Journal of Power Sources 582 (2023) 233519

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Journal of Power Sources

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Rational designs to enable 10-min fast charging and long cycle life in
lithium-ion batteries
Tanvir R. Tanim a, *, Sangwook Kim a, Andrew M. Colclasure b, Zhenzhen Yang c, Kevin Gering a,
Peter J. Weddle b, Michael Evans a, Eric J. Dufek a, Yulin Lin d, Jianguo Wen d, Francois Usseglio-
Viretta b, Alison R. Dunlop c, Stephen E. Trask c, Kandler Smith b, Brian J. Ingram c,
Andrew N. Jansen c
a
Energy Storage and Electric Transportation Department, Idaho National Laboratory, Idaho Falls, ID, 83415, USA
b
Energy Conversion and Storage Systems Center, National Renewable Energy Laboratory, Golden, CO, 80401, USA
c
Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, 60439, USA
d
Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, 60439, USA

H I G H L I G H T S

• Combining multiple solution strategies is the key to enable 10-min fast charging.
• Achieved 600 10- min fast charge cycles with 87.3–92.1% charge acceptance.
• Charge speed remained up to 27 mi/min without lithium plating.
• Driving range equates to 171,00–181,000 miles with aging between 11.5 and 13.9%.
• The study highlights pathways to enable 10-min fast charge in energy-optimized cells.

A R T I C L E I N F O A B S T R A C T

Keywords: A daunting challenge in the design of lithium ion batteries (LiBs) is enabling 10-min extreme fast charging (XFC)
Lithium-ion battery while achieving appreciable charge acceptance and cycle life. This desirable outcome requires both a compre­
Extreme fast charging hensive understanding of LiB operation and aging behavior at different length scales and careful optimization.
Lithium plating
Lithium plating has been a critical bottleneck because, at XFC rates, it consumes cyclable lithium causing distinct
Electrolyte
aging and safety concerns even in moderate-loading LiBs. We propose combining multiple solutions, including
Charging protocol
materials-to-electrode design-to-charging protocols, that are intended to overcome limitations in lithium-ion
transport in the electrolyte phase, thus enabling 10-min XFC in LiBs. Some implemented strategies include
cathode chemistry, optimized carbon binder domain in the cathode, dual layer anode design, improved separator
and advanced electrolyte. Further, innovative charging protocols in moderately loading (∼ 3 mAh/cm2 anode/
2.7 mAh/cm2 cathode) single-layer pouch cells are proposed, together with demonstrated 10-min XFC with
higher charge acceptance between 87.3 and 92.1% (or 2–2.1 mAh/cm2) for 600 cycles without lithium plating.
This methodical study with well-defined cells shows promise in combining multiple solution strategies to enable
10-min XFC, charting a pathway to achieve XFC in higher-loading energy-optimized LiBs.

powered EV adoption [1,2]. A 10-min fast charge, however, would

1. Introduction
Fast charging of batteries (i.e., within 10 min), defines extreme fast
charging (XFC), a capability that is highly desirable to electric vehicle
(EV) owners and considered a necessary catalyst for widespread battery-
require a charging rate of ~6C (roughly equivalent of 6 × the nominal
capacity of current, 1C batteries). This represents significant advances
over existing fast-charging practices (e.g., up to 2C, bound by a 30 min
charge time) [3]. Charging a LiB at ~6C triggers aging mecha­
nisms—notably lithium plating, particle cracking, and surface and

* Corresponding author.
E-mail address: Tanvir.Tanim@inl.gov (T.R. Tanim).

https://doi.org/10.1016/j.jpowsour.2023.233519
Received 13 June 2023; Received in revised form 26 July 2023; Accepted 14 August 2023
Available online 23 August 2023
0378-7753/© 2023 Elsevier B.V. All rights reserved.
T.R. Tanim et al.
List of abbreviations
AM Active material
BOL Beginning of life
CAMP Cell Analysis, Modeling, and Prototyping (Facility)
CBC Cycle-by-cycle
CBD Carbon binder domain
CC Constant current
CEI Cathode electrolyte interphase
CV Constant voltage
DLA Dual-layer anode
DOE Department of Energy
EC Ethylene carbonate
EIS Electrochemical impedance spectroscopy
EOCV End-of-charge rest voltage
EV Electric vehicle
interphase issues—that cause LiBs to reach the end of their useful lives
prematurely. Thus, enabling a 10-min XFC in LiBs with a desired cycle
life is an active area of research [4–10].
The performance bottlenecks and degradation modes and mecha­
nisms associated with XFC have been well-characterized and docu­
mented in the last several years [6,11–18]. However, some pathways to
mitigate these performance bottlenecks and aging effects have recently
emerged [8,12,13,19–23]. Using low-loading cell designs (e.g., 1.9
mAh/cm2 anode), solid-phase diffusion of anode particles was shown
not to be a limiting factor for XFC if Li+ could be supplied to the elec­
trode interface [9,10,24]. Sluggish transport of Li+ through
electrolyte-filled porous medium has been identified as one of the key
bottlenecks causing Li+ depletion (at the anode) or enrichment (at the
cathode) during XFC [13,25]. Such ion depletion or enrichment yields
concentration gradients known as electrolyte-concentration polarization
across a cell, and this can result in distinct voltage loss at both elec­
trodes, subsequently driving the anode potential toward the Li-plating
regime and lower charge acceptance [13,25]. As it is expected to
enable XFC in energy-optimized cells with >4 mAh/cm2 anode loading,
Li+ transport issue and the resultant plating would likely be a key
bottleneck for XFC. These difficulties would require effective mitigation
strategies. Besides Li plating, XFC can trigger cathode degradation (e.g.,
particle cracking and surface-interphase issues) after hundreds of cycles,
and this can distinctly affect battery performance and life [13,24].
Effective solution strategies must consider mitigating both anode- and
cathode-performance bottlenecks, as well as key short- and long-term
degradation issues to enable 10-min XFC.
Researchers have proposed different strategies to alleviate the slug­
gish Li+ transport. Tanim et al. showed that the higher Ni variant of
lithium nickel manganese cobalt oxides (NMC) chemistry (NMC811)
performed better than its low Ni counterpart (NMC532) in both per­
formance and lifespan due to NMC811’s superior physiochemical and
structural properties that effectively reduce overall overpotential at
higher rates [9,10]. Usseglio-Viretta et al. showed that optimizing
electrode compositions can improve Li+ transport behavior and induce
lower overpotential [19]. These authors attribute this improvement to
lower cathode impedance, reduced electrode tortuosity and cathode
thickness [19]. Others have extensively modeled electrodes with sec­
ondary pore networks to provide an anisotropic transport freeway to ion
diffusion. Secondary pore networks can be achieved through
co-extrusion, laser ablation, or freeze-casting [26,27]. Mai et al.
conclude that advanced electrode architecture with secondary pore
networks can increase the fast-charging capability of a LiB [26]. Others
have noted that multilayer electrode designs perform better than single
homogeneous electrode designs and provide incremental benefits in
achieving XFC [27–29].
2
Journal of Power Sources 582 (2023) 233519
LAM Loss of active material
LiB Lithium-ion battery
LLI Loss of li inventory
MSR Material stress reduction (charge protocol)
NE Negative electrode
NMC532 LiNi0.5Mn0.3Co0.2O2
NMC811 LiNi0.8Mn0.1Co0.1O2
PE Positive electrode
RCT Rate capability test
RPT Reference performance test
SEI Solid electrolyte interphase
SEM Scanning electron microscopy
SLPC Single-layer pouch cell
TEM Transmission electron microscope
VR Voltage ramp
XFC Extreme fast charging
Innovative electrolyte formulation—tailored to improve Li + trans­
port properties to facilitate XFC—is another active area of research [25].
Replacing carbonate-based solvents and/or modifying their related
compositions with alternative solvents—such as ethers or nitriles—have
been shown to provide some benefits [30–34]. Gao et al. advocate using
multisolvent systems, which, with careful optimization, have shown a
balanced set of properties conducive to XFC [8]. Other researchers have
resorted to replacing the LiPF6 salt (e.g., with TFSI) to improve Li+
transport [35].
Besides material and electrode-level design modifications, tuning
operational conditions and charging protocols have been shown to
facilitate XFC and reduce degradation. Dufek et al. presented an exten­
sive review of XFC protocols that were designed using advanced phys­
ically derived models and electrochemical and secondary
characterization methods to account for different material constraints,
including lithium plating and cathode-particle degradation [12]. Some
of the novel charging protocols have been shown to increase energy
acceptance by up to three times more than constant current
(CC)-constant voltage (CV) protocols [12]. Partial charging, which
limits the charge acceptance between 80 and 90%, is another avenue
that has been shown to effectively reduce Li plating and cathode
degradation, even at aggressive charging rates [9,10]. Operating cells at
temperatures sufficiently higher to improve transport and kinetics are
suggested as another strategy for improving fast-charging performance
by lowering the tendency toward Li plating [23,25,36,37].
We propose that none of the presented solution strategies alone
would successfully enable XFC for energy-dense cells with high-loading
electrodes. Instead, a combination of strategies that improves lithium-
ion transport could realize XFC in an energy-optimized cell with
desired performance and life [38]. As proof, we implemented multiple
solutions—cathode chemistry, optimized carbon binder domain (CBD)
in the cathode, dual layer anode design in anode, advanced electrolyte,
and innovative charging protocols—in single-layer pouch cells to
demonstrate XFC (up to 6C in 10 min) can be realized for hundreds of
cycles while minimizing the key degradation modes and mechanisms.
2. Methodology
2.1. Experimental
2.1.1. Cell design
The Cell Analysis, Modeling, and Prototyping (CAMP) Facility at
Argonne National Laboratory built 21 single-layer pouch cells (SLPC-
xx3450 format) with three design variants, described in Table 1). The
design variants are determined based on earlier analysis and testing
observations [8,13,19,25,26,39] and are summarized below:
T.R. Tanim et al. Journal of Power Sources 582 (2023) 233519

