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Title: Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide

Abstract

The electrochemical reduction of CO2 is known to be influenced by the identity of the alkali metal cation in the electrolyte; however, a satisfactory explanation for this phenomenon has not been developed. Here we present the results of experimental and theoretical studies aimed at elucidating the effects of electrolyte cation size on the intrinsic activity and selectivity of metal catalysts for the reduction of CO2. Experiments were conducted under conditions where the influence of electrolyte polarization is minimal in order to show that cation size affects the intrinsic rates of formation of certain reaction products, most notably for HCOO, C2H4, and C2H5OH over Cu(100)- and Cu(111)-oriented thin films, and for CO and HCOO– over polycrystalline Ag and Sn. Interpretation of the findings for CO2 reduction was informed by studies of the reduction of glyoxal and CO, key intermediates along the reaction pathway to final products. Density functional theory calculations show that the alkali metal cations influence the distribution of products formed as a consequence of electrostatic interactions between solvated cations present at the outer Helmholtz plane and adsorbed species having large dipole moments. As a result, the observed trends in activity with cation size are attributed to an increase inmore » the concentration of cations at the outer Helmholtz plane with increasing cation size.« less

Authors:
 [1];  [2];  [1];  [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1390621
Alternate Identifier(s):
OSTI ID: 1418306
Grant/Contract Number:  
AC02-76SF00515; DGE-0802270; AC02-05CH11231; SC0004993
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 32; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electrochemical reduction; CO2; copper; silver

Citation Formats

Resasco, Joaquin, Chen, Leanne D., Clark, Ezra, Tsai, Charlie, Hahn, Christopher, Jaramillo, Thomas F., Chan, Karen, and Bell, Alexis T. Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide. United States: N. p., 2017. Web. doi:10.1021/jacs.7b06765.
Resasco, Joaquin, Chen, Leanne D., Clark, Ezra, Tsai, Charlie, Hahn, Christopher, Jaramillo, Thomas F., Chan, Karen, & Bell, Alexis T. Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide. United States. https://doi.org/10.1021/jacs.7b06765
Resasco, Joaquin, Chen, Leanne D., Clark, Ezra, Tsai, Charlie, Hahn, Christopher, Jaramillo, Thomas F., Chan, Karen, and Bell, Alexis T. Mon . "Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide". United States. https://doi.org/10.1021/jacs.7b06765. https://www.osti.gov/servlets/purl/1390621.
@article{osti_1390621,
title = {Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide},
author = {Resasco, Joaquin and Chen, Leanne D. and Clark, Ezra and Tsai, Charlie and Hahn, Christopher and Jaramillo, Thomas F. and Chan, Karen and Bell, Alexis T.},
abstractNote = {The electrochemical reduction of CO2 is known to be influenced by the identity of the alkali metal cation in the electrolyte; however, a satisfactory explanation for this phenomenon has not been developed. Here we present the results of experimental and theoretical studies aimed at elucidating the effects of electrolyte cation size on the intrinsic activity and selectivity of metal catalysts for the reduction of CO2. Experiments were conducted under conditions where the influence of electrolyte polarization is minimal in order to show that cation size affects the intrinsic rates of formation of certain reaction products, most notably for HCOO–, C2H4, and C2H5OH over Cu(100)- and Cu(111)-oriented thin films, and for CO and HCOO– over polycrystalline Ag and Sn. Interpretation of the findings for CO2 reduction was informed by studies of the reduction of glyoxal and CO, key intermediates along the reaction pathway to final products. Density functional theory calculations show that the alkali metal cations influence the distribution of products formed as a consequence of electrostatic interactions between solvated cations present at the outer Helmholtz plane and adsorbed species having large dipole moments. As a result, the observed trends in activity with cation size are attributed to an increase in the concentration of cations at the outer Helmholtz plane with increasing cation size.},
doi = {10.1021/jacs.7b06765},
journal = {Journal of the American Chemical Society},
number = 32,
volume = 139,
place = {United States},
year = {Mon Jul 24 00:00:00 EDT 2017},
month = {Mon Jul 24 00:00:00 EDT 2017}
}

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journal, October 2018

  • Lv, Jing-Jing; Jouny, Matthew; Luc, Wesley
  • Advanced Materials, Vol. 30, Issue 49
  • DOI: 10.1002/adma.201803111

Quantification of Interfacial pH Variation at Molecular Length Scales Using a Concurrent Non-Faradaic Reaction
journal, July 2018

  • Ryu, Jaeyune; Wuttig, Anna; Surendranath, Yogesh
  • Angewandte Chemie, Vol. 130, Issue 30
  • DOI: 10.1002/ange.201802756

FeNC catalysts for CO 2 electroreduction to CO: effect of nanostructured carbon supports
journal, January 2019

