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Conveying Advanced Li-ion Battery Materials into Practice

Review
The Impact of Electrode Slurry Preparation Skills
Alexander Kraytsberg and Yair Ein-Eli*

electrode mixture (binder + electroactive

Li-ion batteries (LIB’s) are of the greatest practical utility for portable electronics powder + conductive additive) onto a cur-
and electric vehicles (EV’s). LIB energy, power and cycle life performances rent collector (without employing liquefied
depend on cathode and anode compositions and morphology, electrolyte com- slurry),[2] all these methods are not com-
mercially employed up to now, and they are
position and the overall cell design. Electrode morphology is influenced by the
out of the scope of the present review.
shape and size of the active material (AM), conductive additive (CA) particles, Currently, most of LIB electrodes are
the polymeric binder properties, and also on the AM/CA/binder mass ratio. produced by coating of the metal foil cur-
At the same time, it also substantially depends on the electrode preparation rent collector with a precursor slurry layer
process. This process is usually comprised of mixing a solvent, a binder, AM followed by the slurry drying; often, these
steps are followed by electrodes roll-mill
and CA powders, and casting the resulting slurry onto a current collector foil
pressing, named frequently as a “calen-
followed by a drying process. Whereas the problems of electrode morphology daring”. This type of technique is being
and their influence on the LIB-electrode performance always receive a proper employed not just in the case of indus-
attention, the influence of slurry properties and slurry preparation techniques trial LIB-production, but also for research
on the electrode morphology is often overlooked or at least underrated. The pre- purposes. The only difference being
sent work summarizes the current state-of-the-art in the field of LIB-electrode that doctor blade coating is common for
research purposes, whereas highly effi-
precursor slurries preparation, characterized by multicomponent compounds
cient slot-die coating equipment is used
and large variations in sizes and shapes of the solid components. Approaches for industrial applications.[3] The slurry is
to LIB-electrode slurry preparation are outlined and discussed in the context of prepared by mixing altogether a liquid sol-
the ultimate LIB-electrode morphology and performance. vent, a polymeric binder, AM powder (for
example, graphite as anode material, and
lithium cobalt oxide as a cathode mate-
rial) and CA (commonly, CA is a carbon conductive material,
1. Introduction or shortly, CCM). Table 1 presents some commercially available
materials for LIB-electrodes: theirs source, brand names and
While Li-ion battery (LIB) performance depends on the composi­ sizes. In some occasions, the addition of a mixing aid (disper-
tion and properties of the electrode components, i.e., electro­ sants) also may be needed. In the case of water-based solvent,
active materials (AM’s), conductive additives (CA’s) and binders, the slurry rheology properties often need to be adjusted by the
the preparation process is also important, since it governs the addition of dispersing aids and thickeners, in accordance with
morphology of the electrode; the electrode preparation technique the coating equipment requirements.[1]
improvements result not only in the cheaper production but Slurry preparation technique, wet electrode precursor drying
also in superior battery capacity and cycleability. Many different characteristics and the subsequent electrode mechanical treat-
methods (chemical vapor deposition, spray deposition, laser ment (rolling and pressing) have a significant influence on the
deposition, spin coating, etc.) were tried in LIB-electrode prepa- electrode performance,[4–8] since the parameters of these pro-
ration on the R&D-scale.[1] Whereas some efforts were devoted cesses control the electrode morphology. On the other hand,
to the development of methods of a direct coating of the dry the slurry properties influence its processability,[9] affecting the
manufacturing equipment productivity and also the finished
electrode morphology, eventually determining the overall elec-
Dr. A. Kraytsberg, Prof. Y. Ein-Eli trode performance and battery operation.
Department of Materials Science and Engineering
Technion-Israel Institute of Technology
Haifa 3200003, Israel
E-mail: eineli@tx.technion.ac.il
2. The Influence of the Precursor Slurry
Prof. Y. Ein-Eli Morphology and the Preparation Process
The Nancy and Stephen Grand Characteristics on Electrode Morphology
Technion Energy Program (GTEP)
Technion-Israel Institute of Technology LIB-cell electrodes have a complex porous structure, comprised
Haifa 3200003, Israel
of AM and CA particles; these are glued all together with a
DOI: 10.1002/aenm.201600655 binder and connected to a current collector (commonly, a copper

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foil for the anodes and an aluminum foil for the cathodes). The
Review

