Approaching 100% Selectivity at Low Potential on Ag for Electrochemical CO 2 Reduction to CO Using a Surface Additive

Buckley, Aya K.; Cheng, Tao; Oh, Myoung Hwan; Su, Gregory M.; Garrison, Jennifer; Utan, Sean W.; Zhu, Chenhui; Toste, F. Dean; Goddard, III, William A.; Toma, Francesca M.

doi:10.1021/acscatal.1c00830

Title: Approaching 100% Selectivity at Low Potential on Ag for Electrochemical CO ₂ Reduction to CO Using a Surface Additive

Abstract

We report the discovery of a quaternary ammonium surface additive for CO2 reduction on Ag surfaces that changes the Faradaic efficiency for CO from 25% on Ag foil to 97%, while increasing the current density for CO production by a factor of 9 from 0.14 to 1.21 mA/cm2 and reducing the current density for H2 production by a factor of 440 from 0.44 to 0.001 mA/cm2. Using ReaxFF reactive molecular dynamics, we find that the surface additive with the highest selectivity, dihexadecyldimethylammonium bromide, promotes substantial population of CO2 near the Ag surface along with sufficient H2O to activate the CO2. While a critical number of water molecules is required in the reduction of CO2 to CO, the trend in selectivity strongly correlates with the availability of CO2 molecules. We demonstrate that the ordering of the cationic modifiers plays a significant role around the active site, thus determining reaction selectivity. The dramatic improvement by addition of a simple surface additive suggests an additional strategy in electrocatalysis.

Authors:

Buckley, Aya K. ^[1]; Cheng, Tao ^[2];

^[3];

^[4]; Garrison, Jennifer ^[1]; Utan, Sean W. ^[1]; Zhu, Chenhui ^[5];

^[1];

^[6];

^[7]

Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States, Chemical Sciences Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States, Department of Chemistry, University of California, Berkeley, California 94720, United States
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, 199 Renai Road, Suzhou, Jiangsu 215123, PR China, Joint Center for Artificial Photosynthesis and Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91125, United States
Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States, Department of Energy Technology, Korea Institute of Energy Technology, Naju 58322, Republic of Korea
Advanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States, Materials Sciences Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States
Advanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States
Joint Center for Artificial Photosynthesis and Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91125, United States
Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States, Chemical Sciences Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States

Publication Date:: Thu Jul 08 00:00:00 EDT 2021

Research Org.:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1806370

Alternate Identifier(s):: OSTI ID: 1812314; OSTI ID: 1825921

Grant/Contract Number:: SC0004993; AC02-05CH11231

Resource Type:: Published Article

Journal Name:: ACS Catalysis

Additional Journal Information:: Journal Name: ACS Catalysis Journal Volume: 11 Journal Issue: 15; Journal ID: ISSN 2155-5435

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electrochemical CO2 reduction; surface additives; interfaces; silver; molecular dynamics; salts; molecules; selectivity; cations

Citation Formats


                    Buckley, Aya K., Cheng, Tao, Oh, Myoung Hwan, Su, Gregory M., Garrison, Jennifer, Utan, Sean W., Zhu, Chenhui, Toste, F. Dean, Goddard, III, William A., and Toma, Francesca M. Approaching 100% Selectivity at Low Potential on Ag for Electrochemical CO 2 Reduction to CO Using a Surface Additive.  United States: N. p., 2021. 
Web.  doi:10.1021/acscatal.1c00830.

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                    Buckley, Aya K., Cheng, Tao, Oh, Myoung Hwan, Su, Gregory M., Garrison, Jennifer, Utan, Sean W., Zhu, Chenhui, Toste, F. Dean, Goddard, III, William A., & Toma, Francesca M. Approaching 100% Selectivity at Low Potential on Ag for Electrochemical CO 2 Reduction to CO Using a Surface Additive.  United States.  https://doi.org/10.1021/acscatal.1c00830

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                    Buckley, Aya K., Cheng, Tao, Oh, Myoung Hwan, Su, Gregory M., Garrison, Jennifer, Utan, Sean W., Zhu, Chenhui, Toste, F. Dean, Goddard, III, William A., and Toma, Francesca M. Thu .  
"Approaching 100% Selectivity at Low Potential on Ag for Electrochemical CO 2 Reduction to CO Using a Surface Additive".  United States.  https://doi.org/10.1021/acscatal.1c00830.

