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Title: CO 2 reduction to acetate in mixtures of ultrasmall (Cu) n ,(Ag) m bimetallic nanoparticles

Abstract

Significance Efficient reduction of carbon dioxide to useful fuels and chemicals is an important research goal in artificial photosynthesis. Significant progress has been made for the C1 products, CO and HCOO − . We report here a procedure based on the use of ultrasmall, monodispersed Cu and Ag bimetallic nanoparticles on thin, electrochemically polymerized poly-Fe(vbpy) 3 (PF 6 ) 2 films. They reduce CO 2 to acetate at pH 7 in aqueous HCO 3 − solutions at relatively high efficiencies with significant rate enhancements with added benzotriazole. In the sequence of clusters, the most efficient results for acetate production were obtained in films of (Cu) 2 ,(Ag) 3 with a faradaic efficiency of 21.2% for acetate from CO 2 at −1.33 V vs. reversible hydrogen electrode in 0.5 M KHCO 3 with 8 ppm of added benzotriazole at 0 °C.

Authors:
 [1];  [1]; ORCiD logo [2];  [1];  [1];  [1]
+ Show Author Affiliations
  1. Department of Chemistry, The University of North Carolina at Chapel Hill, Chapel Hill, NC 27599,
  2. Department of Chemistry and Biochemistry, Florida International University, Miami, FL 31199
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1414879
Alternate Identifier(s):
OSTI ID: 1470063
Grant/Contract Number:  
SC0001011
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 115 Journal Issue: 2; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; catalysis (homogeneous); catalysis (heterogeneous); solar (photovoltaic); solar (fuels); photosynthesis (natural and artificial); hydrogen and fuel cells, electrodes - solar; charge transport; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); CO2 reduction; electrocatalysis; electrodeposition; bimetallic nanoparticles; artificial photosynthesis

Citation Formats

Wang, Ying, Wang, Degao, Dares, Christopher J., Marquard, Seth L., Sheridan, Matthew V., and Meyer, Thomas J. CO 2 reduction to acetate in mixtures of ultrasmall (Cu) n ,(Ag) m bimetallic nanoparticles. United States: N. p., 2017. Web. doi:10.1073/pnas.1713962115.
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Wang, Ying, Wang, Degao, Dares, Christopher J., Marquard, Seth L., Sheridan, Matthew V., & Meyer, Thomas J. CO 2 reduction to acetate in mixtures of ultrasmall (Cu) n ,(Ag) m bimetallic nanoparticles. United States. https://doi.org/10.1073/pnas.1713962115
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Wang, Ying, Wang, Degao, Dares, Christopher J., Marquard, Seth L., Sheridan, Matthew V., and Meyer, Thomas J. Tue . "CO 2 reduction to acetate in mixtures of ultrasmall (Cu) n ,(Ag) m bimetallic nanoparticles". United States. https://doi.org/10.1073/pnas.1713962115.
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@article{osti_1414879,
title = {CO 2 reduction to acetate in mixtures of ultrasmall (Cu) n ,(Ag) m bimetallic nanoparticles},
author = {Wang, Ying and Wang, Degao and Dares, Christopher J. and Marquard, Seth L. and Sheridan, Matthew V. and Meyer, Thomas J.},
abstractNote = {Significance Efficient reduction of carbon dioxide to useful fuels and chemicals is an important research goal in artificial photosynthesis. Significant progress has been made for the C1 products, CO and HCOO − . We report here a procedure based on the use of ultrasmall, monodispersed Cu and Ag bimetallic nanoparticles on thin, electrochemically polymerized poly-Fe(vbpy) 3 (PF 6 ) 2 films. They reduce CO 2 to acetate at pH 7 in aqueous HCO 3 − solutions at relatively high efficiencies with significant rate enhancements with added benzotriazole. In the sequence of clusters, the most efficient results for acetate production were obtained in films of (Cu) 2 ,(Ag) 3 with a faradaic efficiency of 21.2% for acetate from CO 2 at −1.33 V vs. reversible hydrogen electrode in 0.5 M KHCO 3 with 8 ppm of added benzotriazole at 0 °C.},
doi = {10.1073/pnas.1713962115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 2,
volume = 115,
place = {United States},
year = {Tue Dec 26 00:00:00 EST 2017},
month = {Tue Dec 26 00:00:00 EST 2017}
}
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https://doi.org/10.1073/pnas.1713962115
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Works referenced in this record:

