Chemical-Dealloying-Derived PtPdPb-Based Multimetallic Nanoparticles: Dimethyl Ether Electrocatalysis and Fuel Cell Application

Medhanie Gebremedhin Gebru; Palaniappan Subramanian; Petr Bělský; Radhey Shyam Yadav; Itay Pitussi; Sarath Sasi; Rostislav Medlín; Jan Minar; Peter Švec; Haya Kornweitz; Alex Schechter

doi:10.1021/acsami.3c11003

Chemical-Dealloying-Derived PtPdPb-Based Multimetallic Nanoparticles: Dimethyl Ether Electrocatalysis and Fuel Cell Application

Medhanie Gebremedhin Gebru, Palaniappan Subramanian, Petr Bělský, Radhey Shyam Yadav, Itay Pitussi, Sarath Sasi, Rostislav Medlín, Jan Minar, Peter Švec, Haya Kornweitz, Alex Schechter

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5 Scopus citations

Abstract

In this work, we report a novel multimetallic nanoparticle catalyst composed of Pt, Pd, and Pb and its electrochemical activity toward dimethyl ether (DME) oxidation in liquid electrolyte and polymer electrolyte fuel cells. Chemical dealloying of the catalyst with the lowest platinum-group metal (PGM) content, Pt₂PdPb₂/C, was conducted using HNO₃ to tune the catalyst activity. Comprehensive characterization of the chemical-dealloying-derived catalyst nanoparticles unambiguously showed that the acid treatment removed 50% Pb from the nanoparticles with an insignificant effect on the PGM metals and led to the formation of smaller-sized nanoparticles. Electrochemical studies showed that Pb dissolution led to structural changes in the original catalysts. Chemical-dealloying-derived catalyst nanoparticles made of multiple phases (Pt, Pt₃Pb, PtPb) provided one of the highest PGM-normalized power densities of 118 mW mg_PGM^-1 in a single direct DME fuel cell operated at low anode catalyst loading (1 mg_PGM cm^-2) at 70 °C. A possible DME oxidation pathway for these multimetallic catalysts was proposed based on an online mass spectrometry study and the analysis of the reaction products.

Original language	English
Journal	ACS Applied Materials and Interfaces
Early online date	30 Nov 2023
DOIs	https://doi.org/10.1021/acsami.3c11003
State	E-pub ahead of print - 30 Nov 2023
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society

Funding

A.S. and M.G.G. would like to acknowledge Ariel University and Israel National Research Center for Electrochemical Propulsion (INREP) for financially supporting this research. R.S.Y., I.P., and H.K. acknowledge the Ariel HPC Center at Ariel University for providing the computing resources. P.S., S.S., R.M., and J.M. would like to acknowledge the support of the Quantum materials for applications in sustainable technologies (QM4ST), reg. no. CZ.02.01.01/00/22_008/0004572 by Programme Johannes Amos Comenius, call Excellent Research at the New Technologies Research Center, University of West Bohemia, Pilsen. P.Š. acknowledges the support from projects APVV-19-0369 and VEGA 2/0144/21.

Funders	Funder number
Ariel University and Israel National Research Center for Electrochemical Propulsion
Vedecká Grantová Agentúra MŠVVaŠ SR a SAV	2/0144/21
Israel National Research Center for Electrochemical Propulsion	APVV-19-0369

Keywords

chemical dealloying
dimethyl ether
fuel cell
online mass spectrometry
oxidation pathway

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10.1021/acsami.3c11003

Cite this

Gebru, M. G., Subramanian, P., Bělský, P., Yadav, R. S., Pitussi, I., Sasi, S., Medlín, R., Minar, J., Švec, P., Kornweitz, H., & Schechter, A. (2023). Chemical-Dealloying-Derived PtPdPb-Based Multimetallic Nanoparticles: Dimethyl Ether Electrocatalysis and Fuel Cell Application. ACS Applied Materials and Interfaces. Advance online publication. https://doi.org/10.1021/acsami.3c11003

