Gold Nanoparticles on Polymer‐Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO 2

Jhong, Huei‐Ru “Molly”; Tornow, Claire E.; Kim, Chaerin; Verma, Sumit; Oberst, Justin L.; Anderson, Paul S.; Gewirth, Andrew A.; Fujigaya, Tsuyohiko; Nakashima, Naotoshi; Kenis, Paul J. A.

doi:10.1002/cphc.201700815

Title: Gold Nanoparticles on Polymer‐Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO ₂

Abstract

Abstract Multiple approaches will be needed to reduce the atmospheric CO ₂ levels, which have been linked to the undesirable effects of global climate change. The electroreduction of CO ₂ driven by renewable energy is one approach to reduce CO ₂ emissions while producing chemical building blocks, but current electrocatalysts exhibit low activity and selectivity. Here, we report the structural and electrochemical characterization of a promising catalyst for the electroreduction of CO ₂ to CO: Au nanoparticles supported on polymer‐wrapped multiwall carbon nanotubes. This catalyst exhibits high selectivity for CO over H ₂ : 80–92 % CO, as well as high activity: partial current density for CO as high as 160 mA cm ⁻² . The observed high activity, originating from a high electrochemically active surface area (23 m ² g ⁻¹ Au), in combination with the low loading (0.17 mg cm ⁻² ) of the highly dispersed Au nanoparticles underscores the promise of this catalyst for efficient electroreduction of CO ₂ .

Authors:

Jhong, Huei‐Ru “Molly” ^[1]; Tornow, Claire E. ^[2]; Kim, Chaerin ^[3]; Verma, Sumit ^[1]; Oberst, Justin L. ^[2]; Anderson, Paul S. ^[2]; Gewirth, Andrew A. ^[1]; Fujigaya, Tsuyohiko ^[3]; Nakashima, Naotoshi ^[3];

^[1]

Department of Chemistry and Chemical &, Biomolecular Engineering University of Illinois at Urbana Champaign 600 South Mathews Avenue Urbana IL 61801 USA, International Institute for Carbon Neutral Energy Research (WPI-I2CNER) Kyushu University 744 Moto-oka Nishi-ku Fukuoka 819-0395 Japan
Department of Chemistry and Chemical &, Biomolecular Engineering University of Illinois at Urbana Champaign 600 South Mathews Avenue Urbana IL 61801 USA
International Institute for Carbon Neutral Energy Research (WPI-I2CNER) Kyushu University 744 Moto-oka Nishi-ku Fukuoka 819-0395 Japan, Department of Applied Chemistry Kyushu University 744 Moto-oka Nishi-ku Fukuoka 819-0395 Japan

Publication Date:: Tue Oct 17 00:00:00 EDT 2017

Sponsoring Org.:: USDOE

OSTI Identifier:: 1399798

Grant/Contract Number:: FG02005ER46260, DE-SC0004453

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: ChemPhysChem

Additional Journal Information:: Journal Name: ChemPhysChem Journal Volume: 18 Journal Issue: 22; Journal ID: ISSN 1439-4235

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Jhong, Huei‐Ru “Molly”, Tornow, Claire E., Kim, Chaerin, Verma, Sumit, Oberst, Justin L., Anderson, Paul S., Gewirth, Andrew A., Fujigaya, Tsuyohiko, Nakashima, Naotoshi, and Kenis, Paul J. A. Gold Nanoparticles on Polymer‐Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO 2.  Germany: N. p., 2017. 
Web.  doi:10.1002/cphc.201700815.

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                    Jhong, Huei‐Ru “Molly”, Tornow, Claire E., Kim, Chaerin, Verma, Sumit, Oberst, Justin L., Anderson, Paul S., Gewirth, Andrew A., Fujigaya, Tsuyohiko, Nakashima, Naotoshi, & Kenis, Paul J. A. Gold Nanoparticles on Polymer‐Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO 2.  Germany.  https://doi.org/10.1002/cphc.201700815

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                    Jhong, Huei‐Ru “Molly”, Tornow, Claire E., Kim, Chaerin, Verma, Sumit, Oberst, Justin L., Anderson, Paul S., Gewirth, Andrew A., Fujigaya, Tsuyohiko, Nakashima, Naotoshi, and Kenis, Paul J. A. Tue .  
"Gold Nanoparticles on Polymer‐Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO 2".  Germany.  https://doi.org/10.1002/cphc.201700815.

