can optimize their performance in C-N coupling reactions, and discuss the performances and advantages of single-metal catalysts, bimetallic catalysts, and single-atom catalysts under various reaction conditions. By summarizing the latest research achievements, particularly in the development of high-efficiency catalysts, the application of novel catalyst materials, and the in-depth study of reaction mechanisms, this review aims to provide insights for future research in the field of electrochemical C-N coupling, and demonstrates that rationally designed metal catalysts could not only enhance the efficiency and selectivity of electrochemical C-N coupling reactions, but also offer conceptual frameworks for other electrochemical reactions.

摘要

电化学C-N偶联反应在有机化学和绿色化学领域具有重要意义。传统的构建C-N键的方法通常依赖于高温、高压以及其他能源密集型且易产生环境污染物的条件。相比之下,电化学方法利用电能作为驱动力,在环境条件下实现C-N键的形成,是一种更环保、更可持续的选择。电化学C-N偶联的显著优点包括高效率、良好的选择性和温和的反应条件。通过合理设计相应的电催化剂,可以在低电位下实现高效的C-N键偶联。此外,电化学方法能够精确控制反应条件,从而避免传统方法中常见的副反应和副产物,提高选择性和产物纯度。尽管人们为探索电化学C-N偶联的潜力付出了大量研究努力,但设计高效稳定的金属催化剂仍然是一项重大挑战。在这篇综述中,我们总结并评估了为设计金属催化剂而开发的最新策略,以及它们对不同氮源(如N₂和NO)的应用前景。我们阐述了如何控制金属催化剂的纳米级结构、形态和电子性质,以优化其在C-N偶联反应中的性能,并讨论了单金属催化剂、双金属催化剂和单原子催化剂在各种反应条件下的性能和优势。通过总结最新研究成果,特别是在高效催化剂的开发、新型催化剂材料的应用以及反应机理的深入研究方面,本综述旨在为电化学C-N偶联领域的未来研究提供见解,并表明合理设计的金属催化剂不仅可以提高电化学C-N偶联反应的效率和选择性,还能为其他电化学反应提供概念框架。

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