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Triggering C-N Coupling on Metal Oxide Nanocomposite for the Electrochemical Reduction of CO2 and NOx⁻ to Formamide

Journal Article · · Advanced Energy Materials
 [1];  [2];  [3];  [1];  [1];  [4];  [1];  [1];  [5];  [4];  [6];  [1];  [1]
  1. Univ. of New South Wales, Sydney, NSW (Australia)
  2. National Renewable Energy Laboratory (NREL), Golden, CO (United States)
  3. Univ. of Adelaide, SA (Australia)
  4. Univ. of Sydney, NSW (Australia)
  5. Swinburne University of Technology, Melbourne, VIC (Australia)
  6. Monash Univ., Melbourne, VIC (Australia)

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.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE; Australian Research Council (ARC)
Grant/Contract Number:
AC36-08GO28308
OSTI ID:
2371675
Report Number(s):
NREL/JA--5900-90163; MainId:91941; UUID:ddae5065-25e4-4a96-b36d-4bbee1426d40; MainAdminId:72789
Journal Information:
Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 32 Vol. 14; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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