  • Karapinar, Dilan; Tran, Ngoc-Huan; Giaume, Domitille
  • Sustainable Energy & Fuels, Vol. 3, Issue 7
  • DOI: 10.1039/c9se00214f

Role of the Adsorbed Oxygen Species in the Selective Electrochemical Reduction of CO 2 to Alcohols and Carbonyls on Copper Electrodes
journal, September 2017

  • Le Duff, Cécile S.; Lawrence, Matthew J.; Rodriguez, Paramaconi
  • Angewandte Chemie International Edition, Vol. 56, Issue 42
  • DOI: 10.1002/anie.201706463

Carbon‐Nanotube‐Supported Copper Polyphthalocyanine for Efficient and Selective Electrocatalytic CO 2 Reduction to CO
journal, November 2019


Understanding the Heterogeneous Electrocatalytic Reduction of Carbon Dioxide on Oxide-Derived Catalysts
journal, December 2017


Atomic‐Scale Spacing between Copper Facets for the Electrochemical Reduction of Carbon Dioxide
journal, March 2020

  • Jeong, Hyung Mo; Kwon, Youngkook; Won, Jong Ho
  • Advanced Energy Materials, Vol. 10, Issue 10
  • DOI: 10.1002/aenm.201903423

Hydroxide Is Not a Promoter of C 2+ Product Formation in the Electrochemical Reduction of CO on Copper
journal, March 2020


Lateral Adsorbate Interactions Inhibit HCOO while Promoting CO Selectivity for CO 2 Electrocatalysis on Silver
journal, December 2018

  • Bohra, Divya; Ledezma-Yanez, Isis; Li, Guanna
  • Angewandte Chemie, Vol. 131, Issue 5
  • DOI: 10.1002/ange.201811667

Defining a Materials Database for the Design of Copper Binary Alloy Catalysts for Electrochemical CO 2 Conversion
journal, January 2018

  • Lee, Chan Woo; Yang, Ki Dong; Nam, Dae-Hyun
  • Advanced Materials, Vol. 30, Issue 42
  • DOI: 10.1002/adma.201704717

Cover Picture: Hydroxide Is Not a Promoter of C 2+ Product Formation in the Electrochemical Reduction of CO on Copper (Angew. Chem. Int. Ed. 11/2020)
journal, January 2020

  • Li, Jing; Wu, Donghuan; Malkani, Arnav S.
  • Angewandte Chemie International Edition, Vol. 59, Issue 11
  • DOI: 10.1002/anie.202000873

Competition between H and CO for Active Sites Governs Copper-Mediated Electrosynthesis of Hydrocarbon Fuels
journal, July 2018

  • Schreier, Marcel; Yoon, Youngmin; Jackson, Megan N.
  • Angewandte Chemie International Edition, Vol. 57, Issue 32
  • DOI: 10.1002/anie.201806051

Lateral Adsorbate Interactions Inhibit HCOO while Promoting CO Selectivity for CO 2 Electrocatalysis on Silver
journal, January 2019

  • Bohra, Divya; Ledezma‐Yanez, Isis; Li, Guanna
  • Angewandte Chemie International Edition, Vol. 58, Issue 5
  • DOI: 10.1002/anie.201811667

Titelbild: Hydroxide Is Not a Promoter of C 2+ Product Formation in the Electrochemical Reduction of CO on Copper (Angew. Chem. 11/2020)
journal, March 2020


Lateral Adsorbate Interactions Inhibit HCOO while Promoting CO Selectivity for CO 2 Electrocatalysis on Silver
journal, January 2019

  • Bohra, Divya; Ledezma‐Yanez, Isis; Li, Guanna
  • Angewandte Chemie International Edition, Vol. 58, Issue 5
  • DOI: 10.1002/anie.201811667

Plasma-Modified Dendritic Cu Catalyst for CO2Electroreduction
journal, April 2019


In Situ Infrared Spectroscopy Reveals Persistent Alkalinity near Electrode Surfaces during CO 2 Electroreduction
journal, September 2019

  • Yang, Kailun; Kas, Recep; Smith, Wilson A.
  • Journal of the American Chemical Society, Vol. 141, Issue 40
  • DOI: 10.1021/jacs.9b07000

Operando Insight into the Correlation between the Structure and Composition of CuZn Nanoparticles and Their Selectivity for the Electrochemical CO 2 Reduction
journal, November 2019

  • Jeon, Hyo Sang; Timoshenko, Janis; Scholten, Fabian
  • Journal of the American Chemical Society, Vol. 141, Issue 50
  • DOI: 10.1021/jacs.9b10709

Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts
journal, August 2019


Theoretical insights into selective electrochemical conversion of carbon dioxide
journal, March 2019