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@ARTICLE{Brmann:894630,
author = {Bärmann, Peer and Mohrhardt, Marvin and Frerichs, Joop
Enno and Helling, Malina and Kolesnikov, Aleksei and
Klabunde, Sina and Nowak, Sascha and Hansen, Michael Ryan
and Winter, Martin and Placke, Tobias},
title = {{M}echanistic {I}nsights into the {P}re‐{L}ithiation of
{S}ilicon/{G}raphite {N}egative {E}lectrodes in “{D}ry
{S}tate” and {A}fter {E}lectrolyte {A}ddition {U}sing
{P}assivated {L}ithium {M}etal {P}owder},
journal = {Advanced energy materials},
volume = {11},
number = {25},
issn = {1614-6840},
address = {Weinheim},
publisher = {Wiley-VCH},
reportid = {FZJ-2021-03326},
pages = {2100925},
year = {2021},
abstract = {Because of its high specific capacity, silicon is regarded
as the most promising candidate to be incrementally added to
graphite-based negative electrodes in lithium-ion batteries.
However, silicon suffers from significant volume changes
upon (de-)lithiation leading to continuous re-formation of
the solid electrolyte interphase (SEI) and ongoing active
lithium losses. One prominent approach to compensate for
active lithium losses is pre-lithiation. Here, the
“contact pre-lithiation” of silicon/graphite (Si/Gr)
negative electrodes in direct contact with passivated Li
metal powder (PLMP) is studied, focusing on the
pre-lithiation mechanism in “dry state” and after
electrolyte addition. PLMP is pressed onto the electrode
surface to precisely adjust the degree of pre-lithiation
$(25\%,$ $50\%,$ and $75\%).$ By in situ XRD and ex situ 7Li
NMR studies, it is proven that significant lithiation of
Si/Gr electrodes occurs by direct contact to Li metal, that
is, without electrolyte. After electrolyte addition,
de-lithiation of silicon and graphite is confirmed,
resulting in SEI formation. The amount of Li metal highly
impacts the presence and durability of the LixC and LixSi
phases. Finally, the challenges for homogeneous
pre-lithiation and SEI formation are identified, and the
impact of electrolyte addition is assessed by analysis of
the lateral and in-depth lithium distribution within the
Si/Gr electrode.},
cin = {IEK-12},
ddc = {050},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {1221 - Fundamentals and Materials (POF4-122) / SeNSE -
Lithium-ion battery with silicon anode, nickel-rich cathode
and in-cell sensor for electric vehicles (875548)},
pid = {G:(DE-HGF)POF4-1221 / G:(EU-Grant)875548},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000649969200001},
doi = {10.1002/aenm.202100925},
url = {https://juser.fz-juelich.de/record/894630},
}