Table 1
Cell grouping based on designs and charge protocols.
Cell build RCT Cycle Design Modification Charge Protocol Total Charge Time (min)

R2-Gen2 1 Mono layer anode 1–8C, 3–4.1V Variable

R2-Gen2 3 2.6 mAh/cm2 90% AM cathode 6C CC-CV, 3–4.1V 10
Gen2 electrolyte
Celgard 2320 separator

R2+-Gen2 1 DLA 1–8C, 3–4.1V Variable

R2+-Gen2 3 2.7 mAh/cm2 96% AM cathode MSR, 3–4.15V 10
R2+-Gen2 3 Gen2 electrolyte VR, 3–4.15V 10
Celgard 2500 separator

R2+-B26 1 DLA 1–8C, 3–4.1V Variable

R2+-B26 3 2.7 mAh/cm2 96% AM cathode 6C CC-CV, 3–4.1V 10
R2+-B26 3 B26 electrolyte MSR, 3–4.15V 10
R2+-B26 3 Celgard 2500 separator VR, 3–4.15V 10

RCT = Rate capability test, VR = Voltage ramp charge protocol, MSR = Material stress reduction charge protocol.

I. R2-Gen2: a 70 μm, 38.2% porous, 91.8% active material (AM) variation.

mono-layer anode with 2.8 mAh/cm2 loading; a 59 μm, 34.5%
porous, 90% AM cathode with 2.6 mAh/cm2 loading, a Celgard
2320 separator; and Gen2 electrolyte (1.2 M LiPF6 in a 3:7 by wt.
ethylene carbonate (EC): ethyl methyl carbonate electrolyte
[Gen2]).
II. R2+-Gen2: a 72 μm, 25–45% porous, 91.8% AM dual-layer anode
(DLA) with 3 mAh/cm2 loading; a 53 μm, 35.2% porous, 96% AM
cathode with 2.7 mAh/cm2 loading; a Celgard 2500 separator,
and Gen2 electrolyte.
III. R2+-B26: the R2+ electrode designs described as Variant II, with a
Celgard 2500 separator, and using B26 electrolyte [EC: DMC:
DEC: EP: PN (20:40:10:15:15) w/(3%VC, 3%FEC)] + 1.25 M
LiPF6. The B26 electrolyte was reported in greater detail in
Ref. [8].
One cell from each group was used to perform a rate-capability test
(RCT) that included CC-CV charges at different charging rates (or C-rates
based on C/1 capacity at BOL) up to 8C, with a 4.1V cutoff, as shown in
Table 1. After every charge step during RCT, a 15 min rest was allowed
to capture important information about cell impedance and transport
polarizations. Impedance polarization captures the ohmic, and charge-
transfer impedance is obtained from the immediate voltage drop
(within ~12 ms) after each charging step [24,25]. Transport polariza­
tion includes combined Li+ transport-related losses in liquid and solid
phases and is derived from the voltage drop between 12 ms and 15 min
[24,25]. Impedance and transport-polarization measurements contain
useful information about the fast-charge performance bottlenecks of LiB,
provide necessary input data for charge-protocol development, and have
been discussed extensively in earlier publications [13,24,25,39].