Formation of air-stable copper–silver core–shell nanoparticles for inkjet printing
journal, January 2009

  • Grouchko, Michael; Kamyshny, Alexander; Magdassi, Shlomo
  • Journal of Materials Chemistry, Vol. 19, Issue 19
  • DOI: 10.1039/b821327e

Nanostructured Tin Catalysts for Selective Electrochemical Reduction of Carbon Dioxide to Formate
journal, January 2014

  • Zhang, Sheng; Kang, Peng; Meyer, Thomas J.
  • Journal of the American Chemical Society, Vol. 136, Issue 5
  • DOI: 10.1021/ja4113885

Efficient Conversion of CO 2 to CO Using Tin and Other Inexpensive and Easily Prepared Post-Transition Metal Catalysts
journal, April 2015

  • Medina-Ramos, Jonnathan; Pupillo, Rachel C.; Keane, Thomas P.
  • Journal of the American Chemical Society, Vol. 137, Issue 15
  • DOI: 10.1021/ja5121088

Noncovalent Immobilization of a Molecular Iron-Based Electrocatalyst on Carbon Electrodes for Selective, Efficient CO 2 -to-CO Conversion in Water
journal, February 2016

  • Maurin, Antoine; Robert, Marc
  • Journal of the American Chemical Society, Vol. 138, Issue 8
  • DOI: 10.1021/jacs.5b12652

Single catalyst electrocatalytic reduction of CO 2 in water to H 2 +CO syngas mixtures with water oxidation to O 2
journal, January 2014

  • Kang, Peng; Chen, Zuofeng; Nayak, Animesh
  • Energy Environ. Sci., Vol. 7, Issue 12
  • DOI: 10.1039/C4EE01904K

Manganese Electrocatalysts with Bulky Bipyridine Ligands: Utilizing Lewis Acids To Promote Carbon Dioxide Reduction at Low Overpotentials
journal, January 2016

  • Sampson, Matthew D.; Kubiak, Clifford P.
  • Journal of the American Chemical Society, Vol. 138, Issue 4
  • DOI: 10.1021/jacs.5b12215

Electrochemical CO2 Reduction on Metal Electrodes
book, January 2008

Design of Alloy Electrocatalysts for CO[sub 2] Reduction
journal, January 1991

  • Watanabe, Masahiro
  • Journal of The Electrochemical Society, Vol. 138, Issue 11
  • DOI: 10.1149/1.2085417

Electrodeposition of monodisperse copper nanoparticles on highly oriented pyrolytic graphite electrode with modulation potential method
journal, July 2005

  • Huang, Ling; Lee, Eun-Sung; Kim, Kwang-Bum
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 262, Issue 1-3
  • DOI: 10.1016/j.colsurfa.2005.03.023

Understanding Voltammetry
book, December 2011

  • Compton, Richard G.; Batchelor-McAuley, Christopher; Dickinson, Edmund J. F.
  • DOI: 10.1142/p783

XPS study of the Cu@Cu2O core-shell nanoparticles
journal, December 2008

Binding and Reduction of Silver Ions in Thin Polymeric Films of poly-[Fe(vbpy)2(CN)2],poly-vbpy
journal, August 1994

  • Bakir, Mohammed; MacKay, Susan G.; Linton, Richard W.
  • Inorganic Chemistry, Vol. 33, Issue 18
  • DOI: 10.1021/ic00096a019

Photoelectrochemical Reduction of CO 2 Coupled to Water Oxidation Using a Photocathode with a Ru(II)–Re(I) Complex Photocatalyst and a CoO x /TaON Photoanode
journal, October 2016

