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

Abstract

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.

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 Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1433963
Report Number(s):
BNL-203485-2018-JAAM
Journal ID: ISSN 2168-0485
Grant/Contract Number:  
SC0012704
Resource Type:
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:https://doi.org/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:https://doi.org/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 = {2017},
month = {9}
}

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Works referencing / citing this record:

Recent Advances in Electrochemical CO 2 -to-CO Conversion on Heterogeneous Catalysts
journal, August 2018

  • Zheng, Tingting; Jiang, Kun; Wang, Haotian
  • Advanced Materials, Vol. 30, Issue 48
  • DOI: 10.1002/adma.201802066

2D Assembly of Confined Space toward Enhanced CO 2 Electroreduction
journal, July 2018


A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO 2 to Value‐Added Chemicals and Fuel
journal, November 2019

  • Daiyan, Rahman; Saputera, Wibawa Hendra; Masood, Hassan
  • Advanced Energy Materials, Vol. 10, Issue 11
  • DOI: 10.1002/aenm.201902106

Rational Design of Ag‐Based Catalysts for the Electrochemical CO 2 Reduction to CO: A Review
journal, December 2019


Operando EXAFS study reveals presence of oxygen in oxide-derived silver catalysts for electrochemical CO 2 reduction
journal, January 2019

  • Firet, Nienke J.; Blommaert, Marijn A.; Burdyny, Thomas
  • Journal of Materials Chemistry A, Vol. 7, Issue 6
  • DOI: 10.1039/c8ta10412c

Understanding three-dimensionally interconnected porous oxide-derived copper electrocatalyst for selective carbon dioxide reduction
journal, January 2019

  • Nguyen-Phan, Thuy-Duong; Wang, Congjun; Marin, Chris M.
  • Journal of Materials Chemistry A, Vol. 7, Issue 48
  • DOI: 10.1039/c9ta10135g

Heterogeneous catalysts for catalytic CO2 conversion into value-added chemicals
journal, March 2019