Microwave-Assisted Synthesis of Pt-Au Nanoparticles with Enhanced Electrocatalytic Activity for the Oxidation of Formic Acid

Gema Cabello, Rogerio A. Davoglio, Fabian W. Hartl, Jose F. Marco, Ernesto C. Pereira, Sonia R. Biaggio, Hamilton Varela, Angel Cuesta

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Abstract

We report the microwave-assisted hydrothermal synthesis of bimetallic Pt-Au nanoparticles with different Pt/Au mole ratio, and investigate their performance towards the electro-oxidation of formic acid. The as-synthesized Pt-Au sol was dispersed on a graphite electrode, without any binding agents, which allowed us to control the mass of alloy deposited. Pt-Au alloys showed better activity than bulk Pt and/or Pt nanoparticles towards the oxidation of formic acid, as evidenced by the decrease in the onset potential and the higher currents in the corresponding cyclic voltammograms. The higher activity is due both to atomic-ensemble effects, which lead the reaction through the so-called direct pathway with insignificant CO poisoning, and to electronic effects, which optimised the interaction between the catalyst surface and the reactive intermediate in the direct path. Further insight into the individual contributions of atomic-ensemble and electronic effects and their effect on the catalytic activity was provided by the analysis of galvanostatic potential oscillations.
Original languageEnglish
Pages (from-to)56-63
Number of pages8
JournalElectrochimica Acta
Volume224
Early online date7 Dec 2016
DOIs
Publication statusPublished - 10 Jan 2017

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formic acid
Formic acid
Thermodynamic properties
Microwaves
Nanoparticles
Oxidation
Graphite electrodes
Electrooxidation
Hydrothermal synthesis
Polymethyl Methacrylate
Carbon Monoxide
Sols
Catalyst activity
Catalysts

Keywords

  • PtAu alloy
  • electrocatalysis
  • formic acid oxidation
  • microwave hydrothermal synthesis
  • potential oscillators

Cite this

Microwave-Assisted Synthesis of Pt-Au Nanoparticles with Enhanced Electrocatalytic Activity for the Oxidation of Formic Acid. / Cabello, Gema; Davoglio, Rogerio A.; Hartl, Fabian W.; Marco, Jose F.; Pereira, Ernesto C.; Biaggio, Sonia R.; Varela, Hamilton; Cuesta, Angel.

In: Electrochimica Acta, Vol. 224, 10.01.2017, p. 56-63.

Research output: Contribution to journalArticle

Cabello, Gema ; Davoglio, Rogerio A. ; Hartl, Fabian W. ; Marco, Jose F. ; Pereira, Ernesto C. ; Biaggio, Sonia R. ; Varela, Hamilton ; Cuesta, Angel. / Microwave-Assisted Synthesis of Pt-Au Nanoparticles with Enhanced Electrocatalytic Activity for the Oxidation of Formic Acid. In: Electrochimica Acta. 2017 ; Vol. 224. pp. 56-63.
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title = "Microwave-Assisted Synthesis of Pt-Au Nanoparticles with Enhanced Electrocatalytic Activity for the Oxidation of Formic Acid",
abstract = "We report the microwave-assisted hydrothermal synthesis of bimetallic Pt-Au nanoparticles with different Pt/Au mole ratio, and investigate their performance towards the electro-oxidation of formic acid. The as-synthesized Pt-Au sol was dispersed on a graphite electrode, without any binding agents, which allowed us to control the mass of alloy deposited. Pt-Au alloys showed better activity than bulk Pt and/or Pt nanoparticles towards the oxidation of formic acid, as evidenced by the decrease in the onset potential and the higher currents in the corresponding cyclic voltammograms. The higher activity is due both to atomic-ensemble effects, which lead the reaction through the so-called direct pathway with insignificant CO poisoning, and to electronic effects, which optimised the interaction between the catalyst surface and the reactive intermediate in the direct path. Further insight into the individual contributions of atomic-ensemble and electronic effects and their effect on the catalytic activity was provided by the analysis of galvanostatic potential oscillations.",
keywords = "PtAu alloy, electrocatalysis, formic acid oxidation, microwave hydrothermal synthesis, potential oscillators",
author = "Gema Cabello and Davoglio, {Rogerio A.} and Hartl, {Fabian W.} and Marco, {Jose F.} and Pereira, {Ernesto C.} and Biaggio, {Sonia R.} and Hamilton Varela and Angel Cuesta",
note = "Conselho Nacional de Desenvolvimento Cient{\'i}fico e Tecnol{\'o}gico (CNPq) is gratefully acknowledged for financial support under Research Project BJT-2014/400117/2014-2 and for the research support (HV: grant #306151/2010-3). Funda{\cc}{\~a}o de Amparo {\`a} Pesquisa do Estado de S{\~a}o Paulo (FAPESP) is also acknowledged for financial support (grants #2013/07296-2 and #2013/16930-7), and scholarship (FWH: grant #2014/08030-9). GC gratefully acknowledges R. Camargo for his collaboration in the acquisition of the HR-TEM images and for useful discussion and suggestions.",
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T1 - Microwave-Assisted Synthesis of Pt-Au Nanoparticles with Enhanced Electrocatalytic Activity for the Oxidation of Formic Acid

