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@ARTICLE{Nguyen:863371,
author = {Nguyen, Huu-Dat and Kim, Guk-Tae and Shi, Junli and
Paillard, Elie and Judeinstein, Patrick and Lyonnard,
Sandrine and Bresser, Dominic and Iojoiu, Cristina},
title = {{N}anostructured multi-block copolymer single-ion
conductors for safer high-performance lithium batteries},
journal = {Energy $\&$ environmental science},
volume = {11},
number = {11},
issn = {1754-5706},
address = {Cambridge},
publisher = {RSC Publ.},
reportid = {FZJ-2019-03444},
pages = {3298 - 3309},
year = {2018},
abstract = {The greatest challenges towards the worldwide success of
battery-powered electric vehicles revolve around the safety
and energy density of the battery. Single-ion conducting
polymer electrolytes address both challenges by replacing
the flammable and unstable liquid electrolytes and enabling
dendrite-free cycling of high-energy lithium metal anodes.
To date, however, their commercial use has been hindered by
insufficient ionic conductivities at ambient temperature
(commonly not exceeding 10−6 S cm−1) and the limited
electrochemical stability towards oxidation, in particular
when incorporating ether-type building blocks, limiting
their application to rather low-voltage cathode materials
like LiFePO4. Here, we introduce ether-free, nanostructured
multi-block copolymers as single-ion conducting
electrolytes, providing high thermal stability and
self-extinguishing properties and, if plasticized with
ethylene carbonate, ionic conductivities exceeding 10−3 S
cm−1 above 30 °C, i.e., approaching that of
state-of-the-art liquid electrolytes. Moreover, these
single-ion conducting ionomers present highly reversible
lithium cycling for more than 1000 h and, as a result of
their excellent electrochemical stability, highly stable
cycling of Li[Ni1/3Co1/3Mn1/3]O2 cathodes. To the best of
our knowledge, this is the first polymer electrolyte that
presents such remarkable ionic conductivity and outstanding
electrochemical stability towards both reduction and
oxidation, thus, paving the way for advanced high-energy
lithium metal batteries. Remarkably, the realization of
well-defined continuous ionic domains appears to be the key
to efficient charge transport through the electrolyte bulk
and across the electrode/electrolyte interface, highlighting
the importance of the self-assembling nanostructure. The
latter is achieved by carefully (i) designing the copolymer
structure, i.e., introducing alternating ionic blocks with a
very regular distribution of weakly coordinating anions
along the polymer chain and rigid blocks, which are
completely immiscible with ethylene carbonate, and (ii)
choosing the processing solvent, taking into account its
interaction with the different copolymer blocks.},
cin = {IEK-12},
ddc = {690},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {131 - Electrochemical Storage (POF3-131)},
pid = {G:(DE-HGF)POF3-131},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000449843300018},
doi = {10.1039/C8EE02093K},
url = {https://juser.fz-juelich.de/record/863371},
}