Journal of Power Sources 526 (2022) 231129

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Journal of Power Sources

journal homepage: www.elsevier.com/locate/jpowsour

Review article

Developing extreme fast charge battery protocols – A review spanning

materials to systems
Eric J. Dufek a, *, Daniel P. Abraham b, Ira Bloom b, Bor-Rong Chen a, Parameswara R. Chinnam a,
Andrew M. Colclasure c, Kevin L. Gering a, Matthew Keyser c, Sangwook Kim a, Weijie Mai c,
David C. Robertson b, Marco-Tulio F. Rodrigues b, Kandler Smith c, Tanvir R. Tanim a, Francois L.
E. Usseglio-Viretta c, Peter J. Weddle c
a
Energy Storage & Electric Transportation Department, Idaho National Laboratory, Idaho Falls, ID, 83415, USA
b
Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, 60439, USA
c
Center for Energy Conversion & Storage Systems, National Renewable Energy Laboratory, Golden, CO, 80401, USA

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• Overview of critical battery degradation

modes occurring during extreme fast
charging.
• Methods and tools to aid in the devel­
opment of extreme fast charge
protocols.
• Use of advanced analysis and machine
learning for early failure mode
identification.
• Combined use of electrochemical
models and experiments for protocol
development.
• Scaled protocols influence electric
vehicle infrastructure planning.

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

Keywords: Extreme fast charging (XFC) has become a focal research point in the lithium-battery community over the last
Extreme fast charging several years. As adoption of electric vehicles increases, fast charging has become a key driver in enhancing
Li-ion battery consumer recharge experience. Recently, the research community has made significant improvements in
Machine learning
developing charge protocols to support XFC. New charge protocol designs derived using a combination of
Aging
Charge protocol
advanced, physically derived models, and electrochemical and secondary characterization methods, increase
charge acceptance and decrease aging. By coordinating these methods and modifying protocols to account for
different material constraints, including lithium plating and cathode particle degradation, novel charge protocols
have increased the energy accepted during charging by over 25% in 10 min and increased the charge acceptance
prior to a constant-voltage step by approximately 3x. Here, we review several charge-protocol advances, aging
factors which are enhanced by XFC and advances which will enable adoption of XFC capable vehicles. These
advances include implementing machine learning and other detection algorithms to reduce and classify lithium
plating, which is known to significantly degrade cell performance and reduce cell life. The review concludes by
discussing full-system fast charge requirements, including electric vehicle service equipment needs for imple­
menting XFC protocols.

* Corresponding author.
E-mail address: eric.dufek@inl.gov (E.J. Dufek).

https://doi.org/10.1016/j.jpowsour.2022.231129
Received 5 November 2021; Received in revised form 21 January 2022; Accepted 4 February 2022
Available online 23 February 2022
0378-7753/© 2022 Elsevier B.V. All rights reserved.
E.J. Dufek et al. Journal of Power Sources 526 (2022) 231129

Apart from some baseline activities, the standard constant current,

Abbreviations constant voltage (CCCV) profile commonly used for many cycle life
evaluations is seldom used. Instead, for both fast charge and XFC,
Beginning-of-life (BOL) several classes of protocols have been advanced (see Table 1), including
Constant Current (CC) stepped profiles where the current typically decreases during the later
Constant Current Constant Voltage (CCCV) portions of the charge; pulsed profiles where intermittent rest periods or
Constant Voltage (CV) power pulses are applied including both positive and negative current
Electric Vehicles (EVs) pulses; and ramped profiles where either the current or the voltage is
Electric vehicle service equipment (EVSE) ramped during the charge. Other more unique profiles such as the
Extreme Fast Charging (XFC) ‘universal’ charge protocol based on keeping cell overvoltage below
Internal Combustion Engine Vehicles (ICEVs) certain levels have also been developed [25]. Good reviews of different
Lithium Iron Phosphate (LFP) protocol classes are provided by Keil and Jossen [27] and Wassiliadis
Lithium Nickel Manganese Cobalt Oxide (NMC) et al. [28].
Lithium Plating Condition (LPC) In this review, we first discuss cell materials, electrodes and elec­
Plug-in Hybrid Electric Vehicle (PHEV) trolytes, which can influence and be impacted by XFC. We then detail
pseudo-2D (P2D) model how differences in system management, including thermal and me­
Solid Electrolyte Interphase (SEI) chanical management impact performance. We continue and show how
State-of-charge (SOC) experimentally obtained electrochemical information can be used to
U. S. Department of Energy (DOE) develop XFC protocols and advanced detection of aging modes including
lithium plating. The interplay between these different levels of analysis
in the context of fast charging is illustrated schematically in Fig. 1.
Finally, we close with a discussion on how developed protocols could
1. Introduction impact the development of EV infrastructure.
It should also be noted that, even though XFC may be used with many
Electric vehicles (EVs) have seen significant increases in adoption cell chemistries, we primarily focus on NMC-family oxides (LiNi0.xMn0.
over the last several years. With multiple pledges from both industry and yCo0.zO2, NMCxyz, where xyz = 532, 622, and 811) and graphite (C) for
countries across the globe targeting mass adoption of EVs by 2035, there the sake of clarity. Other cell chemistries, such as those based on lithium
is little time to close the gap in consumer experience between EVs and iron phosphate (LFP) or lithium cobalt oxide (LCO), are not extensively
internal combustion engine vehicles (ICEVs). Extreme fast charging discussed. Using the United States Advanced Battery Consortium
(XFC) is one of the most direct means to close the experience gap (USABC) and U.S. Department of Energy (DOE) targets as guidelines,
associated with refueling/charging time. Generally, XFC is defined as cells based on LFP do not meet the 350 Wh/kg energy goal for a long-
the ability to replace at least 80% of the vehicle battery capacity in 15 range EV. These cells typically have gravimetric energy densities on
min or less, or to replenish range at a rate of ~20 miles per minute of the order of 90–120 Wh/kg. Similarly, LCO-based cells exceed the
charge. Extreme fast charging typically uses charge rates of 4.8C or USABC/DOE cost target of $100/kWh [36]. In a similar vein, while
higher [1]. More broadly, fast charging is generally considered charging advances have been made for the use of Si as a negative electrode, it is
80% capacity in 30–50 min. Here we use XFC to denote charging times not included due to limitations which currently exist in achieving long
of less than 15 min in length and the broader fast charging for charging calendar life [37].
of less than 1 h in length. In 2017, a series of perspectives highlighted
many of the complications with enabling high power XFC charging up to
Table 1
350 kW, from cell to infrastructure considerations [1–5]. In the area of
Examples of different Fast Charge and XFC protocol classes.
challenges associated with batteries undergoing XFC, minimizing
Protocol Description References
lithium plating and excessive heat generation were two of the most
prominent of the identified gaps. Since 2017, multiple groups globally Elevated Temperature Heat cells before or during Refs.
have made advancements to address these and other gaps. Core scien­ Charging charging to take advantage of [18–21,29]
enhanced electrolyte Li+ transport
tific advances, including the development of new electrolytes with at elevated temperature
increased lithium transport properties [6–10], unique electrode archi­ Multi-step starting at a high Protocols with a series of constant Refs. [22,27,
tectures and materials [11–17], the beneficial use of heat generation rate current steps which reduce in 30]
[18–21], and the development of advanced charge protocols [22–26], current as the cell approaches
higher voltages
have all occurred and significantly advanced the state of the art for
Multi-step with either an Protocols where a constant Refs. [29,31,
XFC-capable batteries. increase or decrease in current step is used and the 32]
Lithium-ion batteries, as electrochemical cells, rely on the transport current during charging current can both increase or
of lithium ions from the cell positive electrode to the negative electrode decrease during charging, usually
during charging. When transport becomes limited, performance typi­ as determined using a model or
penalty-based system
cally drops due to either lithium plating at the negative electrode, poor Boost Charging Use of 2 constant current (CC) Refs. [22,27]
charge acceptance due to increased cell polarization, or to accelerated steps followed by a constant
degradation as energy is lost due to Joule heating [3]. While there are voltage step.
several ways to alter the materials in the batteries to improve transport, Pulse Charging Use of pulses, usually all at the Refs [22,27,
same current with a defined 33,34]
such as using different electrolyte solvents and salts or altering electrode
periodicity
architecture to reduce tortuosity, it is also possible to adapt the ionic Voltage Controlled Charging Profiles which either ramp voltage Refs. [23,24,
transport within the cell by changing the electrochemical driving force at a controlled rate or which use 35]
during charge. Specifically, how charge profiles are developed can specific voltage controls
distinctly impact each of the negative aspects described above and Voltage Trajectory Current typically starts low, Refs.
increases at intermediate state-of- [25–27]
provide distinctly different aging pathways, while also enhancing
charge (SOCs) and then decreases
charge acceptance. again at high SOC. Similar to
Within the research community, there are several different ap­ Universal and other stress
proaches to adapting charge protocols for both fast charging and XFC. reduction protocols

