Journal
SCIENCE ADVANCES
Volume 8, Issue 3, Pages -Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.abm1899
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Funding
- Australian Research Council (ARC) [DP160104340, DP170100436, DP180102297, DP200101249]
- ARC Discovery Early Career Researcher Award [DE180100036]
- National Key R&D Program of China [2016YFB0100100, 2018YFB0104400]
- National Natural Science Foundation of China [21972055, 21825202, 21575135, 21733012, 21972133]
- Newton Advanced Fellowships [NAF/R2/180603]
- U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office
- DOE Office of Science [DE-AC0206CH11357]
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A new mechanism for operating lithium-oxygen batteries using a versatile molecule has been reported, which improves discharge capacity, energy efficiency, and cycle life. This molecule acts as a redox mediator and a superoxide quencher, addressing parasitic reactions and lithium corrosion.
The advancement of lithium-oxygen (Li-O-2) batteries has been hindered by challenges including low discharge capacity, poor energy efficiency, severe parasitic reactions, etc. We report an Li-O-2 battery operated via a new quenching/mediating mechanism that relies on the direct chemical reactions between a versatile molecule and superoxide radical/Li2O2. The battery exhibits a 46-fold increase in discharge capacity, a low charge overpotential of 0.7 V, and an ultralong cycle life >1400 cycles. Featuring redox-active 2,2,6,6-tetramethyl-1-piperidinyloxy moieties bridged by a quenching-active perylene diimide backbone, the tailor-designed molecule acts as a redox mediator to catalyze discharge/charge reactions and serves as a reusable superoxide quencher to chemically react with superoxide species generated during battery operation. The all-in-one molecule can simultaneously tackle issues of parasitic reactions associated with superoxide radicals, singlet oxygen, high overpotentials, and lithium corrosion. The molecular design of multifunctional additives combining various capabilities opens a new avenue for developing high-performance Li-O-2 batteries.
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