For the baseline R2-Gen2 design, SLC 1506T graphite (D50 = 7–10
μm) from Superior Graphite, LLC, with 91.83% AM content is used. For
the DLA design, SLC 1506T Superior Graphite material with 91.83% AM
content is used for the first layer, and LM2803 graphite (D50 = 3.1 μm)
from American Energy Technology Company (AETC) is used for the
second layer (see SI, Fig. S1). LiNi0.8Mn0.1Co0.1O2 (NMC811, D50 12.5
μm) from Targray is used in all cell builds. All R2+ designs used a
monolayer Celgard 2500 separator with higher porosity (i.e., 55%) as
opposed to the trilayer Celgard 2320 with lower porosity (39%) in the R2
design. Details about the materials, cell designs, build conditions, and
beginning-of-life (BOL) performance are delineated in Supplemental
Tables T1–T3, respectively.
The cells underwent formation and subsequent degassing at the
CAMP facility and were then shipped to Idaho National Laboratory (INL)
for cycle-life evaluation and aging-mode analysis. INL developed the
design of experiments, conducted the cycle-life study and aging-mode
analyses, and confirmed the aging modes with targeted teardown and
electrochemical evaluations in the coin cells. Selected samples were then
sent to Argonne for post-test evaluation to gain more insight into aging
mechanisms.
2.1.2. Initial characterization and fast charge cycling
Upon receipt, INL performed some initial evaluations to quantify
BOL cell-to-cell variation. The cells were fixtured to apply 15–30 kPa
pressure (see Ref. [24] for fixturing details). The fixtured assembly was
then placed in a thermal chamber (TestEquity 1007C) at 30 ± 1 ◦ C. A
MACCOR Series 4000 automated test system was used for all
charge-discharge tests. A Solartron 1287 potentiostat and analyzer,
Model 1260, were used for electrochemical impedance spectroscopy
(EIS) measurements. Table T3 lists the average and 1σ standard devia­
tion of different metrics—such as mass, open circuit voltage, and
high-frequency impedance—in the as-received cells. These show a tight
spread; measured capacities at C/20 and C/1 also show lower cell-to-cell
2.1.3. Charge-protocol development
Table 1 lists different charge protocols and upper charge-cutoff
voltages evaluated in this study. Besides the standard 6C CC-CV, two
advanced-charge protocols—namely, voltage ramp (VR) and material-
stress reduction (MSR)—are developed and evaluated [3]. These
charge protocols are summarized as follows:
• 6C CC-CV Protocol: CC charged at 6C up to 4.1V, then CV charged at
4.1V until a 10-min total charge time (CC + CV) has elapsed. First-
cycle voltage and current progression during 6C CC-CV charge pro­
tocol is provided in SI Figure S3(a).
• VR Protocol: CC charge at 7C to 4.06V, voltage ramp at 3.5 mV/10s
(or 0.35 mV/s), with 4.15V upper limit. Go to CV@4.15V step and
continue charging until the total charge time reaches 10 min. The
Newman model is used to derive the VR charge protocol using BOL
and RCT test data for the final cell builds, as reported by Mai et al.
[20]. The protocol was selected to give adequate buffer to avoid
lithium plating with 5% capacity improvement over conventional 6C
CC-CV. See “Additional information on charge protocol develop­
ment” in the supplemental section for more information. First-cycle
voltage and current progression during 6C CC-CV charge protocol
is provided in SI Figure S3(b).
• MSR Protocol: This protocol uses a series of CC steps to maximize the
CC phase and minimize cell overpotential as charging progresses.
This strategy helps maximize charge acceptance and reduce over­
potential while lowering the mechanical and electrochemical
stresses on the materials within the cell. MSR protocol is a refined
and more-granular version of this research team’s earlier multistep
charge protocol [6], except applying the highest current (6.7C) in the
mid-state-of-charge range when cell overpotential remains the
lowest. Each current step of the MSR protocol is 30 s. If 4.15V is
reached before 10 min, the cell enters a CV step at 4.15V. The full
description is provided in “Additional information on charge

3
T.R. Tanim et al.
protocol” in the supplemental section. First-cycle voltage and current
progression during 6C CC-CV charge protocol is provided in SI Figure
S3(c).
2.1.4. Cycling
The following cycling loop was used to cycle all the cells:
• C/2 discharge, 15 min rest, charge to 4.1V/4.15V using 6C CC-CV,
VR, or MSR charge protocol, rest for 15 min
• Each cell accumulated 600 cycles with reference performance tests
(RPTs) at predefined and uniform cycle counts.
2.1.5. Reference performance tests
A slow-rate C/20 charge-discharge test between 3 and 4.1V and an
EIS test at 3.8V were performed as part of reference performance tests to
quantify the individual cell’s state of health.
2.1.6. Post-testing
• Electrochemical Characterization: INL performed targeted testing to
quantify the electrochemical performance and aging in the elec­
trodes at different cycling intervals using electrodes harvested after
the protocols were run. The harvested electrodes were coordinated
between INL and Argonne; i.e., the electrodes were cut vertically at
the middle of each full electrode, and INL kept half of each electrode,
and Argonne received the remaining half. Either Li/NMC811 or Li/
Gr half cells were used to quantify change in electrode performance.
Prior to tear-down, the SLPCs were discharged to 3V at C/2, followed
by a CV hold for 2h or until a C/50 current was achieved. The cells
were then torn down in an Ar-filled glovebox. Following that, the
electrodes were washed twice with excess EMC for 1 min each and
dried at ambient temperature in the glovebox. The dried electrodes
were then used to build CR2032 coin cells with a 1.27 cm diameter
working electrode, and a 1.43 cm diameter 170-μm-thick Li refer­
ence negative electrode. INL punched three electrode samples
(cathode or anode) from the middle sections of the half electrodes.
Fresh electrolyte and separator, as shown in Table 1, were used in the
coin cells. The coin cells went through three C/10 charge-discharge
formation cycles between 2.8 and 4.3V, for Li/NMC811, or 0.005V
and 1.5V for Li/Gr, followed by EIS testing at 3.9V (for Li/NMC811)
or 0.1V (for Li/Gr). Another C/20 charge-discharge cycle was per­
formed after the EIS test to measure the capacity at degraded states.
The performance of the harvested cells was compared with similarly
built coin cells with fresh electrodes.
• Physical Characterization: Cross-sectional anodes were prepared
using Ar + ion beam at 4 kV for 6 h with a cross-section polisher,
located in CAMP in a dry room. The cross-sectioned samples were
loaded onto the airtight holder to minimize air and moisture expo­
sure during transfer. After the sample was mounted, the sealed
holder was evacuated before it was inserted into the scanning elec­
tron microscopy (SEM) chamber. The JEOL JSM-6610LV SEM in­
strument was used to image the generated cross-section samples.
Transmission electron microscopy (TEM) using ACAT, an FEI Titan
80–300 instrument equipped with the capability to correct both
spherical and chromatic aberrations was performed at Argonne to
characterize the surface features of cathodes selected at various cycle
conditions. ACAT was used to capture electron energy-loss spec­
troscopy data while it was running in image-coupled scanning/
transmission electron microscopy mode at 200 kV. Ar + ion-milling
with an accelerating voltage of 4 kV and ion-milling polishing with
an accelerating voltage of 0.3 kV were used to prepare the TEM
specimens.
2.2. Modeling
A previously reported electrochemical macro-homogeneous
4
Journal of Power Sources 582 (2023) 233519
Newman model was used to suggest changes that could be made to cell
builds to improve fast-charge performance [8,25]. The baseline R2
predictions used parameters for 1506T graphite, NMC532 cathode, and
Gen2 electrolyte materials, as reported in Ref. [25]. The effect of
changing active cathode material was investigated using model pa­
rameters for open-circuit potential, solid-state diffusion coefficient, and
exchange current density of NMC811 [9]. The porosity and thickness of
the Celgard 2320 was assumed to be 40% and 20 μm while the Celgard
2500 separator was taken to be 55% porous and 25 μm thick. An
important, but difficult to measure parameter for the separators is the
McMullin number. Based on extensive fitting to electrochemical data,
the McMullin number for the Celgard 2320 was estimated as ~9 while
that of the Celgard 2500 was estimated as ~3.3. These values are similar
to direct measurements made by Gasteiger using impedance in a unique
blocking setup [40].
Previously, microstructure modeling tools used by the National
Renewable Energy Laboratory (NREL) suggested lowering the amount of
CBD can improve fast-charge performance by both reducing cathode
thickness and reducing tortuosity and McMullin number [39]. Based on
these tools, the McMullin number for cathodes with 10% CBD is esti­
mated to be ~8, and cathodes with 4% CBD are estimated to be ~6, with
both electrodes having a porosity near 35%. The DLA is represented in
the macrohomogeneous model with distinct porosities and McMullin
numbers for each layer. The low-porosity region next to the current
collector has a porosity of 25% while the McMullin number that is based
on microstructure analysis is estimated to be 15. The high-porosity re­
gion near the current collector has a porosity of 45% and is estimated to
have a McMullin number of 5.5. Transport properties for the Gen2 and
B26 electrolytes are taken from predictions of INL’s Advanced Electro­
lyte Model. The detailed polynomial fits are reported in Ref. [8]. The
Newman model is also used to derive an advanced charge protocol with
voltage ramping for the final cell builds, as reported by Mai et al. [20].
The protocol was selected to give a similar buffer of a couple megavolts
for lithium plating as the standard CC-CV protocol, but it is also pre­
dicted to improve capacity by about 5%. More details about
charge-protocol development can be found in the SI section, “Additional
information on charge protocol development.”
3. Results
3.1. Improvement in fast-charging and plating performance with different
cell-design attributes
Fig. 1(a) and (b) illustrate model predictions for how each change to
the cell build improves fast-charge capacity and lessens lithium-plating
onset with a 3–4.1V voltage constraint. The standard R2 with NMC532
cathode, which was reported on extensively in our earlier publications
[6,14,15,41,42], is predicted to only achieve 36% capacity (scaled by
BOL C/1 capacity) during 6C CC charging, and significant plating is
expected with the graphite anode/lithium plating potential reaching
− 24 mV (see Table SI T4). Changing from NMC532 to NMC811 reduces
cell overpotential due to enhanced kinetics/diffusion for higher Ni
material [9,13] and is predicted to improve 6C CC capacity by about 4%.
Further, due to a thinner cathode design and the associated reduction of
salt-concentration gradients, the graphite anode potential is signifi­
cantly improved: predicted to be − 10 mV. Next, exchanging the Celgard
2320 separator for a Celgard 2500 is predicted to improve CC capacity
by 11% because the minimum graphite anode potential would be
slightly improved. Reducing the CBD in the cathode is projected to
improve capacity by about 4%. Interestingly, the further reduction in
cathode thickness is not projected to significantly enhance graphite
anode potential because severe salt depletion no longer occurs in the
anode when using the Celgard 2500 separator. The DLA anode is ex­
pected to improve capacity by another 5%, which brings the graphite
anode potential to well above 0V at +5.8 mV. Finally, incorporating a
higher-transport B26 electrolyte is predicted to give a 6C CC capacity of
T.R. Tanim et al. Journal of Power Sources 582 (2023) 233519