2
E.J. Dufek et al.
2. Material and electrode consideration for XFC
2.1. Positive electrodes
From both supply chain and specific energy considerations, there has
been a recent interest in increasing the amount of Ni in positive elec­
trode materials. Comparing performance of NMC532 with the higher-Ni
NMC811 shows significant improvement in charge acceptance during
XFC for the latter when similar electrode loadings are used. A key reason
for improved charge acceptance is that, at comparable electrode po­
tentials, the NMC811 has higher specific capacity, solid-state diffusion
and electric conductivity when compared to NMC532 [39]. Combined,
the enhancements allow higher Ni positive electrodes to outperform
lower-Ni systems. In recent work comparing the two NMCs using similar
areal loading, it was found that NMC811 outperformed NMC532 by
3.2%, 5.2%, 3.2%, and 1.7% when charging at rates of 1, 4, 6, and 9C
with a cell Vmax of 4.1V [40]. Part of the improved performance of
NMC811 is that its higher specific capacity enabled thinner electrodes to
be used.
Degradation of NMC, as evidenced by loss of active material (LAM)
through particle cracking and delamination, is a significant set of failure
modes that leads to performance decay during fast charging and XFC.
During lithiation and delithiation cycles, the electrode materials un­
dergo significant mechanical stress due to the frequent volume expan­
sion and contraction as lithium ions are extracted and inserted from/into
the lattices [41–43]. In practice, the extent of LAM increases as C-rate
increases as shown in the work of Tanim et al. [22,40], where NMC532
cathode particles were found to crack when cycled at rates between 1
and 9C. According to these studies, as cycling advances beyond 400
cycles, the rate of cathode capacity loss due to mechanical disintegration
of the cathode particles increases and significant growth in internal
resistance occurs. Interparticle separation or cracking of cathode ma­
terials induces many other side effects, such as fresh contact area with
electrolyte and changes in electrolyte wetting [41,44]. More severe
cracking of NMC811 particles (vs. low-Ni alternatives) has also been
reported, though a commensurate loss of performance was not observed,
likely due to the enhanced diffusion and electrical conductivity for the
higher-Ni material. The mechanical expansion and contraction also
impact the binders used in the electrodes, which adhere the active
electrode materials to each other and to the current collector, and can
also suffer when exposed to significant levels of fast charging [45].
Separation and disintegration of secondary cathode particles com­
plicates aging for cells undergoing XFC. However, there are differences
Fig. 1. Key considerations which impact charge acceptance, aging and performance when performing XFC. Portions adapted from Ref. [38].
3
Journal of Power Sources 526 (2022) 231129
which emerge when using secondary particles with aligned grains. Early
studies, not specifically focused on fast charge and XFC, have shown that
by aligning the cathode particle grains or by using single crystalline
materials, a reduction in the mechanical stresses on the cathode can be
achieved, enhancing overall performance [46–48]. Due to the increased
mechanical stresses which occur during XFC, it is anticipated that
similar advances in the materials would have a beneficial impact on life
and retention of cathode performance over extended XFC cycling.
Mechanical degradation is not the only route by which NMC de­
grades during XFC. When lithium is irreversibly plated at the negative
electrode, the inability to fully lithiate the NMC results in lattice volume
strain which progresses with cycling, as shown by Son et al. [49].
Additionally, the effects of XFC on the electrodes have been reported to
be heterogeneous in cells containing nickel-rich positive electrodes.
Indeed, Yang, et al. [50] performed a systematic study on cells con­
taining NMC cathodes with different compositions. The anisotropic
change in unit cell volume was found to correlate with the Ni content
when electrodes with lower areal loading (1.5 mAh/cm2) were used,
while it leveled off for higher areal loadings (2.5 mAh/cm2). The change
in unit cell volume was due to lithium plating on the negative electrode
which resulted in incomplete particle lithiation during cell discharge. As
one might expect, the heterogeneous changes in the positive electrode
align with heterogeneous lithium deposition on the negative electrode.
Other positive electrode materials including lithium iron phosphate
(LFP) and lithium cobalt oxide (LCO) have also been investigated.
Recent interest in LFP for lower cost and shorter range EVs warrants its
consideration for both fast charge and XFC. Some studies have looked at
the ability to use it as a cathode material with minimal impact to aging
[18,51]. These reports suggest minimal degradation to the LFP material.
Other aspects related to aging for these cells primarily center on lithium
plating and losses at the negative electrode.
2.2. Negative electrodes
As fast charging is more aggressive than standard cycling, the aging
and degradation phenomena are often exacerbated when compared to
cells cycled under milder conditions. The most significant issue with XFC
is that lithium plating on the negative electrode is a possible, life-
limiting factor. If plated lithium becomes irreversibly isolated it can
lead to both increased capacity loss and decreased safety [52–54].
Lithium plating is a complex phenomenon driven by the interaction
of thermodynamics and the kinetics of intercalation. Lithium can plate
on the graphite surface if the local potential is less than 0 V (vs. Li/Li+)
E.J. Dufek et al.
[55–57], which can happen if the observed cell voltage is greater or
equal to 4 V at sufficiently high rates for most C/NMC cells. As one
would expect, plating is exacerbated at higher currents and lower tem­
peratures. However, plating has been observed at charge rates as low as
C/6 at about room temperature [55].
We note that lithium plating can also be a partially reversible pro­
cess, where stripping efficiency can be improved by changing electrolyte
properties, the rest period and the rate at which the charging event
occurs [58]. When stripping efficiency is high, the total capacity loss due
to lithium plating is minimal during early cycles, but the combined ef­
fect of even minor loss due to irreversible lithium plating and additional
SEI formation does eventually lead to increased capacity loss [59]. Due
to the loss of lithium and the complexity of achieving high reversibility
for plated lithium, lithium plating has been identified as a significant
inhibitor to reliable fast charging and XFC cells and has been a subject of
intense recent research [1]. As described more thoroughly in a recent
review, methods to characterize and quantify lithium plating are sig­
nificant and include a suite of different analysis methods spanning
invasive cell tear down to in operando analysis [60].
Unlike positive electrode material changes, alteration of the type of
graphite in the negative electrode of cells for XFC does not lead to sig­
nificant impacts on performance, as graphitic materials have relatively
similar voltage responses. However, morphological features (such as
particle size) can affect anode performance at high currents. The work of
Zhang et al. [61] found that, while the use of smaller graphite particles
improved the life of cells that underwent XFC, the smaller particles did
not significantly alter rate capability.
Changing to higher energy materials like Si may provide some
improvement in reducing lithium plating, as Li-Si alloy formation occurs
at potentials that are further removed from lithium plating and a high
areal loading can be achieved with a thinner negative electrode. How­
ever, while Si may provide some benefit, there are other concerns that
