energies
Article
Study on the Extensibility of Voltage-Plateau-Based Lithium
Plating Detection for Electric Vehicles
Nithin Somasundaran *, Nessa Fereshteh Saniee
Citation: Somasundaran, N.;
Fereshteh Saniee, N.; Dinh, T.Q.;
Marco, J. Study on the Extensibility of
Voltage-Plateau-Based Lithium
Plating Detection for Electric Vehicles.
Energies 2023, 16, 2537. https://
doi.org/10.3390/en16062537
Academic Editor: Carlos Miguel
Costa
Received: 19 January 2023
Revised: 24 February 2023
Accepted: 26 February 2023
Published: 8 March 2023
Copyright: © 2023 by the authors.
Licensee MDPI, Basel, Switzerland.
This article is an open access article
distributed under the terms and
conditions of the Creative Commons
Attribution (CC BY) license (https://
creativecommons.org/licenses/by/
4.0/).
Energies 2023, 16, 2537. https://doi.org/10.3390/en16062537
, Truong Quang Dinh * and James Marco
Warwick Manufacturing Group (WMG), University of Warwick, Coventry CV4 7AL, UK
* Correspondence: nithin.somasundaran@warwick.ac.uk (N.S.); t.dinh@warwick.ac.uk (T.Q.D.);
Tel.: +44-7760857606 (N.S.)
Abstract: Lithium plating is an undesirable side reaction in lithium-ion cells during fast charging at
lower temperatures. The voltage plateau of the open-circuit voltage (OCV) of cells after charging
is widely used to infer the onset of lithium plating. The differential analysis of post-charge OCV
has been shown to yield greater insights into the Li stripping characteristics. Though this method
is continuously evaluated for single cells in open circuit, a battery module can have a series and
parallel connection of cells. The effectiveness and scalability of the voltage-plateau-based technique
for battery modules is presented here. The study focuses on individual cells in open circuit, cells in
parallel connection, and cells in a series-parallel connection. The results validate the scalability of
the technique, yet the reliability and sensitivity were observed to be inferior to the single cell results
published previously.
Keywords: lithium plating; voltage plateau; battery management system
1. Introduction
Electric vehicles (EV) employing lithium-ion batteries have gained huge popularity
over the years. However, the range anxiety and long charging time have hindered EVs’
extensive public acceptance [1,2]. To address these concerns, manufacturers often depend
on energy dense cells and their fast-charging (FC) strategies. FC targets differ between
manufacturers; however, many wish to charge the battery from 20 to 80% capacity [3]
within 1 h. Li-ion batteries, when charged at a faster rate, have significant drawbacks [2].
One such aspect is the onset of undesirable side reactions, which leads to metallic lithium
plating (LP) [4] on the graphite anode. LP is largely connected to FC and is aggravated at
low operating temperatures [5]. At low temperatures and FC, the reduced charge kinetics
lowers the anode potential less than the Li+ reference and favors Li ions to be deposited as
metallic lithium on the surface of the anode [6,7]. The contiguous plating and intercalation
potential of graphite anodes make them prone to LP.
The effect of LP on the safety and cycle life of a cell is known to be significant,
as LP in dendrite formation [7] can pierce through the separator and cause an internal
short circuit [8]. Furthermore, metallic lithium deposits can isolate from further chemical
reactions and lead to loss of lithium inventory (LLI) and energy and capacity fade [6]. Hence,
the detection and prevention of LP during FC is deemed to be crucial. Metallic Li plated
on the graphite anode can be subdivided as reversible and irreversible. The irreversible
part of LP detaches from the anode and interacts with the electrolyte and contributes
to LLI, whereas the reversible part undergoes further reactions and re-intercalates into
the anode. This metallic lithium stripping and re-intercalation of reversible Li produces
a voltage plateau in the open-circuit voltage (OCV) during the relaxation phase after a
charging event [9]. The time differential of the voltage plateau of OCV (∂V/∂t), generally
referred to as the voltage relaxation profile (VRP), can be used to estimate the Li stripping
time [10] and, in turn, be employed as a proxy-metric to quantify the volume of reversible
https://www.mdpi.com/journal/energies
 Energies 2023, 16, x FOR PEER REVIEW 2 of

Energies 2023, 16, 2537 2 of 15

and, in turn, be employed as a proxy-metric to quantify the volume of reversible LP [1

There exist several other means of LP detection [12]; however, the majority of them su
LP [11]. There exist several other means of LP detection [12]; however, the majority
as (a) reference electrode, (b) neutron diffraction, (c) measurement of cell thickness, a
of them such as (a) reference electrode, (b) neutron diffraction, (c) measurement of cell
(d) accurate coulombic efficiency, etc., require sophisticated equipment and test enviro
thickness, and (d) accurate coulombic efficiency, etc., require sophisticated equipment and
ments [9].
test environments [9].
VRP, being a non-invasive and an easy-to-use technique, is widely used by researc
VRP, being a non-invasive and an easy-to-use technique, is widely used by researchers
ers to develop and compare new FC charging strategies [13–15] that are appropriate f
to develop and compare new FC charging strategies [13–15] that are appropriate for deploy-
deployment within a battery management system (BMS). However, most of the existi
ment within a battery management system (BMS). However, most of the existing literature
literature focuses on cell-level analysis within a laboratory and the scalability of VRP
focuses on cell-level analysis within a laboratory and the scalability of VRP to cells in
cells in series-parallel combinations has not been widely considered. Furthermore, VRP
series-parallel combinations has not been widely considered. Furthermore, VRP is defined
defined and evaluated for cells in open circuit after charging. There are few reported stu
and evaluated for cells in open circuit after charging. There are few reported studies on
ies on improving the detection capability of VRPs. U. Rao Koleti et al. [10] indicated th
improving the detection capability of VRPs. U. Rao Koleti et al. [10] indicated that the
the current limits set during the constant voltage (CV) phase at the end of a constant cu
current limits set during the constant voltage (CV) phase at the end of a constant current
rent charge period greatly influence the detection capability. This is due to the initiati
charge period greatly influence the detection capability. This is due to the initiation of Li
of Li stripping in the CV phase itself and demonstrated the increase in LP detection cap
stripping in the CV phase itself and demonstrated the increase in LP detection capability
bility with a higher CV cut-off. However, this study was also limited to single cells.
with a higher CV cut-off. However, this study was also limited to single cells.
Within an EV battery pack, generally there will be a parallel combination of cells th
Within an EV battery pack, generally there will be a parallel combination of cells
make up modules and subsequent modules connected in series to form the pack. The co
that make up modules and subsequent modules connected in series to form the pack.
plex electrical connection within a battery pack will induce stray inductance. In additi
The complex electrical connection within a battery pack will induce stray inductance. In
to this, the cells in a pack will have current imbalance and cell-to-cell current flow existi
addition to this, the cells in a pack will have current imbalance and cell-to-cell current flow
even after charging [16], which invalidates the ideal open-circuit requirement for the VR
existing even after charging [16], which invalidates the ideal open-circuit requirement for
The only reported literature on VRP that considered cells in parallel is by the authors
the VRP. The only reported literature on VRP that considered cells in parallel is by the
this article in [17].
authors of this article in [17].
Considering these factors, the study presented in this article aims to gain insight in
Considering these factors, the study presented in this article aims to gain insight into
the effectiveness of VRPs for inferring the onset of LP when cells are connected in seri
the effectiveness of VRPs for inferring the onset of LP when cells are connected in series-
parallel combination as part of a module. The preliminary research conducted in [17]
parallel combination as part of a module. The preliminary research conducted in [17] is
further extended, analyzed in detail, and presented here. The focus here is on the scalab
further extended, analyzed in detail, and presented here. The focus here is on the scalability
ity of VRP; improving the LP detection sensitivity is not considered.
of VRP; improving the LP detection sensitivity is not considered.
The article is structured as follows: Section 2 explains the experimental set-up a
The article is structured as follows: Section 2 explains the experimental set-up and
details of the tests performed on individual cells, cells in parallel, and cells in series p
details of the tests performed on individual cells, cells in parallel, and cells in series parallel.
allel. Section 3 presents the test results and analysis. Finally, Sections 4 and 5 present t
Section 3 presents the test results and analysis. Finally, Sections 4 and 5 present the further
further work and conclusions from this study.
work and conclusions from this study.