Fig. 1. (a) Modeled cell voltage evolutions at 6C for different battery designs. (b) Predicted Li plating potentials at 6C.

68% and 10-min CC-CV capacity of 89%, with only very small amounts
of lithium plating predicted from local heterogeneities. A table sum­
marizing the improvements can be found in SI T4.
3.2. BOL 10-min fast-charge performance
Fig. 2 displays the experimental and incremental improvement in
fast-charge performance for different cell-design attributes using
different charge protocols. Fig. 2(a) shows one critical metric,

Fig. 2. (a, b) BOL impedance and transport polarizations, obtained from RCTs for different cell designs between 3 and 4.1V [9]. (c) BOL charge acceptance with
different charging protocols. Charge acceptance is normalized by BOL C/1 discharge capacity between 3 and 4.1V.

5
T.R. Tanim et al.
impedance-polarization voltage, which captures the combined ohmic
and charge-transfer polarization losses at different CC charging rates
during RCT. Impedance polarization trends linearly, but varies distinctly
for different builds. The R2 Gr/NMC532-Gen2 build, which was
described earlier, shows the highest impedance polarization [6,41–43].
Replacing the NMC532 chemistry with NMC811 shows up to a
32–35.5% reduction in impedance polarization for the C-rates investi­
gated. The R2+ electrode design—with optimized CBD in the cathode,
DLA, a Celgard 2500 separator, and the same Gen2 electrolyte—further
reduced the impedance polarization, to between 47 and 52.7% of the
impedance seen in the R2 Gr/NMC532-Gen2 design. As shown in Fig. 2
(a), replacing the Gen2 electrolyte with B26 in the R2+ build showed the
best performance, reducing impedance polarization between 55 and
60.7% of that measured in the R2 Gr/NMC532-Gen2 design.
Fig. 2(b) shows another critical performance metric: transport po­
larization voltage. This measurement captures the combined Li+
transport-related losses in liquid and solid phases. Once again, the R2
Gr/NMC532-Gen2 build shows the poorest performance: having highest
losses, up to 4C, and a distinct plateau after that. The plateau was linked
to distinct nonuniform concentration effects (i.e., depletion of Li+ in the
electrolyte) near the anode-current collector and enrichment of Li+ in
the electrolyte near the cathode-current collector area [13,25]. Earlier
studies also reported Li plating on the anode when cells were
fast-charged at rates within the plateau region [6,15,42]. The R2 build
with an NMC811 cathode shows improved performance: between 30
and 34% up to 4C better than the baseline design. Nevertheless, the
better build still indicates a plateau-like trend once reaching 5C. The R2+
build with the Gen2 electrolyte further improves transport polarization:
between 40 and 48% up to 4C as compared to the R2 Gr/NMC532-Gen2
design. R2+ appears to show the emergence of a plateau after 6C, as well
as switching without showing any distinct plateau up to 8C.
Fig. 2(c) shows the first cycle amp-hr-based charge acceptance (as a
percentage) for the different cell builds with different charging rates and
upper charge-cutoff voltages. The capacity charge (or percentage charge
acceptance) is scaled by BOL C/1 discharge capacity of the respective
cells between 3 and 4.1V. The R2 designs, irrespective of cathode
chemistry, show a comparable charge acceptance of 78% at 6C and 10
min with a 3–4.1V voltage limit. The best-performing build, R2+-B26,
shows a 9.3% increase in total CC + CV charge acceptance in 10 min,
with a 21% reduction in CV charge acceptance under the same voltage
limit.
Because improved performance was both predicted by the pseudo-
two dimensional model and shown in early observations in RCTs, we
studied two advanced charge protocols, VR and MSR, with an expanded
voltage window of 3–4.15V for the R2+ cell designs. Using the R2+
design with a Gen2 electrolyte resulted in an increase in total charge
acceptance—between 9.3% MSR to 11.4% VR—over the R2-Gr/
NMC811 Gen2 design and between 2.1% MSR to 4.8% VR better than
the R2+-B26 design with a 6C 4.1V charge protocol. CV charge accep­
tance reduced to 20.2% and 9.9% for the MSR and VR charge profiles,
respectively, even with a higher charge cutoff of 4.15V. In line with the
polarization data in Fig. 2(a) and (b), the R2+ design with the B26
electrolyte shows the best total charge acceptance, which increases to
between 90.8% MSR and 92.1% VR with the CV portion between 11.6%
MSR to 3.1% VR. When compared to the R2-Gr/NMC811-Gen2 design,
this indicates an increase of 12.8% and 14.1% total charge acceptance,
for MSR and VR, respectively, as well as a reduction of 27.3% for MSR
and of 36.3% for VR in CV charge acceptance.
3.3. Cycle life performance
The R2 design with Gr/NMC532-Gen2 cell build that had up to 78.1%
charge acceptance experienced a distinct capacity fade after 450 cycles
of 6C CC-CV charging between 3 and 4.1V with the three cells exhibiting
fade to between 19.8 and 42% of BOL C/20 capacity. Several publica­
tions have reported these results and identified the key aging modes and
6
Journal of Power Sources 582 (2023) 233519
mechanisms with extensive characterizations at different length scales
[6,14–16,42–44]. Distinct plating-induced loss of Li inventory (LLI) has
been confirmed to be the dominating aging mode responsible for ca­
pacity fade in these cells. The loss of active material (LAM) in the
cathode was minor and limited to (at most) roughly 8% after 450 cycles.
Hence, we do not include the R2-Gr/NMC532-Gen2 cycle-life data in this
article and focus instead on presenting the cycle life data and analysis of
the latest builds presented in Table 1.
Fig. 3 shows the cycle-life performance of different cell builds with
Gr/NMC811 chemistry. Fig. 3(a) compares the 6C CC-CV cycle-life ca­
pacity fade between the R2-Gen2 and the R2+-B26 cell groups, with a
4.1V charge cutoff. Fig. 3(c) and (d) show the EIS spectra at BOL and
after 600 cycles for the same two builds. The average capacity fade in
each build (∼ 9.5%) is significantly lower than in the R2 Gr/NMC532-
Gen2 cell build at 450 cycles, which was between 19.8 and 42% [6,
42]. Interestingly, the average capacity fade between the R2-Gen2 and
R2+-B26 builds overlaps; however, the R2+ build with a B26 electrolyte
shows much less variability in aging (up to 0.2% 1σ standard deviation)
than the R2 build (up to 3% 1σ standard deviation) when employing the
Gen2 electrolyte.
In line with the polarization data in Fig. 2(a) and (b), EIS data at BOL,
as indicated in Fig. 3(c) show the lowest ohmic/bulk resistance with a
high-frequency zero-crossing intercept and the smallest mid- and low-
frequency depressed semicircles in the R2+ design with B26 electro­
lyte, followed closely by the R2+ design with the Gen2 electrolyte.
Ohmic/bulk resistance is the combined resistant effect from the current
collector, electrode, electrolyte, and separator. Thus, the size of the mid-
and low-frequency depressed semicircles can be attributed to solid-
electrolyte interphase (SEI) and cathode-electrolyte interphase (CEI)
processes in the anode and cathodes, respectively [45]. The R2 design