electrode performance and lifetime are as much dependent on Alexander Kraytsberg

the properties of these compounds as on the electrode mor- graduated from the Moscow
phology.[10–14] CA often comprises of carbon conductive material Institute of Physics and
(CCM) particles of various types; eventually, CA particles hook Technology in 1972 and
AM particles up to the current collector. The requirements to joined the Russian Academy
the well-prepared LIB-electrode (see Figure 1) are: of Science to study the
electrochemistry of oxides,
(i). AM particles should be finely dispersed without forming ag- semiconductors, and
glomerates, and CA particles form diaphanous percolated photoelectro-chemistry.
conductive network, leading to that a maximum or most of During 1994–2002 he worked
AM particles are hooked up to the current collector;[16–22] for Tracer Technologies Inc.
practically, CA often comprised of various types of carbon (Somerville, MA, USA) con-
particles, and an excellent consideration of particularities ducting Li-ion battery-related research. During 2003–2008
of conductivity of such multiscale systems are presented he was a Chief Scientist of Hi-Cell Ltd. (Israel) and studied
in.[23,24] The purpose of the binder is to secure a mechani- DMFC technology. In 2009 he joined the Department of
cal stability of the electrode structure. Practically, the binder Materials Science and Engineering at the Technion-Israel
often belongs to the polyvinyliden fluoride (PVDF) – based institute of Technology. Currently his work is focused on
polymer family. Besides, the electrode has to be adequately the electrochemistry of oxides, non-aqueous electrochem-
porous, providing an access of the electrolyte to all (or at istry, and materials for power storage.
least the most) of the AM particles.
The optimal electrode design also implies that the mass
ratios of AM to the CA and to the binder are maintained as After graduating from Bar-Ilan
high as possible. University (Israel) in 1995,
Yair Ein-Eli was a post-
(ii). AM particles are better to be small, enabling the cell to oper- doctoral fellow between the
ate at high current rates. From the common sense point, the years 1995–1997 at Covalent
suggestion that Li+-diffusion inside a solid AM determines Associates Inc., USA. He
the current rate looks natural, and since smaller particles of- headed the Li-ion research
fer the shorter Li+-diffusion paths, AM-particle downsizing group until 1998 and then
favors the current performance and Coulombic efficiency. returned to Israel, joined
Recently, some works have revised the traditionally accepted Electric Fuel Ltd. and was
values of the Li+-diffusivity (and thus, the ionic conductivity) appointed VP of Research and
of such cathode materials as LiFePO4 and Li(Ni⅓Mn⅓Co⅓) Technology. In 2001 he joined
O2, and have demonstrated that Li+-diffusion may not be the the Department of Materials Science & Engineering at
rate-determining step, even if AM-particles are micrometer- the Technion. Current research projects involve advanced
scaled.[25,26] At the same time, the enhancement of the over- materials for Li-ion batteries, metal-air cells and fuel cells.
all ionic conduction of the AM grains is not the only driving Prof. Ein-Eli is also engaged in research and development
force for AM particle downsizing, and there are two other of electroplating methods and corrosion science.
aspects which favor downsizing of AM particles, aiming the
high current rates battery applications:
The low electronic conductivity of some AM materials; e.g.,
the conductivity of LiFePO4 is ≈10−10 S cm−1 and it also
some major challenges and concerns emerge when deliber-
noteworthy that smaller particles – 2μ- have higher specific
ating AM-particle downsizing:
conductivity then larger – 15μ – particles.[27] Such low AM
a. Small (and particularly nanosized) AM and CA have a
electronic conductivity requires the employment of small
large surface area, which facilitate electrolyte catalytic
AM particles in any case, since low ionic conductivity and
decomposition resulting in gel-like films onto AM and
low electronic conductivity, both equally compromise the
CA surface if anode and/or cathode potentials are beyond
overall power performance.
the thermodynamic stability windows of the cell electro-
The morphology of the electrode laminate (conductive com- lytes[36,37]; these films are interfering Li+ transport and con-
posite); to this end, it is also advantageous to employ small sume electrolyte.
AM particles (along with small conductive additive parti- b. Solid electrolyte interface film (SEI) is always being formed
cles), because the smaller these particles are, the lower the onto LIB’s AM and CA of LIB electrodes during operation,
laminate percolation threshold is expected to be.[28,29] consuming lithium and electrolyte.[38] SEI thickness doesn’t
depend on AM/CA particle size, and thus, this lithium and
(iii). All of these provisions explain the drive for diminishing the electrolyte consumption is proportional to AM/CA surface
AM particle sizes, and the vast employment of the micron, area. This aspect is particularly problematic for high surface
sub-micron, and nanosized AM.[30–35] At the same time, area nano-AM’s/CA’s.[39–41]

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Table 1.  Some commercially available materials for LIB – electrodes; source, brand names and sizes.

Review
Material Brand Size (D50) Available from
Anode AM, Graphite RGPT100 18–21 μm Targray, http://www.targray.com/li-ion-battery/anode-materials/
anode-active-materials
Anode AM, Carbon TIMREX® KS 6 3.4 μm Timcal, http://www.mtixtl.com/msds/Leaflet%20C-NERGY%20C65%20
&%2045.pdf
Anode AM, Li4Ti5O12 NANOMYTE(R) Clusters, 1.5–3 μm NEI Corporation, http://www.neicorporation.com/
BE10
Primary particles, 50–90 nm
Cathode AM, LiMn2O4 NANOMYTE BE30 Clusters, 6–7 μm
Primary particles, 30–50 nm
Cathode AM, LiMn1.5Ni0.5O4 NANOMYTE SP-10 Clusters, 5–7 μm
Primary particles, 50–70 nm
Cathode AM, LiNi0.8Co0.15Al0.05O2 NANOMYTE BE 45 Clusters, 11–13 μm
Primary particles, 50–70 nm
Cathode AM, Li(NiMnCo)O2 PLB-H5 8.0–12.0 μm Limyi Gelon Lib Co., http://www.libgroup.net/
Cathode AM, LiCoO2 X10N ≈12 μm L&F Material Co., Ltd, http://landf.co.kr/
Cathode AM, Ni-Mg – Co oxide 8–13 μm BASF http://aerospace.basf.com/common/pdfs/BASF_HED_NCMs_
Aerospace_Data_Sheet_sfs.pdf
LiFePO4 ≈2 μm MTI Co., http://www.mtixtl.com/LiFePO4PowderforLi-ionbatteryCath-
ode200g/bag-EQ-Lib-LFPO.aspx
CB additive VULCAN XC-72 ≈50 nm Cabot Co., http://www.cabotcorp.com/solutions/products-plus/
carbon-blacks-for-elastomer-reinforcement/conductive
CB additive UF-G5 ≈6 μm Showa Denko K.K, http://www.sdk.co.jp/english/prod-
ucts/137/15641/2096.htm
CB additive HS100 ≈48 nm DENKI KAGAKU KOGYO K.K., http://www.denka.com.sg/denka_black/

c. Another hurdle is that nanosized material

implementation results in a lower elec-
trode packaging density.

All of these facts suggest that AM/CA par-

ticle sizes are to be optimal for each particular
combination of electrolyte and AM/CA mate-
rials and electrode morphologies.[1,11,42–44]
The determination of these optimal AM/CA
particle sizes is particularly important from
the slurry preparation points, since smaller
powder particles dispersion is more diffi-
cult[45]; also, smaller particles are more prone
to segregation inside the slurry (this point is
explained in detail below).

(iv). Practical thickness of the active electrode

layer lies in the range between 40 and
300 μm[48,49] with tolerance in the range
of 1–2 μm; doctor blade coating or slot-
die coating (the method, which actually is
the outgrowth of the desktop-scale doctor
blade coating) is the most common coat-
Figure 1.  Schematics of the idealized LIB-electrode. a) The electrode with a favorable mor-
ing method for LIB-electrodes.[3] The even phology, AM particles are dispersed, contacting with a current collector and an electrolyte,
active layer thickness is a sine qua non re- CA is evenly dispersed and involved in forming a conductive net, and the binder is adequately
quirement for good cell performance, and spreads across the material. b) A poorly prepared electrode, AM and CA are agglomerated.
an even slurry wet coating is a prerequisite Reproduced with permission and modified.[15] Copyright 2016, Electrochemical Society.