2. Experimental 2. Experimental
Details Details
LP is known LP to beis highly
knowninfluenced
to be highly influenced
by ambient by ambient
operating operating
temperature temperature
[8], and hence, [8], a
hence, it is important to validate the tests at different temperatures.
it is important to validate the tests at different temperatures. The temperatures considered The temperatures co
for the study sidered for5,
are 25, 10, the study
and 0 ◦ Care 25, 10,
inside an 5, and 0 environmental
ESPEC °C inside an ESPEC environmental
chamber. The charging chamber. T
charging rates (C rates) used were 0.3, 0.5, and 1C. The electrochemical performance of t
rates (Crates ) used were 0.3, 0.5, and 1C. The electrochemical performance of the cells was
benchmarkedcells withwas benchmarked
a reference with a reference
test (defined in Sectiontest 2.2)(defined in Sectionover
at the beginning, 2.2) at
thethe beginning, ov
course
of the experiment, and at the end. The overall experimental process is depicted in Figure 1 is depict
the course of the experiment, and at the end. The overall experimental process
in Figureplatform
and the experimental 1 and the inexperimental
Figure 2. The platform
setup andinVRP Figure 2. The setup
evaluation and
of cells VRP evaluation
in various
cells in various
scenarios are presented below. scenarios are presented below.

Cells Cells Cells

Conditioning Tested Tested as Tested as
Cyles Individually 1S3Ps 3S3P

RPT-1 RPT-2 RPT-3 RPT-4

Figure 1. Experiment stages.

Energies 2023, 16, x FOR PEER REVIEW 3 of 15

Energies 2023, 16, 2537 3 of 15

Figure 1. Experiment stages.

ESPEC
Environment Chamber

Test jig

Cell/Module Cycler

Figure2.
Figure 2. Experimental
Experimental platform.
platform.

2.1.
2.1. Cell
Cell Preparation
Preparation
Commercially
Commerciallyavailable
availableINR21700
INR21700 cells
cells with
with aa rated
rated capacity
capacity ofof 4.8
4.8 Ah
Ah were
were used
used for
for
the
the study.
study. These
These cells have NCA
cells have NCA chemistry
chemistrywithwithaagraphite
graphiteanode
anodeandandthe therated
ratedvoltage
voltage is
is 4.2 V. The manufacturer’s recommended charging strategy is constant
4.2 V. The manufacturer’s recommended charging strategy is constant current (CC) up to current (CC) up
to
4.24.2
V, V, followed
followed by by constant
constant voltage
voltage (CV) (CV)
withwith a cut-off
a cut-off of 0.05C.
of 0.05C. The C The Crate
rate of 1C of 1C A.
is 4.8 is
4.8 A. Similarly, the discharging protocol is CC mode till 2.5 V. Nine cells
Similarly, the discharging protocol is CC mode till 2.5 V. Nine cells of similar mass and of similar mass
and internal
internal resistance
resistance were were selected
selected for for
the the experiment.
experiment. TheThe cells
cells areare labelled
labelled from
from 1 to
1 to 9 in9
in order. Theresistance
resistancewas
wasmeasured
measuredwhenwhencells
cellswere
werefully
fully discharged
discharged at at 25 ◦ C using
order. The 25 °C using aa
HIOKI-BT3563 at 1kHz. The average resistance of the cells was
HIOKI-BT3563 at 1kHz. The average resistance of the cells was around 16 mΩ. around 16 mΩ.

