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Title: Silver Nanoparticles with Surface-Bonded Oxygen for Highly Selective CO2 Reduction

Journal Article · · ACS Sustainable Chemistry & Engineering
ORCiD logo [1];  [2];  [3];  [1];  [1];  [4];  [4]; ORCiD logo [1]
  1. Harvard Univ., Cambridge, MA (United States)
  2. Harvard Univ., Cambridge, MA (United States); Hamilton College, Clinton, NY (United States)
  3. Harvard Univ., Cambridge, MA (United States); Univ, of Science and Technology of China, Anhui (China)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
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Here, the surface electronic structures of catalysts need to be carefully engineered in CO2 reduction reaction (CO2RR), where the hydrogen evolution side reaction usually takes over under a significant overpotential, and thus dramatically lows the reaction selectivity. Surface oxides can play a critical role in tuning the surface oxidation state of metal catalysts for a proper binding with CO2RR reaction intermediates, which may significantly improve the catalyst activity and selectivity. Here, we demonstrate the importance of surface-bonded oxygen on silver nanoparticles in altering the reaction pathways and improving the CO2RR performances. A comparative investigation on air-annealed Ag (Air-Ag) catalyst with or without the post-treatment of H2 thermal annealing (H2-Ag) was performed. In Air-Ag, the subsurface chemically bonded O species (O-Agδ+) was identified by angle resolved X-ray photoelectron spectroscopy and X-ray absorption spectroscopy techniques, and contributed to the improved CO selectivity rather than H2 in CO2RR electrolysis. As a result, while the maximal CO Faradaic efficiency of H2-Ag is at ~ 30 %, the Air-Ag catalyst presented a high CO selectivity of more than 90 % under a current density of ~ 21 mA/cm2.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704
OSTI ID:
1433963
Report Number(s):
BNL-203485-2018-JAAM
Journal Information:
ACS Sustainable Chemistry & Engineering, Vol. 5, Issue 10; ISSN 2168-0485
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 47 works
Citation information provided by
Web of Science

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  • Stephens, Ifan E. L.; Bondarenko, Alexander S.; Perez-Alonso, Francisco J.
  • Journal of the American Chemical Society, Vol. 133, Issue 14 https://doi.org/10.1021/ja111690g
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Cited By (6)

2D Assembly of Confined Space toward Enhanced CO 2 Electroreduction journal July 2018
Recent Advances in Electrochemical CO 2 -to-CO Conversion on Heterogeneous Catalysts journal August 2018
Understanding three-dimensionally interconnected porous oxide-derived copper electrocatalyst for selective carbon dioxide reduction journal January 2019
Heterogeneous catalysts for catalytic CO2 conversion into value-added chemicals journal March 2019
A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO 2 to Value‐Added Chemicals and Fuel journal November 2019
Rational Design of Ag‐Based Catalysts for the Electrochemical CO 2 Reduction to CO: A Review journal December 2019

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