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Title: Silver Nanoparticles with Surface-Bonded Oxygen for Highly Selective CO 2 Reduction

Abstract

Here, the surface electronic structures of catalysts need to be carefully engineered in CO 2 reduction reaction (CO 2RR), 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 CO 2RR 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 CO 2RR performances. A comparative investigation on air-annealed Ag (Air-Ag) catalyst with or without the post-treatment of H 2 thermal annealing (H 2-Ag) was performed. In Air-Ag, the subsurface chemically bonded O species (O-Ag δ+) was identified by angle resolved X-ray photoelectron spectroscopy and X-ray absorption spectroscopy techniques, and contributed to the improved CO selectivity rather than H 2 in CO 2RR electrolysis. As a result, while the maximal CO Faradaic efficiency of H 2-Ag is at ~ 30 %, the Air-Ag catalyst presented a high CO selectivity of more than 90 % under a current density of ~ 21 mA/cm 2.

Authors:
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)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1433963
Report Number(s):
BNL-203485-2018-JAAM
Journal ID: ISSN 2168-0485
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Sustainable Chemistry & Engineering
Additional Journal Information:
Journal Volume: 5; Journal Issue: 10; Journal ID: ISSN 2168-0485
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Jiang, Kun, Kharel, Priti, Peng, Yande, Gangishetty, Mahesh K., Lin, Hao-Yu Greg, Stavitski, Eli, Attenkofer, Klaus, and Wang, Haotian. Silver Nanoparticles with Surface-Bonded Oxygen for Highly Selective CO2 Reduction. United States: N. p., 2017. Web. doi:10.1021/acssuschemeng.7b02380.
Jiang, Kun, Kharel, Priti, Peng, Yande, Gangishetty, Mahesh K., Lin, Hao-Yu Greg, Stavitski, Eli, Attenkofer, Klaus, & Wang, Haotian. Silver Nanoparticles with Surface-Bonded Oxygen for Highly Selective CO2 Reduction. United States. doi:10.1021/acssuschemeng.7b02380.
Jiang, Kun, Kharel, Priti, Peng, Yande, Gangishetty, Mahesh K., Lin, Hao-Yu Greg, Stavitski, Eli, Attenkofer, Klaus, and Wang, Haotian. Tue . "Silver Nanoparticles with Surface-Bonded Oxygen for Highly Selective CO2 Reduction". United States. doi:10.1021/acssuschemeng.7b02380. https://www.osti.gov/servlets/purl/1433963.
@article{osti_1433963,
title = {Silver Nanoparticles with Surface-Bonded Oxygen for Highly Selective CO2 Reduction},
author = {Jiang, Kun and Kharel, Priti and Peng, Yande and Gangishetty, Mahesh K. and Lin, Hao-Yu Greg and Stavitski, Eli and Attenkofer, Klaus and Wang, Haotian},
abstractNote = {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.},
doi = {10.1021/acssuschemeng.7b02380},
journal = {ACS Sustainable Chemistry & Engineering},
number = 10,
volume = 5,
place = {United States},
year = {Tue Sep 12 00:00:00 EDT 2017},
month = {Tue Sep 12 00:00:00 EDT 2017}
}

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