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Review

Figure 2.  a) A degraded slot-die coated Li(Ni) 1(Mn) 3 (Co) 1 O 2 cathode performance caused by the presence of the large powder agglomerates in the
2 10 5
laminate. b) A degraded slot-die coated Li(Ni) 1(Mn) 3 (Co) 1 O 2 cathode performance caused by the presence of the pinhole-type defects in the laminate.
2 10 5
Reproduced and modified with permission from the US Goverment.[46] c) The electrode defects (stripes) occurring once the slurry solid substance
concentration is excessively large. Reproduced with permission from Elsevier, 2016.[50] d) pinhole-type defects. Reproduced and modified with permis-
sion from In Core Systems.[47]

for getting an even dry electrode active material layer. In any
case, it is clear that the slurry should contain solid issues,
which are fairly smaller than electrode thickness. It was dem-
onstrated that powder agglomerates should be substantially
smaller than the slurry coating thickness, otherwise the per-
formance of the electrode is compromised (Figure 2a). The
presence of large particle agglomerates also results in the ap-
pearance of slot-die coating defects (Figure 2b).[50]
It worth noting that besides the fisico-chemical slurry
parameters (viscosity, granulonetric parameters of the solid
fraction, etc.), such extensive processing parameter, as electrode
laminate thick ness also plays a significant role. It was reported
that electrode laminates with higher thickness are more prone
to the thickness inhomogeneity and also to the appearance of
pinhole-type defects[51] (Figure 2d).
(v). CA should form conductive pathways in the LIB electrodes,
which suggests that CA needs to be uniformly distributed all
over the slurry volume (macro-mixing) and also against AM
particles (micro-mixing). It should be taken in the consid-
eration, though, that CA distribution depends not solely on
the mixing efforts, but also on the CA nature[52]; some types
of carbon black particles may stabilize the slurry against
segregation effects (sedimentation or agglomeration)[53] as-
sisting also the uniformity of AM/CA/binder slurry.[8,54,55]
These circumstances imply that an optimal slurry prepara-
tion approach depends not only on the sizes of the AM and
CA components but also on the particular properties of CA.
The electrode structure resulting from a poorly mixed AM/
CA/binder slurry is shown in Figure 1(b) – AM and CA par-
ticles are agglomerated and the binder is forming a relatively
large globules; in this case, a substantial part of AM is not
hooked up and/or accessible for Li+, and a substantial part of
CA and the binder are not working as they should. Therefore,
electrodes with such a morphology cannot provide a good per-
formance (see, e.g.,[56]).
The bottom line is that slurry should be evenly mixed
without AM/CA separation to maintain the electrode active
layer patters shown in Figure 1(a). The drying is also important
for preparing a performing electrode,[1,6] and an inappropriate
drying mode may result in disadvantageous electrode active
layer morphology. However, poorly mixed slurry always results
in meagre electrode active layer morphology.
The production of a well-prepared slurry of fine powders is
usually a strenuous, difficult and lengthy process; small parti-
cles (micro-sized particles and particularly nanosized particles)
tend to form inhomogeneous structured slurries with hier-
archical cluster sets on preparation (i.e., such slurries consist
of agglomerates, which in turn consist of aggregates, as it is
explained below). Slurries having particles of different kinds
particularly tend to segregate (i.e., if the slurry contains particles
having different sizes and/or densities and/or shapes).[52,57–61]
This aspect is especially important in the case of LIB-elec-
trode precursor slurries, since AM and CA particles often
differ in size, shape and density significantly (usually CA par-
ticles are smaller), which may result in CA separation and
agglomeration.[62]

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3. Basics of Micro- and Nano-Powder Slurry
Morphology
Upon dispersion, powder usually forms the slurry, which is
comprised of particle clusters suspended inside the solvent;
these clusters have two-level structure, as shown in Figure 3.
This structure consists of larger agglomerates suspended in the
solvent, which, in turn, comprised of smaller aggregates made
of primary particles.[63–65] The agglomerates are the assemblies
of aggregates, which are consolidated into the agglomerates
by weak Van der Waals forces, whereas the aggregates are the
assemblies of the primary particles consolidated into aggregates
by stronger (often electrostatic) bonds. The agglomerates are
also often referred to as “soft agglomerates” in the literature, and
the aggregates are often referred to as “hard agglomerates”.[66]
Theoretical considerations illustrating the formation of this
two-level slurry structure are reported. Namely, it was demon-
strated that upon cluster forming by assembling the prime par-
ticles, the initial dense packing begins to adopt defects (dislo-
cations, voids, etc.), and these defects compromise the cluster
strength. Finally, the particle cluster strength declines down to
the extent that further cluster build-up results in a separation
of the cluster (now it may be named agglomerate) into distinct
parts. These parts are strongly interconnected inside (now it
may be named aggregates) and weakly connected with the
neighboring aggregates.[53]
The market-available AM powder typically comprises of the
particles of 2–10 μm in size, which are often agglomerated in
globules of 50–90 μm[67] in size, as shown in Table 1. During
slurry preparation these powders are dispersed down to the
smaller sizes, as this is important from the electrochemical
points, as discussed in Section 2 (i)–(ii) as well as from the tech-
nological point.
The goals of the viable LIB-slurry preparation procedure are:
(a). Dispersing the AM/CA agglomerates
Figure 3.  Hierarchical agglomerate/aggregate structure of a slurry. a) Schematics of the structure. Reproduced and modified with permission.[68]
b) SEM images the silica clusters from practical slurry, mean primary particle size ≈650 nm, after spray drying; an agglomerate (upper image) consists of
aggregates, the detailed agglomerate structure is presented in the lower image. Reproduced and modified with permission.[69] Copyright 2016, Elsevier.
Adv. Energy Mater. 2016, 1600655 © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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(b). Reducing the size of AM/CA aggregates to the utmost pos-
Review
sible degree
(c). Providing the most favorable mutual arrangement of AM,
CA and a binder suppressing their separation and agglom-
eration.
(d). Preserving the most favorable structure and composition of
the AM, CA and binder preventing the material degradation
in the course of mixing
The outlined objectives are to be attained by application of
the adequate mixing procedure (i.e., the adequate sequences
of mixing steps and/or implementation of suitable surfactants;
the surfactant usage is discussed in details below), by the
implementation of the appropriate mixing equipment and the
employment of a proper slurry solvent. It worth to be noted that
generally, LIB-electrode related slurries are non-equilibrium
entities, and the slurry parameters degrade in time after the
end of the treatment, and AM/CA and binder often revert to
the agglomerated state as time passes[55,70–73]; the stability of
the slurry may be enhanced by binder modification (e.g., by
implementation of PVDF – binder with a high molecular chain
length[53]).
4. Mixing Approaches and Mixing Equipment
The process of slurry preparation by dispersing particle clus-
ters (agglomerates and aggregates) is similar to the process
of solid grains comminution because similar types of stresses
should be harnessed in these both cases; smaller stress inten-
sities are often needed to be applied for particle clusters dis-
persing since intra-agglomerate Van-der-Waals forces, and even
more powerful intra-aggregate forces, are weaker than inter-
crystallite and intra – crystallite forces inside grains of solid
materials. This circumstance suggests that the processes and
equipment, which are used for solid material comminution,
are also adequate for slurry preparation. Indeed, the employing
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Figure 5.  Schematic representation of the stress intensity vs cluster size