still exist for Si including calendar life considerations [37]. To date,
lithium metal anodes have not been thoroughly investigated for XFC,
though there are distinct performance and life differences which emerge
as it is cycled at different rates. There have also been studies looking at
both lithium titanates and niobates for XFC [15]. While good for high
rates, much like LFP cells, these cells tend to present lower energy and
are not as directly applicable to long-range EV applications.
2.3. Electrode structure considerations
Altering the electrode morphology can also improve its performance
under high currents. As one might expect, random porosity in the
negative electrode creates a tortuous path for lithium transport.
Conceptually, if a less tortuous path in the porous laminate was present,
there should be reduced impact from lithium plating during XFC.
Indeed, Robertson et al. [62] reported that increased porosity of the
graphite electrode does lead to a decrease in observed lithium plating.
The performance of structured porosity in the graphite electrode was
investigated theoretically by Usseglio-Viretta et al. [63], and by Mai
et al. [64]. These works indicate that a relatively low amount of struc­
turing would be needed to increase diffusion and reduce the likelihood
of lithium plating.
Experimentally, researchers have investigated the effect of struc­
tured porosity in both the positive and negative materials to achieve
both high energy and to aid in fast charge capability. While some of the
approaches were not directly used to advance XFC capability, the gen­
eral processes and methods could ultimately be used to enhance charge
acceptance during a fast charging event. Approaches to create structured
porosity include powder processing, freeze casting, laser ablation, and
magnetic orientation [11,65–68]. For example, post electrode-casting
processes, such as laser ablation, can create a highly ordered pattern
of vertical pores (perpendicular to the current collector) [12]. Pouch
cells (>2 Ah) containing laser ablated graphite negative electrodes have
shown good capacity retention (86%) after 600 cycles at a 6C charge
4
Journal of Power Sources 526 (2022) 231129
rate.
The structure of the electrode has also been shown to change the
progression of material level degradation modes. The most direct way to
understand how modifications to the electrode and cell impact aging is
to quantify the different aging modes, including LLI (loss of lithium in­
ventory, such as the losses due to SEI formation and irreversible losses
from Li plating and deposition) and LAM [69]. In Chinnam et al.‘s [70]
work, cells with higher weight loadings for both the positive and
negative electrodes tended to display higher rates of LLI even at current
densities that were on the same order as lower loading cells. For the
lower loading cells, LAM at the positive electrode (LAMPE) was a
dominant aging mode. As higher C-rates were achieved without plating,
the increased mechanical stresses in the positive electrode particles led
to greater particle fracture [70]. The study also found that even small
changes in the porosity of the negative electrode due to either SEI
growth or lithium plating can significantly impact the likelihood that
further lithium plating will occur.
2.4. Electrolyte
In most lithium-ion cells, the electrolyte is a mixture of organic
carbonates containing a lithium-bearing salt, like lithium hexa­
fluorophosphate, LiPF6. Additives are sometimes used to change elec­
trolyte properties and/or reactivity. During XFC, transport limitations
can arise as the cell polarizes. Under such polarization there is an
enrichment of electrolyte salt in proximity to the positive electrode and
a depletion near the negative electrode. This difference in salt concen­
tration across the cell causes a corresponding spatial variance in elec­
trolyte properties, such as viscosity, conductivity, and diffusivity, which,
in turn, affect the lithium flux between the electrodes. Toward that end,
recommendations have been given for electrolytes intended for XFC to
have twice the conductivity and up to 4 times the diffusivity of con­
ventional electrolytes if other cell design features such as electrode
thickness and porosity are held constant [71]. This has been successfully
demonstrated in recent work that developed XFC electrolytes [6,17].
In addition to being an ionic transport medium, the electrolyte also
contributes to the formation and chemistry of the SEI layer, which are a
source of impedance and lithium consumption. Indeed, there is a lot of
published work on the connection between electrolyte composition and
SEI layer chemistry. The reader is referred to the comprehensive reviews
by Aurbach for more information [72–74]. As an example of how
different electrolyte compositions change the nature of the SEI, Fig. 2
compares how the anode and cathode potentials behave when using
LiPF6 and lithium bis(oxalate)borate (LiBOB) as salt. When compared to
LiPF6, LiBOB is known to form a highly resistive SEI on the graphite
electrode, causing most of the polarization to originate from the anode.
Fig. 2 shows that the anode potentials for the cells are similar at a C/5
rate, but the differences become very pronounced above a 3C rate,
leading to the LiPF6 and LiBOB cells meeting the thermodynamic lithium
plating condition (LPC) at ~120 and ~10 mAh/g, respectively. Thus, in
addition to high Li+ conductivity in the bulk, the electrolyte should yield
low impedance SEI layers that allows rapid transport of Li+ ions into the
graphite particles in order to minimize overpotentials at the anode [75].
While modifications to the SEI have been well studied, there have
been few reports on the effect of fast-charging and XFC on the changes to
the bulk electrolyte composition. Most studies, such as that given in
Ref. [76], have focused on the impact of the charge rate on the SEI layer
formed by electrolyte decomposition. Yang et al. [77] showed that,
using C/NMC532 cells, at charge rates in the range of 1–8C there was no
change in the relative amounts of electrolyte decomposition products, as
shown in Fig. 3. Here, three components were identified, corresponding
to m/e values of 317, 535 and 563 Da. The uncharged (m-1), empirical
formulae for these components were C11H22O7PF, C14H33O15P3, and
C16H37O15P3, respectively.
E.J. Dufek et al.
Fig. 2. The (a,b) anode and (c,d) cathode potentials φa and φc , respectively, for constant current charging of a full cell from 3 to 4.4 V at C/5 and 3C rates. The black
and red lines are for cells with 1.2 M LiPF6 and 0.7 M LiBOB salts, respectively, in a 3:7 w/w mixture of EC and ethyl methyl carbonate (EMC). The lithium-plating
condition (LPC) is indicated by the dotted line in (b). (For interpretation of the references to color in this figure legend, the reader is referred to the Web version of
this article.)
3. Pack and battery management considerations
Comparison of cells and packs undergoing fast charge has shown that
the pack can experience greater fade than individual cells due to
increased heterogeneity and how the pack is managed by the battery
management system as it ages [78]. This heterogeneity is partly due to
differences in the thermal environment of the cells throughout the pack.
Temperature has a complex relationship with XFC, as elevated temper­
atures can improve cell kinetics but also decrease cycle and calendar
lives. To minimize the impacts of high temperature degradation while
maximizing the benefits of higher temperature during XFC, Yang et al.
[21] estimate that battery thermal management systems (BTMS) will
need to be resized from the current 1–5 kW range to around 15–25 kW,
depending on the design and charge rates. It has been suggested that
deliberately pre-heating cells could be a viable approach to decrease the