with Gen2 electrolyte shows the highest ohmic resistance and largest
low- and mid-frequency depressed semicircles at BOL, as indicated in
Fig. 3(c).
At the end of 600 cycles, irrespective of cell design, the high-
frequency zero-crossing intercept moved toward the right, and the
low- and mid-frequency semicircles grew, as shown in Fig. 3(b), indi­
cating an increase in ohmic, charge-transfer, and SEI/CEI impedances.
The nearly comparable impedance spectra at 600 cycles for the two
builds suggest that the R2-Gen2 design, despite showing slightly higher
impedance at the BOL, experienced a lower rate of impedance growth as
compared to the R2+-B26 build, as indicated in Fig. 3(d).
Fig. 3(b) and (e) show the aging data of the R2+ builds. These were
cycled using advanced charge protocols (i.e., MSR and VR up to 4.15V
charge-cutoff voltage). Despite cycling up to a 4.15V charge cut off,
these cells experience from 0.3% up to 11.9% higher capacity fade than
the corresponding build cycled with a 4.1V charge cutoff, as shown in
Fig. 3(e). The higher capacity fade can be attributed to the higher
charge-cutoff voltage.
Depending on the electrolyte and charge protocol, the extent of ca­
pacity fade varies. For instance, the R2+ build with B26 electrolyte
outperforms the build of the R2+ with Gen2 for capacity fade cycled for
the MSR protocols. The R2+-Gen2 with the MSR charge protocol aged
23.6 ± 12% (1σ) as compared to the R2+-B26 cell build, which aged only
16.2 ± 5.1%, cycled under the same MSR protocol after 600 cycles.
The R2+ cell builds cycled under the VR protocol show less capacity
fade: between 12.1% in the Gen2 build and 13.9% in the B26 build at
600 cycles. They also show less variability than those cycled under the
MSR protocol, as shown in Fig. 3(b). This indicates an incremental
benefit from an appropriately designed advanced charge protocol. For
the VR profile, the capacity fade after 600 cycles remains within 1.8% in
the R2+-Gen2 and R2+-B26 builds. The R2+-B26 build, however, shows
the lowest aging variability—up to 2.33% aging variability in the Gen2
cells is reduced to no more than 0.4% in the B26 cells.
The EIS results in Fig. 3(e) show a comparable high-frequency
impedance spectra, indicating a comparable ohmic-resistance increase
in all builds after 600 cycles. However, R2+ cells with B26 electrolyte
T.R. Tanim et al.
Fig. 3. (a, b) C/20 Ah-based capacity fade between 3 and 4.1V. (c–e) Impedance data. EIS performed at 3.9V.
show slightly wider mid-frequency depressed semicircles than in the
4.1V condition, as observed in Fig. 3(d), indicating slightly aggravated
anode and cathode surface/interface issues may have presented.
3.4. Dominating aging modes and mechanisms
Our team used multiple techniques and prior observations to classify
and quantify the dominating aging modes and mechanisms, as reported
in greater detail in our earlier publications. First, we used an earlier
developed deep-learning technique to classify the dominant aging
modes in cells tested with different charge protocols [44]. As in this
earlier study, we used synthetic data generated by the
incremental-capacity (IC) model to train a deep-learning model. The IC
model relied on the slow-rate charge-discharge data from the
Li/NMC811 and Li/Gr half cells (CR2032) with the same fresh elec­
trodes and electrolytes—identical to the pouch cells—to create synthetic
data associated with various modes of aging in pairs (e.g., LLI + LAMPE
or LLI + LAMNE). Once trained, the deep-learning classification model
takes experimental IC data for a given cell and cycle number as an input
and provides an output to the category (i.e., LLI + LAMPE or LLI +
LAMNE) that the dominant aging mode belongs to Ref. [44]. The specific
mechanism for LLI (i.e., plating or normal SEI growth), was determined
by evaluating the cycle-by-cycle (CBC) end-of-charge rest voltage
(EOCV) and coulombic efficiency (CE) trends. Earlier research has
correlated these two parameters with the occurrence of Li plating [6,15,
43,46]. Finally, targeted cell teardown was performed to verify aging
modes and mechanisms.
Fig. 4(a) shows the classification results of the deep-learning model
using t-distributed stochastic neighbor-embedding (t-SNE)
7
Journal of Power Sources 582 (2023) 233519
visualization. The t-SNE method converts similarities between data
points to joint probabilities, minimizing the Kullback-Leibler divergence
between the joint probabilities of two-dimensional embedding and even
higher dimensional data and illustrates classification based on the dif­
ferences between synthetic and experimental IC curves [44,47] derived
from the deep-learning model. As shown in Fig. 4, the
synthetic-data-based aging-mode classification is well divided between
the LLI + LAMPE (shown as faded cyan markers) and LLI + LAMNE
(shown as faded pink markers) modes. The deep-learning model outputs
using experimental IC obtained from C/20 discharge tests during RPT
falls onto the LLI + LAMPE classification zone (shown as grey, blue, and
red markers), confirming that LLI + LAMPE was the dominating aging
mode in cells tested up to 600 cycles irrespective of cell design. More­
over, the probability of LLI + LAMPE is calculated and remains very close
to 100% throughout 600 cycles. It is important to note that because we
only provided two choices (i.e., LLI + LAMPE or LLI + LAMNE) to the
deep-learning model, the results do not necessarily imply that LAMNE is
not present—i.e., a minor extent of LAMNE can still be present.
The LLI that consumes the cyclable Li is caused by two distinct
mechanisms: (1) SEI growth, which is a normal aging phenomenon in
LiBs; and (2) Li plating, which is an undesirable aging phenomenon (an
example would be Li- plating caused by fast-charging). A decrease in
CBC CE and an increase in EOCV have been used to detect the occur­
rence of Li plating [6,15,43,46]. A distinct decrease in CE indicates
higher rate of LLI commonly occurs due to Li plating [15,46]. The mixed
potential effect of graphite and electrochemically active plated Li metal
was attributed to the reduction of anode potential, which eventually
leaves the cell at an elevated voltage after relaxation following charge
[6,15,46]. After examining all CBC data, we have identified three trends
T.R. Tanim et al.
Fig. 4. (a) Deep-learning classification. (b) CBC EOCV. (c) CBC CE. (d) Summary of Li plating. Figs. 4 and 5 present corresponding-cell data.
of CBC CE and EOCV, which are shown in Fig. 4(b) and (c). The three
trends are linked with their associated aging mechanisms below:
• Case I: A gradually reducing trend of EOCV and near 100% CE, which
indicates no Li plating, as shown by the R2+-B26 6C 4.1V and R2+-
B26 VR 4.15V cases in Fig. 4(b) and (c).
• Case II: A gradually increasing trend of EOCV and <100% CE, which
indicates Li plating, as illustrated by the R2-Gen2 6C 4.1V case in
Fig. 4(b) and (c).
• Case III: EOCV remains flat, with nearly 100% CE up to a particular
cycle number, after which Case II manifests. This is depicted in the
