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@ARTICLE{Haneke:1025928,
author = {Haneke, Lukas and Pfeiffer, Felix and Bärmann, Peer and
Wrogemann, Jens and Peschel, Christoph and Neumann, Jonas
and Kux, Fabian and Nowak, Sascha and Winter, Martin and
Placke, Tobias},
title = {{I}nsights into {E}lectrolytic {P}re‐{L}ithiation: {A}
{T}horough {A}nalysis {U}sing {S}ilicon {T}hin {F}ilm
{A}nodes},
journal = {Small},
volume = {19},
number = {8},
issn = {1613-6810},
address = {Weinheim},
publisher = {Wiley-VCH},
reportid = {FZJ-2024-03206},
pages = {2206092},
year = {2023},
note = {Unterstützt durch BMBF Projekt “PräLi” (03XP0238X).},
abstract = {Pre-lithiation via electrolysis, herein defined as
electrolytic pre-lithiation, using cost-efficient
electrolytes based on lithium chloride (LiCl), is
successfully demonstrated as a proof-of-concept for enabling
lithium-ion battery full-cells with high silicon content
negative electrodes. An electrolyte for pre-lithiation based
on γ-butyrolactone and LiCl is optimized using
boron-containing additives (lithium bis(oxalato)borate,
lithium difluoro(oxalate)borate) and CO2 with respect to the
formation of a protective solid electrolyte interphase (SEI)
on silicon thin films as model electrodes. Reversible
lithiation in Si||Li metal cells is demonstrated with
Coulombic efficiencies (CEff) of $95–96\%$ for optimized
electrolytes comparable to 1 m LiPF6/EC:EMC 3:7. Formation
of an effective SEI is shown by cyclic voltammetry and X-ray
photoelectron spectroscopy (XPS). electrolytic
pre-lithiation experiments show that notable amounts of the
gaseous product Cl2 dissolve in the electrolyte leading to a
self-discharge Cl2/Cl− shuttle mechanism between the
electrodes lowering pre-lithiation efficiency and causing
current collector corrosion. However, no significant
degradation of the Si active material and the SEI due to
contact with elemental chlorine is found by SEM, impedance,
and XPS. In NCM111||Si full-cells, the capacity retention in
the 100th cycle can be significantly increased from $54\%$
to $78\%$ by electrolytic pre-lithiation, compared to
reference cells without pre-lithiation of Si.},
cin = {IEK-12},
ddc = {620},
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},
pubmed = {36504320},
UT = {WOS:000896906000001},
doi = {10.1002/smll.202206092},
url = {https://juser.fz-juelich.de/record/1025928},
}