likelihood of Li plating during XFC [18]. Since the BTMS resizing esti­
mates provided above (15–25 kW) are based only on the heat generated
by the XFC event, even larger thermal management systems would be
required in cases of adoption of pre-heating approaches, to ensure rapid
return to ambient or optimal operating temperatures for driving.
Non-uniform thermal management due to either pack or cell design
Fig. 3. Area fraction of the major electrolyte degradation products as a func­
tion of apparent molecular weight and charge rate. The error bars represent the
area fraction maxima and minima for each component [77]. The x-axis is given
in units of mass/charge (Daltons, Da) to indicate the approximate formula
weight of the protonated molecular ion, assuming a charge of +1. Copyright ©
Wiley-GmbH. Reproduced with permission.
5
Journal of Power Sources 526 (2022) 231129
can also have localized impacts within a cell. Thermal gradients within
the cell can create local hot spots, which have elevated levels of
degradation such as SEI growth [79,80]. Development of such hot spots
can result in a cascading failure where the accumulated heat further
leads to high current density and accelerated chemical reaction kinetics,
or even thermal runaway hazards [81].
In a similar vein, heterogenous management of pressure can also
impact aging for cells undergoing fast charge [82]. When pressure is not
homogenously applied to a cell, variations in pressure have been shown
to lead to localized lithium deposition and subsequent enhanced rates of
failure. Should lithium deposit locally, the ability to maintain revers­
ibility is also impacted by pressure. Several recent works on lithium
metal cycling have shown that uniform, moderate pressure of at least
~300–350 kPa significantly enhance plating and stripping efficiency
while lower levels of pressure lead to reduced stripping efficiency
[83–86].
4. Protocol development
4.1. Cell format and information considerations
Presented in Fig. 4 is a general summation of the different aging
effects associated with XFC. The figure also includes different design
solutions which can be used to mitigate the aging impacts and be har­
nessed to increase the amount of charge which can be accepted during
XFC. At each of the different length scales listed there are distinct areas
where improvements can be made to increase XFC performance and
minimize aging.
Before developing charge protocols researchers need to first under­
stand the type of cells that will be used. Understanding how new charge
protocols impact cell performance can be difficult to directly compare
across studies due to the different types of cells used for evaluation.
Within the research community, the three main cell configurations used
are coin cells, research pouch cells (both single and multilayer), and
commercial cylindrical cells. Other studies using 3-electrode cells are
also performed and provide detailed information on the state of both
electrodes during cycling [24,35,75,87–89]. Of the different cell types,
all have some distinct positive and negative attributes making them
more suited for different types of studies. As an example, coin cells are
easy to prepare and test, but they also have significantly higher
impedance than pouch cells and typically contain excess electrolyte. To
enable easier comparison of coin cells to other cell types consideration of
the amount of electrolyte added to the cell and reporting cell impedance
are advisable. R&D pouch cells, on the other hand, have lower imped­
ance and usually more closely resemble what would be found in auto­
motive settings. Like coin cells, the full details of the contents of the cell,
E.J. Dufek et al.
Fig. 4. Key degradation modes and aging effects which occur during XFC across different length scales within a battery and routes to enhance performance and
minimize aging.
including electrolyte blends and electrode loading, porosity, and mate­
rial content, are known. But R&D pouch cells do, at times, have higher
variability than commercial cells and, as one scales from a single layer to
a multi-layer cell, thermal aspects including heating due to high-rate
charging change considerably. Commercial cells can be highly repre­
sentative (assuming they are in line with automotive specific energy and
energy densities), but they come with the downside of limited infor­
mation related to many key design aspects, including electrode thickness
and electrolyte formulation. When evaluating XFC protocols, either
R&D pouch cells or commercial cells provide the closest representations
to what would be deployed in a vehicle. New XFC protocols should, at a
minimum, be evaluated using these cell formats to allow more direct
comparison across efforts and to show the most immediate benefit of
new protocol advances.
Information available in the open literature is immensely beneficial
when looking to expand and build upon the work of others. Yet, the
benefit of data is limited by the extent of information provided that
details the specifics of experiments and cells used. For all cases, but
especially for non-commercial cells, the inclusion of critical metadata, or
data about the cells and experiments, including specifics on both the
positive and negative electrode materials, loadings and electrode
porosity, provide critical information to better understand the key lim­
itations which may emerge as a specific set of cells undergoes XFC.
Recent work highlighted that there is a need to go beyond just reporting
materials, as the extent of specific aging modes can change considerably
as the cell loading increases [70]. In addition to reporting the active
materials, adding details on the type of electrolyte used and its volume
with respect to either void space in the cell or to the total cell capacity
(in g/Ah) is critical for cross study comparison. Additionally, this in­
formation helps ensure that cell life is not artificially extended by excess
electrolyte volume, especially when lithium metal is plated [89–91].
Lastly, specifics on how cells are fixtured and thermally controlled is
pertinent when reporting XFC data. Non-uniform temperature, or
slightly elevated or depressed temperatures, can dramatically alter how
cells perform [62]. Similarly, pressure and compression related to cell
design and fixturing can also impact performance [82]. Examples of how
to structure the information for reporting in a straightforward tabular
format and the benefit of sharing information can be found in several
recently published manuscripts [70,92,93].
4.2. Characterization of cell response at beginning-of-life
When significant information about the cell and electrodes is un­
available, there are still ways to develop and advance high performing
6
Journal of Power Sources 526 (2022) 231129
XFC protocols using beginning-of-life (BOL) characterization data,
including rate capability, voltage relaxation and cell impedance as a
function of SOC at different rates [22,25]. From the information gath­
ered during the BOL characterization, it becomes possible to construct
charge protocols that have some grounding in the physics of the cell,
even if the protocols do not fully approximate the exact state of the
respective positive and negative electrodes. In work by Guo et al. [25], a
“universal” fast charge protocol was developed using a combination of
cell characterization data and a mathematical model. This work resulted
in a protocol that applied a current during charge that was inversely
proportional to the cell impedance (Table 1). In doing so, the researchers
were able to extend life while still allowing high charge rates. Other
work looking to reduce the stress on particles used BOL characterization
coupled with cell-level models to first apply high currents followed by
current reduction at discrete voltages to maintain a constant stress on
active material particles [26]. Using this approach, it was possible to
