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dc.contributor.author
Dey, Subal
dc.contributor.author
Masero, Fabio
dc.contributor.author
Brack, Enzo
dc.contributor.author
Fontecave, Marc
dc.contributor.author
Mougel, Victor
dc.date.accessioned
2022-02-14T14:30:58Z
dc.date.available
2022-01-10T15:20:46Z
dc.date.available
2022-02-14T14:30:58Z
dc.date.issued
2021-07-06
dc.identifier.issn
2573-2293
dc.identifier.other
10.33774/chemrxiv-2021-18tth
en_US
dc.identifier.uri
http://hdl.handle.net/20.500.11850/524340
dc.identifier.doi
10.3929/ethz-b-000524340
dc.description.abstract
The electrochemical generation of metal hydride (M H) species remains one of the major hurdles for a wide range of catalytic reactions to be carried out electrochemically. We introduce here a new strategy for electrocatalytic M H generation using concerted proton electron transfer (CPET) mediators. We investigate the combination of a series of CPET mediators with the CO2 electroreduction catalyst [MnI(bpy)(CO)3Br] (bpy = 2,2’-bipyridine), probing the reversal of the product selectivity from CO to HCOOH to evaluate the efficiency of the M H generation step. We demonstrate the formation of the manganese-hydride by in-situ spectroscopic techniques and determine the thermodynamic boundary conditions for this mechanism to occur. A synthetic iron-sulfur cluster is identified as the best CPET-mediator for that system, enabling the preparation of a benchmark catalytic system for HCOOH generation.
en_US
dc.format
application/pdf
en_US
dc.language.iso
en
en_US
dc.publisher
Cambridge University Press
en_US
dc.rights.uri
http://creativecommons.org/licenses/by-nc-nd/4.0/
dc.title
Electrocatalytic metal hydride generation using concerted proton electron transfer mediators
en_US
dc.type
Working Paper
dc.rights.license
Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International
ethz.journal.title
ChemRxiv
ethz.size
14 p.
en_US
ethz.grant
Hybrid Electrocatalysts Inspired by the Nitrogenase Enzyme
en_US
ethz.grant
Molecules and materials for tandem electroreduction of N2 and CO2 to complex molecules
en_US
ethz.publication.place
Cambridge
en_US
ethz.publication.status
published
en_US
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02513 - Laboratorium für Anorganische Chemie / Laboratory of Inorganic Chemistry::09654 - Mougel, Victor / Mougel, Victor
en_US
ethz.leitzahl.certified
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02513 - Laboratorium für Anorganische Chemie / Laboratory of Inorganic Chemistry::09654 - Mougel, Victor / Mougel, Victor
en_US
ethz.grant.agreementno
853064
ethz.grant.agreementno
197153
ethz.grant.fundername
EC
ethz.grant.fundername
SNF
ethz.grant.funderDoi
10.13039/501100000780
ethz.grant.funderDoi
10.13039/501100001711
ethz.grant.program
H2020
ethz.grant.program
Projekte MINT
ethz.date.deposited
2022-01-10T15:20:52Z
ethz.source
FORM
ethz.eth
yes
en_US
ethz.availability
Open access
en_US
ethz.rosetta.installDate
2022-02-14T14:31:07Z
ethz.rosetta.lastUpdated
2024-02-02T16:19:35Z
ethz.rosetta.versionExported
true
ethz.COinS
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