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@article{osti_1399798,

  title        = {Gold Nanoparticles on Polymer‐Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO 2},

  author       = {Jhong, Huei‐Ru “Molly” and Tornow, Claire E. and Kim, Chaerin and Verma, Sumit and Oberst, Justin L. and Anderson, Paul S. and Gewirth, Andrew A. and Fujigaya, Tsuyohiko and Nakashima, Naotoshi and Kenis, Paul J. A.},

  abstractNote = {Abstract Multiple approaches will be needed to reduce the atmospheric CO 2 levels, which have been linked to the undesirable effects of global climate change. The electroreduction of CO 2 driven by renewable energy is one approach to reduce CO 2 emissions while producing chemical building blocks, but current electrocatalysts exhibit low activity and selectivity. Here, we report the structural and electrochemical characterization of a promising catalyst for the electroreduction of CO 2 to CO: Au nanoparticles supported on polymer‐wrapped multiwall carbon nanotubes. This catalyst exhibits high selectivity for CO over H 2 : 80–92 % CO, as well as high activity: partial current density for CO as high as 160 mA cm −2 . The observed high activity, originating from a high electrochemically active surface area (23 m 2  g −1 Au), in combination with the low loading (0.17 mg cm −2 ) of the highly dispersed Au nanoparticles underscores the promise of this catalyst for efficient electroreduction of CO 2 .},

  doi          = {10.1002/cphc.201700815},

  journal      = {ChemPhysChem},

  number       = 22,

  volume       = 18,

  place        = {Germany},

  year         = {Tue Oct 17 00:00:00 EDT 2017},

  month        = {Tue Oct 17 00:00:00 EDT 2017}

}

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Title: Gold Nanoparticles on Polymer‐Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO 2

Abstract

Citation Formats

Electrochemical conversion of CO2 to useful chemicals: current status, remaining challenges, and future opportunities journal, May 2013

Diesel Production from Fischer−Tropsch: The Past, the Present, and New Concepts journal, May 2009

The Fischer–Tropsch process: 1950–2000 journal, January 2002

Efficient Electrochemical Flow System with Improved Anode for the Conversion of CO2 to CO journal, January 2014

Design of an Assembly of Poly(benzimidazole), Carbon Nanotubes, and Pt Nanoparticles for a Fuel-Cell Electrocatalyst with an Ideal Interfacial Nanostructure journal, March 2009

Tuning of Silver Catalyst Mesostructure Promotes Selective Carbon Dioxide Conversion into Fuels journal, November 2016

Exceptional Size-Dependent Activity Enhancement in the Electroreduction of CO 2 over Au Nanoparticles journal, November 2014

Influence of dilute feed and pH on electrochemical reduction of CO2 to CO on Ag in a continuous flow electrolyzer journal, June 2015

Support materials for PEMFC and DMFC electrocatalysts—A review journal, June 2012

Electrocatalytic process of CO selectivity in electrochemical reduction of CO2 at metal electrodes in aqueous media journal, August 1994

Towards sustainable fuels and chemicals through the electrochemical reduction of CO 2 : lessons from water electrolysis journal, January 2015

A selective and efficient electrocatalyst for carbon dioxide reduction journal, January 2014

Design of an assembly of pyridine-containing polybenzimidazole, carbon nanotubes and Pt nanoparticles for a fuel cell electrocatalyst with a high electrochemically active surface area journal, November 2009

Fuel Cell Electrocatalyst Using Polybenzimidazole-Modified Carbon Nanotubes As Support Materials journal, February 2013

Real surface area measurements in electrochemistry journal, January 1991

Preparation and characterisation of platinum- and gold-coated copper, iron, cobalt and nickel deposits on glassy carbon substrates journal, September 2008

Tuning of Silver Catalyst Mesostructure Promotes Selective Carbon Dioxide Conversion into Fuels journal, November 2016

Operation of a Pressurized System for Continuous Reduction of CO 2 journal, January 2012

Monodisperse Au Nanoparticles for Selective Electrocatalytic Reduction of CO 2 to CO journal, October 2013

Activity Descriptors for CO 2 Electroreduction to Methane on Transition-Metal Catalysts journal, January 2012

The Effects of Catalyst Layer Deposition Methodology on Electrode Performance journal, February 2013

A Gross-Margin Model for Defining Technoeconomic Benchmarks in the Electroreduction of CO 2 journal, June 2016

Future CO 2 Emissions and Climate Change from Existing Energy Infrastructure journal, September 2010

New trends in the development of heterogeneous catalysts for electrochemical CO 2 reduction journal, July 2016

Effect of Cations on the Electrochemical Conversion of CO2 to CO journal, November 2012

Bottom-up design of carbon nanotube-based electrocatalysts and their application in high temperature operating polymer electrolyte fuel cells journal, January 2011

Quantum Description of the Plasmon Resonances of a Nanoparticle Dimer journal, February 2009

Stabilization Wedges: Solving the Climate Problem for the Next 50 Years with Current Technologies journal, August 2004

Greenhouse Gas Emissions, Energy Efficiency, and Cost of Synthetic Fuel Production Using Electrochemical CO 2 Conversion and the Fischer–Tropsch Process journal, June 2016

Electrocatalytic activity of carbon-supported Pt–Au nanoparticles for methanol electro-oxidation journal, May 2007

Prospects of CO2 Utilization via Direct Heterogeneous Electrochemical Reduction journal, December 2010