extend the life of the battery by avoiding lithium plating and reducing
excessive material stress and degradation, including reducing loss of
active material at the positive electrode of the cell [26].
Other advanced protocols have been developed based on calculated
voltage relaxation after fast charge to determine lumped overvoltage
parameters, which incorporated overvoltage from both electrodes due to
ohmic, charge-transfer and mass-transport impedances in both the solid
and liquid state [22,94]. These protocols look to identify charging cur­
rents in regimes that are below levels where mass-transport limitations
arise. To develop the protocols, voltage relaxation data was collected by
charging a cell at different rates and examining how the voltage relaxes
after a cell reaches the maximum voltage (Vmax). Using high-rate data
acquisition during rate capability evaluation makes it possible to
approximate both the transport and impedance contributions to the cell
voltage. This information can then be used to develop multi-step or
boost protocols that reduce aging by decreasing the likelihood of lithium
plating [22,95].
4.3. Three-electrode studies
Where more complete information on electrode and electrolyte
components are available, direct methods can be used to guide charge
protocol development. These include the use of microprobe reference
electrodes (REs) that monitor the positive and negative electrode po­
tentials (φc and φa, respectively) during electrochemical cycling of the
cell [75,87,88].
Electrode potential profiles obtained at 30 and 45 ◦ C on C/NMC532
cells containing a LiPF6 electrolyte are displayed in Fig. 5 [35]. In these
E.J. Dufek et al.
experiments, the cells were charged at constant currents, ranging from
0.2 to 6C, to a specified capacity. Fig. 5 shows that the positive electrode
(cathode) accounts for a major portion of the cell polarization at all
states-of-charge [35]. This polarization causes the cell to reach its upper
cut-off voltage (UCV) before Li+ ions are fully extracted from the oxide
thereby decreasing charge acceptance by the cell in a given voltage
window. It should be noted that excessive polarization at the positive
electrode can also result in electrolyte oxidation and cause permanent
structural changes in the layered oxide. In addition, the cathode can be
the main contributor to heat generation in the cell, which is greater at
higher charging currents. For these reasons, charge protocol design must
also consider the effective potentials to which the cathode will be
exposed.
The negative electrode (anode) polarization causes its voltage to dip
below the lithium plating potential, creating conditions that are favor­
able for lithium nucleation and growth on the graphite surface. The
effect of polarization can be especially severe in thick, high-capacity
electrodes: here, only anode portions closer to the separator interface
are effectively utilized, causing large and persistent lithium concentra­
tion gradients that promote non-uniform aging in the electrode. Raising
cell temperature is one approach to lower electrode polarization; the
higher temperature facilitates charge migration by enhancing rates of
diffusion and interfacial transport. Fig. 5 shows that the anode potential
crosses zero (vs. Li/Li+) at 3.4 and 4.6C at 30 and 45 ◦ C, respectively,
which indicates that, for the same C-rate, lithium plating is less likely at
higher temperatures. This type of information can be used to adapt
charging protocols considering temperature changes experienced by
cells under high currents, or when pre-heating methods are employed
(see section 3).
The ability to experimentally determine conditions that are condu­
cive to lithium plating makes REs very useful to the design of XFC
protocols. Indeed, previous works have demonstrated that charging al­
gorithms obtained by using a RE to avoid lithium plating potentials can
be successfully implemented in large-format cells, with clear benefits to
charging time and cell life [96,97]. The issue with deriving realistic
charging protocols using potentials measured vs. a RE is that such values
are inexact when high currents are applied. The finite separation be­
tween the RE and the electrodes, along with the low ionic conductivity
of typical lithium-ion battery electrolytes, creates an offset between the
measured potentials and the ones experienced at the anode surface
(Fig. 6b). Hence, the potentials measured by the RE can be greater than
those at the anode surface by several mV per C-rate; this difference
Fig. 5. The (a,b) anode and (c,d) cathode potentials φa and φc , respectively, for constant current charging of a full cell from 3 V to a fixed capacity of 87 mAh/g, at 30
and 45 ◦ C. The lines of different color correspond to different C-rates given in the legend in panel a. After charge, the cells rested for 1 h at zero current before being
discharged to 3 V at a C/5 rate (dashed lines). Note that the electrode potentials at the beginning of discharge are similar even though the charge rates vary from C/5
to 6-C [35]. (For interpretation of the references to color in this figure legend, the reader is referred to the Web version of this article.)
7
Journal of Power Sources 526 (2022) 231129
causes the RE to overestimate the onset of lithium plating by tens of
millivolts when high currents are applied [75]. As a result, charging
protocols derived from conventional three-electrode measurements are
intrinsically conservative with respect to the onset of
lithium-deposition. By estimating the difference between the potential
measured by the RE and actual potentials at the anode, protocols can be
designed that minimize charging times without exposing the anode to
lithium plating conditions [24].
The ideal charging mode to exclude lithium-plating is shown in
Fig. 6c. This CCCη (constant current, constant anode surface potential)
protocol charges the cell until the graphite potential reaches 0 V vs. Li/
Li+ and then maintains this potential until the desired capacity is
reached. However, this protocol cannot be practically implemented
because the true anode surface potential cannot be determined
experimentally.
Other charging modes are displayed in Fig. 6d and the associated
currents in Fig. 6e. For example, in the CCCφ protocol (grey plots), the
cell is charged until the anode potential, φ (measured by the RE), rea­
ches 0 V vs Li/Li+ and then cell held at this potential until the desired
capacity is reached. This approach is conservative as the potential
measured by the RE is lower than the actual anode surface potential, as
mentioned earlier. In the “seesaw” protocol, an initial high current (e.g.,
6C) is applied until φ reaches a set potential and then the current is
decreased by xC (e.g., x = 0.25) until the set value is met again; this
operation continues until the cell reaches the desired SOC. In Fig. 6d and
e, the set values are φ = 0 (blue plots), φ = (6C rate)*R (black plots), and
φ = − |iR| (red plots), where R is the electrolyte resistance between the
RE and anode surface.
4.4. Electrochemical modeling
More detailed information on cell and electrode design and material
selection provides the opportunity to use electrochemical models, which
give insight into the physical phenomenon responsible for reduced
charge acceptance and accelerated degradation typically seen during
XFC. Three key degradation modes observed during fast charging are
lithium plating, secondary cathode particle cracking, and enhanced SEI
growth due to elevated temperatures and large thermal gradients. These
factors are strongly influenced by the active material chemistry, the
electrolyte and the electrode loading [71]. By better understanding the
underlying cause of these degradation modes, advanced protocols can be
developed to maximize charge acceptance while reducing cell aging.
E.J. Dufek et al. Journal of Power Sources 526 (2022) 231129

