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Improving the catalytic activity of Pt-Rh/C towards ethanol oxidation through the addition of Pb

Improving the catalytic activity of Pt-Rh/C towards ethanol oxidation through the addition of Pb
Improving the catalytic activity of Pt-Rh/C towards ethanol oxidation through the addition of Pb
This paper describes the effect of composition on the catalytic activity of carbon-supported Pt-Pb, Pt-Rh, and Pt-Rh-Pb catalysts towards ethanol oxidation in acid media. The catalysts were synthesised by a polyol reduction method and characterised using several experimental techniques, including X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray absorption near edge structure, and X-ray energy dispersive spectroscopy. The catalytic activity towards ethanol oxidation was evaluated by cyclic voltammetry, chronoamperometry, and in situ Fourier transform infrared spectroscopy (FTIR) experiments. XRD data indicate the presence of Pb in both alloyed and oxide forms. TEM images reveal nanoparticles well-dispersed on the carbon support, with spherical shapes and particle sizes around 2.0–6.5 nm. The Pt3RhPb/C catalyst showed the highest catalytic activity for ethanol oxidation, reaching current densities 6.0 times higher than the commercial Pt/C catalyst. The trimetallic catalyst showed the highest CO2 and acetic acid formation, explaining the higher current densities presented during cyclic voltammetry and chronoamperometry. Additionally, since the oxidation appears to follow a non-selective path, the role of Pb in the trimetallic catalyst is not related to driving the reaction towards the production of CO2. The improvement in catalytic activity occurred due to the synergy between the metals.
Bimetallic catalysts, Ethanol oxidation reaction, FTIR, Fuel cells, Trimetallic catalysts
0013-4686
Almeida, Caio V.S.
718ae32a-23a1-4a8d-8248-a66d6f96f5fc
Huang, Haoliang
132a8eda-b800-4fa7-9583-6b4306f30247
Russell, Andrea E.
b6b7c748-efc1-4d5d-8a7a-8e4b69396169
Eguiluz, Katlin I.B.
59d40318-d101-44e0-b00c-b8f30aa1baf4
Salazar-Banda, Giancarlo R.
80800367-cb82-42ad-8137-83e98dbf4ecb
Almeida, Caio V.S.
718ae32a-23a1-4a8d-8248-a66d6f96f5fc
Huang, Haoliang
132a8eda-b800-4fa7-9583-6b4306f30247
Russell, Andrea E.
b6b7c748-efc1-4d5d-8a7a-8e4b69396169
Eguiluz, Katlin I.B.
59d40318-d101-44e0-b00c-b8f30aa1baf4
Salazar-Banda, Giancarlo R.
80800367-cb82-42ad-8137-83e98dbf4ecb

Almeida, Caio V.S., Huang, Haoliang, Russell, Andrea E., Eguiluz, Katlin I.B. and Salazar-Banda, Giancarlo R. (2022) Improving the catalytic activity of Pt-Rh/C towards ethanol oxidation through the addition of Pb. Electrochimica Acta, 431, [141089]. (doi:10.1016/j.electacta.2022.141089).

Record type: Article

Abstract

This paper describes the effect of composition on the catalytic activity of carbon-supported Pt-Pb, Pt-Rh, and Pt-Rh-Pb catalysts towards ethanol oxidation in acid media. The catalysts were synthesised by a polyol reduction method and characterised using several experimental techniques, including X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray absorption near edge structure, and X-ray energy dispersive spectroscopy. The catalytic activity towards ethanol oxidation was evaluated by cyclic voltammetry, chronoamperometry, and in situ Fourier transform infrared spectroscopy (FTIR) experiments. XRD data indicate the presence of Pb in both alloyed and oxide forms. TEM images reveal nanoparticles well-dispersed on the carbon support, with spherical shapes and particle sizes around 2.0–6.5 nm. The Pt3RhPb/C catalyst showed the highest catalytic activity for ethanol oxidation, reaching current densities 6.0 times higher than the commercial Pt/C catalyst. The trimetallic catalyst showed the highest CO2 and acetic acid formation, explaining the higher current densities presented during cyclic voltammetry and chronoamperometry. Additionally, since the oxidation appears to follow a non-selective path, the role of Pb in the trimetallic catalyst is not related to driving the reaction towards the production of CO2. The improvement in catalytic activity occurred due to the synergy between the metals.

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Accepted/In Press date: 23 August 2022
e-pub ahead of print date: 24 August 2022
Published date: 1 November 2022
Additional Information: Funding Information: The authors thank FAPITEC, FINEP, and the Brazilian National Council of Technological and Scientific Development-CNPq (grants: 305438/2018-2 and 311856/2019-5) for the financial support. This study was financed in part by the Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - Brazil (CAPES) - Finance Code 001. Additionally, we thank Diamond Light Source for instrument access on B18 (SP20354-1) and the station scientist Veronica Celorrio for her assistance. HH acknowledges fellowship support from the China Scholarship Council (201608440295) and the University of Southampton, and the Young Potential Program of Shanghai Institute of Applied Physics, Chinese Academy of Sciences. Funding Information: The authors thank FAPITEC, FINEP, and the Brazilian National Council of Technological and Scientific Development-CNPq (grants: 305438/2018-2 and 311856/2019-5) for the financial support. This study was financed in part by the Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - Brazil (CAPES) - Finance Code 001. Additionally, we thank Diamond Light Source for instrument access on B18 (SP20354-1) and the station scientist Veronica Celorrio for her assistance. HH acknowledges fellowship support from the China Scholarship Council (201608440295) and the University of Southampton, and the Young Potential Program of Shanghai Institute of Applied Physics, Chinese Academy of Sciences. Publisher Copyright: © 2022 Elsevier Ltd
Keywords: Bimetallic catalysts, Ethanol oxidation reaction, FTIR, Fuel cells, Trimetallic catalysts

Identifiers

Local EPrints ID: 469746
URI: http://eprints.soton.ac.uk/id/eprint/469746
ISSN: 0013-4686
PURE UUID: c7f68e5f-231f-4d8d-b90d-8dba2f22860d
ORCID for Andrea E. Russell: ORCID iD orcid.org/0000-0002-8382-6443

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Date deposited: 23 Sep 2022 17:14
Last modified: 17 Mar 2024 07:28

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Contributors

Author: Caio V.S. Almeida
Author: Haoliang Huang
Author: Katlin I.B. Eguiluz
Author: Giancarlo R. Salazar-Banda

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