curves in relation to the processes of powder dispersion; mixers with
solid grinding issues are represented with a dash line, and hydrodynamic
shear mixers are represented with dotted line; an exemplified intra-cluster
particles adhesion vs cluster size curve is given here for the comparison,
and it is represented with solid line. Reproduced and modified with per-
mission.[74] Copyright 2016, Elsevier.

Consequently, mixers (mills) with solid grinding issues offer

higher dispersing efficiency than other dispersing machines
(ultrasonic mixing is a special case, though); the relations
Figure 4.  Schematics of the most common dispersing equipment: a) the between the minimal cluster size in the mixing slurry and
most often employed hydrodynamic shear-based mixers, also named dis- the applied specific mixing energy for alumina powder slurry
solvers, b) kneaders and c) stirred ball mills (generalization of a common prepared by different mixers are presented in Figure 6. LIB-
ball mill), d) 3-roller mills, e) disc (colloid) mills, f) ultrasonic homog- manufacturers are usually reluctant to disclose the types of
enizers. Reproduced and modified with permission.[74] Copyright 2016,
Elsevier.
their mixing equipment, and other details of their slurry-
preparation technology. The analysis of published patents
and offerings from suppliers of LIB-electrode manufacturing
of shear fluid flow is common for powder slurry preparation; equipment makes it reasonable to suggest that industrial LIB-
ultrasonic mixing also is often employed.[74–76] According to,[74] slurry mixing processes are mostly based on various versions of
the dispersing equipment may be classified under two types. hydrodynamic shear mixing; ball-mill mixing also is employed
The mixers, which are applying shear stresses to the clusters
of dispersing material through the solid grinding issues (e.g.,
stirred ball mills), are to be assigned to the first type, and the
mixers, which are applying shear stresses through the liquid
media (e.g., hydrodynamic shear-based mixers, disc mills,
3-roller mills, kneaders and ultrasonic homogenizers), are to be
assigned to the second type. Schematics of the most common
mixing devices of these types are given in Figure 4.
Kneaders (and extruders, which are actually a kneader ver-
sion) and 3-roller mills are to be used for dispersing of the
slurries with very high solid fractions and large viscosities;
these mixers are sparsely used for LIB-electrode slurry prepa-
ration, though.[56,77–79] Disc (colloid) mills also are rarely used
for LIB-electrode slurry preparation.[80–82] The reason for this
classification is that the applied stress intensity dependence
on the size of the treating clusters is different for these two
types of mixers (stress intensity is determined as the ratio of
stress force to the cluster surface, or as the stress energy per
unit cluster volume). Specifically, the shear stress conveyed to
the cluster by fluid flow is not related to the cluster diameter,
Figure 6.  The relations of the achievable minimal cluster size and the
while the stress conveyed by a mixer with solid grinding issues applied specific energy for different mixers in the case of alumina powder
is inversely proportional to the cube of the cluster size[74] as dispersing. Reproduced and modified with permission.[74] Copyright
illustrated in Figure 5. 2016, Elsevier.

