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Modulating CO2 Electrocatalytic Conversion to the Organics Pathway by the Catalytic Site Dimension

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.3c12722· OSTI ID:2341256
 [1];  [2];  [3];  [4];  [4];  [4];  [5];  [6];  [4];  [7];  [5]
  1. Argonne National Laboratory (ANL), Argonne, IL (United States); Northern Illinois University, DeKalb, IL (United States); Northern Illinois University
  2. Argonne National Laboratory (ANL), Argonne, IL (United States); Northern Illinois University, DeKalb, IL (United States)
  3. Valparaiso University, IN (United States)
  4. Argonne National Laboratory (ANL), Argonne, IL (United States)
  5. Argonne National Laboratory (ANL), Argonne, IL (United States); University of Chicago, IL (United States)
  6. Northern Illinois University, DeKalb, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
  7. Northern Illinois University, DeKalb, IL (United States)
+ Show Author Affiliations
Electrochemical reduction of carbon dioxide to organic chemicals provides a value-added route for mitigating greenhouse gas emissions. Here, we report a family of carbon-supported Sn electrocatalysts with the tin size varying from single atom, ultrasmall clusters to nanocrystallites. High single-product Faradaic efficiency (FE) and low onset potential of CO2 conversion to acetate (FE = 90% @ –0.6 V), ethanol (FE = 92% @ –0.4 V), and formate (FE = 91% @ –0.6 V) were achieved over the catalysts of different active site dimensions. The CO2 conversion mechanism behind these highly selective, size-modulated p-block element catalysts was elucidated by structural characterization and computational modeling, together with kinetic isotope effect investigation.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States); Northern Illinois University, DeKalb, IL (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357; EE0009418
OSTI ID:
2341256
Alternate ID(s):
OSTI ID: 2502010
OSTI ID: 2574814
Report Number(s):
DOE-NIU-9418--1
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 15 Vol. 146; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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