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@ARTICLE{Bobrov:917131,
author = {Bobrov, Gleb and Kedzior, Stephanie A. and Pervez, Syed
Atif and Govedarica, Aleksandra and Kloker, Gabriele and
Fichtner, Maximilian and Michaelis, Vladimir K. and Bernard,
Guy M. and Veelken, Philipp M. and Hausen, Florian and
Trifkovic, Milana},
title = {{C}oupling {P}article {O}rdering and {S}pherulitic {G}rowth
for {L}ong-{T}erm {P}erformance of
{N}anocellulose/{P}oly(ethylene oxide) {E}lectrolytes},
journal = {ACS applied materials $\&$ interfaces},
volume = {15},
number = {1},
issn = {1944-8244},
address = {Washington, DC},
publisher = {Soc.},
reportid = {FZJ-2023-00363},
pages = {1996–2008},
year = {2023},
abstract = {Development of lithium-ion batteries with composite solid
polymer electrolytes (CPSEs) has attracted attention due to
their higher energy density and improved safety compared to
systems utilizing liquid electrolytes. While it is well
known that the microstructure of CPSEs affects the ionic
conductivity, thermal stability, and mechanical
integrity/long-term stability, the bridge between the
microscopic and macroscopic scales is still unclear. Herein,
we present a systematic investigation of the distribution of
TEMPO-oxidized cellulose nanofibrils (t-CNFs) in two
different molecular weights of poly(ethylene oxide) (PEO)
and its effect on Li+ ion mobility, bulk conductivity, and
long-term stability. For the first time, we link local
Li-ion mobility at the nanoscale level to the morphology of
CPSEs defined by PEO spherulitic growth in the presence of
t-CNF. In a low-MW PEO system, spherulites occupy a whole
volume of the derived CPSE with t-CNF being incorporated in
between lamellas, while their nuclei remain particle-free.
In a high-MW PEO system, spherulites are scarce and their
growth is arrested in a non-equilibrium cubic shape due to
the strong t-CNF network surrounding them. Electrochemical
strain microscopy and solid-state 7Li nuclear magnetic
resonance spectroscopy confirm that t-CNF does not partake
in Li+ ion transport regardless of its distribution within
the polymer matrix. Free-standing CSPE films with low-MW PEO
have higher conductivity but lack long-term stability due to
the existence of uniformly distributed, particle-free,
spherulite nuclei, which have very little resistance to Li
dendrite growth. On the other hand, high-MW PEO has lower
conductivity but demonstrates a highly stable Li cycling
response for more than 1000 h at 0.2 mA/cm2 and 65 °C and
more than 100 h at 85 °C. The study provides a direct link
between the microscopic dynamic, Li-ion transport, bulk
mechanical properties and long-term stability of the derived
CPSE and, and as such, offers a pathway towards design of
robust all-solid-state Li-metal batteries.},
cin = {IEK-9},
ddc = {600},
cid = {I:(DE-Juel1)IEK-9-20110218},
pnm = {1223 - Batteries in Application (POF4-122)},
pid = {G:(DE-HGF)POF4-1223},
typ = {PUB:(DE-HGF)16},
pubmed = {36592370},
UT = {WOS:000908362500001},
doi = {10.1021/acsami.2c16402},
url = {https://juser.fz-juelich.de/record/917131},
}