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

Abstract

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.

Authors:
 [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)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1580239
Alternate Identifier(s):
OSTI ID: 1581860
Report Number(s):
BNL-212468-2019-JAAM
Journal ID: ISSN 0044-8249
Grant/Contract Number:  
SC0012704; FG02-13ER16381; SC0009476
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie
Additional Journal Information:
Journal Volume: 132; Journal Issue: 8; Journal ID: ISSN 0044-8249
Publisher:
German Chemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; CO2 electroreduction; selectivity control; syngas production; high activity; density functional theory

Citation Formats

He, Qun, Liu, Daobin, Lee, Ji Hoon, Liu, Yumeng, Xie, Zhenhua, Hwang, Sooyeon, Kattel, Shyam, Song, Li, and Chen, Jingguang G. Electrochemical Conversion of CO2 to Syngas with Controllable CO/H2 Ratios over Co and Ni Single-Atom Catalysts. United States: N. p., 2019. Web. doi:10.1002/ange.201912719.
He, Qun, Liu, Daobin, Lee, Ji Hoon, Liu, Yumeng, Xie, Zhenhua, Hwang, Sooyeon, Kattel, Shyam, Song, Li, & Chen, Jingguang G. Electrochemical Conversion of CO2 to Syngas with Controllable CO/H2 Ratios over Co and Ni Single-Atom Catalysts. United States. doi:https://doi.org/10.1002/ange.201912719
He, Qun, Liu, Daobin, Lee, Ji Hoon, Liu, Yumeng, Xie, Zhenhua, Hwang, Sooyeon, Kattel, Shyam, Song, Li, and Chen, Jingguang G. Wed . "Electrochemical Conversion of CO2 to Syngas with Controllable CO/H2 Ratios over Co and Ni Single-Atom Catalysts". United States. doi:https://doi.org/10.1002/ange.201912719. https://www.osti.gov/servlets/purl/1580239.
@article{osti_1580239,
title = {Electrochemical Conversion of CO2 to Syngas with Controllable CO/H2 Ratios over Co and Ni Single-Atom Catalysts},
author = {He, Qun and Liu, Daobin and Lee, Ji Hoon and Liu, Yumeng and Xie, Zhenhua and Hwang, Sooyeon and Kattel, Shyam and Song, Li and Chen, Jingguang G.},
abstractNote = {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.},
doi = {10.1002/ange.201912719},
journal = {Angewandte Chemie},
number = 8,
volume = 132,
place = {United States},
year = {2019},
month = {12}
}

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