2.2. Reference Performance Test

2.2. Reference Performance Test
A detailed description of the reference performance test (RPT) process is defined in [18]
A detailed description of the reference performance test (RPT) process is defined in
but is included here for completeness. The RPT involves discharge capacity measurements
[18] but is included here for completeness. The RPT involves discharge capacity measure-
and resistance measurements at different SoCs using discharge pulses. Cells are connected
ments and resistance measurements at different SoCs using discharge pulses. Cells are
individually to 9 channels of a Maccor 4209 multirange cycler for RPT and kept inside an
connected individually to 9 channels of a Maccor 4209 multirange cycler for RPT and kept
environmental chamber at 25 ◦ C.
inside an environmental
Cells are temperaturechamber at 25adequately
soaked and °C. rested to stabilize before and after each
Cells are temperature soaked and adequately
step in the process. The rest periods were 2 h before rested to stabilize
and after beforeand
a full charge anddischarge
after each
step in the process. The rest periods were 2 h before and after a full charge
for capacity measurement. The charging and discharging limits are the same as highlighted and discharge
forSection
in capacity2.1.measurement.
Discharge capacity The charging
is measured andfordischarging limits till
0.3C in CC mode are2.5
theV.same as high-
For discharge
lighted in Section 2.1. Discharge capacity is measured for 0.3C in
pulses and SoC adjustments, the rest period considered is 1 h, which is the same as CC mode till 2.5 V.that
For
discharge pulses
employed in [18].andTheSoC adjustments,
discharge pulsetheused
rest period considered
for resistance is 1 h, which
measurement is is0.5C,
the same
and
as that employed in [18]. The discharge pulse used for resistance
the SoCs considered for measurements are 100, 80, 50, and 30%. SoC adjustments measurement is were
0.5C,
and the SoCs
performed considered
with for measurements
a 0.3C discharge in CC mode. areFour
100, 80, 50,were
RPTs and 30%. SoC adjustments
performed over the course were
performed with a 0.3C discharge in CC
of this study, and they are labelled as RPT-1 to 4.mode. Four RPTs were performed over the course
of this study, and they are labelled as RPT-1 to 4.
2.3. Individual Cell Test for VRP
2.3. Individual
The unused Cellcells
Testwere
for VRP
cycled three times before the actual tests to facilitate condition-
Theprotocol
ing. The unused followed
cells were wascycled
0.3C three
CC mode times tillbefore
4.2 V andthe actual
CV withtests to facilitate
a 0.05C limit, andcondi-
the
discharge
tioning. Thewasprotocol
0.3C in followed
CC with 2.5 wasV0.3C
as the CClower
modelimit. The
till 4.2 cells,CV
V and after conditioning
with a 0.05C limit,cycles,
and
underwent
the discharge an RPT. The average
was 0.3C in CC withcell capacity
2.5 V as from RPT-1limit.
the lower was 4.66
The Ah and
cells, resistances
after were
conditioning
16.17
cycles,and 16.35 mΩ an
underwent at 100
RPT. and 30%
The SoC, respectively.
average cell capacity from RPT-1 was 4.66 Ah and re-
The cells
sistances werewere
16.17mounted
and 16.35on mΩ a customized
at 100 and 30% PerspexSoC, jig with brass connectors, placed
respectively.
insideThean ESPEC chamber, and wired to a Maccor
cells were mounted on a customized Perspex jig with cycler. The cellsbrass
were connectors,
charged in CC-CV
placed
mode ◦ C.
inside an ESPEC chamber, and wired to a Maccor cycler. The cells were 10,
at rates of 0.3, 0.5, and 1C for 3 cycles under temperatures of 25, 5, andin0CC-
charged
Afterwards,
CV mode atcells rateswere rested
of 0.3, 0.5, with
and 1Cno for
electrical load
3 cycles for atemperatures
under duration of 4 hofto25,
achieve electrical
10, 5, and 0 °C.
equilibrium. The OCV
Afterwards, cells were during rest was
rested with recordedload
no electrical by theforMaccor cycler
a duration of at
4 hantointerval
achieveof 1s.
elec-
The VRP
trical was computed
equilibrium. The OCVfrom during
the rest rest
periodwasOCV. The VRP
recorded of individual
by the cellsat
Maccor cycler and
ananalysis
interval
is
ofgiven
1s. Thein VRP
Section
was3.1.
computed from the rest period OCV. The VRP of individual cells and
analysis is given in Section 3.1.
 Energies2023,
Energies 2023,16,
16,2537
x FOR PEER REVIEW 44 of
of 15
15

2.4.Scaling
2.4. Scalingtoto1-Series
1-Seriesand
and3-Parallel
3-Parallel(1S3P)
(1S3P)Configuration
Configuration
Thecells
The cellsafter
afterindividual
individualtests
testsfor
forVRP
VRPwere
weredischarged
dischargedand andsubjected
subjectedto toRPT-2.
RPT-2.The
The
average internal resistance increased by 1.22% and capacity reduced
average internal resistance increased by 1.22% and capacity reduced by 2.12% from the by 2.12% from the
initial value. It is assumed that this is mainly due to accelerated ageing
initial value. It is assumed that this is mainly due to accelerated ageing associated with LP. associated with
LP. However,
However, the changes
the changes in capacity
in capacity and resistance
and resistance were were
uniformuniform
acrossacross
all theallcells.
the cells.
Thecells
The cells after
after RPT
RPT were discharged
discharged completely
completelyand andformed
formedinto intoparallel
parallelmodules
modules of
three.
of three.Three
Three 1S3P1S3Pmodules
modules wereweremademade with thethe
with help of brass
help blocks
of brass blocksconnected
connected on the
on neg-
the
ative terminal
negative terminal andand
a 6mm
a 6mm 2 copper
2 copper cable of 20
cable of cm length
20 cm having
length 0.90.9
having mΩmΩ resistance
resistance on on
the
positive side. The reason for using cables at the positive terminal is
the positive side. The reason for using cables at the positive terminal is to facilitate theto facilitate the inclu-
sion of anofadditional
inclusion clamp-on
an additional clamp-oncurrent sensor
current connection.
sensor connection.Cells 1, 2,1,and
Cells 3 formed
2, and 3 formedthe first
the
1S3P;
first 4, 5,4,and
1S3P; 6 formed
5, and the the
6 formed second;
second;andand
7, 8,7,and 9 were
8, and connected
9 were connected as the third
as the 1S3P.
third 1S3P.
TwoTektronix
Two TektronixTCP312A
TCP312Acurrent
currentprobes
probes(CT)(CT)were
wereusedusedwith
withTCPA300
TCPA300amplifiers
amplifiers
for
foreach
each1S3P;
1S3P;the theoutput
outputof ofthese
thesewerewereinterfaced
interfacedtotoaaPicoPicoLog
LogADC-24
ADC-24data dataacquisition
acquisition
system
systeminterfaced
interfacedtotoa alaptop
laptopforfordata recording
data recording at at
a rate of 1Hz.
a rate TheThe
of 1Hz. sensors
sensors areare
capable of
capable
accurately measuring currents with a sensitivity of ± 1 mA. The circuit
of accurately measuring currents with a sensitivity of ±1 mA. The circuit and connections and connections
of
ofthe
the1S3P
1S3Pmodules
modulesare areshown
shownininFigure
Figure3.3.The
Thecurrents
currentsof ofCell
Cell3,3,Cell
Cell6,6,and
andCellCell99were
were
computed
computedbased basedononKirchhoff’s
Kirchhoff’s current
currentlaw (KCL),
law (KCL),considering
considering the the
current recorded
current by the
recorded by
Maccor cycler
the Maccor for respective
cycler modules.
for respective modules.

ESPEC Chamber

1S3P -1
CT CT

Cell1 Cell2 Cell3

Channel 1

1S3P -2

CT CT

Cell4 Cell5 Cell6 Channel 2

Pico Log
ADC-24
Maccor
Cycler
1S3P -3
CT CT

Cell7 Cell8 Cell9

Channel 3

Figure3.3.Schematic
Figure Schematicand
andconnection
connectionofofcells
cellsinin1S3P
1S3Pmodule.
module.

