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@ARTICLE{Shaji:909212,
author = {Shaji, Ishamol and Diddens, Diddo and Winter, Martin and
Nair, Jijeesh Ravi},
title = {{M}echanistically {N}ovel {F}rontal‐{I}nspired in situ
{P}hotopolymerization: {A}n {E}fficient
{E}lectrode|{E}lectrolyte {I}nterface {E}ngineering {M}ethod
for {H}igh {E}nergy {L}ithium {M}etal {P}olymer {B}atteries},
journal = {Energy $\&$ Environmental Materials},
volume = {6},
number = {6},
issn = {2575-0356},
address = {Hoboken},
publisher = {Wiley},
reportid = {FZJ-2022-03072},
pages = {e12469},
year = {2023},
abstract = {The solvent-free in situ polymerization technique has the
potential to tailor-make conformal interfaces that are
essential for developing durable and safe lithium metal
polymer batteries (LMPBs). Hence, much attention has been
given to the eco-friendly and rapid ultraviolet (UV)-induced
in situ photopolymerization process to prepare solid-state
polymer electrolytes. In this respect, an innovative method
is proposed here to overcome the challenges of UV-induced
photopolymerization (UV-curing) in the zones where UV-light
cannot penetrate, especially in LMPBs where thick electrodes
are used. The proposed frontal-inspired photopolymerization
(FIPP) process is a diverged frontal-based technique that
uses two classes (dual) of initiators to improve the slow
reaction kinetics of allyl-based monomers/oligomers by at
least $50\%$ compared with the conventional UV-curing
process. The possible reaction mechanism occurring in FIPP
is demonstrated using density functional theory calculations
and spectroscopic investigations. Indeed, the initiation
mechanism identified for the FIPP relies on a photochemical
pathway rather than an exothermic propagating front forms
during the UV-irradiation step as the case with the
classical frontal photopolymerization technique. Besides,
the FIPP-based in situ cell fabrication using dual
initiators is advantageous over both the sandwich cell
assembly and conventional in situ photopolymerization in
overcoming the limitations of mass transport and active
material utilization in high energy and high power LMPBs
that use thick electrodes. Furthermore, the LMPB cells
fabricated using the in situ-FIPP process with high mass
loading LiFePO4 electrodes (5.2 mg cm-2) demonstrate
higher rate capability, and a $50\%$ increase in specific
capacity against a sandwich cell encouraging the use of this
innovative process in large-scale solid-state battery
production.},
cin = {IEK-12},
ddc = {333.7},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {1221 - Fundamentals and Materials (POF4-122)},
pid = {G:(DE-HGF)POF4-1221},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000934985700001},
doi = {10.1002/eem2.12469},
url = {https://juser.fz-juelich.de/record/909212},
}