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Critical appraisal on the role of catalysts for the oxygen reduction reaction in lithium-oxygen batteries

Critical appraisal on the role of catalysts for the oxygen reduction reaction in lithium-oxygen batteries
Critical appraisal on the role of catalysts for the oxygen reduction reaction in lithium-oxygen batteries
This work reports a detailed characterization of the reduction of oxygen in pyrrolidinium-based ionic liquids for application to lithium-oxygen batteries. It is found that, in the absence of Li+, all electron transfer kinetics are fast, and therefore, the reactions are limited by the mass transport rate. Reversible reduction of O2 to O2•- and O2•- to O22- take place at E0 = 2.1 V and 0.8 V vs. Li+/Li, respectively. In the presence of Li+, O2 is reduced to LiO2 first and then to Li2O2. The solubility product constant of Li2O2 is found to be around 10-51, corroborating the hypothesis that electrode passivation by Li2O2 deposition is an important issue that limits the capacity delivered by lithium-oxygen batteries. Enhancing the rate of Li2O2 formation by using different electrode materials would probably lead to faster electrode passivation and hence smaller charge due to oxygen reduction (smaller capacity of the battery). On the contrary, soluble redox catalysts can not only increase the reaction rate of Li2O2 formation but also avoid electrode passivation since the fast diffusion of the soluble redox catalyst would displace the formation of Li2O2 at a sufficient distance from the electrode surface
0013-4686
168-173
Lodge, Andrew W.
2612eca4-d8bd-4029-9ccc-19a54c22619a
Lacey, Matthew J.
d474e53b-ac9c-4e75-abe9-cdd1d9d549b0
Fitt, Matthew
d608a73e-a96d-43b6-8b0b-04aa01931c8f
Garcia-Araez, Nuria
9358a0f9-309c-495e-b6bf-da985ad81c37
Owen, John R.
067986ea-f3f3-4a83-bc87-7387cc5ac85d
Lodge, Andrew W.
2612eca4-d8bd-4029-9ccc-19a54c22619a
Lacey, Matthew J.
d474e53b-ac9c-4e75-abe9-cdd1d9d549b0
Fitt, Matthew
d608a73e-a96d-43b6-8b0b-04aa01931c8f
Garcia-Araez, Nuria
9358a0f9-309c-495e-b6bf-da985ad81c37
Owen, John R.
067986ea-f3f3-4a83-bc87-7387cc5ac85d

Lodge, Andrew W., Lacey, Matthew J., Fitt, Matthew, Garcia-Araez, Nuria and Owen, John R. (2014) Critical appraisal on the role of catalysts for the oxygen reduction reaction in lithium-oxygen batteries. Electrochimica Acta, 140, 168-173. (doi:10.1016/j.electacta.2014.05.026).

Record type: Article

Abstract

This work reports a detailed characterization of the reduction of oxygen in pyrrolidinium-based ionic liquids for application to lithium-oxygen batteries. It is found that, in the absence of Li+, all electron transfer kinetics are fast, and therefore, the reactions are limited by the mass transport rate. Reversible reduction of O2 to O2•- and O2•- to O22- take place at E0 = 2.1 V and 0.8 V vs. Li+/Li, respectively. In the presence of Li+, O2 is reduced to LiO2 first and then to Li2O2. The solubility product constant of Li2O2 is found to be around 10-51, corroborating the hypothesis that electrode passivation by Li2O2 deposition is an important issue that limits the capacity delivered by lithium-oxygen batteries. Enhancing the rate of Li2O2 formation by using different electrode materials would probably lead to faster electrode passivation and hence smaller charge due to oxygen reduction (smaller capacity of the battery). On the contrary, soluble redox catalysts can not only increase the reaction rate of Li2O2 formation but also avoid electrode passivation since the fast diffusion of the soluble redox catalyst would displace the formation of Li2O2 at a sufficient distance from the electrode surface

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e-pub ahead of print date: 14 May 2014
Published date: 10 September 2014
Organisations: Electrochemistry

Identifiers

Local EPrints ID: 371762
URI: http://eprints.soton.ac.uk/id/eprint/371762
ISSN: 0013-4686
PURE UUID: c7c72598-a7e4-49e2-aa69-3abfcfec9a8f
ORCID for Andrew W. Lodge: ORCID iD orcid.org/0000-0001-5004-208X
ORCID for Nuria Garcia-Araez: ORCID iD orcid.org/0000-0001-9095-2379
ORCID for John R. Owen: ORCID iD orcid.org/0000-0002-4938-3693

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Date deposited: 14 Nov 2014 14:42
Last modified: 15 Mar 2024 03:46

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Contributors

Author: Andrew W. Lodge ORCID iD
Author: Matthew J. Lacey
Author: Matthew Fitt
Author: John R. Owen ORCID iD

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