Abstract
We demonstrate by Raman Spectroscopy that simultaneous reduction of NO3- and CO2 on Cu surfaces leads to formation of Cu-C[tbnd]N–like species, showing Raman bands at 2080 and 2150 cm−1 when associated with reduced or oxidized Cu surfaces, respectively. Furthermore Cu-C[tbnd]N–like species are soluble, explaining vast restructuring of the Cu surface observed after co-electrolysis of CO2 and nitrate. Oxidation of deposited Cu-C[tbnd]N–like species results in the formation of NO. Cu-C[tbnd]N–like species do not form in electrolytes containing i) NH4+ and CO2, or ii) NO3- and HCOO-, suggesting these likely originate from Cu-CO, the commonly accepted intermediate in electrochemical reduction of CO2, and Cu-NHx species, previously identified in the literature as intermediate towards C-N bond formation. The implications of the previously unresolved formation of Cu-C[tbnd]N–like species for the development of electrodes and processes for electrochemical formation of carbon-nitrogen bonds, including urea, amines or amides, are briefly discussed.
Original language | English |
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Article number | 121512 |
Journal | Applied catalysis B: environmental |
Volume | 316 |
Early online date | 2 Jun 2022 |
DOIs | |
Publication status | Published - 5 Nov 2022 |
Keywords
- C-N bond formation
- Co-electrolysis
- Cu electrodes
- Cyanide
- Raman
- SERS
- Urea
- UT-Hybrid-D