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  The oxygen reduction reaction on palladium with low metal loadings: The effects of chlorides on the stability and activity towards hydrogen peroxide

Fortunato, G. V., Pizzutilo, E., Cardoso, E. S. F., Lanza, M. R., Katsounaros, I., Freakley, S. J., et al. (2020). The oxygen reduction reaction on palladium with low metal loadings: The effects of chlorides on the stability and activity towards hydrogen peroxide. Journal of Catalysis, 389, 400-408. doi:10.1016/j.jcat.2020.06.019.

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Fortunato, Guilherme Vilalba1, 2, 3, Author           
Pizzutilo, Enrico1, Author           
Cardoso, Eduardo S. F.2, Author           
Lanza, , Marcos R.V.3, Author
Katsounaros, Ioannis4, Author           
Freakley, Simon J.5, Author           
Mayrhofer, Karl Johann Jakob1, 6, 7, Author           
Maia, Gilberto2, Author           
Ledendecker, Marc1, 8, Author           
1Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society, ou_1863354              
2Institute of Chemistry, Universidade Federal de Mato Grosso Do sul, Av. Senador Filinto Muller, 1555, Campo Grande MS, Brazil, ou_persistent22              
3Institute of Chemistry of São Carlos, Universidade de São Paulo, Avenida Trabalhador São-Carlense 400, São Carlos, SP 13566-590, Brazil, ou_persistent22              
4Forschungszentrum Jülich, Helmholtz-Institute Erlangen-Nürnberg for Renewable Energy (IEK-11), Egerlandstr. 3, 91058 Erlangen, Germany, ou_persistent22              
5Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, U.K., ou_persistent22              
6Helmholtz-Institute Erlangen-Nuremberg for Renewable Energy (IEK-11), Forschungszentrum Jülich, Egerlandstrasse 3, 91058 Erlangen, Germany, ou_persistent22              
7Department of Chemical and Biological Engineering, Friedrich-Alexander-Universität Erlangen-Nürnberg, 91058 Erlangen, Germany, ou_persistent22              
8Department of Technical Chemistry, Technical University Darmstadt, 64287 Darmstadt, Germany, ou_persistent22              


Free keywords: Catalyst selectivity; Chlorine compounds; Electrocatalysts; Electrodes; Electrolytic reduction; Graphene nanoribbon; High resolution transmission electron microscopy; Hydrogen peroxide; Ketones; Nanoribbons; Oxidation; Oxygen reduction reaction; Palladium; Peroxides, Accelerated stress; Catalyst degradation; Catalysts oxidation; Commodity chemicals; Graphene nanoribbons; Noble metal loading; Production methods; Rotating ring-disk electrode, Molecular oxygen
 Abstract: Hydrogen peroxide is considered one of the most important commodity chemicals worldwide but its main production method, the anthraquinone process, poses serious logistical, environmental and safety challenges. Electrocatalytic synthesis through the reduction of molecular oxygen is a promising H2O2 production route. However, the reduction of molecular oxygen is kinetically hindered and stable electrocatalysts with a high activity and selectivity towards the 2-electron transfer reaction are needed. In this work, we evaluated the influence of chloride on catalysts with low palladium loadings on the ORR selectivity towards H2O2. We report the factors and dynamics that influence H2O2 production and highlight synthesis strategies to obtain close to 100 selectivity. By probing the electrode surface after various degradation cycles, we evaluate the role of adsorbing species and the catalysts oxidation states on the hydrogen peroxide selectivity. We systematically modified the catalyst synthesis using different Pd-precursors that were reduced and supported on high surface area graphene nanoribbons. Identical location transmission electron microscopy was used to probe catalyst dynamics during reaction and the activities and selectivities were measured by a rotating ring disk electrode. We probe the potential boundary conditions that lead to catalyst degradation during accelerated stress tests and potentiostatic polarisation and demonstrate how the catalytically active surface can be revived after degradation. The obtained insights can be used as guideline for the development of active, selective and stable catalysts with low noble metal loadings. © 2020 Elsevier Inc.


Language(s): eng - English
 Dates: 2020-09
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: -
 Identifiers: DOI: 10.1016/j.jcat.2020.06.019
 Degree: -



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Title: Journal of Catalysis
  Abbreviation : J. Catal.
Source Genre: Journal
Publ. Info: Amsterdam : Elsevier
Pages: - Volume / Issue: 389 Sequence Number: - Start / End Page: 400 - 408 Identifier: ISSN: 0021-9517
CoNE: https://pure.mpg.de/cone/journals/resource/954922645027