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for LIB-electrode production.[83–86] The operation of a good
number of the lab-scale slurry preparation equipment is also
based on these two mixing methods, or on the combination of
these mixing methods; it is worth noting that a popular manual
mortar-and-pestle mixing procedure is actually a combination
of these two mixing processes.[87]
4.1. Hydrodynamic Shear Mixing – Based Slurry Preparation
This type of mixing treatment is often conducted by such hydro-
dynamic shear-based mixers as low energy magnetic stirrers/
dissolvers,[56,88,89] rotary drum mixers,[90] high energy homog-
enizers and Rushton turbines,[5,53,73,90] static stirrers,[85] etc. The
detailed explanation of the basics of such hydrodynamic shear
mixers may be found in.[91] Slurry preparation takes place by the
action of the hydrodynamic-based forces; the forces are controlled
by the flow shear rate, cluster cross-sectional area and the dynamic
viscosity of the fluid. The slurry preparation process comprised of
two (reciprocally related) sub-processes, i.e., the clusters break-up
and the suspended clusters re-association; the suspended clusters
undergo restructuring in the course of this re-assembling.[75,92,93]
Cluster brake-up is a complex process, which combines
three parallel paths – erosion, rupture and shattering, as illu­
strated in Figure 7.[94–102] It depends on the particularities of
particle – particle interaction, slurry solvent – particle interac-
tion, and the applied shear force, which path prevails; the shear
force, in turn, depends on a combination of the solvent viscosity
and velocity. Erosion commonly takes place under a low energy
input; small fragments are gradually shearing off from larger
agglomerates in the course of erosion. Rupture, is related to
high energy input; the clusters are separated into few parts of
comparable sizes in the course of rupture; this process starts
sharply if a threshold stress is surpassed. Shuttering is the spe-
cial variant of the rupture wherein the cluster simultaneously
separates into a substantial amount of smaller fragments. The
agglomerate re-association depends on the parameters of par-
ticle – particle interaction, solvent – particle interaction and on
the slurry solid fraction ratio.[103]
The balance between re-association and partition rates
is often governing the equilibrium size of the clusters in the
Figure 7.  a) Schematics of rotor-stator mixer and b) particle size distribution on mixing; fumed silica powder with average primary particles size 12 nm
(Aerosil R816) dispersed in water. Reproduced and modified with permission.[102] Copyright 2016, Taylor & Francis.
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slurry[104–106]; this suggests the existence of a critical size below
Review
which the cluster comminution rate becomes insignificant.[103]
This balance explains the fact that hydrodynamics-based pro-
cessing provides the slurries with the agglomerates not smaller
than ∼100 nm (under the reasonable treatment time and specific
energy input) in the most of the reported studies,[17,102,107–109]
and thus this type of processing allows complete dispersing of
the powder (down to the primary particles) only if the primary
particles are not smaller than ∼100 nm.[110] This conclusion is
supported by comparison of several specific versions of hydro-
dynamic shear mixers, and also by a theoretical modeling of
the processes inside such mixers.[74,111] The preparation of the
slurry with the median cluster diameters down to 40 nm–60 nm
is also possible by implementing motionless Ramond super-
mixer[112]; a surfactant addition also is also useful for shifting
the balance between cluster association and dissociation toward
smaller cluster sizes thus enhancing the slurry fineness.
Finally, whatever the mixing thoroughness is, a slurry
commonly comprises of re-arranged clusters (aggregates or
two-level agglomerate/aggregate issues); for LIB-electrode
morphology, the important point is that the rebuild slurry
agglomerates are more dense than the precursor AM/CA-
clusters, and thus have lower porosity.[92,96,113–115] It was dem-
onstrated, though, that the final LIB-electrode performance
strongly depends on the porosity of AM/CA clusters, so the
delicate compromise between mixing intensity (high mixing
intensity is beneficial for AM/CA dispersing) and preserving
the optimal internal structure of the AM/CA clusters inside
the slurry is to be maintained.[65,116–123] The other issue is that
the binder molecules often degrade under a very high intensity
flow conditions[124–128]; this effect may compromise the starting
binder properties. This circumstance ground is also to be taken
into consideration determining the optimal mixing intensity.
Commercially available cathode materials, anode materials
and conductive additives present considerably broad spec-
trum of powders of various sizes. Conductive CB powders
are usually small (within a nanometric scale), while the sizes
of graphite and carbon AM are often in the range of several
micro­meters (mcm). Other anode AM powder materials (for
example, Li4Ti5O12) often comprises of a primary particle
clusters of a several micrometers in size whereas, the primary
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particles are of several tenth of nanometers in size. Some of
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the cathode AM powders also comprise of micrometer-size
particles, but some of these powders actually also comprise
of primary particle agglomerates, and the primary particles
are several tenth of nanometers in size; some examples of the
commercially available AM’s and CB’s are presented in Bottom
line is that a hydrodynamic shear – based mixing is well-spread
technique, and it is a convenient method of slurry preparation,
but it usually can provide mixing only on the sub-micrometer
scale. Namely, even if the precursor AM and CA powders are
made of fine primary particles down to several nanometers is
size, the slurry consist of the intermixed AM and CA particle
clusters, usually no less than 100 nm in size; further increasing
of the flow intensity may result in a binder degradation. Thus,
the decision whether or not the hydrodynamic shear – based
mixing is an appropriate slurry preparation technique, depends
on the particular AM and CA powder fineness and binder
properties.
4.2. Ball-Mill Mixing – Based Slurry Preparation
The different versions of ball-milling mixing are the accepted
methods of slurry preparation[74,129]; this method is also in
a common use for LIB-electrode slurry preparation.[5,130–139]
As in the case of hydrodynamic-based milling, the dispersing
ability of the ball-milling process (i.e., the final fineness of
the solid clusters in the slurry) is determined by the balance
of cluster breaking down rate and the rate of fine cluster asso-
ciation.[140,141] This balance depends on the nature of the dis-
persing powder[142] and also may be shifted toward cluster
dispersing by a surfactant addition (the detailed consideration
of the surfactant action is presented below).
In the course of ball milling, though, the powder particles are
involved in the substantial surface and volume modification;
these modifications may go as far as to mechanochemical
transformation of the material (e.g., carbon nanotubes may be
a subject of scission, and their aspect ratio and structure may
change substantially[143–145]), and such processes may take place
even under prolonged low-energy ball milling[146]). Also, reac-
tions between particles, between powder and dispersing media
(solvent and/or binder),[147–149] and even between dispersing
material and the mill vial material[150] may take place; ball colli-
sions and local liquid high-shear turbulence may also result in