Fig. 6. Cell voltage at the relaxation period and cell potential measured using a reference electrode. (a) Cell voltage U at relaxation after charging at rates ranging
from 0.2C to 6C to 4.39 V. Observe that the higher the charge rate, the greater the voltage drop as soon as the charging current is terminated. (b) The electrolyte
potential sensed by the RE differs from that experienced at the surface of the anode by ~iR, leading to a difference of this same magnitude between the measured
potential φ and the surface electrode potential η. (c) The ideal charging protocol that maintains the anode at the thermodynamic limit for lithium plating. (d) Anode
potentials and (e) C-rates during the charging using various φ cutoff conditions. In both (d) and (e), the grey, blue, red, and black plots correspond to the CCCφ,
seesaw (φ = 0), iR corrected seesaw (φ = − |iR|), and 6C corrected seesaw profiles (φ = 6C*R), respectively (Adapted from Refs. [24,88]). (For interpretation of the
references to color in this figure legend, the reader is referred to the Web version of this article.)

Part of the challenge of developing advanced charging protocols
experimentally is that very large parameter space exists for novel cur­
rent/voltage protocols [23]. Models are a quick and low-cost tool for
screening novel protocols and provide physical insight into how novel
protocols mitigate or exacerbate specific aging modes like lithium
plating.
Electrochemical models have predicted that electrolyte transport
limitations and the resulting heterogeneous current distribution through
the electrode depth accelerate aging. A major issue with fast charging,
especially for high energy density cells undergoing XFC, is the non-
uniform utilization of the of the electrodes, which can lead to local­
ized degradation and lithium plating [98–100]. Heterogeneous utiliza­
tion can also lead to differences in relaxation processes complicating
electrochemical analysis [101]. Thus, protocols should be developed to
overcome this specific limitation.
The BMW group has used pseudo-2D (P2D) models to develop novel
fast charging protocols to prevent lithium plating and shown their val­
idity for large format, prismatic, plug-in hybrid electric vehicle (PHEV)
cells [102]. Models were used to develop both multi-step protocols
where the current was reduced when a certain anode potential was
reached, and a constant anode potential protocol that keeps the anode
potential near a set value. The latter is termed constant current constant
anode potential (CCCA) and the current and voltage profiles for this
protocol are shown in Fig. 7a. The proposed CCCA is very similar to the
voltage/current profile developed by Mai et al. [23] using voltage
ramping shown in Fig. 7b. These advanced protocols reduced the
required charging time to prevent plating by several minutes. Further,
the BMW group investigated the effect of positive electrode active ma­
terial choice on the selection of novel charge protocols. By using a P2D
model, the group designed charge protocols for NMC622 and NMC811,
showing that a more aggressive advanced charge protocol can be used
for the NMC811 material. The main cause of this is the reduced elec­
trode/cell thickness leading to lower gradients in electrolyte salt
concentration.
Significant progress has been made in advanced charging protocols
that help prevent lithium plating, much of it guided by P2D [24,96,102,
103] or battery management system (BMS)-compatible, predictive
transmission line modeling [100,104]. For closed-loop, real-time
implementation, several authors have developed reduced-order elec­
trochemical models and integrated them with state-estimation algo­
rithms [105,106]. Combined with model-predictive control, the
physics-based estimation algorithms predict and control the battery to
the internal anode potential of 0 V vs. Li/Li+ to avoid the lithium plating
side reaction [107,108]. The work of Song et al. [107] further proposes

