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Title: Electrochemical Conversion of CO2 to Syngas with Controllable CO/H2 Ratios over Co and Ni Single-Atom Catalysts

Journal Article · · Angewandte Chemie
 [1];  [2];  [3];  [3];  [4];  [4];  [5];  [6];  [7]
  1. Univ. of Science and Technology of China, Anhui (China); Columbia Univ., New York, NY (United States)
  2. Nanyang Technological Univ. (Singapore)
  3. Columbia Univ., New York, NY (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
  5. Florida A & M University, Tallahassee, FL (United States)
  6. Univ. of Science and Technology of China, Anhui (China)
  7. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
+ Show Author Affiliations

The electrochemical CO2 reduction reaction (CO2RR) to yield synthesis gas (syngas, CO and H2) has been considered as a promising method to realize the net reduction in CO2 emission. However, it is challenging to balance the CO2RR activity and the CO/H2 ratio. To address this issue, nitrogen-doped carbon supported single-atom catalysts are designed as electrocatalysts to produce syngas from CO2RR. While Co and Ni single-atom catalysts are selective in producing H2 and CO, respectively, electrocatalysts containing both Co and Ni show a high syngas evolution (total current 74 mA cm-2) with CO/H2 ratios (0.23-2.26) that are suitable for typical downstream thermochemical reactions. Density functional theory calculations provide insights into the key intermediates on Co and Ni single-atom configurations for the H2 and CO evolution. The results present a useful case on how non-precious transition metal species can maintain high CO2RR activity with tunable CO/H2 ratios.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0012704
OSTI ID:
1580239
Alternate ID(s):
OSTI ID: 1581860
Report Number(s):
BNL-212468-2019-JAAM
Journal Information:
Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 8 Vol. 132; ISSN 0044-8249
Publisher:
German Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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