the binder molecules scission.[151,152]
All these mechanochemical modifications must be thor-
oughly watched and considered in the course of the slurry ball
milling; it was reported that ball milling – related AM/CA mod-
ification may be beneficial for LIB-electrode performance, but
may also impair the properties of the starting CA/AM.[117,153–157]
Besides, ball-milling action often has a complex and ambivalent
character, which depend on the specific ball-milling and mate-
rial parameters[158]; e.g., ball milling treatment may impair the
low current rate performance enhancing the high current rate
performance.[159]
The conclusion is that the ball-milling provides finely inter-
mixed slurry with smaller AM and CA clusters if compared
with hydrodynamic shear – based mixing; at the same time,
the ball-milling tends to compromise the AM and CA particles
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morphology. In fact, this slurry preparation technique may not
be recommended if the particular morphology of AM and CA
particles is suggested to be essential for electrode performance.
4.3. Ultrasonic Mixing – Based Slurry Preparation
Currently, it is accepted that ultrasound has a mixing action
at the micro-scale because of transient acoustic cavitation; the
cavitation takes place at considerably high ultrasound intensi-
ties (regarding water, it takes place at ultrasonic powers over
1 W/cm2 at normal ambient conditions). The microbubbles
are forming and growing thru the low-pressure half periods
of the sound wave; the bubble growth rate increases rapidly
on reaching some critical bubble size, and then bubbles force-
fully collapse for a very short time during the high-pressure
half period of the sound wave creating shock waves. Such fast
bubble collapse is nearly adiabatic, so the substantial local
pressure and temperature growth with large gradients are
initiated.[160]
Another process that takes place into the working volume
of the ultrasonic mixer is the macro-scale liquid flow. It occurs
because the concentration of the cavitation bubbles decreases
outward the emitter along its axis, and the bubbles diffuse
toward areas with low babble concentration drugging of the
liquid; the liquid flow rate may be as high as 2 m/s. This liquid
flow is often sufficient for providing a fair stirring inside the
working volume of small ultrasonic mixers securing uniform
dispersing of the slurry all over device working volume without
installing additional stirring equipment.[160]
The relatively low ultrasound frequencies (down to 20 kHz)
are advantageous for slurry preparation[160,161]; generally the
ultrasonic mixing offers the same mixing quality as the hydro-
dynamic–based mixing but under substantially lower energy
input conditions[162] (see Figure 6). However, the specific
advantages of ultrasonic mixer implementation depend on
the particular dispersing material.[163] The dispersion proce-
dures, which combine ultrasound and ball-milling,[164] and also
surfactant-assisted ultrasonic mixing[165,166] may be particularly
advantageous.
The characteristic feature of the ultrasonic mixing is the
possibility of the preparation of well-dispersed slurries with
low solvent content[163,167]; besides, the preparation of highly
concentrated slurries may be even more energy-efficient than
preparation of diluted slurries.[166] Regarding LIB-electrode
slurries, the ability to obtain slurries with high AM/CA and
binder contents is advantageous because the settling of the
solid fraction of the slurry can create uneven distribution of
the electrode component (AM/CA/binder) and inhomogeneous
pore distribution across the electrode thickness in the course
of the electrode drying. Slurry solids settle to the bottom of the
slurry layer concentrating in the vicinity of the current collector;
this is the electrode area, which is less accessible for Li+ ions.
Thus, this electrode inhomogeneity aggravates the local Li+-ions
shortage depriving AM in this area from absorbing Li+-ions.[168]
The higher is the slurry concentration, the shorter is the slurry
drying time,[56] and the smaller are the unwanted AM con-
centration changes.[88,169–171] Long drying time also effects in
binder distribution inhomogeneity, so that the binder runs low
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near the current collector,[171,172] which compromises the adhe-
sion of the active electrode mass to the current collector.
Bottom line, shortening the drying time improves the adhe-
sion. Besides increasing the slurry solid fraction, slurry drying
may be accelerated by elevating of the drying temperature and
also by drying under vacuum.[173] Although from the indus-
trial perspective, such drying process modifications are not
rewarding. Moreover, there are indications that whereas the
elevation of the drying temperature is beneficial for the active
layer adhesion toward current collector in the case of in-oven
drying,[173] the high temperature hot-plate (or hot roll) drying
results in a decrease in the active layer adhesion toward current
collector.[174]
Appropriate consideration must be given to possible chem-
ical actions of intensive ultrasound in the course of ultrasonic
treatment. This is particularly important in the case of water-
based slurries because of the vast generation of highly reactive
free radicals, such as H·, OH·, O· and HO2· under the ultra-
sonic irradiation conditions.[175] Within the subject of LIB-elec-
trode ultrasonic slurry dispersing, the important points are the
binder polymer chain scission and the binder grafting on the
AM and CA particles under the action of ultrasound. Popular
LIB-electrode binders such as methyl cellulose, poly acrylic acid
and polyvinyl alcohol[176–180] are prone to the ultrasonic-induced
de-polymerization, whereas the length of chain of polymeric
binder is an important parameter, which controls the electrode
quality.[181,182] Binder chemisorption and grafting, which take
place in the course of ultrasonic treatment of AM/CA slur-
ries,[183] play an ambiguous role in LIB-electrode performance;
the processes may increase the electrode integrity, which is
advantageous (this is particularly useful if AM undergoes
volume changes during the electrochemical lithiation), but may
also degrade CA/AM contacts and thus compromise the elec-
trode conductivity.[184,185] Ultrasonic treatment is a promising
method of LIB-electrode slurry preparation, and such mixing
was employed for LIB-electrode slurry preparation.[12,117,186–188]
The method is in the opening stage of development, though,
and the accurate comparison of ultrasonic slurry dispersion
method and other dispersion methods for LIB-electrode slurry
preparation is not still available.
Summing up, whereas ultrasonic mixing is less common
technique of slurry preparation than hydrodynamic shear –
based mixing and ball-milling, it has advantage of fine par-
ticle clusters disintegration and also offers the opportunity
of the slurry preparation with a very low solvent content but
enough low viscosity (such slurries are advantageous for the
further preparation processing). Also, the binder adhesion
toward AM and CA surfaces may be improved under the
ultrasound action in the course of mixing. At the same time,
the application of the high intensity ultrasound may result in
degradation of some polymeric molecules so this technique
may not be a good choice for slurries with certain particular
binders.
5. Dispersant and Surfactant Influence
Surfactants have a substantial impact on the partition of powder
clusters in the course of slurry preparation. A surfactant may
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tackle powder agglomeration and thus provide better AM/CA
Review
intermixing and slurry homogeneity in two ways.
1. The partition of the powder clusters is controlling by the
