It was found that copper-modified covalent triazine frameworks (Cu-CTF) efficiently catalyze the electrochemical reduction of nitrate and promote N-N bond formation of nitrous oxide (N2O), a key intermediate for N2 formation (denitrification). A Cu-CTF electrode exhibited an onset potential of -50 mV versus RHE for the electrochemical nitrate reduction reaction (NRR). The faradaic efficiency for N2O formation by Cu-CTF reached 18% at -200 mV versus RHE, whereas that for Cu metal was negligible. On the basis of density functional calculations for Cu-CTF, both solvated and surface-bound nitric oxide (NO) were generated by the NRR due to the moderate adsorption strength of Cu atoms for NO, a property that facilitated the effective dimerization of NO through an Eley-Rideal-type mechanism.
ASJC Scopus subject areas
- Electronic, Optical and Magnetic Materials
- Physical and Theoretical Chemistry
- Surfaces, Coatings and Films