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@ARTICLE{Holtstiege:851135,
author = {Holtstiege, Florian and Wilken, Andrea and Winter, Martin
and Placke, Tobias},
title = {{R}unning out of lithium? {A} route to differentiate
between capacity losses and active lithium losses in
lithium-ion batteries},
journal = {Physical chemistry, chemical physics},
volume = {19},
number = {38},
issn = {1463-9076},
address = {Cambridge},
publisher = {RSC Publ.},
reportid = {FZJ-2018-04837},
pages = {25905 - 25918},
year = {2017},
abstract = {Active lithium loss (ALL) resulting in a capacity loss
(QALL), which is caused by lithium consuming parasitic
reactions like SEI formation, is a major reason for capacity
fading and, thus, for a reduction of the usable energy
density of lithium-ion batteries (LIBs). QALL is often
equated with the accumulated irreversible capacity (QAIC).
However, QAIC is also influenced by non-lithium consuming
parasitic reactions, which do not reduce the active lithium
content of the cell, but induce a parasitic current. In this
work, a novel approach is proposed in order to differentiate
between QAIC and QALL. The determination of QALL is based on
the remaining active lithium content of a given cell, which
can be determined by de-lithiation of the cathode with the
help of the reference electrode of a three-electrode set-up.
Lithium non-consuming parasitic reactions, which do not
influence the active lithium content have no influence on
this determination. In order to evaluate this novel
approach, three different anode materials (graphite, carbon
spheres and a silicon/graphite composite) were investigated.
It is shown that during the first charge/discharge cycles
QALL is described moderately well by QAIC. However, the
difference between QAIC and QALL rises with increasing cycle
number. With this approach, a differentiation between
“simple” irreversible capacities and truly detrimental
“active Li losses” is possible and, thus, Coulombic
efficiency can be directly related to the remaining useable
cell capacity for the first time. Overall, the exact
determination of the remaining active lithium content of the
cell is of great importance, because it allows a statement
on whether the reduction in lithium content is crucial for
capacity fading or whether the fading is related to other
degradation mechanisms such as material or electrode
failure.},
cin = {IEK-12},
ddc = {540},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {131 - Electrochemical Storage (POF3-131)},
pid = {G:(DE-HGF)POF3-131},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:28926044},
UT = {WOS:000412275200011},
doi = {10.1039/C7CP05405J},
url = {https://juser.fz-juelich.de/record/851135},
}