  • Sahara, Go; Kumagai, Hiromu; Maeda, Kazuhiko
  • Journal of the American Chemical Society, Vol. 138, Issue 42
  • DOI: 10.1021/jacs.6b09212

Particle Size Effects in the Catalytic Electroreduction of CO 2 on Cu Nanoparticles
journal, May 2014

  • Reske, Rulle; Mistry, Hemma; Behafarid, Farzad
  • Journal of the American Chemical Society, Vol. 136, Issue 19
  • DOI: 10.1021/ja500328k

Efficient Electrochemical Reduction of Carbon Dioxide to Acetate on Nitrogen-Doped Nanodiamond
journal, September 2015

  • Liu, Yanming; Chen, Shuo; Quan, Xie
  • Journal of the American Chemical Society, Vol. 137, Issue 36
  • DOI: 10.1021/jacs.5b02975

Mesoscopic Metal Particles and Wires by Electrodeposition
journal, April 2002

  • Penner, Reginald M.
  • The Journal of Physical Chemistry B, Vol. 106, Issue 13
  • DOI: 10.1021/jp013219o

Polyethylenimine-Enhanced Electrocatalytic Reduction of CO 2 to Formate at Nitrogen-Doped Carbon Nanomaterials
journal, May 2014

  • Zhang, Sheng; Kang, Peng; Ubnoske, Stephen
  • Journal of the American Chemical Society, Vol. 136, Issue 22
  • DOI: 10.1021/ja5031529

Cu(ii)/Cu(0) electrocatalyzed CO2 and H2O splitting
journal, January 2013

  • Chen, Zuofeng; Kang, Peng; Zhang, Ming-Tian
  • Energy & Environmental Science, Vol. 6, Issue 3
  • DOI: 10.1039/c3ee24487c

A sensitive nonenzymatic glucose sensor in alkaline media with a copper nanocluster/multiwall carbon nanotube-modified glassy carbon electrode
journal, April 2007

Gold–Copper Nanoalloys Supported on TiO 2 as Photocatalysts for CO 2 Reduction by Water
journal, October 2014

  • Neaţu, Ştefan; Maciá-Agulló, Juan Antonio; Concepción, Patricia
  • Journal of the American Chemical Society, Vol. 136, Issue 45
  • DOI: 10.1021/ja506433k

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

  • Zhu, Wenlei; Michalsky, Ronald; Metin, Önder
  • Journal of the American Chemical Society, Vol. 135, Issue 45
  • DOI: 10.1021/ja409445p

Active and Selective Conversion of CO 2 to CO on Ultrathin Au Nanowires
journal, November 2014

  • Zhu, Wenlei; Zhang, Yin-Jia; Zhang, Hongyi
  • Journal of the American Chemical Society, Vol. 136, Issue 46
  • DOI: 10.1021/ja5095099

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

  • Peterson, Andrew A.; Nørskov, Jens K.
  • The Journal of Physical Chemistry Letters, Vol. 3, Issue 2
  • DOI: 10.1021/jz201461p

Highly electrocatalytic reduction of nitrite ions on a copper nanoparticles thin film
journal, April 2009

  • Ko, Wen-Yin; Chen, Wei-Hung; Cheng, Ching-Yuan
  • Sensors and Actuators B: Chemical, Vol. 137, Issue 2
  • DOI: 10.1016/j.snb.2009.01.014

Photochemical and Photoelectrochemical Reduction of CO 2
journal, May 2012

Surfactant-free preparation of supported cubic platinum nanoparticles
journal, January 2012

  • Peng, Zhenmeng; Kisielowski, Christian; Bell, Alexis T.
  • Chemical Communications, Vol. 48, Issue 13
  • DOI: 10.1039/c2cc16962b

Nickel/Copper nanoparticles modified TiO2 nanotubes for non-enzymatic glucose biosensors
journal, May 2013

CO 2 Capture by a Rhenium(I) Complex with the Aid of Triethanolamine
journal, October 2013