R2+-Gen2 MSR 4.15V case in Fig. 4(b) and (c). This indicates a point
where Li plating happens after a certain cycling period.
Based on the above observations, we can have early indications as to
which cells experience Li plating; this summary is provided in Fig. 4(d).
Earlier reports concluded distinct heterogeneity in capacity fade in cells
that experience Li plating, which itself happens non-uniformly [6,10,
15]. The relatively large cell-to-cell aging variability in the two condi­
tions (R2-Gen2 6C 4.1V and R2+-Gen2 MSR 4.15V, see Fig. 3(a) and (b)
and Fig. 4(d)] that had largely experienced Li plating is consistent with
earlier reports [6,10,15].
3.5. Post-testing
3.5.1. Optical images and Li deposition
We opened six cells to verify the Li plating conclusions that were
shown in Fig. 4. Optical images of the anode are shown in Fig. 5, and
they provide direct visual evidence of Li plating. Deposited metallic Li
on the graphite-anode surface, if connected electronically, can
8
Journal of Power Sources 582 (2023) 233519
intercalate to graphite matrix through chemical intercalation, can be
stripped back during discharge step following charge, or becomes
disconnected, dead Li, consuming reversible Li and electrolyte [46,49].
Paramesh et al. report that at fast charging rates above 3C, plated Li
predominantly becomes irreversible, dead Li [46]. All cells in this study
were discharged to 3V at C/3 following a 2h constant voltage hold.
Hence, the Li deposits shown in Fig. 5 primarily refer to the irreversibly
disconnected or dead Li.
Two cells from the R2 Gen2 build show Li deposits on a graphite
surface after 600 6C-4.1V cycles. These are shown in Fig. 5(a) and (b).
The R2+ design with B26 electrolyte shows no Li-plating deposits after
600 6C-4.1V cycles, even with a higher fast-charge acceptance of ~78%
(Fig. 5(c)). Therefore, an advanced electrode design with a B26 elec­
trolyte was able to avoid Li plating even at an aggressive 6C charge rate
up to 600 cycles.
Increasing charge-cutoff voltage to 4.15V undoubtedly makes the
charging conditions more aggressive. Our analysis in the prior section
concluded that the build of an R2+ cell design with Gen2 electrolyte
shows some non-uniformity in Li plating behavior—i.e., in two of the
three cells from the R2+-Gen2 group cycled using MSR protocol plates
and in one of three cells from the R2+-Gen2 group that were cycled using
VR plates. This may be due to local heterogeneities (porosity, thickness,
electron conductivity, etc.) in the electrode microstructure driving
small-scale lithium deposition [48]. Fig. 5(d) and (e) also confirm the
presence of Li deposits in two of the cells showing relevant Li-plating
electrochemical signatures (e.g., CBC CE and EOCV). Therefore, the
R2+ design with Gen2 electrolyte may not be sufficient to enable XFC
capability even with advanced charge protocols when charge cut off
voltage is higher (i.e., >4.1V).
The R2+ design and B26 electrolyte, when cycled with this advanced
T.R. Tanim et al.
charge protocol, could avoid Li plating. Fig. 5(f) shows no deposits of Li
when cycled 600 times using the VR protocol with a 4.15V charge cutoff;
this can be taken as evidence to support this conclusion.
3.5.2. DLA structural integrity
Next, we present cross-sectional images of pristine and cycled anode
samples as shown in Fig. 6. All samples show well-defined dual-layer
structure where the smaller-particle layer is at the top and the larger-
particle layer is at the bottom. Fig. 6 shows that even after 600 fast-
charge cycles, the structural integrity of the anode was well-
maintained (i.e., neither delamination nor exfoliation is present).
3.5.3. Electrochemical performance of cycled electrodes
We measured both capacity fade and impedance growth in har­
vested, aged electrodes in (Li/NMC811 and Li/Gr) coin cells. The per­
formance of the aged cells was compared with coin cells built with fresh
electrode and electrolyte. The C/20 capacity fade and EIS spectra are
presented in Figs. 7(a) and (b) for Li/NMC811 cells.
3.5.3.1. NMC811 cathode. Average capacity fade in NMC811 remains
within 4–6% for cells cycled at 6C up to 4.1V. The B26 build shows a
capacity fade slightly higher (e.g., 2% more) than the Gen2 system for
the 6C-4.1V cycling condition after 600 cycles. For the 4.15V conditions,
the R2+ cathode fade was between 3.5 and 4.5% with a Gen2 electrolyte
irrespective of VR or MSR charge protocol. Like the 6C-4.1V condition,
the R2+ build with B26 electrolyte shows an elevated capacity fade of
9.13 ± 3.3% (1σ) at the end of cycling. Therefore, the capacity-fade data
for cycling to 4.15 V indicate that B26 electrolyte may induce slightly
more damage to the NMC811 cathode. EIS spectra in Fig. 7(b) show an
overall increased growth over fresh cells in depressed-semi-circles,
Fig. 5. Optical images of anode samples after 600 cycles. (a and b) R2-Gen2 6C-4.1V, (c) R2+-B26 6C 4.1V (9), (d) R2+-Gen2 MSR 4.15V, (e) R2+-Gen2 VR 4.15V, and
(f) R2+-B26 VR 4.15V. Figs. 4 and 5 present corresponding-cell data. All the cells in this study were discharged to 3V at C/3 following a 2h CV hold.
9
Journal of Power Sources 582 (2023) 233519
which are related to surface/interphase issues, but the difference
among builds remains low. Thus, ranking them conclusively was not
possible.
Fig. S4 shows sub-particle damage to the cathode after 600 fast-
charge cycles. The interprimary particle separation (IPPS)—also
commonly referred to as particle cracking—seems qualitatively indis­
tinct and comparable in all the samples irrespective of electrolyte (e.g.,
Gen2 vs. B26) and voltage conditions (e.g., 4.1V vs. 4.15V). The TEM
images in Fig. S5 show comparable CEI thickness after 600 cycles for the
cathode samples cycled at 6C-4.1V, irrespective of electrolyte. However,
thicker CEI can be observed for the cathode samples cycled at the higher
voltage (4.15V), regardless of the electrolyte used. Moreover, the cath­
ode sample with the B26 electrolyte shows a thicker CEI layer in the
4.15V than its counterpart. We also present the rock-salt layer thickness
between the R2-Gen2 and R2+-B26 cathode samples after 600 cycles, as
shown in Fig. S6. A comparison between the two pieces indicates that
the NMC811 cathode with the B26 electrolyte experiences a much
thicker rock-salt and mixed layer at the interface than does the NMC811
with the Gen2 electrolyte.
3.5.3.2. Anode. Fig. 7(c and d) show the capacity fade and impedance
growth of aged graphite anode samples in coin cells. The R2 and R2+
cells with the Gen2 electrolyte showed evidence of Li deposition, as
indicated in Fig. 5, so we did not test them in the coin cells. Thus, Fig. 7
(c) and (d) only include the R2+ anode sample data with the B26 elec­
trolyte. The R2+ B26 anode samples after 600 6C-4.1V cycles show
minor improvement in performance after 600 cycles (i.e., the capacity
fade is − 3.5%, and depressed semicircles were smaller). The higher-
voltage condition (i.e., 4.15V, with an advanced charge protocol),
shows an increased capacity fade after 600 cycles, but the fade remains
T.R. Tanim et al. Journal of Power Sources 582 (2023) 233519

