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@ARTICLE{Wu:1024361,
author = {Wu, Yi−Shiuan and Pham, Quoc-Thai and Yang, Chun-Chen and
Chern, Chorng-Shyan and Babulal, Lakshmipriya Musuvadhi and
Seenivasan, Manojkumar and Jeyakumar, Juliya and Mengesha,
Tadesu Hailu and Placke, Tobias and Brunklaus, Gunther and
Winter, Martin and Hwang, Bing Joe},
title = {{C}oating of a {N}ovel {L}ithium-{C}ontaining {H}ybrid
{O}ligomer {A}dditive on {N}ickel-{R}ich {L}i{N}i 0.8 {C}o
0.1 {M}n 0.1 {O} 2 {C}athode {M}aterials for
{H}igh-{S}tability and {H}igh-{S}afety {L}ithium-{I}on
{B}atteries},
journal = {ACS sustainable chemistry $\&$ engineering},
volume = {10},
number = {22},
issn = {2168-0485},
address = {Washington, DC},
publisher = {ACS Publ.},
reportid = {FZJ-2024-02117},
pages = {7394 - 7408},
year = {2022},
note = {Zudem unterstützt durch BMBF Projekt: 03XP0304D},
abstract = {In this study, we synthesized a Li-containing “BTJ-L”
hybrid oligomer─obtained through polymerization of
bismaleimide (BMI) with a polyether monoamine (i.e.,
Jeffamine-M1000, JA), trithiocyanuric acid (TCA), and
LiOH─and coated it as an additive in various amounts
(0.5–2 wt $\%)$ onto the surface of a Ni-rich
LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode active material,
forming BTJ-L@NCM811 electrodes for lithium-ion batteries
(LIBs). Relative to CR2032 coin-type cells incorporating a
pristine NCM811 electrode, the cells with the 1 wt $\%$
BTJ-L@NCM811 electrode demonstrated a slightly higher
initial discharge capacity (173 mAh g–1 vs171 mAh g–1)
and higher values of average Coulombic efficiency, CEavg
$(99.5\%$ $vs98.9\%)$ and capacity retention, CR $(86.1\%$
$vs72.9\%)$ after 100 cycles at 1C. Electrochemical
impedance spectroscopy revealed that the decrease in the
charge transfer resistance (Rct: 46.7 Ω vs171.1 Ω) and the
superior Li+ ion diffusivity (DLi+: ∼1.09 × 10–12 cm2
s–1 vs ∼1.61 × 10–13 cm2 s–1) of the cells
incorporating the BTJ-L@NCM811 electrode after cycling at 1C
could be attributed to the excellent wettability toward the
electrolyte and the extra Li+ ions contributed by the hybrid
BTJ-L oligomer additive. Therefore, the BTJ-L oligomer
coating layer functioned much like an artificial cathode
electrolyte interphase (CEI) layer, impairing the
dissolution of transition metals (TMs) from the cathode
materials into the carbonate-based electrolytes.
Furthermore, insitu microcalorimetry manifested that the
total exothermic heat generation (Qt) of the coin cells
containing the 1 wt $\%$ BTJ-L@NCM811 electrode operating at
1C in isothermal modes (35 and 55 °C) during the charging
process was dramatically lower (by ca. $45\%)$ relative to
that of the cells incorporating the pristine NCM811
electrode. On the basis of an ARC-HWS analysis, the
delithiated pristine NCM811 electrode shows thermal
reactivity with the electrolyte at a much earlier stage in
comparison to the 1 wt $\%$ BTJ-L@NCM811 counterpart (843
min vs 1039 min) between 171 and 192 °C. Thus, Ni-rich
NCM811 cathode materials coated with trace amounts (i.e., 1
wt $\%)$ of the BTJ211-L1 hybrid oligomer additives
displayed both enhanced electrochemical performance and
remarkably improved thermal stability. Accordingly, this
Li-containing BTJ-L hybrid oligomer appears to be a great
candidate material for coating high-Ni oxide cathode
materials to enhance the safety and electrochemical
performance of LIB cells.},
cin = {IEK-12},
ddc = {540},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {1223 - Batteries in Application (POF4-122) / 1222 -
Components and Cells (POF4-122) / LiBEST2 -
Lithium-Batterie-Konzepte mit hoher Energiedichte, Leistung
und Sicherheit (13XP0304A)},
pid = {G:(DE-HGF)POF4-1223 / G:(DE-HGF)POF4-1222 /
G:(BMBF)13XP0304A},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000809046600018},
doi = {10.1021/acssuschemeng.2c01712},
url = {https://juser.fz-juelich.de/record/1024361},
}