Fig. 7. Example of novel XFC protocols developed to minimize recharge time and prevent lithium plating using P2D models for graphite/NMC cells. (a) Constant
current constant anode potential (CCCA) from BMW group. Reproduced from Ref. [52]. (b) “Voltage ramping” protocol developed by Mai et al. Reproduced
from Ref. [23].

8
E.J. Dufek et al.
the use of current-reversal pulses that strip and recover plated lithium
from the anode. Ahmed et al. [109] used a genetic algorithm to adapt
reduced-order electrochemical model parameters as the battery aged.
Further work is needed to adapt the electrochemical models and
model-based fast charge algorithms as the battery ages. This is difficult,
as many electrochemical model parameters are not readily observed
from normal cycling data.
As mentioned above, novel protocol development to prevent lithium
plating often relies on methods to maintain the anode potential above 0
V vs. Li/Li+. Three-dimensional modeling is needed to help provide
insight into how to translate these protocols to large capacity cells,
which have significantly more current and temperature heterogeneity.
Further, protocols to avoid lithium plating usually consist of several
distinct decreasing current steps. Modeling has suggested that an alter­
native strategy would be to linearly ramp the cell voltage, which may be
easier to implement, especially when charging needs to be modified to
account for cell aging. Unlike lithium plating, other aging modes, like
LAM, do not have a readily available set of indicators to monitor in real
time. For instance, it is difficult for battery management systems to
interpret electrochemical signals as indicators for the fracture of cathode
particles. Models can provide insight into cathode particle stress and
how charging protocol affects this difficult to measure quantity.
Moving forward, advanced protocols need to be developed that
minimize aging from lithium plating, LAM, and SEI growth from
elevated temperature simultaneously. Modeling can provide key in­
sights into how to modulate current/voltage to balance competing fac­
tors for these aging mechanisms. Modeling can also be key to
understanding how to adapt advanced protocols with different aging
modes. That is, how should advanced protocols change to accommodate
expected aging phenomena like SEI growth, LAM, and increases in
electrode tortuosity?
5. Analysis of aging data
During XFC, multiple physical, chemical, and electrochemical re­
actions in the cell are occurring. With time, these aging mechanisms
eventually lead to irreversible loss of capacity and power. Thus, battery
degradation is a set of complex phenomena, which can vary based on
how cells are used, designed and on what environmental conditions they
are exposed to Ref. [38]. Complicating understanding aging data is
electrode heterogeneity: the different modes may not uniformly occur
across an electrode [50,95,110,111]. Other influences, such as battery
design and production methods, may contribute to performance degra­
dation or may even alter the rate at which degradation occurs or how
quickly fade is seen. A key example of this is when excess electrolyte is
present and the life of a cell is artificially extended beyond what would
be expected from a commercial cell operated in the same use regime [90,
91]. Furthermore, the various aging phenomena usually couple with
each other, making aging processes even more complicated and difficult
to interpret [38]. Thus, identifying the root causes of battery aging re­
mains extremely challenging. To address such a complexity in aging,
various aging mechanisms are categorized in three major aging modes:
loss of lithium inventory (LLI), loss of active materials in the cathode
(LAMPE), and loss of active materials in the anode (LAMNE) [112].
To better understand and ideally mitigate degradation phenomena
from the earliest onset, aging detection methodologies are required to
identify the onset of degradation. Early detection is key to minimize
impact prior to the evolution of aging to the point where a cell is no
longer able to meet its expected use. Conventional experimental
methods to confirm aging causes and where the aging occurs often rely
on destructive post-test experiments [113], in situ measurements [111],
and operando measurements [60,114]. Analysis of the electrochemical
signatures also often involves the use of physics-based modeling, where
the actual kinetics and thermodynamic drivers of degradation reactions
in a cell are captured either empirically or semi-empirically [23,63,64,
70,71]. Both experimental and model-based activities have positive and
9
Journal of Power Sources 526 (2022) 231129
negative attributes. Experimental measurements are usually invasive,
time/resource intensive, and need expert knowledge to interpret the
results but can provide detailed information spanning several length
scales. Physics-based models usually need extensive computational re­
sources, and the models are not as flexible when the cell design and
usage condition change, however, they often provide information that is
hard to experimentally probe.
Battery state-of-health, which is aligned with materials-level degra­
dation, is often tracked using cell level electrochemical performance
data including capacity degradation, voltage changes at the end of rest
periods, coulombic efficiency, pulse impedance, electrochemical
impedance spectroscopy and an assortment of derivatives of data, such
as differential voltage and incremental capacity curves [51,112,
115–119]. These signatures provide distinct opportunity to understand
and predict life using data science approaches. Using data-driven
methodologies, hundreds of thousands of battery performance data
sets or points can be analyzed by computational algorithms, from which
high dimensional patterns correlated with lifetime or aging mechanisms
can be recognized [120–122]. In 2019, Severson et al. [115] developed
cycle life prediction within 5% of error from the first 5 life cycles from
125 C/LFP, fast charging cells. Other work related to data-driven pre­
dictions have looked at the comparison of different charge protocols to
predict performance at different cycle counts [123], or to identify
optimal charge protocols as was done by Attia et al. [31] and more
recently by Park et al. [124]. Each of these methods has provided
distinct advances in either life prediction or in the ability to reduce the
time needed to optimize charge protocols. However, analysis from pure
data-driven methods usually fails to provide insights into the
cause-effect relationship for battery aging. Data-driven techniques that
solely use cycle life data have often been found to insufficiently account
for calendar aging, which when projecting life to 10+ years can create
significant differences in prediction [123,125]. Without understanding
of the causes of aging and the role of different types of aging, battery
developers and users may miss opportunities for employing corrective
measures at early stages to prevent more dramatic capacity loss or cell
failure from occurring.
Establishing degradation-mechanism-informed battery lifetime esti­
mation frameworks is an emerging field as noted in several recent ar­
ticles [126–128]. With respect to XFC protocol development and
evaluation, degradation-mechanism-informed methods provide tools
which enable researchers and developers the opportunity to quickly
evaluate and modify protocols. The methods also provide opportunity
for high-throughput analysis without the need for destructive analysis or
for labor intensive characterization methods. One of the emerging
methods that enhances aging understandings is integration of
physics-based models and machining learning approaches that rely on
electrochemical signals. When integrated, the beginning of life physics,
input parameters, and boundary conditions provided by experimental
data or physics-based models can be extrapolated to account for aging
by machine learning.
Another approach promotes the use of physically explainable fea­
tures from the battery performance data [125,129,130]. These data are
collected as time-dependent data streams, such as voltage, current, or
temperature, and features in these data streams that correlate to specific
aging mechanisms/modes, which can then be analyzed as lifetime or
aging phenomena describers. For example, Chen et al. [93] developed a
classification framework targeting early lithium plating identification.
This machine learning classification methodology was constructed using
several electrochemical data signatures collected in a cycle-by-cycle
basis during pouch cell testing, including capacity fade, voltage during
rest period, and coulombic efficiency, across various protocols and
charging rates from 4C to 9C. The linearity of the cycle-by-cycle be­
haviors provided the opportunity to separate cells where the primary
loss of lithium inventory was due to lithium plating as opposed to
normal SEI formation. In cases with lithium plating, the electrochemical
data exhibits strong non-linear signatures, enabling the direct
E.J. Dufek et al.
classification between cells dominated by SEI growth and those where
lithium plating occurs. Using this framework, the classification identifies
cells where plating occurs within 25 cycles. This provides the ability to
either change protocol or battery use early during the aging process or to
enable more rapid characterization of new protocols.
Other examples of detecting lithium plating due to fast charging have
used combined model-based analysis and differential voltage analysis.
Using the data from the end of rest, Katzer et al. [131] were able to
develop a detection algorithm and apply it for both C/LFP and C/NMC
commercial cells. The incremental capacity (IC) analysis detailed by
Dubarry et al. [69,132] is another example of how big data and
physical-based modeling can be combined to elucidate aging modes. In