Fig. 6. Cross-sectional SEM images of DLA: (a) Pristine, uncycled DLA after calendaring, (b) R2+-B26 6C-4.1V DLA, (c) R2+-Gen2 VR 4.15V DLA, and (d) R2+-B26
VR 4.15V DLA.

Fig. 7. (a and b) Cathode capacity-fade and EIS (at 3.9V) data in coin cells (Li/NMC811). (c and d) Anode capacity-fade and EIS (at 0.1V) data in coin cells (Li/Gr).

below 5%. However, the EIS data show a shrunken semicircle after 600
cycles. This verifies the conclusion of the DL model that LAMNE is not a
dominant aging mode for the cells in this study. Still, the slight perfor­
mance improvement (or decrease in degradation) in the anode material
after 600 fast cycles requires further evaluation, characterization, and
validation. This will be a topic for future investigation. We hypothesize
that a small amount of cracking could enable better access to active
graphite material, resulting in higher-capacity and lower charge-
transfer resistance. It might also be due to incomplete electrolyte wet­
ting in the fresh samples, which improved as cycling progressed.

10
T.R. Tanim et al.
4. Discussion
The results and analysis validate that a combination of rational
material, design change, and advanced charge protocols can enable VFC
(≥6C) without lithium plating for hundreds of cycles. The materials and
design changes investigated in this study include switching from the
NMC532 to the NMC811 cathode with optimized CBD, DLA, a separator
with more pore volume, and advanced electrolytes. These material and
design improvements showed a 2.6 × and 2.1 × reduction in impedance
polarization and transport polarization at 6C without signs of Li-plating-
related transport plateau, as observed in Fig. 2, which compares favor­
ably to the performance of Gr/NMC532 cells without those modifica­
tions [41,42,49]. 6C CC charge acceptance increased from 36 to 68%
with a 4.1V limit, as discussed in Section 4, improving Li-plating po­
tential from − 24mV to above zero. The total charge acceptance in the
optimized build increased to 87.3% in 10 min, which is about 9% higher
than Gr/NMC532 and Gr/NMC811 cell builds without optimization, but
with a CC-CV 6C-4.1V charge protocol.
The 6C-4.1V cycle-life aging data, as observed in Figs. 3 and 4, show
only 11.5% aging, with no lithium plating after 600 cycles in the opti­
mized cell build that incorporates all design improvements. This is
significantly better than the performance of the Gr/NMC532 cell, which
experienced up to 42% capacity fade at 450 cycles and much lower
utilization (78%) due to distinct plating [41,42,49]. The Gr/NMC811
cells without CBD, a separator, DLA, and the B26 electrolyte did show
lower capacity fade. Still, they could not avoid Li plating at 6C, high­
lighting the benefit of those additional design modifications.
Increasing the charge voltage cutoff to 4.15V necessitates the
advanced charge protocols (e.g., VR and MSR) for cells with an opti­
mized design. These two advanced charge protocols show between 3.5
and 4.8% improvement in charge acceptance in the optimized cells.
However, while the VR protocol avoided Li plating entirely, the MSR
protocol could not do so in all cells after 600 cycles. Plating in MSR cells
did not start immediately after cycling; instead, it occurred in later
cycling stages. Therefore, a more-refined version of the MSR charge
protocol or an adaptation with aging could improve performance. For
example, allowing the MSR CC steps to be adapted or scaled in either
magnitude or duration (or both) to emerging polarization during XFC
(which worsens with aging) would avoid instances of overpotential that
foster conditions for lithium plating.
Consistent with our earlier studies, material and design modifica­
tions in the optimized cells show that LLI and LAMPE are the two
dominant aging modes. LLI occurred due to both normal and plating-
related inventory loss in the SEI. Most notably, we did not see struc­
tural damage in the DLA, and its electrochemical performance shows no
distinct aging effects. Cathode capacity loss occurred primarily due to
IPPS (or cracking) and degraded surface and interphase issues. Multiple
studies extensively evaluated this NMC811 material under fast-charging
conditions (up to 9C) with Gen2 electrolyte and observed that NMC811
could retain its performance even after distinct IPPS [9,13]. These
studies partially attributed this behavior to the superior physiochemical
makeup of NMC811 (i.e., higher diffusion and electronic conductivity)
and its structural properties (i.e., radially oriented subparticles) [9,13].
In a separate study, Ruess et al. concluded that an increase in electro­
chemically active surface area due to IPPS/cracking could help retain
performance in NMC811 as well [50].
Scaling the performance of the best-performing cell build, which did
not show Li plating, to a realistic EV pack could be useful to battery
developers and original-equipment manufacturers (OEMs). Fig. 8 shows
the cell-to-pack scaling performance metrics (e.g., the equivalent fast-
charge miles for 600 cycles and charging speed). After 600 cycles, the
equivalent fast-charge driving miles reach 171,000 and 181,000 miles
for the 6C-4.1V and the VR-4.15V charge profiles, respectively. There­
fore, higher-voltage operation for these investigated cells could provide
up to 10,000 more fast-charge miles than the low-voltage counterpart at
the expense of only 2.4% additional capacity fade. Most battery
11
Journal of Power Sources 582 (2023) 233519
Fig. 8. Equivalent fast-charge miles and charging speed are calculated based on
a 100 kWh battery pack and 300 Wh/mile efficiency for a full-size sedan [54].
We used an energy (Wh)-based scaling from cell-to-pack and considered total
energy throughput over 600 cycles. Charging speed is estimated using
fast-charge energy at 600 cycles. More information about the calculation can be
found in Refs. [3,13] and the section entitled “Equivalent miles calculation”
in SI.
warranties and vehicle life in EVs fall within a range of
100,000–200,000 miles [51,52]. Therefore, these cells would meet the
current EV warranty and life goals with exclusive fast charging.
Fig. 8 also shows the fast-charging speed at 600 cycles for the two
optimized cell builds, which indicates that the 6C-4.1V condition has at
least 26 miles/min charging speed, and the VR-4.15V condition stayed
above 27 miles/min charging speed throughout the cycling. The U.S.
Department of Energy (DOE) has set a fast-charge goal (average) of 20