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abstract = "In this work, we report a novel multimetallic nanoparticle catalyst composed of Pt, Pd, and Pb and its electrochemical activity toward dimethyl ether (DME) oxidation in liquid electrolyte and polymer electrolyte fuel cells. Chemical dealloying of the catalyst with the lowest platinum-group metal (PGM) content, Pt2PdPb2/C, was conducted using HNO3 to tune the catalyst activity. Comprehensive characterization of the chemical-dealloying-derived catalyst nanoparticles unambiguously showed that the acid treatment removed 50% Pb from the nanoparticles with an insignificant effect on the PGM metals and led to the formation of smaller-sized nanoparticles. Electrochemical studies showed that Pb dissolution led to structural changes in the original catalysts. Chemical-dealloying-derived catalyst nanoparticles made of multiple phases (Pt, Pt3Pb, PtPb) provided one of the highest PGM-normalized power densities of 118 mW mgPGM-1 in a single direct DME fuel cell operated at low anode catalyst loading (1 mgPGM cm-2) at 70 °C. A possible DME oxidation pathway for these multimetallic catalysts was proposed based on an online mass spectrometry study and the analysis of the reaction products.",

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AU - Gebru, Medhanie Gebremedhin

AU - Subramanian, Palaniappan

AU - Bělský, Petr

AU - Yadav, Radhey Shyam

AU - Pitussi, Itay

AU - Sasi, Sarath

AU - Medlín, Rostislav

AU - Minar, Jan

AU - Švec, Peter

AU - Kornweitz, Haya

AU - Schechter, Alex

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N2 - In this work, we report a novel multimetallic nanoparticle catalyst composed of Pt, Pd, and Pb and its electrochemical activity toward dimethyl ether (DME) oxidation in liquid electrolyte and polymer electrolyte fuel cells. Chemical dealloying of the catalyst with the lowest platinum-group metal (PGM) content, Pt2PdPb2/C, was conducted using HNO3 to tune the catalyst activity. Comprehensive characterization of the chemical-dealloying-derived catalyst nanoparticles unambiguously showed that the acid treatment removed 50% Pb from the nanoparticles with an insignificant effect on the PGM metals and led to the formation of smaller-sized nanoparticles. Electrochemical studies showed that Pb dissolution led to structural changes in the original catalysts. Chemical-dealloying-derived catalyst nanoparticles made of multiple phases (Pt, Pt3Pb, PtPb) provided one of the highest PGM-normalized power densities of 118 mW mgPGM-1 in a single direct DME fuel cell operated at low anode catalyst loading (1 mgPGM cm-2) at 70 °C. A possible DME oxidation pathway for these multimetallic catalysts was proposed based on an online mass spectrometry study and the analysis of the reaction products.

AB - In this work, we report a novel multimetallic nanoparticle catalyst composed of Pt, Pd, and Pb and its electrochemical activity toward dimethyl ether (DME) oxidation in liquid electrolyte and polymer electrolyte fuel cells. Chemical dealloying of the catalyst with the lowest platinum-group metal (PGM) content, Pt2PdPb2/C, was conducted using HNO3 to tune the catalyst activity. Comprehensive characterization of the chemical-dealloying-derived catalyst nanoparticles unambiguously showed that the acid treatment removed 50% Pb from the nanoparticles with an insignificant effect on the PGM metals and led to the formation of smaller-sized nanoparticles. Electrochemical studies showed that Pb dissolution led to structural changes in the original catalysts. Chemical-dealloying-derived catalyst nanoparticles made of multiple phases (Pt, Pt3Pb, PtPb) provided one of the highest PGM-normalized power densities of 118 mW mgPGM-1 in a single direct DME fuel cell operated at low anode catalyst loading (1 mgPGM cm-2) at 70 °C. A possible DME oxidation pathway for these multimetallic catalysts was proposed based on an online mass spectrometry study and the analysis of the reaction products.

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Chemical-Dealloying-Derived PtPdPb-Based Multimetallic Nanoparticles: Dimethyl Ether Electrocatalysis and Fuel Cell Application

Abstract

Bibliographical note

Funding

Keywords

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