2.5.
2.5.Scaling
Scalingtoto3-Series
3-Seriesand
and3-Parallel
3-Parallel(3S3P)
(3S3P)Configuration
Configuration
The
The cells in 1S3Ps were disconnected andRPT-3
cells in 1S3Ps were disconnected and RPT-3was
wasperformed.
performed.Later,
Later,the
thecells
cellswere
were
connected
connectedtotoform
formthethe3S3P
3S3Pmodule,
module, asas
seen
seenin in
Figure 4. Rows
Figure 4. Rows1, 2,
1, and 3 represent
2, and 3 representeach of
each
the 1S3Ps
of the within
1S3Ps the the
within 3S3P system,
3S3P respectively.
system, The The
respectively. 3S3P3S3P
module was was
module placed in aninESPEC
placed an ES-
chamber
PEC chamberand wasandwired to a Chroma
was wired 17020 module
to a Chroma cycler. cycler.
17020 module The currents of Cell 3,
The currents of Cell
Cell 6,
3,
and Cell 9 were computed based on KCL, considering the current recorded
Cell 6, and Cell 9 were computed based on KCL, considering the current recorded by theby the Chroma
cycler
Chroma for cycler
the module.
for the module.
To prevent over charging and over discharging of cells, a generic BMS (Orion Jr 2)
was used. The BMS was configured according to the module specifications and was set to
transmit the lowest cell voltage and highest cell voltage data measured in the module.
Additional ISO224 precision voltage sensing isolation amplifiers were used to measure
the voltages of each row in the 3S3P. The output from the voltage sensors was interfaced
 to PicoLog ADC-24. The isolation amplifier prevents short circuit of cell negative termi-
nals via the ground pin of ADC-24 and thus ensures the safety of cells and measuring
Energies 2023, 16, 2537 5 of 15
equipment. The voltages of rows 1, 2, and 3 (1S3P-1 to 3) of 3S3P is represented as V_H,
V_M, and V_L, respectively.

ESPEC Chamber
ISO224
CT
V_H 1S3P-1 +
Voltage sensing
CT CT
BMS
Cell1 Cell2 Cell3

V_M 1S3P-2

ISO224 CT CT

(V_H) Channel 1
Cell4 Cell5 Cell6 Chroma
ISO224
(V_M) module
Pico Log cycler
ADC-24 V_L 1S3P-3

CAN
CT CT

V_H
Cell7 Cell8 Cell9
ISO224
(V_L) V_M
BMS
V_L
GND

-
Figure4.4.Schematic
Figure Schematicand
andconnections
connectionsof
of3S3P
3S3Pmodule.
module.

To prevent over
3. Experimental Resultscharging and over discharging of cells, a generic BMS (Orion Jr 2)
and Discussions
was used. The BMS
3.1. VRP of Individual Cells was configured according to the module specifications and was set
to transmit the lowest cell voltage and highest cell voltage data measured in the module.
The OCVs recorded during the 4 h of rest after charging at a different Crate were pro-
Additional ISO224 precision voltage sensing isolation amplifiers were used to measure the
cessed and the VRP was computed. The results from the individual cell tests were ana-
voltages of each row in the 3S3P. The output from the voltage sensors was interfaced to
lyzed and it was seen that the cell VRPs exhibited lithium stripping only for 0.5 and 1C at
PicoLog ADC-24. The isolation amplifier prevents short circuit of cell negative terminals via
ambient temperatures of 5 and 0 °C. The VRPs for these scenarios are depicted in Figure
the ground pin of ADC-24 and thus ensures the safety of cells and measuring equipment.
5. The
The pointers
voltages in the1,figures
of rows 2, andshow the deflection
3 (1S3P-1 to 3) of 3S3Pin VRP, indicating as
is represented theV_H,
end of Li strip-
V_M, and
ping.
V_L, respectively.
It can be seen in Figure 5a, for 25 and 10 °C, the Li stripping characteristics are not
observed
3. Experimentalin the OCV,
Results even
andfor a higher Crate of 1C. This is due to improved charge kinet-
Discussions
ics and diffusion at
3.1. VRP of Individual Cells high temperatures. The two-stage decay in OCV is predominantly
seenThein theOCVsVRPrecorded
at lower temperatures.
during the 4 hAll ofthe
restcells were
after maintained
charging at the same
at a different temper-
Crate were
processed and the VRP was computed. The results from the individual cell testscell-to-
ature, and the maximum deviation from the setpoint value was ±0.5 °C. However, were
cell variations
analyzed and itwere
was prominent
seen that the in the
cell result
VRPs obtained.
exhibited Cells
lithium 1 tostripping
3 exhibited higher,
only for 0.5cells
and4
to 6 had moderate, and cells 7 to 9 had minimum
◦ levels of stripping.
1C at ambient temperatures of 5 and 0 C. The VRPs for these scenarios are depicted in
Figure An 5.ambient temperature
The pointers in the of 0 °C stimulated
figures more Li stripping
show the deflection in VRP,associated
indicatingwith
the reversi-
end of
ble LP for
Li stripping. the cells considered, even for lower currents of 0.3C. The influence of C rate on Li

stripping
It canat be0 seen
°C is in
revealed
Figure in5a,Figure
for 255b.
and From these
10 ◦ C, theresults, it could
Li stripping be seen that the
characteristics are VRP
not
is only effective in detecting the possible onset of LP for temperatures
observed in the OCV, even for a higher Crate of 1C. This is due to improved charge kinetics of 5 °C and below
when
and cells areatcharged
diffusion at 0.5 and 1C.The
high temperatures. Hence, it is possible
two-stage decay that
in OCVthe VRP may only be effec-
is predominantly seen
tive
in thefor
VRP similar scenarios
at lower when these
temperatures. cells
All the arewere
cells connected in series-parallel
maintained combination.
at the same temperature,
Thisthe
and is evaluated
maximumindeviationthe following the setpoint value was ±0.5 ◦ C. However, cell-to-cell
fromsections.
variations were prominent in the result obtained. Cells 1 to 3 exhibited higher, cells 4 to 6
had moderate, and cells 7 to 9 had minimum levels of stripping.
 Energies 2023, 16, x FOR PEER REVIEW 6 of 15
Energies 2023, 16, 2537 6 of 15

V/ T (Vh -1)
V/ T (Vh -1)
V/ T (Vh -1)

(a) (b)
Figure 5. VRP of individual cells. (a) Effect of temperature when cells are charged at 1C. (b) Effect
Figure 5. VRP of individual cells. (a) Effect of temperature when cells are charged at 1C. (b) Effect of
of Crate when cells are kept at 0 °C.
Crate when cells are kept at 0 ◦ C.

