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@ARTICLE{Roitzheim:909187,
author = {Roitzheim, Christoph and Sohn, Yoo Jung and Kuo, Liang-Yin
and Häuschen, Grit and Mann, Markus and Sebold, Doris and
Finsterbusch, Martin and Kaghazchi, Payam and Guillon,
Olivier and Fattakhova-Rohlfing, Dina},
title = {{A}ll-{S}olid-{S}tate {L}i {B}atteries with
{NCM}–{G}arnet-{B}ased {C}omposite {C}athodes: {T}he
{I}mpact of {NCM} {C}omposition on {M}aterial
{C}ompatibility},
journal = {ACS applied energy materials},
volume = {5},
number = {6},
issn = {2574-0962},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {FZJ-2022-03055},
pages = {6913 - 6926},
year = {2022},
abstract = {Garnet-based all-solid-state batteries (ASBs) with high
energy density require composite cathodes with high areal
loading and high-capacity cathode active materials. While
all ceramic cathodes can typically be manufactured via
cosintering, the elevated temperatures necessary for this
process pose challenges with respect to material
compatibility. High-capacity cathode active materials like
Ni-rich LiNixCoyMn1–x–yO2 (NCM) show insufficient
material compatibility toward the solid electrolyte
Li6.45Al0.05La3Zr1.6Ta0.4O12 (LLZO:Ta) during cosintering,
leading to the formation of highly resistive interphases. We
investigated this secondary phase formation both
experimentally and via density functional theory calculation
to get a mechanistic understanding of the cosintering
behavior of LLZO:Ta with NCM111 and Ni-rich NCM811.
Furthermore, we employed B doping of both NCM materials in
order to assess its impact on the cation interchange and
subsequent secondary phase formation. While secondary phases
were formed for all four NCM materials, their onset
temperature, nature, and amount strongly depend on the NCM
composition and doping. Surprisingly, Ni-rich NCM811 turned
out to be the most promising cathode active material for the
combination with garnet-type LLZO:Ta. As proof of concept,
fully inorganic, ceramic all-solid-state lithium batteries
featuring only a Li-metal anode, an LLZO:Ta separator, and a
composite cathode, consisting of LLZO:Ta, Li3BO3, and
NCM811, were prepared by conventional sintering. The purely
inorganic full cells delivered a high specific areal
discharge capacity of 0.7 mA h cm–2 in the initial cycle.},
cin = {IEK-1 / IEK-12},
ddc = {540},
cid = {I:(DE-Juel1)IEK-1-20101013 / 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:000819121400001},
doi = {10.1021/acsaem.2c00533},
url = {https://juser.fz-juelich.de/record/909187},
}