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Promoting solution phase discharge in Li–O2 batteries containing weakly solvating electrolyte solutions

Abstract:
On discharge, the Li–O2 battery can form a Li2O2 film on the cathode surface, leading to low capacities, low rates and early cell death, or it can form Li2O2 particles in solution, leading to high capacities at relatively high rates and avoiding early cell death. Achieving discharge in solution is important and may be encouraged by the use of high donor or acceptor number solvents or salts that dissolve the LiO2 intermediate involved in the formation of Li2O2. However, the characteristics that make high donor or acceptor number solvents good (for example, high polarity) result in them being unstable towards LiO2 or Li2O2. Here we demonstrate that introduction of the additive 2,5-di-tert-butyl-1,4-benzoquinone (DBBQ) promotes solution phase formation of Li2O2 in low-polarity and weakly solvating electrolyte solutions. Importantly, it does so while simultaneously suppressing direct reduction to Li2O2 on the cathode surface, which would otherwise lead to Li2O2 film growth and premature cell death. It also halves the overpotential during discharge, increases the capacity 80- to 100-fold and enables rates >1 mA cmareal−2 for cathodes with capacities of >4 mAh cmareal−2. The DBBQ additive operates by a new mechanism that avoids the reactive LiO2 intermediate in solution.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1038/nmat4629

Authors


More by this author
Department:
Oxford,MPLS,Materials
Role:
Author
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Institution:
University of Oxford
Oxford college:
St Edmund Hall
Role:
Author


Publisher:
Springer Nature
Journal:
Nature Materials More from this journal
Volume:
15
Issue:
8
Pages:
882-888
Publication date:
2016-04-25
Acceptance date:
2016-03-21
DOI:
EISSN:
1476-4660
ISSN:
1476-1122
Pmid:
27111413


Language:
English
Keywords:
Pubs id:
pubs:619678
UUID:
uuid:9e6be1c1-257b-431f-b9b0-9b9334602f17
Local pid:
pubs:619678
Source identifiers:
619678
Deposit date:
2016-12-16

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