3.2. VRP of 1S3P Configuration

An ambient temperature of 0 ◦ C stimulated more Li stripping associated with re-
versible LP for the cellsdischarge
The charge and considered, protocols
even forprogrammed
lower currents in of
the0.3C.
Maccor were modified
The influence of Crateto
suit
on Lithe
stripping ◦
1S3P configuration of cells.
at 0 C is revealed inThe charge–discharge
Figure 5b. From thesecurrents and
results, it CV be
could cut-off
seenlimits
that
were
the VRP scaled
is onlyupeffective
by a factor of three the
in detecting to suit 1S3P onset
possible cycling. Thefor
of LP test 5 ◦ C and
scenarios ofofindividual
temperatures
cell tests
below whenwere repeated
cells on allatthe
are charged 0.51S3P
and modules
1C. Hence,and the
it is VRP was
possible computed
that fromonly
the VRP may the rest
be
effective for similar
period OCV. scenariosthe
In addition, when these cells
inter-cell are flow
current connected
duringin series-parallel combination.
cycling and relaxation was
This is evaluated in the following sections.
monitored.
As the cells under consideration showed signs of stripping only for lower tempera-
3.2. VRP
tures of 1S3P
during Configuration
individual cycling, only those scenarios are repeated for 1S3P configurations.
The The charge OCV
relaxation and discharge
of cells inprotocols programmed
1S3P connection in the
differed Maccor
from theirwere modified
individual to for
tests suit5
the
and1S3P
0 °C,configuration of cells.6.The
as seen in Figure Thecharge–discharge
VRP of modulescurrents and CV cut-off
from relaxation OCV forlimits
the were
same
scaled up by a factor
temperatures of three
are shown to suit 7.
in Figure 1S3P cycling. The test scenarios of individual cell tests
were repeated on all the 1S3P modules and the VRP was computed from the rest period
OCV. In addition, the inter-cell current flow during cycling and relaxation was monitored.
As the cells under consideration showed signs of stripping only for lower temperatures
during individual cycling, only those scenarios are repeated for 1S3P configurations. The
relaxation OCV of cells in 1S3P connection differed from their individual tests for 5 and 0 ◦ C,
as seen in Figure 6. The VRP of modules from relaxation OCV for the same temperatures
are shown in Figure 7.
The VRP of 1S3P modules deviated significantly from the individual cell results shown
in Figure 5a, especially for 5 ◦ C. The 1S3P’s OCVs and corresponding VRPs did not reveal
any signs of Li stripping at 5 ◦ C in Figures 6a and 7a. Although stripping was observed for
0 ◦ C, the characteristics are different from the individual cell results seen in Figure 7b. To
understand if this varied OCV and VRP behavior is due to unbalanced charging of cells
within each 1S3P, charging and relaxation currents at 0 ◦ C are also analyzed.
 Energies 2023, 16, x FOR PEER REVIEW 7
Energies 2023, 16, x FOR PEER REVIEW 7 of
Energies 2023, 16, 2537 7 of 15

(a) (b)
(a) (b)
Figure 6. OCV of cells charged at 1C, individually and in 1S3Ps: (a) At 5 °C. (b) At 0 °C.
Figure 6. OCV
Figure 6. OCV of cells of cells
charged charged
at 1C, at 1C, individually
individually and in 1S3Ps:and
(a)in
At1S3Ps: (a) At
5 ◦ C. (b) At 05 ◦°C.
C. (b) At 0 °C.

(a) (b)
(a) (b) ◦ C.
Figure 7.
Figure 7. Comparison ofComparison of VRPs
VRPs when cells when cells
are charged are individually
at 1C, charged at 1C, individually
and and
in 1S3Ps: (a) Atin5 1S3Ps: (a) At
◦
(b) At 0 C. (b)
Figure At
7. 0 °C.
Comparison of VRPs when cells are charged at 1C, individually and in 1S3Ps: (a) At 5 °
(b) At 0 °C.
Energies 2023, 16, 2537 8 of 15

The charging currents recorded by ADC-24 for an ambient temperature of 0 ◦ C charged

at 1C were processed and coulomb counting was employed to estimate the SoC based on
(1). The ampere hour of each cell, when tested in 1S3P for 0 ◦ C and 1C, is computed. As the
energy capacity of each cell for 1C at 0 ◦ C is unknown prior to the 1S3P test, the relative
SoC is computed with the capacity from RPT-2 as per Equation (1). C_1S3P is the capacity
of cells when charged at 1C in 1S3P at 0 ◦ C. Similarly, C_RPT2 is the cell capacity from
RPT-2 performed before the experiment. Though the capacity from RPT is measured at
a different temperature and Crate , it is a reliable reference to effectively assess the cells.
Table 1 shows the computed values based on (2).

∆t × i(t)
SoC (t) = SoC (t − 1) + (1)
3600 × Cell_capacity

SoC_1S3PRelative = (C_1S3P/C_RPT2) × 100 (2)

Table 1. Relative SoC of cells in 1S3Ps after 1C charging at 0 ◦ C.

Module 1S3P 1 1S3P 2 1S3P 3

Cells cell1 cell2 cell3 cell4 cell5 cell6 cell7 cell8 cell9
SoC_1S3PRelative (%) 90.68 92.68 88.19 90.80 91.14 90.23 91.25 92.28 90.53

The average of cell capacities from RPT-2 was 4.39 Ah, with a standard deviation of
0.17 Ah. From the SoC_1S3PRelative (%) it is implied that the cells in 1S3Ps are balanced,
especially in 1S3P-2 and 3. The variations seen in 1S3P-1 cells may primarily be due to the
parasitic resistances from jig fixtures and brass blocks at lower temperatures.
The analysis of rest phase currents showed an interesting relationship with the OCV
during rest. Ideally, stripping of metallic lithium and the re-intercalation into the anode
will cause a voltage plateau that can be clearly seen in the OCV of an individual cell. When
the cells are connected in parallel as part of a module, they are not in open circuit and
the voltage plateau of an individual cell will cause current flow within the module. The
correlation of current flow and voltage plateau was significant for 0 ◦ C. During the 5 ◦ C
rest period in Figure 8a, the current flow seems to be steady, without dynamic changes.
The initial current flow between cells was noticed to be influenced by the voltage plateau,
as seen in Figure 8b. The start and end of the voltage plateau in OCV is indicated by
red arrowheads. Positive and negative currents indicate cells charging and discharging,
respectively. Only the significant first 1 h of the current flow is shown here.
The steady current flow during rest seems to affect the Li stripping process, and hence,
the voltage plateau is negligible at 5 ◦ C and not captured in the VRP. However, as seen
during individual cell tests, stripping is prevalent at 0 ◦ C and this explains the plateau
in Figure 8b. Stripping is initiated within each cell in 1S3Ps, there will be variations in
the plateaus of the individual cells, as observed in Figure 5a in Section 3.1. Nevertheless,
since cells are connected in parallel, they cannot have different voltages and this leads
to counteracting current flow within each 1S3P branch. Once stripping is completed, the
dynamics in current flow settles down and steady balancing current flow continues to exist
till the end of 4 h rest.
Energies 2023, 16, x FOR PEER REVIEW 9 of 15

Energies 2023, 16, 2537 9 of 15

Current(mA)

OCV(V)
Current(mA)

OCV(V)
Current(mA)

OCV(V)
(a) (b)
Figure
Figure 8.
8. OCV
OCVand
andrest
restphase
phase currents
currents after
after 1C
1C charge:
charge: (a)
(a) At
At 55 °C.
◦ C.(b)
(b)At
At00°C.
◦ C.

