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Elucidating the role of Ni to enhance the methanol oxidation reaction on Pd electrocatalysts
Stockholm Univ, AlbaNova Univ Ctr, FYSIKUM, SE-10691 Stockholm, Sweden..
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemical Engineering, Applied Electrochemistry. Univ Warwick, Dept Chem, Coventry CV4 7AL, W Midlands, England..ORCID iD: 0000-0002-9385-7577
Stockholm Univ, AlbaNova Univ Ctr, FYSIKUM, SE-10691 Stockholm, Sweden..
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemical Engineering, Applied Electrochemistry.ORCID iD: 0000-0001-5816-2924
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2020 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 360, article id 136954Article in journal (Refereed) Published
Abstract [en]

Amongst promising available technologies enabling the transition to renewable energy sources, electrochemical oxidation of alcohols, in a direct fuel cell or in an electrolysis reaction (H-2 production), can be an economically and sustainable alternative to currently used technologies. In this work, we highlight the advantages of a Pd-Ni bimetallic electrocatalyst for methanol electrooxidation - a convenient choice due to the low cost of Ni combined with the observed acceptable catalytic performance of Pd. We report a synergistic effort between experiments and theoretical calculations based on density functional theory to provide an in-depth understanding - at the atomistic level - of the origin of the enhanced electrochemical activity of methanol electrooxidation using the bimetallic catalysts Pd3Ni and PdNi over pure Pd. Cyclic voltammograms and High-Performance Liquid Chromatography (HPLC) demonstrate higher activity towards methanol electrooxidation with increased Ni concentration and, furthermore, higher selectivity for CO2. These effects are understood by: 1) changes in the methanol oxidation reaction mechanism. 2) Mitigation or suppression of CO poisoning on the Pd-Ni alloys as compared to the pure Pd catalyst. 3) A stronger tendency towards highly oxidized intermediates for the alloys. These findings elucidate the effects of a bimetallic electrocatalyst for alcohol electrooxidation as well as unambiguously suggest PdNi as a more cost-effective alternative electrocatalyst.

Place, publisher, year, edition, pages
Elsevier BV , 2020. Vol. 360, article id 136954
Keywords [en]
Electrocatalysis, Methanol oxidation, Density functional theory, Pd catalyst, Energy conversion
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-285719DOI: 10.1016/j.electacta.2020.136954ISI: 000576817900004Scopus ID: 2-s2.0-85090219872OAI: oai:DiVA.org:kth-285719DiVA, id: diva2:1504096
Note

QC 20201126

Available from: 2020-11-26 Created: 2020-11-26 Last updated: 2022-06-25Bibliographically approved

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Martín-Yerga, DanielCornell, Ann M.

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