---
_id: '7280'
abstract:
- lang: eng
text: Non-aqueous lithium-oxygen batteries cycle by forming lithium peroxide during
discharge and oxidizing it during recharge. The significant problem of oxidizing
the solid insulating lithium peroxide can greatly be facilitated by incorporating
redox mediators that shuttle electron-holes between the porous substrate and lithium
peroxide. Redox mediator stability is thus key for energy efficiency, reversibility,
and cycle life. However, the gradual deactivation of redox mediators during repeated
cycling has not conclusively been explained. Here, we show that organic redox
mediators are predominantly decomposed by singlet oxygen that forms during cycling.
Their reaction with superoxide, previously assumed to mainly trigger their degradation,
peroxide, and dioxygen, is orders of magnitude slower in comparison. The reduced
form of the mediator is markedly more reactive towards singlet oxygen than the
oxidized form, from which we derive reaction mechanisms supported by density functional
theory calculations. Redox mediators must thus be designed for stability against
singlet oxygen.
article_number: '1380'
article_processing_charge: No
article_type: original
author:
- first_name: Won-Jin
full_name: Kwak, Won-Jin
last_name: Kwak
- first_name: Hun
full_name: Kim, Hun
last_name: Kim
- first_name: Yann K.
full_name: Petit, Yann K.
last_name: Petit
- first_name: Christian
full_name: Leypold, Christian
last_name: Leypold
- first_name: Trung Thien
full_name: Nguyen, Trung Thien
last_name: Nguyen
- first_name: Nika
full_name: Mahne, Nika
last_name: Mahne
- first_name: Paul
full_name: Redfern, Paul
last_name: Redfern
- first_name: Larry A.
full_name: Curtiss, Larry A.
last_name: Curtiss
- first_name: Hun-Gi
full_name: Jung, Hun-Gi
last_name: Jung
- first_name: Sergey M.
full_name: Borisov, Sergey M.
last_name: Borisov
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Yang-Kook
full_name: Sun, Yang-Kook
last_name: Sun
citation:
ama: Kwak W-J, Kim H, Petit YK, et al. Deactivation of redox mediators in lithium-oxygen
batteries by singlet oxygen. Nature Communications. 2019;10. doi:10.1038/s41467-019-09399-0
apa: Kwak, W.-J., Kim, H., Petit, Y. K., Leypold, C., Nguyen, T. T., Mahne, N.,
… Sun, Y.-K. (2019). Deactivation of redox mediators in lithium-oxygen batteries
by singlet oxygen. Nature Communications. Springer Nature. https://doi.org/10.1038/s41467-019-09399-0
chicago: Kwak, Won-Jin, Hun Kim, Yann K. Petit, Christian Leypold, Trung Thien Nguyen,
Nika Mahne, Paul Redfern, et al. “Deactivation of Redox Mediators in Lithium-Oxygen
Batteries by Singlet Oxygen.” Nature Communications. Springer Nature, 2019.
https://doi.org/10.1038/s41467-019-09399-0.
ieee: W.-J. Kwak et al., “Deactivation of redox mediators in lithium-oxygen
batteries by singlet oxygen,” Nature Communications, vol. 10. Springer
Nature, 2019.
ista: Kwak W-J, Kim H, Petit YK, Leypold C, Nguyen TT, Mahne N, Redfern P, Curtiss
LA, Jung H-G, Borisov SM, Freunberger SA, Sun Y-K. 2019. Deactivation of redox
mediators in lithium-oxygen batteries by singlet oxygen. Nature Communications.
10, 1380.
mla: Kwak, Won-Jin, et al. “Deactivation of Redox Mediators in Lithium-Oxygen Batteries
by Singlet Oxygen.” Nature Communications, vol. 10, 1380, Springer Nature,
2019, doi:10.1038/s41467-019-09399-0.
short: W.-J. Kwak, H. Kim, Y.K. Petit, C. Leypold, T.T. Nguyen, N. Mahne, P. Redfern,
L.A. Curtiss, H.-G. Jung, S.M. Borisov, S.A. Freunberger, Y.-K. Sun, Nature Communications
10 (2019).
date_created: 2020-01-15T12:12:26Z
date_published: 2019-03-26T00:00:00Z
date_updated: 2021-01-12T08:12:44Z
day: '26'
ddc:
- '540'
doi: 10.1038/s41467-019-09399-0
extern: '1'
file:
- access_level: open_access
checksum: 123dd33e7f26761c82c74e10811a1e4d
content_type: application/pdf
creator: dernst
date_created: 2020-01-22T15:58:54Z
date_updated: 2020-07-14T12:47:55Z
file_id: '7355'
file_name: 2019_NatureComm_Kwak.pdf
file_size: 1003676
relation: main_file
file_date_updated: 2020-07-14T12:47:55Z
has_accepted_license: '1'
intvolume: ' 10'
language:
- iso: eng
license: https://creativecommons.org/licenses/by/4.0/
month: '03'
oa: 1
oa_version: Published Version
publication: Nature Communications
publication_identifier:
issn:
- 2041-1723
publication_status: published
publisher: Springer Nature
quality_controlled: '1'
status: public
title: Deactivation of redox mediators in lithium-oxygen batteries by singlet oxygen
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 10
year: '2019'
...