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@article{osti_1806370,

  title        = {Approaching 100% Selectivity at Low Potential on Ag for Electrochemical CO 2 Reduction to CO Using a Surface Additive},

  author       = {Buckley, Aya K. and Cheng, Tao and Oh, Myoung Hwan and Su, Gregory M. and Garrison, Jennifer and Utan, Sean W. and Zhu, Chenhui and Toste, F. Dean and Goddard, III, William A. and Toma, Francesca M.},

  abstractNote = {We report the discovery of a quaternary ammonium surface additive for CO2 reduction on Ag surfaces that changes the Faradaic efficiency for CO from 25% on Ag foil to 97%, while increasing the current density for CO production by a factor of 9 from 0.14 to 1.21 mA/cm2 and reducing the current density for H2 production by a factor of 440 from 0.44 to 0.001 mA/cm2. Using ReaxFF reactive molecular dynamics, we find that the surface additive with the highest selectivity, dihexadecyldimethylammonium bromide, promotes substantial population of CO2 near the Ag surface along with sufficient H2O to activate the CO2. While a critical number of water molecules is required in the reduction of CO2 to CO, the trend in selectivity strongly correlates with the availability of CO2 molecules. We demonstrate that the ordering of the cationic modifiers plays a significant role around the active site, thus determining reaction selectivity. The dramatic improvement by addition of a simple surface additive suggests an additional strategy in electrocatalysis.},

  doi          = {10.1021/acscatal.1c00830},

  journal      = {ACS Catalysis},

  number       = 15,

  volume       = 11,

  place        = {United States},

  year         = {Thu Jul 08 00:00:00 EDT 2021},

  month        = {Thu Jul 08 00:00:00 EDT 2021}

}

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Title: Approaching 100% Selectivity at Low Potential on Ag for Electrochemical CO 2 Reduction to CO Using a Surface Additive

Abstract

Citation Formats

Surface Ligand Promotion of Carbon Dioxide Reduction through Stabilizing Chemisorbed Reactive Intermediates journal, May 2018

Carbon Dioxide Reduction in Room-Temperature Ionic Liquids: The Effect of the Choice of Electrode Material, Cation, and Anion journal, November 2016

Development and Validation of a ReaxFF Reactive Force Field for Cu Cation/Water Interactions and Copper Metal/Metal Oxide/Metal Hydroxide Condensed Phases journal, September 2010

Effects of temperature and gas–liquid mass transfer on the operation of small electrochemical cells for the quantitative evaluation of CO 2 reduction electrocatalysts journal, January 2016

Molecular tuning of CO2-to-ethylene conversion journal, November 2019

Crystal structures of three new N -halomethylated quaternary ammonium salts journal, September 2015

Ionic Liquid-Mediated Selective Conversion of CO2 to CO at Low Overpotentials journal, September 2011

Structural Transition in an Ionic Liquid Controls CO 2 Electrochemical Reduction journal, July 2015

Insights into the electrocatalytic reduction of CO 2 on metallic silver surfaces journal, January 2014

CO 2 Reduction Selective for C ≥2 Products on Polycrystalline Copper with N-Substituted Pyridinium Additives journal, July 2017

New Insights Into the Role of Imidazolium-Based Promoters for the Electroreduction of CO 2 on a Silver Electrode journal, June 2016

Understanding cation effects in electrochemical CO 2 reduction journal, January 2019

Some Topics in the Theory of Fluids journal, December 1963

The influence of chain configuration and, in turn, chain packing on the sorption and transport properties of poly(tert-butyl acetylene) journal, September 1993

Electrochemical CO2-to-ethylene conversion on polyamine-incorporated Cu electrodes journal, December 2020

How cations affect the electric double layer and the rates and selectivity of electrocatalytic processes journal, October 2019

Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products journal, March 2019

In Situ Spectroscopic Examination of a Low Overpotential Pathway for Carbon Dioxide Conversion to Carbon Monoxide journal, July 2012

Hydronium-Induced Switching between CO 2 Electroreduction Pathways journal, February 2018

Insight into the Microenvironments of the Metal–Ionic Liquid Interface during Electrochemical CO 2 Reduction journal, January 2018

Dynamic Boundary Layer Simulation of Pulsed CO 2 Electrolysis on a Copper Catalyst journal, March 2021

Electrocatalysis at Organic–Metal Interfaces: Identification of Structure–Reactivity Relationships for CO 2 Reduction at Modified Cu Surfaces journal, March 2019

