Triggering C-N Coupling on Metal Oxide Nanocomposite for the Electrochemical Reduction of Co2 and Nox- to Formamide

Putri Ramadhany, Thanh Tran-Phu, Jodie Yuwono, Zhipeng Ma, Chen Han, Thi Kim Anh Nguyen, Josh Leverett, Priyank Kumar, Rosalie Hocking, Antonio Tricoli, Alexandr Simonov, Rose Amal, Rahman Daiyan

Research output: Contribution to journalArticlepeer-review

Abstract

The co-electroreduction of CO2 and NOx- (NO3-/NO2-) to generate formamide (HCONH2) offers an opportunity for downstream chemical and polymer manufacturing decarbonization; however, significant challenges lie in the C-N coupling and the associated low product selectivity. Herein, p-block metal oxides are incorporated in copper oxides to provide more accessible active sites for reactant adsorption and activation, tuning the reaction selectivity toward the formamide production. Through in situ Raman and synchrotron-based infrared spectroscopy measurements, C-N bond formation is demonstrated in real-time with the CuOx/BiOx catalyst, where the C-N bond is detected via a *CHO and *NH2 intermediates formation, in agreement with the density functional theory calculations. When tested in a flow electrolyzer, a formamide yield rate of 134 +- 11 mmol h-1 gcat-1 is reported, the first report of co-electroreduction of CO2 and NOx- to formamide beyond conventional H-cell measurements. These new insights on the C-N coupling mechanisms and scale-up capability provide directions for further development of electrocatalysts for the formamide production.
Original languageAmerican English
Number of pages14
JournalAdvanced Energy Materials
DOIs
StatePublished - 2024

NREL Publication Number

  • NREL/JA-5900-90163

Keywords

  • electrocatalytic C-N coupling
  • formamide
  • metal oxides
  • nanocomposite

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