  • Morimoto, Tatsuki; Nakajima, Takuya; Sawa, Shuhei
  • Journal of the American Chemical Society, Vol. 135, Issue 45
  • DOI: 10.1021/ja409271s

An unconventional pathway for reduction of CO2 to methane in CO-grown Methanosarcina acetivorans revealed by proteomics
journal, November 2006

  • Lessner, D. J.; Li, L.; Li, Q.
  • Proceedings of the National Academy of Sciences, Vol. 103, Issue 47
  • DOI: 10.1073/pnas.0608833103

Artificial Z-Scheme Constructed with a Supramolecular Metal Complex and Semiconductor for the Photocatalytic Reduction of CO 2
journal, March 2013

  • Sekizawa, Keita; Maeda, Kazuhiko; Domen, Kazunari
  • Journal of the American Chemical Society, Vol. 135, Issue 12
  • DOI: 10.1021/ja311541a

Photoelectrochemical CO 2 Reduction to Acetate on Iron–Copper Oxide Catalysts
journal, December 2016

New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces
journal, January 2012

  • Kuhl, Kendra P.; Cave, Etosha R.; Abram, David N.
  • Energy & Environmental Science, Vol. 5, Issue 5
  • DOI: 10.1039/c2ee21234j

Self-assembly of acetate adsorbates drives atomic rearrangement on the Au(110) surface
journal, October 2016

  • Hiebel, Fanny; Shong, Bonggeun; Chen, Wei
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13139

Electrochemical Synthesis of Silver Nanoparticles under Protection of Poly( N -vinylpyrrolidone)
journal, August 2003

  • Yin, Bingsheng; Ma, Houyi; Wang, Shuyun
  • The Journal of Physical Chemistry B, Vol. 107, Issue 34
  • DOI: 10.1021/jp0349031

Electrocatalytic Reduction of Carbon Dioxide: Let the Molecules Do the Work
journal, November 2014

Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane
journal, December 2015

  • Zhang, Sheng; Kang, Peng; Bakir, Mohammed
  • Proceedings of the National Academy of Sciences, Vol. 112, Issue 52
  • DOI: 10.1073/pnas.1522496112

Electrochemical Reduction of Carbon Dioxide on Various Metal Electrodes in Low-Temperature Aqueous KHCO3 Media
journal, January 1990

  • Azuma, Masashi; Hashimoto, Kazuhito; Hiramoto, Masahiro
  • Journal of The Electrochemical Society, Vol. 137, Issue 6, p. 1772-1778
  • DOI: 10.1149/1.2086796

Tuning the Selectivity of Carbon Dioxide Electroreduction toward Ethanol on Oxide-Derived Cu x Zn Catalysts
journal, November 2016

Probing the Active Surface Sites for CO Reduction on Oxide-Derived Copper Electrocatalysts
journal, July 2015

  • Verdaguer-Casadevall, Arnau; Li, Christina W.; Johansson, Tobias P.
  • Journal of the American Chemical Society, Vol. 137, Issue 31
  • DOI: 10.1021/jacs.5b06227

Controlling the Thickness of the Surface Oxide Layer on Cu Nanoparticles for the Fabrication of Conductive Structures by Ink-Jet Printing
journal, March 2008

  • Jeong, Sunho; Woo, Kyoohee; Kim, Dongjo
  • Advanced Functional Materials, Vol. 18, Issue 5
  • DOI: 10.1002/adfm.200700902

Recognition of dimethoate carried by bi-layer electrodeposition of silver nanoparticles and imprinted poly-o-phenylenediamine
journal, September 2008

Synthetic and mechanistic investigations of the reductive electrochemical polymerization of vinyl-containing complexes of iron(II), ruthenium(II), and osmium(II)
journal, July 1983

  • Calvert, Jeffrey M.; Schmehl, Russell H.; Sullivan, B. Patrick
  • Inorganic Chemistry, Vol. 22, Issue 15
  • DOI: 10.1021/ic00157a013

One-step electrosynthesis of ethylene and ethanol from CO2 in an alkaline electrolyzer
journal, January 2016

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