The electrochemical C‐N coupling process, facilitating the production of organic nitrogen substances (such as urea, methylamine, formamide, and ethylamine) via the simultaneous reduction of carbon dioxide (CO2) and small nitrogen‐based substances, stands at the forefront of advancing carbon neutrality and the artificial nitrogen cycle. This method has garnered substantial interest due to its potential economic and environmental benefits. Although considerable progress has been achieved in this emerging field, it still faces challenges, including slow reactant adsorption, competing side reactions, and complex multi‐step pathways, resulting in low yields and selectivity. Strategically designing and developing low‐cost and exceptionally performant catalysts is crucial for cost‐effective and precise electrochemical C─N bonding. This article offers an in‐depth review of the electrosynthesis of valuable organic nitrogen compounds at ambient conditions from earth‐abundant resources/wastes, such as CO2 and small nitrogenous molecules (nitrogen: N2, nitrite: NO2−, nitrate: NO3−, ammonia: NH3, etc.), via electrochemical C─N bond formation reactions, especially using carbon‐based catalysts. The relevant electrochemical C─N bond formation mechanisms, the design principles of advanced carbon‐based electrocatalysts, and the impact of different electrolyser designs are discussed, along with the present obstacles and upcoming prospects in this dynamic field.

中文翻译：

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合理设计的碳基电化学C-N偶联催化剂

电化学C-N偶联过程，通过同时还原二氧化碳（CO2）和小型氮基物质，站在推进碳中和和人工氮循环的最前沿。这种方法由于其潜在的经济和环境效益而引起了人们的广泛兴趣。尽管这一新兴领域已经取得了相当大的进展，但它仍然面临着挑战，包括缓慢的反应物吸附、竞争性副反应和复杂的多步骤途径，导致产率和选择性较低。战略性地设计和开发低成本且性能优异的催化剂对于经济高效且精确的电化学 C─N 键合至关重要。本文深入回顾了在环境条件下从地球丰富的资源/废物（例如二氧化碳）电合成有价值的有机氮化合物2和小氮分子（氮：N2、亚硝酸盐：NO2-，硝酸盐：NO3-，氨：NH3等），通过电化学C─N键形成反应，特别是使用碳基催化剂。讨论了相关的电化学C─N键形成机制、先进碳基电催化剂的设计原理、不同电解槽设计的影响，以及该动态领域目前的障碍和未来的前景。