Carbon-nitrogen bond formation on Cu electrodes during CO2 reduction in NO3- solution

Piotr M. Krzywda, Ainoa Paradelo Rodríguez, Nieck E. Benes, Bastian T. Mei, Guido Mul*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

26 Citations (Scopus)
113 Downloads (Pure)

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 languageEnglish
Article number121512
JournalApplied catalysis B: environmental
Volume316
Early online date2 Jun 2022
DOIs
Publication statusPublished - 5 Nov 2022

Keywords

  • C-N bond formation
  • Co-electrolysis
  • Cu electrodes
  • Cyanide
  • Raman
  • SERS
  • Urea
  • UT-Hybrid-D

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