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Source of magnetic field effects on the electrocatalytic reduction of CO2

Abstract:
We present an analysis of reported magnetic field effects on the yield of formic acid produced by electrocatalytic reduction of carbon dioxide at a nanoparticle tin electrode (Pan et al., J. Phys. Chem. Lett. 11 (2020) 48–53). Radical pair spin dynamics simulations are used to show that: (1) the g mechanism favoured by Pan et al. is not sufficient to explain the observed magneto-current. (2) Field-dependent spin relaxation, resulting from the anisotropy of the g-tensor of CO2  , combined with the coherent singlet-triplet interconversion arising from isotropic hyperfine and Zeeman interactions, can quantitatively account for the observed magnetic field effect. (3) Modification of hyperfine interactions by isotopic substitution (1H  2H and/or 12C  13C) could be used to test both the proposed reaction mechanism and the interpretation presented here.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1063/5.0021643

Authors

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Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Physical & Theoretical Chem
Role:
Author
ORCID:
0000-0001-5901-1722
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Physical & Theoretical Chem
Role:
Author
ORCID:
0000-0002-8863-570X


Publisher:
AIP Publishing
Journal:
Journal of Chemical Physics More from this journal
Volume:
153
Issue:
2020
Article number:
084303
Publication date:
2020-08-24
Acceptance date:
2020-08-05
DOI:
EISSN:
1089-7690
ISSN:
0021-9606


Language:
english
Keywords:
Pubs id:
1123774
Local pid:
pubs:1123774
Deposit date:
2020-08-06
ARK identifier:

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