3.3. VRP of 3S3P current

The steady Configuration
flow during rest seems to affect the Li stripping process, and
hence,Thetheexperiments
voltage plateau is negligible
on individual atwere
cells 5 °C repeated
and not captured
for 3S3P, in thethe
with VRP. However,
Chroma moduleas
seen during individual cell tests, stripping is prevalent at 0 °C and
cycler programmed appropriately with revised charge/discharge limits. The controllerthis explains the plat-
eau
areainnetwork
Figure 8b. Stripping
(CAN) messages is initiated
from the within
BMS each
were cell
usedinas
1S3Ps,
limitsthere will
for the be variations
cycler in
in real time.
the
Theplateaus of the
highest cell individual
voltage measuredcells,byasBMS
observed in Figure
was used as the 5a in Section
limit 3.1. Nevertheless,
for CC charging. Similarly,
since cells are
the lowest cellconnected
voltage datain parallel,
from BMS they
was cannot
set ashave different
the limit duringvoltages and thisThis
CC discharge. leadsis to
to
counteracting currentand
avoid over charging flow within
over each 1S3P branch. Once stripping is completed, the dy-
discharging.
namics TheinVRP
current flow1S3P
of each settles down
in the and was
module steady balancing
computed current
from flow continues
the respective ISO224to exist
voltage
till the end
sensor data.ofIn4 addition
h rest. to this, the VRP of 3S3P was computed from the module OCV data
recorded by the Chroma cycler.
3.3. VRP
Theofresults from 3S3P testing showed Li stripping only for 0 ◦ C with 1C charging, as
3S3P Configuration
noticed
Thein 1S3P testing
experiments on(Section
individual3.2).cells
The were
VRPsrepeated
of the 3S3Pfor module andthe
3S3P, with 1S3Ps within
Chroma the
mod-
module are depicted in Figure 9. Rows 1, 2, and 3 represent 1S3P-1, 2,
ule cycler programmed appropriately with revised charge/discharge limits. The controller and 3, respectively.
area network (CAN) messages from the BMS were used as limits for the cycler in real time.
The highest cell voltage measured by BMS was used as the limit for CC charging. Simi-
larly, the lowest cell voltage data from BMS was set as the limit during CC discharge. This
is to avoid over charging and over discharging.
The VRP of each 1S3P in the module was computed from the respective ISO224 volt-
age sensor data. In addition to this, the VRP of 3S3P was computed from the module OCV
data recorded by the Chroma cycler.
Energies 2023, 16, x FOR PEER REVIEW 10 of 15

The results from 3S3P testing showed Li stripping only for 0 °C with 1C charging, as
Energies 2023, 16, 2537 10 of 15
noticed in 1S3P testing (Section 3.2). The VRPs of the 3S3P module and 1S3Ps within the
module are depicted in Figure 9. Rows 1, 2, and 3 represent 1S3P-1, 2, and 3, respectively.

10-5 10-5
0 0

-2

-5 -4

-6

-10 -8
Row1-Cells 1-2-3
Row2-Cells 4-5-6 -10
Row3-Cells 7-8-9
-15 -12
3S3P
-14
0 0.5 1 1.5 2 2.5 3 3.5
Time(Hrs)
Figure 9.
Figure 9. VRPs
VRPs from
from 3S3P
3S3P module.
module.

In Figure 9, the VRP of the 3S3P module is an algebraic algebraic sum

sum ofof individual
individual 1S3P
1S3P VRPs.
VRPs.
Hence, it is important to compute the VRP of each row of a bigger module, as there could
be varied levels of LP and the VRP computed from net module OCV need need not
not reflect
reflect this.
this.
This
This is crucial when performance
performance of of FC strategies are monitored
monitored based
based on on VRP as detailed
in [9]. The stripping time for row 3 (1S3P-3) is seen to be slightly more than rows 2 and 1,
indicating varied levels of of LP
LP within
within the
the module.
module.
The stripping
strippingtimes
timesmeasured
measuredfrom fromFigure
Figure9 are given
9 are in Table
given 2. Compared
in Table 2. Compared withwith
row
1,
rowthe1,stripping time time
the stripping for rows 2 and2 3and
for rows were 1.36 and
3 were 1.36 1.6
andtimes higher,
1.6 times respectively.
higher, The
respectively.
VRP of 3S3P
The VRP computed
of 3S3P from from
computed the module OCV showed
the module OCV showeda stripping time oftime
a stripping 24.6 of
min,
24.6which
min,
is 1.3 times less than row 3. This clearly shows the significance of computing
which is 1.3 times less than row 3. This clearly shows the significance of computing row row wise
VRPs, ratherrather
wise VRPs, than one
thanfrom
one module OCV. To
from module investigate
OCV. the varied
To investigate levels of
the varied plating
levels within
of plating
3S3P, the surface temperature and charging current of each cell are
within 3S3P, the surface temperature and charging current of each cell are analyzed analyzed and given
and
in Figure
given 10.
in Figure 10.

Table 2. Stripping
Table 2. Stripping time
time from
from VRPs
VRPs of
of3S3P.
3S3P.

Module Name
Module Name Details
Details Stripping Time
Stripping Time (Min)
(mins)
1S3P-1
1S3P-1 OCV
OCVfrom ISO224(V_H)
from ISO224 (V_H) 19.8
19.8
1S3P-2
1S3P-2 OCVfrom
OCV from ISO224
ISO224 (V_M)
(V_M) 27
27
1S3P-3 OCV from ISO224 (V_L) 31.8
1S3P-3 OCV from ISO224 (V_L) 31.8
3S3P Module OCV from cycler 24.6
3S3P Module OCV from cycler 24.6
Current and temperature variation during the CC phase is focused on here. A tem-
Current
perature and temperature
gradient variation
of 1 ◦ C is observed during
within the the CC phase
module beforeis1Cfocused on here.
charging; A tem-
this may be
perature
due gradient ofcirculation
to non-uniform 1 °C is observed
withinwithin the module
the chamber. Cellsbefore 1C charging;
in 1S3P-2 and 3 werethisat amay be
lower
due to non-uniform
◦ circulation within the chamber. Cells in 1S3P-2 and
temperature (<0 C) than 1S3P-1. Furthermore, during charging the rise in temperature3 were at a lower
temperature
(∆T) is small (<0 °C) thanThe
for 1S3P-3. 1S3P-1. Furthermore,
dependence of LP onduring charging[19,20]
temperature the rise in temperature
favored more LP,
and this resulted in the extended stripping time in Table 2. In the case of 1S3P-2,more
(∆T) is small for 1S3P-3. The dependence of LP on temperature [19,20] favored LP,
though
and this resulted in the extended stripping time in Table 2. In the case
the cells were initially at lower temperature, during charging the ∆T increased. of 1S3P-2, though
the cells were initially at lower temperature, during charging the ∆T increased.
Energies 2023, 16, x FOR PEER REVIEW 11 of 15
Energies 2023, 16, 2537 11 of 15