AU - Cabello, Gema

AU - Davoglio, Rogerio A.

AU - Hartl, Fabian W.

AU - Marco, Jose F.

AU - Pereira, Ernesto C.

AU - Biaggio, Sonia R.

AU - Varela, Hamilton

AU - Cuesta, Angel

N1 - Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq) is gratefully acknowledged for financial support under Research Project BJT-2014/400117/2014-2 and for the research support (HV: grant #306151/2010-3). Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP) is also acknowledged for financial support (grants #2013/07296-2 and #2013/16930-7), and scholarship (FWH: grant #2014/08030-9). GC gratefully acknowledges R. Camargo for his collaboration in the acquisition of the HR-TEM images and for useful discussion and suggestions.

PY - 2017/1/10

Y1 - 2017/1/10

N2 - We report the microwave-assisted hydrothermal synthesis of bimetallic Pt-Au nanoparticles with different Pt/Au mole ratio, and investigate their performance towards the electro-oxidation of formic acid. The as-synthesized Pt-Au sol was dispersed on a graphite electrode, without any binding agents, which allowed us to control the mass of alloy deposited. Pt-Au alloys showed better activity than bulk Pt and/or Pt nanoparticles towards the oxidation of formic acid, as evidenced by the decrease in the onset potential and the higher currents in the corresponding cyclic voltammograms. The higher activity is due both to atomic-ensemble effects, which lead the reaction through the so-called direct pathway with insignificant CO poisoning, and to electronic effects, which optimised the interaction between the catalyst surface and the reactive intermediate in the direct path. Further insight into the individual contributions of atomic-ensemble and electronic effects and their effect on the catalytic activity was provided by the analysis of galvanostatic potential oscillations.

AB - We report the microwave-assisted hydrothermal synthesis of bimetallic Pt-Au nanoparticles with different Pt/Au mole ratio, and investigate their performance towards the electro-oxidation of formic acid. The as-synthesized Pt-Au sol was dispersed on a graphite electrode, without any binding agents, which allowed us to control the mass of alloy deposited. Pt-Au alloys showed better activity than bulk Pt and/or Pt nanoparticles towards the oxidation of formic acid, as evidenced by the decrease in the onset potential and the higher currents in the corresponding cyclic voltammograms. The higher activity is due both to atomic-ensemble effects, which lead the reaction through the so-called direct pathway with insignificant CO poisoning, and to electronic effects, which optimised the interaction between the catalyst surface and the reactive intermediate in the direct path. Further insight into the individual contributions of atomic-ensemble and electronic effects and their effect on the catalytic activity was provided by the analysis of galvanostatic potential oscillations.

KW - PtAu alloy

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KW - microwave hydrothermal synthesis

KW - potential oscillators

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JO - Electrochimica Acta

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