their work, a look-up table, which contains simulated IC curves across
different electrode chemistries and extent of aging, was developed. This
synthetic data enables diagnosis and determination of relative amounts
of LLI and LAM for aged batteries. Kim et al. [133] further implemented
a deep learning-based framework to understand aging in cells that have
undergone fast charging. Their approach extracts and differentiates
unique features from IC curves over the course of LLI + LAMPE and LLI +
LAMNE. From this framework, major aging phenomena in the cathode or
anode can be pinpointed and quantified.
An ongoing challenge is to refine the sensitivity of methods to cap­
ture the extent of aging at the very initial stages and in capturing mul­
tiple signatures at the same time (e.g., both lithium plating and positive
electrode particle fracture). Being able to make such a determination
within as few cycles as possible presents the opportunity for both more
intelligent control of battery packs and the more rapid development and
ultimate validation of new protocols.
6. Considerations for charging infrastructure
Thus far, this review has focused of how fast charge and XFC pro­
tocols impact cell-level aging and performance. While fast charge pro­
tocols designed for prolonged cell-life is distinctly important to facilitate
the mass adoption of EVs, it is also necessary to consider that a battery or
EV also needs corresponding EV service equipment (EVSE) infrastruc­
ture. As new charging protocols are developed at the cell level, there is a
need to understand how these protocols scale to infrastructure needs.
The desire to have larger vehicles that are capable of XFC and that can
charge at the rates needed to replace 200 miles of range in a short time
makes it even more critical to understand appropriate EVSE power
levels. To better understand fast charge infrastructure needs, recent
work has developed methods to scale early-stage protocol development
to the vehicle level [134]. As shown in Fig. 8, the maximum power
needed for next generation EVs, especially those using advanced pro­
tocols, exceeds the power levels of current installed EVSE. In several
instances, the power needed exceeds 350 kW when scaled to the charger
level. There are three main reasons for this higher power requirement
when compared to the original XFC perspective articles [1–5]. First, the
original work was based on a battery pack of 60 kWh. Second, as ve­
hicles and their battery packs become larger, the energy needed on a kW
per mile basis increases. Third, the nature of advanced profiles, which
have non-uniform currents, leads to portions of the charge that often
exceed 6C. Power levels above 350 kW, especially for some of the
multi-step and pulsed profiles, suggest that a key consideration for re­
searchers developing protocols at the cell level is the need to understand
how advancements will impact system level needs and performance.
This is especially true as larger and longer-range vehicles are developed.
In addition to considering how protocols scale to the vehicle level,
there is also a need to consider the impacts of fast charging on EVSE and
other associated infrastructure planning. Mitigating peak power can be
achieved using several different means, including time-of-use (TOU)
pricing, the use of behind-the-meter stationary energy storage, and
smart charging algorithms that reduce charging rates or timing based on
the power available [135]. Each of the methods is a different approach
to shift or reduce power needs for EV infrastructure: TOU motivates
10
Journal of Power Sources 526 (2022) 231129
Fig. 8. Comparison of maximum power for several charge protocols after
scaling from the cell level to vehicle level for 65 kWh battery packs. MS5 9C is a
multi-step profile described in Tanim et al. [22] and the voltage ramp is
described in Mai et al. [23]. The material stress reduction profiles is a multi-step
profile means to minimize high currents at low SOC where impedance is high.
Power levels align with next generation XFC capable vehicles able to replace
range at 20 miles per min and are scaled based on experimental data captured
at the cell level. Adapted from data in Ref. [134].
people to shift charging to off-peak hours when lower cost would be
incurred; smart charging algorithms instead scale the power available to
ensure that power limits are not exceeded [136]. Another consideration
that impacts EVSE is that the peak power ratio (the ratio of peak power
to the average power) should be minimized to increase stability of the
charging system [137–139].
7. Remaining gaps and future opportunities
Over the last several years, there has been significant improvements
in fast charge protocols. Using a combination of physical characteriza­
tion and advanced models, protocols have been developed that can be
readily adapted to new cell designs and chemistries. Close coordination
of cell designs including the use of different positive electrode materials,
like NMC811, and advanced electrolytes, which have improved trans­
port, have impacted how protocols are developed. As new designs and
materials have entered the XFC realm, modifications to protocols have
enabled ramped and variable rate charge protocols to adopt lower
maximum rates without decreasing charge acceptance in a fixed time
period (e.g. 10 min). The lower maximum rates are possible as a more
uniform rate is possible for the duration of the charge. Indeed, over the
last three years, such improvements have increased the amount of en­
ergy accepted by cells tested by our team by over 25% in 10 min and,
more distinctly, have increased energy accepted prior to any constant
voltage step by close to 3x [22,23,35,140]. These advances have also
enabled key failure mechanisms such as lithium plating to be signifi­
cantly reduced [22,35,70,93,95].
While clear advances have been made, there is still a need to
continue to develop new and higher performing protocols. While some
of the impacts from lithium plating and from positive electrode aging
have been addressed, most studies currently have only evaluated out to
400–500 cycles. This cycle count is only about half of what many
automotive manufacturers desire [36]. The current protocols also are
almost entirely developed based on BOL characterization of systems.
Extended evaluation to higher cycle counts and including additional
aging considerations, such as calendar aging, will be important as higher
energy cell designs and chemistries are commercialized. With respect to
aging and failure modes, several new machine learning and character­
ization advances have been made which reduce the time needed to
E.J. Dufek et al.
understand the benefit of different charge protocols. Given that distinct
aging from both positive and negative electrode contributions have been
identified during XFC, protocols need to be developed that not only have
high performance at BOL, but that can also be adapted later in life as the
cells age. The key to achieving age-informed fast charging protocols is
the incorporation of many of the machine learning techniques described
above and the joint continued advancement of robust electrochemical
models that can be updated with specific aging constraints to adapt
protocols based on a case-by-case basis.
As new protocols are developed, including those that can potentially
adapt with aging, it is vital that researchers maintain system-level
considerations to understand how improvements may scale to both the
vehicle and EVSE level. Taking infrastructure-level limitations into ac­
count will help ensure that the rapid advancement in battery technology
is not limited by hardware or other charging infrastructure stability is­
sues. In-line with a focus on system configuration and design, the last
key area that needs an increased level of attention soon is more discrete
planning and coordination on the use of XFC charge protocols that
mirror expected use conditions. It has been shown with DC fast charging
that charging immediately after a driving event instead of right before
the driving event can change the extent of aging [78,123]. The timing of
fast charging with respect to driving events and partial charging from
intermediate states-of-charge are going to be important to investigate,
especially as more complex and physics-based charge protocols are
developed. For more vehicle-relevant scenarios, understanding how to
appropriately consider environmental conditions such as temperature
will be vital, as will consideration of how to beneficially use thermal
management to both minimize aging and improve charge acceptance.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgements
The authors thank Samuel Gillard from the U.S. Department of En­
ergy for supporting this project. Funding provided by the Vehicle
Technologies Office of the U.S. Department of Energy’s Office of Energy
Efficiency and Renewable Energy under the guidance of the Advanced
Battery Cell Research Program (eXtreme fast charge Cell Evaluation of
Lithium ion batteries, XCEL). This manuscript has been authored by
Battelle Energy Alliance, LLC under Contract No. DE-AC07-05ID14517
for Idaho National Laboratory with the U.S. Department of Energy, the
National Renewable Energy Laboratory operated by Alliance for Sus­
tainable Energy, LLC for the U.S. Department of Energy under Contract
No. DE-AC36-08GO28308, and by Argonne National Laboratory, which
is a U.S. Department of Energy Office of Science Laboratory operated by
UChicago Argonne, LLC under Contract No. DE-AC02-06CH11357. The
United States Government retains and the publisher, by accepting the
article for publication, acknowledges that the United States Government
retains a non-exclusive, paid-up, irrevocable, worldwide license to
publish or reproduce the published form of this manuscript, or allow
others to do so, for United States Government.
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