电催化NO与碳氧化物共还原合成尿素的理论研究进展

Advances in Theoretical Research on Synthesis of Urea by Electrocatalytic Co-Reduction of Nitric Oxide and Carbon Oxides

摘要: 电化学方法由于能在温和条件下进行、低耗、清洁，成为解决人类所面临的能源和环境问题的有效手段之一。一氧化氮(NO)造成了严重的环境问题，碳氧化合物(如CO₂和CO)是主要的空气污染物，科学家一直致力于研究有效的方法减少或转化这些有毒害的氧化物。在环境条件下，通过一氧化氮和碳氧化合物的电化学共还原合成尿素可以实现碳/氮中和、减轻环境污染，是一种环境友好策略，具有广阔应用前景。近期虽然越来越多的研究在电化学尿素合成方面取得了一些突破，但存在法拉第效率低、尿素产率不高、C-N耦联反应机理不清楚等问题，这些问题制约其大规模应用。本文从实验化学和理论计算化学领域，综述了环境条件下基于NO和碳氧化合物电化学尿素合成的最新进展，并从理论化学层面揭示C-N耦联反应机理，为之后该反应提供实验与理论的指导与支撑。

Abstract: Electrochemical methods have become one of the effective means of solving the energy and envi-ronmental problems facing mankind due to their ability to be carried out under mild conditions, low consumption and cleanliness. Nitric oxide (NO) causes serious environmental problems, and carbon oxides (e.g., CO₂ and CO) are major air pollutants, and scientists have been working on effec-tive methods to reduce or convert these toxic oxides. The synthesis of urea by electrochemical co-reduction of nitric oxide and carbon oxides under ambient conditions can achieve Car-bon/Nitrogen neutralisation and reduce environmental pollution, which is an environmentally friendly strategy with broad application prospects. Recently, although more and more researches have made some breakthroughs in electrochemical urea synthesis, there are problems such as low Faraday efficiency, low urea yield, and unclear mechanism of C-N coupling reaction, which restrict its large-scale application. In this paper, we review the recent progress of electrochemical urea synthesis based on NO and carbon-oxygen compounds under ambient conditions from the fields of experimental chemistry and theoretical computational chemistry, and reveal the mechanism of the C-N coupling reaction from the level of theoretical chemistry, so as to provide experimental and theoretical guidance and support for this reaction afterwards.