Electrochemical synthesis of C-N bond-containing com-pounds(e.g.,urea,amino acid,amide,amine,and their de-rivates)from CO2/N2 and their derivates is emerging as a promising sustainable strategy[1-7].CO2 and its derived products,CO,HCOOH,(COOH)2,etc.,could serve as car-bon sources(Figure 1)[8].N2,making up 80%of air,is an appealing nitrogen source.However,the low solubility of N2 and the high dissociation energy for the N≡N bond limit its application.The recent advances in renewable energy-driven nitrogen fixation techniques are expected to provide green active nitrogen sources.Specifically,photocatalytic or elec-trocatalytic oxidation of N2 to NOx/NO3-has been achieved recently by our group[9-12].Now,the development of clean electricity has reawakened the interest in plasma-/electro-catalytic nitrogen fixation.Combining the renewable-en-ergy-driven C/N precursor activation/conversion with the subsequent electrocatalytic C-N coupling is an alternative way to realize high selectivity synthesis of the target pro-ducts.The bottleneck for this technique lies in the compe-titive relationship between the C-N coupling reaction and the sole reduction of the C/N precursor.To obtain a high current density,a big applied potential is usually required,accompanied by the occurrence of side reactions,resulting in the decrease of Faradaic efficiency.