contact angle at border between particle surface and slurry
solvent (αwet). The αwet actually depends on the interaction of
the particle material and the solvent; specifically, the smaller
is the αwet, the higher is the affinity of the solvent for the solid
surface, and the finer the powder may be dispersed.[189] Sur-
factants reduce the αwet diminishing the difference between
the energy of particle attraction inside the cluster and the en-
ergy of particle-solvent interaction (ΔGpartition) thus facilitat-
ing cluster partition.[65,190–193] It worth to be noted that this
thermodynamic condition doesn’t rule out the existence of
the activation energy for the powder partition, so the disper-
sion of the powder may generally depend on the mixing en-
ergy intensity even if the surfactant reduces the contact angle
to zero.
2. The ultimate cluster sizes, AM/CA distribution, slurry ho-
mogeneity and the morphology of clusters in slurry, is also
controlling by the process of the particle association; this
association is caused by the attraction of the colliding clus-
ters.[104–106,194,195] Surfactant adsorption results in modifi-
cation of the inter-cluster interaction; specifically, charged
(anionic/cationic) surfactants hinders cluster merging (i.e.,
provides slurry stabilization) by electrostatic force, and non-
ionic and polymeric-type surfactants provide steric hindrance
of cluster merging.[192,196–198]
The AM/CA intermixing improvements and thus the ulti-
mate enhancement of electrode performance were reported
by many researches[17,18,199–202] in the case of surfactant addi-
tion into the slurry. A modification of the surfactant-assistance
mixing (substrate induced coagulation, SIC) was reported
in[16,19,203–205]; SIC assisted the even distribution of small CA
particles over substantially larger AM by adding a surfactant to
the AM suspension strictly in the amount of the AM absorp-
tion capacity. The surfactant (gelatin or polyvinyl alcohol) has
a strong affinity to CA, and so CA evenly distributes over AM
surface being added to the suspension; this results in improve-
ments of the fabricated electrode performance.
A similar approach may be implemented if the AM-nanopar-
ticles are substantially smaller then CA. A high aspect ratio CA
(carbon nanotubes, CNT’s) were mixed with binder solution
(polyacrylic acid, PAA), and the CNT’s turn to be enclosed with
the binder molecules. Subsequently, nano-AM particles were
added to the PAA-enclosed CNT’s suspension, and the AM par-
ticles turns to be evenly pasted across CA surface (the process
was named polymer-assisted assembly).[206] Figure 8a illustrates
the process, and Figure 8(b) demonstrates the excellence of the
resulting electrode.
As outlined above, LIB-electrode slurries contain not only
solid fractions (AM/CA), solvent and (sometimes) surfactant
but also a dissolved polymer (binder). Importantly, the binder
has a sounding impact onto the AM/CA dispersion process.
First, the binder often interacts with AM/CA surfaces[207,208]
providing steric and/or electrostatic protection against sec-
ondary AM/CA merging and agglomeration; this feature
depends on the binder and AM/CA-surface properties. The
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Figure 8.  a) Schematics of the of CNTs/AM composite electrode preparation by polymer-assisted assembly. b) The specific capacity vs cycle number
graph, red squares and circles show data for CNTs/PAA/Fe3O4 electrode prepared by polymer assisted assembly, and data for commonly prepared
reference Fe3O4/PVDF/CB electrode are marked with black squares and circles. Reproduced and modified with permission.[206] Copyright 2016, J. Wiley
& Sons.
binder may diminish αwet assisting the wetting of AM/CA sur-
faces by the slurry solution,[139,209–213] and thus, the dissolved
binders may serve as surfactants.[214] The binder solution with
low αwet also assists the formation of highly conductive binder/
CA bridges between adjacent AM particles on drying due to the
capillary effect of the CA/binder slurry; these bridges improve
the inter-AM conductivity increasing the electrode performance
and cycle life.[215] Second, the elastic properties of the binder
solutions have a substantial influence on the mixing process,
particularly in case of hydrodynamic shear stress driven mixing
processes.[100] Third, the binder polymer chains may interact
forming interconnected net and thus facilitating particle
agglomerate fusion and slurry flocculation.[70] The bottom line
is that the binder modifies AM/CA surface interaction with the
slurry solvent; this may support AM/CA particles association or,
on the contrary, may assist fine dispersion of AM/CA powders
depending on the particularities of this modification.[216]
Nowadays, there is a tendency for implementation of water-
based slurry solvents in LIB-production; indeed, water-based
solvents are cheaper, non-flammable and more environmentally
safe than organic solvents.[195,217–221] The change-over to the
aqueous slurries requires the implementation of water-soluble
binders; besides, pooling away from the most common PVDF
binder (which needs a non-aqueous solvent) may be advanta-
geous by itself, because this binder and its solvent (NMP) are
a subject of safety concerns.[222,223] It was also reported that
the electrodes being prepared with the water-based slurry
have more uniform binder distribution (and hence better per-
formance) than electrodes prepared with the non-aqueous
slurry.[171] Furthermore, water-soluble binders are preferable for
high-capacity Si-based anodes.[182,224]
The specific feature of aqueous solvents is that many AM and
CA materials have low affinity to water; this provision is particu-
larly related to silicone powder and CA’s, such as graphite. The
solution of this problem often facilitates by the fact that most
of frequently employed water-soluble binders are active at the
surfaces of the common AM’s and CA’s; this is related to such
binders as poly acrylates, gelatin, chitosan/chitosan derivatives,
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cellulose/cellulose derivatives, alginates, etc.[16,217,225–229]. It was
reported that many of these binders provide protection against
AM/CA agglomeration, and are assisting AM/CA powder dis-
persion by diminishing αwet[16,19,139,211,216,228–232]; some widely
employed water-soluble binders may even serve as dispersing
aids in wet ultrafine grinding of industrial minerals.[233] The
binder – assisted penetration of solvent inside the powder clus-
ters (infiltration) also has a sounding impact on the cluster dis-
solution. The infiltration may act in two opposite directions: it
may densify the clusters increasing cluster resistance toward
dispersion, and may favor the reduction of overall cluster cohe-
sion, thereby enhancing dispersion depending on the binder
solution viscosity and particularities of the binder interaction
with AM/CA surfaces.[97,234,235] Binder solutions don’t always
demonstrate adequate dispersing ability toward employed
AM’s, though. In many cases, the application of surfactants/
dispersants improves dispersity and homogeneity of AM/CA
slurries.[46,135,195,200,237–241] However, the implementation of sur-
factants may hit snags. The first issue is that the surfactant per-
sists on the AM/CA surfaces after slurry drying and thus it may
compromise electrode conductivity[202,237,238,240]; in this relation
the employment of fugitive surfactants (such as ethanol[242]),
which fade out in course of electrode drying, may be advanta-
geous. The second issue is that many anionic/cationic sur-
factants/dispersants used in water-based slurries may induce
the corrosion of aluminum current collectors.[200]
In conclusion, a surfactant implementation may substan-
tially improve slurry homogeneity and enhance AM and CA