Aqueous CO 2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles journal, November 2012

A comprehensive review on PEM water electrolysis journal, April 2013

The effect of electrolyte composition on the electroreduction of CO 2 to CO on Ag based gas diffusion electrodes journal, January 2016

Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO 2 Fixation journal, June 2013

Rethinking wedges journal, January 2013

Bench-scale electrochemical system for generation of CO and syn-gas journal, March 2011

Microfluidic Reactor for the Electrochemical Reduction of Carbon Dioxide: The Effect of pH journal, January 2010

Title: Gold Nanoparticles on Polymer‐Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO ₂

Electrochemical conversion of CO2 to useful chemicals: current status, remaining challenges, and future opportunities
journal, May 2013

Diesel Production from Fischer−Tropsch: The Past, the Present, and New Concepts
journal, May 2009

The Fischer–Tropsch process: 1950–2000
journal, January 2002

Efficient Electrochemical Flow System with Improved Anode for the Conversion of CO₂ to CO
journal, January 2014

Design of an Assembly of Poly(benzimidazole), Carbon Nanotubes, and Pt Nanoparticles for a Fuel-Cell Electrocatalyst with an Ideal Interfacial Nanostructure
journal, March 2009

Tuning of Silver Catalyst Mesostructure Promotes Selective Carbon Dioxide Conversion into Fuels
journal, November 2016

Exceptional Size-Dependent Activity Enhancement in the Electroreduction of CO ₂ over Au Nanoparticles
journal, November 2014

Influence of dilute feed and pH on electrochemical reduction of CO₂ to CO on Ag in a continuous flow electrolyzer
journal, June 2015

Support materials for PEMFC and DMFC electrocatalysts—A review
journal, June 2012

Electrocatalytic process of CO selectivity in electrochemical reduction of CO₂ at metal electrodes in aqueous media
journal, August 1994

Towards sustainable fuels and chemicals through the electrochemical reduction of CO ₂ : lessons from water electrolysis
journal, January 2015

A selective and efficient electrocatalyst for carbon dioxide reduction
journal, January 2014

Design of an assembly of pyridine-containing polybenzimidazole, carbon nanotubes and Pt nanoparticles for a fuel cell electrocatalyst with a high electrochemically active surface area
journal, November 2009

Fuel Cell Electrocatalyst Using Polybenzimidazole-Modified Carbon Nanotubes As Support Materials
journal, February 2013

Real surface area measurements in electrochemistry
journal, January 1991

Preparation and characterisation of platinum- and gold-coated copper, iron, cobalt and nickel deposits on glassy carbon substrates
journal, September 2008

Tuning of Silver Catalyst Mesostructure Promotes Selective Carbon Dioxide Conversion into Fuels
journal, November 2016

Operation of a Pressurized System for Continuous Reduction of CO ₂
journal, January 2012

Monodisperse Au Nanoparticles for Selective Electrocatalytic Reduction of CO ₂ to CO
journal, October 2013

Activity Descriptors for CO ₂ Electroreduction to Methane on Transition-Metal Catalysts
journal, January 2012

The Effects of Catalyst Layer Deposition Methodology on Electrode Performance
journal, February 2013

A Gross-Margin Model for Defining Technoeconomic Benchmarks in the Electroreduction of CO ₂
journal, June 2016

Future CO ₂ Emissions and Climate Change from Existing Energy Infrastructure
journal, September 2010

New trends in the development of heterogeneous catalysts for electrochemical CO 2 reduction
journal, July 2016

Effect of Cations on the Electrochemical Conversion of CO₂ to CO
journal, November 2012

Bottom-up design of carbon nanotube-based electrocatalysts and their application in high temperature operating polymer electrolyte fuel cells
journal, January 2011

Quantum Description of the Plasmon Resonances of a Nanoparticle Dimer
journal, February 2009

Stabilization Wedges: Solving the Climate Problem for the Next 50 Years with Current Technologies
journal, August 2004

Greenhouse Gas Emissions, Energy Efficiency, and Cost of Synthetic Fuel Production Using Electrochemical CO ₂ Conversion and the Fischer–Tropsch Process
journal, June 2016

Electrocatalytic activity of carbon-supported Pt–Au nanoparticles for methanol electro-oxidation
journal, May 2007

Prospects of CO₂ Utilization via Direct Heterogeneous Electrochemical Reduction
journal, December 2010

Aqueous CO ₂ Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles
journal, November 2012

A comprehensive review on PEM water electrolysis
journal, April 2013

The effect of electrolyte composition on the electroreduction of CO ₂ to CO on Ag based gas diffusion electrodes
journal, January 2016

Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO ₂ Fixation
journal, June 2013

Rethinking wedges
journal, January 2013

Bench-scale electrochemical system for generation of CO and syn-gas
journal, March 2011

Microfluidic Reactor for the Electrochemical Reduction of Carbon Dioxide: The Effect of pH
journal, January 2010