Current(A)

Current(A)

Current(A)
Temperature( oC)

Temperature( oC)

Temperature( oC)
10. Charging current and surface temperature of cells in 3S3P, 1C0 at ◦
Figure
Figure 10. Charging current and surface temperature of cells in 3S3P, 1C at °C.0 C.

The relative SoC of each cell in 3S3P is computed based on RPT-3 as per Equation (3)
The relative SoC of each cell in 3S3P is computed based on RPT-3 as per Equation (3)
and given in Table 3.
and given in Table 3.
SoC_3S3PRelative
𝑆𝑜𝐶_3𝑆3𝑃 (%) (= %) 𝐶_3𝑆3𝑃 × 100
= (C_3S3P/C_RPT3) ×100 (3) (3)
𝐶_𝑅𝑃𝑇3

3. Relative ◦
Table
Table 3. Relative SoC SoC of cells
of cells in 3S3P
in 3S3P afterafter 1C charging
1C charging at 0 at
°C.0 C.

Module
Module 1S3P 1S3P
1 1 1S3P1S3P2 2 1S3P1S3P3 3
Cells Cells cell1 cell1
cell2 cell2
cell3 cell3cell4cell4cell5cell5
cell6cell6cell7cell7cell8cell8cell9cell9
𝑆𝑜𝐶_3𝑆3𝑃
SoC_3S3PRelative 85.07 85.07
(%) (%) 86.43 86.43
84.0784.0789.0389.03
85.1685.1681.9781.9784.7184.71
86.3986.3983.9483.94

𝑆𝑜𝐶_3𝑆3𝑃
The The SoC_3S3PRelative datadata
in Table 3 suggest
in Table 3 suggestcell cell
unbalance
unbalance in 3S3P. Yet,Yet,
in 3S3P. the average
the average
of cell
of cell SoCs within each row of 3S3P is 85.19, 85.38, and 85.01%. Similarly, standard
SoCs within each row of 3S3P is 85.19, 85.38, and 85.01%. Similarly, the the standard
deviation of cell
deviation SoCs
of cell SoCsin each row
in each rowis is
1.18,
1.18,3.53,
3.53,and
and1.25%.
1.25%.Cells
Cellsin in1S3P-1
1S3P-1 andand 33 are
are relatively
rela-
tively balanced compared with 1S3P-2. During charging, the voltage
balanced compared with 1S3P-2. During charging, the voltage of 1S3P-3 reached the CC of 1S3P-3 reached
the CC
limitlimit (4.2First,
(4.2 V). V). First,
this wasthissensed
was sensed by the
by the BMS, and BMS, and subsequently,
subsequently, the cycler the cyclerfrom
changed
changed
CC tofrom CC to CV mode.
CV mode.
The The
1S3P-1 and and
1S3P-1 3 were at a at
3 were lower voltage
a lower and and
voltage laterlater
at a at
CVa limit
CV limit of 0.15C charging
of 0.15C charging
stopped. This led to the unbalance in cell SoCs at lower ambient
stopped. This led to the unbalance in cell SoCs at lower ambient temperatures. Also, temperatures. Also, the the
variations in the test jig connections and parasitic resistances changes
variations in the test jig connections and parasitic resistances changes the current flow the current flow
within
withinmodule. Although
module. Although care care
has been
has beentaken to minimize
taken to minimize the error
the errorin measurements,
in measurements,
minor errors
minor in current
errors in current measurement
measurementcan canaffect
affectthethe computations based basedon onKCL
KCLand, and,when
when aggregated
aggregated during
during coulomb
coulomb counting,
counting, cancan
leadleadto to variations
variations in in
cellcell SoCs.
SoCs.
The The
rest rest
phase phase current
current afterafter charging
charging was was comparable
comparable withwith the results
the results fromfrom the 1S3P
the 1S3P
experiment as seen in Figure 8b. The dynamics in current
experiment as seen in Figure 8b. The dynamics in current flow and OCV were correlated, flow and OCV were correlated,
and and
afterafter stripping
stripping the currents
the currents stabilized
stabilized and and continued
continued to flow
to flow tillend
till the the of
end of4the
the 4 h rest.
h rest.
The The dynamics
dynamics in current
in current andand OCV OCV
duringduring relaxation
relaxation are depicted
are depicted in Figure
in Figure 11. 11.
Energies 2023, 16, x FOR PEER REVIEW 12 of 15

Energies 2023, 16, 2537 12 of 15

1S3P-1
4.18
OCV I-Cell2
4.16 I-Cell1 I-Cell3 50

4.14
0
4.12

4.1 -50

4.08
0.2 0.4 0.6 0.8 1 1.2 1.4
Time(Hrs)
1S3P-2
4.2
OCV I-Cell5
4.18 I-Cell4 I-Cell6 50

4.16
0
4.14

4.12 -50

4.1
0.2 0.4 0.6 0.8 1 1.2 1.4
Time(Hrs)
1S3P-3
4.18
OCV I-Cell8
I-Cell7 I-Cell9 50
4.16

4.14
0
4.12

4.1 -50

4.08
0.2 0.4 0.6 0.8 1 1.2 1.4
Time(Hrs)
Figure 11. OCV and rest phase currents in 3S3P after 1C charge at 0 ◦ C.

