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Title: The Role of Subsurface Oxygen on Cu Surfaces for CO2 Electrochemical Reduction

Abstract

Under ambient conditions, copper with oxygen near the surface displays strengthened CO2 and CO adsorption energies. This finding is often used to rationalize differences seen in product distributions between Cu-oxide and pure Cu electrodes during electrochemical CO2 reduction. However, little evidence exists to confirm the presence of oxygen within first few layers of the Cu matrix under relevant experimental reducing conditions. As a result, using density functional theory calculations, we discuss the stability of subsurface oxygen from thermodynamic and kinetic perspectives, and show that under reducing potentials, subsurface oxygen alone should have negligible effects on the activity of crystalline Cu.

Authors:
 [1];  [2];  [1];  [3]
  1. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Zhejiang Univ., Hangzhou (China)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1457147
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 28; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Fields, Meredith, Hong, Xin, Norskov, Jens K., and Chan, Karen. The Role of Subsurface Oxygen on Cu Surfaces for CO2 Electrochemical Reduction. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b04983.
Fields, Meredith, Hong, Xin, Norskov, Jens K., & Chan, Karen. The Role of Subsurface Oxygen on Cu Surfaces for CO2 Electrochemical Reduction. United States. doi:10.1021/acs.jpcc.8b04983.
Fields, Meredith, Hong, Xin, Norskov, Jens K., and Chan, Karen. Tue . "The Role of Subsurface Oxygen on Cu Surfaces for CO2 Electrochemical Reduction". United States. doi:10.1021/acs.jpcc.8b04983. https://www.osti.gov/servlets/purl/1457147.
@article{osti_1457147,
title = {The Role of Subsurface Oxygen on Cu Surfaces for CO2 Electrochemical Reduction},
author = {Fields, Meredith and Hong, Xin and Norskov, Jens K. and Chan, Karen},
abstractNote = {Under ambient conditions, copper with oxygen near the surface displays strengthened CO2 and CO adsorption energies. This finding is often used to rationalize differences seen in product distributions between Cu-oxide and pure Cu electrodes during electrochemical CO2 reduction. However, little evidence exists to confirm the presence of oxygen within first few layers of the Cu matrix under relevant experimental reducing conditions. As a result, using density functional theory calculations, we discuss the stability of subsurface oxygen from thermodynamic and kinetic perspectives, and show that under reducing potentials, subsurface oxygen alone should have negligible effects on the activity of crystalline Cu.},
doi = {10.1021/acs.jpcc.8b04983},
journal = {Journal of Physical Chemistry. C},
number = 28,
volume = 122,
place = {United States},
year = {2018},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

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Cited by: 5 works
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Figures / Tables:

Table 1 Table 1: Oxygen Free Energies in a Cu (111) slab.

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Works referencing / citing this record:

Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design
journal, December 2018

  • Kibria, Md Golam; Edwards, Jonathan P.; Gabardo, Christine M.
  • Advanced Materials, Vol. 31, Issue 31
  • DOI: 10.1002/adma.201807166

Paramelaconite‐Enriched Copper‐Based Material as an Efficient and Robust Catalyst for Electrochemical Carbon Dioxide Reduction
journal, June 2019

  • Martić, Nemanja; Reller, Christian; Macauley, Chandra
  • Advanced Energy Materials, Vol. 9, Issue 29
  • DOI: 10.1002/aenm.201901228

Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels
journal, September 2019

  • Birdja, Yuvraj Y.; Pérez-Gallent, Elena; Figueiredo, Marta C.
  • Nature Energy, Vol. 4, Issue 9
  • DOI: 10.1038/s41560-019-0450-y

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.