mi/min [53] or more. The charging speed is well over that limit for this
moderate-loading cell build.
5. Conclusions
This study shows that implementing multiple solution strategies can
achieve a 10 min XFC, up to 6C, without Li plating and distinct degra­
dation in extended cycling settings. The solution strategies implemented
in the cell builds investigated in this are (1) choosing NMC811 over
NMC532, (2) using optimized carbon binder domain (CBD) in NMC811,
(3) dual layer anode (DLA), (4) switching to a higher-pore-volume
separator, (5) using an advanced electrolyte (e.g., B26), and (6) using
advanced charge protocols. These solution strategies improve lithium-
ion transport within the cell, reducing associated cell overpotential
losses, which minimizes cell degradation at different length scales and
avoids Li plating after hundreds of cycles.
Cells that implemented the six solution strategies showed as much as
an 87.3% charge acceptance in 10 min with a 6C CC-CV charge protocol
when the cutoff voltage was constrained to 4.1V. This optimized cell
degraded 11.5% after 600 cycles without showing any evidence of Li
plating. This cycle life scales to an equivalent driving range of 171,000
miles, achieving a charging speed of up to 26 mi/min. These results
highlight the extent of distinct improvement accomplished by imple­
menting innovative materials and electrode design. Going to a 4.15V
charge cutoff voltage showed a slightly better charge acceptance for the
advanced material stress reduction (MSR) and voltage ramp (VR) pro­
tocols, up to 3.5–4.8%, but at the expense of more aging. A cycle-life
study shows that MSR protocol, even with all the above design modifi­
cations, was not able to entirely avoid Li plating (although two of the
three cells showed no Li plating) because one cell experienced small-
scale Li plating toward the later stage of cycling. This was possibly
due to local heterogeneities (porosity, thickness, electron conductivity,
T.R. Tanim et al.
etc.) in the electrode microstructure. Therefore, the MSR protocol could
be refined further, or an adaptive version could be implemented to
provide a buffer to the local heterogeneities that might avoid Li plating.
When applied to the optimized cell build, the VR profile resulted in up to
a 92.1% charge acceptance in 10 min and 13.9% capacity fade after 600
cycles at a 4.15V charge cutoff avoiding Li plating. This equates to a
181,000 mile fast-charge range with at least 27 mi/min charging speed.
Therefore, the XFC range of 171,000–181,000 miles with up to 13.9%
fade can meet current EV warranty and life goals, which nominally fall
between 100,000 and 200,000 miles [51,52]. The charging speed (be­
tween 26 and 27 mi/min) also meets DOE’s XFC goal of 20 mi min− 1
[53].
This study finds two dominant aging modes: LLI in the negative
electrode and loss of active material (LAMPE) in the positive electrode.
The structural integrity of the DLA remains intact, showing no distinct
degradation after 600 fast-charge cycles in the two best cases discussed
above. Cathode fade is primarily dominated by secondary subparticle
separation or cracking and surface/interphase degradation. However,
their effects on electrochemical performance are minor, between 6 and
11% fade for the 6C-4.1V and VR-4.15V conditions, respectively. These
results extensively align with our earlier studies on the same cathode
materials [9,13].
This study validates the benefits of implementing multiple solution
strategies in moderate-loading cells (3 mAh/cm2 anode vs. 2.7 mAh/cm2
cathode). The promising results show a pathway to enable 10 min XFC in
energy-optimized cells with ≥4 mAh/cm2 loading. The solution strate­
gies are not necessarily limited to the ones identified in this study.
CRediT authorship contribution statement
Tanvir R. Tanim: Conceptualization, Methodology, Validation,
Formal analysis, Investigation, Data curation, Writing – original draft,
Supervision, Project administration, Funding acquisition. Sangwook
Kim: Formal analysis, Data curation, Validation, Writing – review &
editing. Andrew M. Colclasure: Methodology, Software, Formal anal­
ysis, Writing – review & editing. Zhenzhen Yang: Resources, Data
curation, Validation, Writing – review & editing. Kevin Gering: Meth­
odology, Writing – review & editing, Funding acquisition. Peter J.
Weddle: Methodology, Software, Formal analysis, Writing – review &
editing. Michael Evans: Data curation, Validation. Eric J. Dufek:
Conceptualization, Methodology, Writing – review & editing, Project
administration, Funding acquisition. Yulin Lin: Resources, Data cura­
tion, Validation, Writing – review & editing. Jianguo Wen: Resources,
Data curation, Validation, Writing – review & editing. Francois Usse­
glio-Viretta: Methodology, Software, Formal analysis, Writing – review
& editing. Alison R. Dunlop: Resources, Data curation, Validation,
Writing – review & editing. Stephen E. Trask: Resources, Data curation,
Validation, Writing – review & editing. Kandler Smith: Methodology,
Software, Formal analysis, Writing – review & editing. Brian J. Ingram:
Resources, Data curation, Validation, Writing – review & editing.
Andrew N. Jansen: Resources, Data curation, Validation, Writing –
review & editing.
Declaration of competing interest
The authors declare no conflict of interest.
Data availability
Data will be made available on request.
Acknowledgments
The authors thank Samuel Gillard from DOE for supporting this
project. Funding was provided by the DOE Office of Energy Efficiency
and Renewable Energy’s Vehicle Technologies Office under the
12
Journal of Power Sources 582 (2023) 233519
guidance of the Advanced Battery Cell Research XCEL Program. This
manuscript was authored by Battelle Energy Alliance, LLC, under Con­
tract No. DE-AC07-05ID14517 for INL; the Alliance for Sustainable
Energy, LLC, under Contract No. DE-AC36-08GO28308 for NREL; and
the University of Chicago–Argonne, LLC, under Contract No. DE-AC02-
06CH11357 for Argonne, all of which are DOE-Office of Science Labo­
ratories. Work performed at the Center for Nanoscale Materials, a U.S.
Department of Energy Office of Science User Facility, was supported by
the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-
AC02-06CH11357. This article has been contributed to by U.S. Gov­
ernment subcontractors and their work is in the public domain in the
USA.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.jpowsour.2023.233519.
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