Using Microenvironments to Control Reactivity in CO2 Electrocatalysis journal, February 2020

Efficient electroreduction of CO 2 on bulk silver electrode in aqueous solution via the inhibition of hydrogen evolution journal, March 2017

Organo-vermiculites: synthesis, structure and properties. Platelike nanoparticles with high aspect ratio journal, January 2006

Progress and Perspectives of Electrochemical CO 2 Reduction on Copper in Aqueous Electrolyte journal, April 2019

Dramatic HER Suppression on Ag Electrodes via Molecular Films for Highly Selective CO 2 to CO Reduction journal, March 2021

In Situ Monitoring Using ATR-SEIRAS of the Electrocatalytic Reduction of CO 2 on Au in an Ionic Liquid/Water Mixture journal, May 2018

Title: Approaching 100% Selectivity at Low Potential on Ag for Electrochemical CO ₂ Reduction to CO Using a Surface Additive

Surface Ligand Promotion of Carbon Dioxide Reduction through Stabilizing Chemisorbed Reactive Intermediates
journal, May 2018

Carbon Dioxide Reduction in Room-Temperature Ionic Liquids: The Effect of the Choice of Electrode Material, Cation, and Anion
journal, November 2016

Development and Validation of a ReaxFF Reactive Force Field for Cu Cation/Water Interactions and Copper Metal/Metal Oxide/Metal Hydroxide Condensed Phases
journal, September 2010

Effects of temperature and gas–liquid mass transfer on the operation of small electrochemical cells for the quantitative evaluation of CO ₂ reduction electrocatalysts
journal, January 2016

Molecular tuning of CO2-to-ethylene conversion
journal, November 2019

Crystal structures of three new N -halomethylated quaternary ammonium salts
journal, September 2015

Ionic Liquid-Mediated Selective Conversion of CO₂ to CO at Low Overpotentials
journal, September 2011

Structural Transition in an Ionic Liquid Controls CO ₂ Electrochemical Reduction
journal, July 2015

Insights into the electrocatalytic reduction of CO ₂ on metallic silver surfaces
journal, January 2014

CO ₂ Reduction Selective for C _≥2 Products on Polycrystalline Copper with N-Substituted Pyridinium Additives
journal, July 2017

New Insights Into the Role of Imidazolium-Based Promoters for the Electroreduction of CO ₂ on a Silver Electrode
journal, June 2016

Understanding cation effects in electrochemical CO ₂ reduction
journal, January 2019

Some Topics in the Theory of Fluids
journal, December 1963

The influence of chain configuration and, in turn, chain packing on the sorption and transport properties of poly(tert-butyl acetylene)
journal, September 1993

Electrochemical CO2-to-ethylene conversion on polyamine-incorporated Cu electrodes
journal, December 2020

How cations affect the electric double layer and the rates and selectivity of electrocatalytic processes
journal, October 2019

Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products
journal, March 2019

In Situ Spectroscopic Examination of a Low Overpotential Pathway for Carbon Dioxide Conversion to Carbon Monoxide
journal, July 2012

Hydronium-Induced Switching between CO ₂ Electroreduction Pathways
journal, February 2018

Insight into the Microenvironments of the Metal–Ionic Liquid Interface during Electrochemical CO ₂ Reduction
journal, January 2018

Dynamic Boundary Layer Simulation of Pulsed CO ₂ Electrolysis on a Copper Catalyst
journal, March 2021

Electrocatalysis at Organic–Metal Interfaces: Identification of Structure–Reactivity Relationships for CO ₂ Reduction at Modified Cu Surfaces
journal, March 2019

Using Microenvironments to Control Reactivity in CO2 Electrocatalysis
journal, February 2020

Efficient electroreduction of CO 2 on bulk silver electrode in aqueous solution via the inhibition of hydrogen evolution
journal, March 2017

Organo-vermiculites: synthesis, structure and properties. Platelike nanoparticles with high aspect ratio
journal, January 2006

Progress and Perspectives of Electrochemical CO ₂ Reduction on Copper in Aqueous Electrolyte
journal, April 2019

Dramatic HER Suppression on Ag Electrodes via Molecular Films for Highly Selective CO ₂ to CO Reduction
journal, March 2021

In Situ Monitoring Using ATR-SEIRAS of the Electrocatalytic Reduction of CO ₂ on Au in an Ionic Liquid/Water Mixture
journal, May 2018