The
Figure 11. rest
OCVperiod current
and rest phase flow in 1S3P-3
currents in 3S3Pin Figure
after 11 was
1C charge at significantly
0 °C. higher than when
the same cells were tested as an independent 1S3P in Figure 8b. The cells in 1S3P-3, when
The
tested rest periodshowed
individually, currentlower
flow stripping
in 1S3P-3time,
in Figure
as seen11inwas significantly
Figure higher
5. These cell than
variations
when the same
can induce cells
varied were
levels oftested
LP for as an within
cells independent
1S3P-3 1S3P in Figure
and lead 8b. The
to distinct restcells
phaseincurrents.
1S3P-3,
when tested individually,
The arrowhead in Figure 11 showed
specifieslower
the stripping
end of thetime, as seeninin
dynamics Figureand
current 5. These
relatescell
to
variations
the end ofcanthe induce
voltagevaried levels
plateau. Theofcells
LP for cells within
in 1S3P-3 were1S3P-3
chargedandto lead to distinct
similar rest
SoCs, with
phase currents.
a deviation The 1.25%
of only arrowhead
from in Figure
the mean,11yetspecifies the end
the current of during
flow the dynamics
the restinphase
currentis
prevalent.
and relatesAs
to these
the end cells
of experienced varied levels
the voltage plateau. of plating,
The cells in 1S3P-3thewere
voltage plateau
charged to of each
similar
duringwith
SoCs, restamay have been
deviation distinct,
of only 1.25% and
fromthis
theled to the
mean, yetdynamics
the currentinflow
current flow,the
during asrest
the
parallel
phase is connection
prevalent. Asforces
thesecell voltages
cells to be same.
experienced varied levels of plating, the voltage plateau
of each during rest may have been distinct, and this led to the dynamics in current flow,
4. Future
as Works
the parallel connection forces cell voltages to be same.
4.1. Evaluation on Different Cell Chemistries
4. Future Worksconducted here focused on cells with NCA as the cathode material. Though
The study
the VRP
4.1. should
Evaluation onideally work
Different Cellfor any cells with graphite anode, it is to be studied in detail
Chemistries
for other cell chemistries and material ratios. The comparison of the relaxation behavior
The study conducted here focused on cells with NCA as the cathode material.
of different chemistries is not yet studied and compared. Another important aspect to
Though the VRP should ideally work for any cells with graphite anode, it is to be studied
consider is the influence of differently aged cells within a module.
in detail for other cell chemistries and material ratios. The comparison of the relaxation
behavior of different chemistries is not yet studied and compared. Another important as-
pect to consider is the influence of differently aged cells within a module.
Energies 2023, 16, 2537 13 of 15

4.2. Module Formats, Representative Bus Bars, and Interconnections

The results from testing individual 1S3Ps and when they were in series to form 3S3P
showed variations in charging currents and lithium stripping. This clearly suggests the
dependence of LP and anode potential on module formats and interconnections. The
efficacy of the VRP for lithium stripping detection when more cells are connected in series-
parallel are to be investigated and substantiated.
The scale-up performed for the study utilized generic jigs to facilitate additional
current and voltage measurements, and the effect of parasitic circuit parameters were
noticeable. A battery module with actual bus bars, interconnections, and with multi sensor
array boards for measurements discussed in [16] can drastically reduce these and aid in
future assessments.
One of the main challenges is to have accurate current measurements during cycling
and during rest. The sensors utilized should be capable of measuring current in the range
of milliamperes during rest and measure large currents up to 1C. A single sensor might not
be feasible for this. Hence, a combination of sensors with different ranges could be utilized.
The sensitivity and accuracy of voltage measurement is equally important, as the whole
VRP analysis depends on it.

4.3. Temperature Gradient within the Pack

It is evident from the experiment results and existing literature that LP is highly influ-
enced by temperature. The study here focused on cells/modules kept in an environmental
chamber and ambient temperature was maintained constant as much as possible. Tem-
perature gradients in a battery pack could be due to unbalanced charging or even due
to ineffective cooling mechanisms. Cells tend to degrade within a parallel system due to
uneven current distribution [21], and the temperature gradient [22] is a prime factor for this.
As considered by Zilberman et al., a much larger temperature gradient could be induced
within a small module in a controlled environment and the occurrence of voltage plateau
and stripping could be studied.

5. Conclusions
The study presented here focused on assessing the ability of the VRP to detect LP
for cells and cells in series-parallel connections. The test conditions considered various
charging scenarios and temperatures, with current flow measurements within the battery
modules. It was found that the VRP detects lithium stripping associated with LP even if
cells are not ideally in open circuit. The transferability of the VRP from individual cells to
modules proved to be feasible. However, the detection capability and sensitivity of the VRP
at the module level was severely reduced in comparison to single cell tests. Low levels of
LP did not show any plateaus in the OCV during rest. The promising results obtained from
the study were limited to lower temperatures and a high Crate , both are known to cause
severe plating. This result implies that BMS algorithms designed and calibrated within a
laboratory using single cell experiments will need to be recalibrated for deployment on
multicell systems relative to the actual architecture of the battery pack employed.
FC strategies usually incorporate Crates well above 1C and gradually reduce based
on SoC and temperature during charging. Hence, for such studies the VRP will be useful,
particularly for temperatures lower than 5 ◦ C. The VRP could be scaled and used within
a BMS as a tool to detect LP. Yet, the role of it in a BMS is limited and it can only act as a
binary indicator of LP. As seen from the results, analyzing a single voltage plateau from
module OCV may lead to inaccurate estimation of LP. It is highly recommended to consider
OCVs of each series branch to distinguish variations within the module. These voltages are
normally measured by BMS to find the highest and lowest cell voltages in a pack.
For high temperatures and a lower Crate , the VRP failed to provide necessary insights
and the incidence of LP could be misinterpreted. The VRP of single cells and cells in parallel
for the study in [17] were comparable. However, the experimental results presented here
disagree with the findings. One reason for this is the calendar ageing of cells; cells from
Energies 2023, 16, 2537 14 of 15

different manufacturing batches tend to be aged differently. Furthermore, the cathode and
anode thickness also play a vital role in LP. Small deviations in these can lead to different
stripping behavior and VRPs. The detection capability of the VRP is known to improve
when cut-off current in the CV phase is adjusted appropriately. The influence of this on
cells in series-parallel connection is a topic that needs to be researched.

Author Contributions: Conceptualization, N.S., N.F.S. and J.M.; methodology, N.S. and N.F.S.;
validation, N.S.; formal analysis, N.S.; investigation, N.S. and N.F.S.; resources, J.M.; data curation,
N.S.; writing—original draft preparation, N.S. and N.F.S.; writing—review and editing, J.M. and
T.Q.D.; supervision, J.M. and T.Q.D. All authors have read and agreed to the published version of
the manuscript.
Funding: This research is supported by Innovate UK through the Electric BSA (eBSA), Project
Number: 75281.
Data Availability Statement: The data presented in this study are available on request from the
corresponding author.
Acknowledgments: The authors record their sincere gratitude to James Mathew, project engineer at
WMG, for his contributions during module testing.
Conflicts of Interest: The authors declare no conflict of interest.

Abbreviations

LP Lithium plating
FC Fast charging
VRP Voltage relaxation profile
CC Constant current
CV Constant Voltage
Crate Charging rate
OCV Open-circuit voltage
RPT Reference performance test
1S3P 1 cell in series and 3 in parallel
3S3P 3 cells in series and 3 in parallel
BMS Battery management system

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