Electrocatalytic synthesis of C–N coupling compounds from CO₂ and nitrogenous species

Abstract

The electrocatalytic synthesis of C–N coupling compounds from CO2 and nitrogenous species not only offers an effective avenue to achieve carbon neutrality and reduce environmental pollution, but also establishes a route to synthesize valuable chemicals, such as urea, amide, and amine. This innovative approach expands the application range and product categories beyond simple carbonaceous species in electrocatalytic CO2 reduction, which is becoming a rapidly advancing field. This review summarizes the research progress in electrocatalytic urea synthesis, using N2, NO2−, and NO3− as nitrogenous species, and explores emerging trends in the electrosynthesis of amide and amine from CO2 and nitrogen species. Additionally, the future opportunities in this field are highlighted, including electrosynthesis of amino acids and other compounds containing C–N bonds, anodic C–N coupling reactions beyond water oxidation, and the catalytic mechanism of corresponding reactions. This critical review also captures the insights aimed at accelerating the development of electrochemical C–N coupling reactions, confirming the superiority of this electrochemical method over the traditional techniques.

Efficient Electrochemical Co‐Reduction of Carbon Dioxide and Nitrate to Urea with High Faradaic Efficiency on Cobalt‐Based Dual‐Sites

“…This approach enables us to directly observe the bonding of nitrogen and carbon from the reactants to the product, providing definitive evidence that the synthesis of urea is indeed the result of the C-N coupling reaction. Figure S23, Supporting Information illustrates the 1 H NMR spectrum of the electrolyte with Na 15 NO 3 , displaying the typical double peaks of 15 N-urea at 5.53 and 5.76 ppm, while the 1 H NMR spectrum of the electrolyte with Na 14 NO 3 only exhibits a single peak of 14 N-urea at 5.65 ppm. The 1 H NMR results confirm that there are urea productions in the coupling electrolysis of CO 2 and NO 3 − on Co NPs@C. Recycling tests were performed to examine the stability of the Co NPs@C/CC electrode.…”

“…− concentrations during the urea electrosynthesis process. In addition, we have included isotope-labeling experiments, utilizing 15 N-labeled and 14 N-labeled nitrogen sources to trace their formation of urea molecules. This approach enables us to directly observe the bonding of nitrogen and carbon from the reactants to the product, providing definitive evidence that the synthesis of urea is indeed the result of the C-N coupling reaction.…”