The asymmetric orbital hybridization in single-atom-dimers for urea synthesis by optimizing the C-N coupling reaction pathway

Electrocatalytic reduction from nitrate (NO3-) and carbon dioxide (CO2) parades great prospects in substituting traditional process for urea synthesis, but challenges remain due to the arduous C-N coupling and multistage protonation. Unlike common design strategies, our study utilized synergistic effect between asymmetrical sites to reduce coupling barrier and promote urea production. Herein, we anchor dual single-atom Ru and Co on N-doped carbon for fixing the C/N group respectively and minimizing the generation energy for intermediates. As a result, the CoRuN6 electrocatalyst successfully restricts the parrel reaction (CO2/NO3- reduction) and affords a urea yield of 8.98 mmol h−1g−1 and a faradic efficiency (FE) of 25.31% at − 0.6 V versus RHE. Our research provides novel insights into capitalizing on spatial regulation of active sites for efficient urea electrosynthesis.