intermixing being combined with the above slurry preparation
techniques. At the same time, the choice of the surfactant is to
be done with care; it should be kept in mind that the surfactant
leftovers may compromise the electrode performance.
6. The Sequence of Multicomponent Slurry
Preparation Steps Matters
It was reported that the performance of the electrodes, which
are prepared of the same AM, CA and binders, markedly
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Figure 9.  The effect of the mixing sequence of LIB-electrode slurry. a) Cathode, AM – LiCoO2 (≈10 μm), CA – carbon black (≈35 nm), binder – PVDF
(Mw = 7 × 104), AM : CB : binder = 95:2.5:2.5 wt. ratio, solvent – NMP, 65 wt. % of solids. Reproduced and modified with permission.[244] b) anode,
AM – 88.8 wt. % graphite, CB – 3.2 wt. % acetylene black, binder – 8 wt. % PVDF, solvent – NMP. Reproduced and modified with permission.[248]
c) cathode, AM –LiNi0,80Co0,15Al0,05O2/Li(Li-Mn-Al)2O4 mix, 2/1 w. ratio, 92 w.%, CB – 4 w.%, binder PVDF – 4 w.%. Reproduced and modified with
permission.[116] Copyright 2016, Elsevier.
depends on the mixing sequence of the electrode slurry (i.e., the
different orders of adding AM, CB and a binder in the course
of slurry mixing-preparation); the effect is confirmed for dif-
ferent slurries (for various cathode slurries and anode slurries
with a variety of AM’s, CB’s and binders).[5,116,132,243–247] Some
examples of such influence are presented in Figure 9. The
numerical modeling demonstrates the advantages of multistage
mixing if one starts the process with the less viscous solvent
(the binder is added at the second and third steps for two- and
multi-step processes, respectively) with a gradual addition
of the solid slurry components (see Figure 10a).[4] Figure 10b
demonstrates that for AM particle of each shape and size, one-
step mixing provides electrodes with a lower conductivity than
two- and multi-step mixing procedures. At the same time, all
two- and multi-step mixing procedures produce electrodes with
similar conductivities.
The most distinguished feature is that both conductivities
and binder distribution depend on AM shape and size in the
same or even at a greater extent than these parameters depend
on the process variations. This means that the implementation
of multi-step 2 increases the conductivity (1.35 times) of the
electrode made of small polyhedral AM particles, if compared
with a one-step production. At the same time, the electrode’s
conductivity is increased (in 1.30 times) if polyhedral AM’s are
changed for cuboid AM’s, preserving the preparation process
(see Figure 10b). These circumstance suggest that the shape
of AM particles are to be taken into considerations for a cor-
rect comparison of the results emerging from the different
works discussing the influence of slurry mixing processing
sequence. The alteration in the sequence of slurry preparation
steps results in a modification of the prepared electrode mor-
phology, which in turn, affects the electrode performance; such
alteration may be used as a powerful tool for electrode perfor-
mance improvements. Electrode laminate morphology modifi-
cation may comprise in a variation of AM vs CB distribution,
in a variation of AM/CB vs binder distribution, in a variation
of the electrode laminate pore structure, and in some combina-
tions, all of these parameters. In this regard, it worth to note
that the binder solubility and the interaction of the binder and
surface of the dispersing powder (expectably) plays a pivotal
part in the distribution of the slurry components.[249] Thus, it
is suggested that for different slurries (i.e., for different CB’s,
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Review
different AM’s, different binders and different solvents), the
optimal mixing process would be different.
The potentiality of the variation of sequence of slurry prepa-
ration steps were demonstrated in the work of Zheng et. al.[248]
Slurry components were graphite powder (AM), CB and PVDF,
while NMP was used as slurry solvent. Two different sequences
of slurry preparation steps were employed: first sequence
comprised of dispersing AM and CB in NMP followed by dis-
solving binder in the prepared AM/CB/NMP slurry; the other
sequence comprised of dispersing of CB into a pre-prepared
PVDF/NMP solution followed by dispersing the AM powder
into the CB/PVDF/NMP slurry (Figure 9b). The authors related
the apparent difference in cycle life of the anodes prepared with
these two types of slurries to the difference in the mechanical
properties of these electrode laminates, which originates from
the variance between the morphology of these laminates. This
assumption was supported with the observation that electrodes
prepared from both slurries had similar conductivity, but sub-
stantially different Young modulus, and the Young modulus of
the electrode, which was prepared in the second method, was
substantially lower (the electrode laminate being less rigid).
Since the viscosity of PVDF/NMP solution was substantially
higher than the viscosity of NMP solution, it is problematic for
the viscous PVDF/NMP to penetrate inside AM clusters and
spreading over all AM’s surface upon AM addition (though, it
may be suggested that the surface inside CB cluster also was
not adequately accessible for binder).
This assumption is in agreement with the provisions that
in the course of powder dispersing by rotating impeller that
the larger is the shear rate the smaller are the final size of the
clusters of the dispersing powder; G, the global shear rate is
expressed in Equation (1):
ωT
G= (1)
µV
where, T stands for the impeller torque, ω stands for the
angular velocity of the impeller, μ stands for the dynamic vis-
cosity, and V stands for the volume of the aggregation space.
Thus, the lower is the viscosity the larger is the shear rate.[92]
This means that if the viscosity of the solvent is high, it is dif-
ficult to take apart AM particles and properly coat their surface
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Figure 10.  a) Mixing sequences and suggested AM particles shapes. b) Parameters of ultimate electrode prepared from the different processed slur-
ries – the binder distribution homogeneity index (binder distributed more homogeneous into electrodes if the index is lower) and conductive interfacial
area of the electrode (the parameter, which is proportional to the electrode conductivity). Reproduced and modified with permission.[4] Copyright 2016,
ACS Publications.

with a binder integrating all AM into a laminate upon drying.
As a result, PVDF molecules contacted mostly to the external
AM particle surface and upon drying, the polymer chains were
not stretched along all AM surface. Therefore, the binder is
not entrenched inside the pores and is being mostly tangled
all together outside the AM particles, thus having a limited
free space available for absorbing the mechanical stretching
and stresses accompanied the AM lithiation/de-lithiation pro-
cesses; consequently, the electrode laminate had demonstrated
substantial rigidity. Contrary to this, the powder agglomerates
were smaller in the course of dispersing the AM/CB in a low
viscous NMP first, and then the binder freely spread all over
AM powder surface upon PVDF addition; the binder molecule
segments penetrate inside AM pores entrenching there. Thus,
binder molecules have more contacts with AM particles, set-
tling in a more ordered fashion, leaving extra free space for
absorbing stretch/stress load on the AM upon consecutive lithi-
ation/de-lithiation cycling. This explanation correlates well with
the work of Cho et al.,[70] reporting that the PVDF molecules
formed relatively large and separated clews right after slurry
preparation; these polymer molecules were finely dissolved and
it was reported that the binder spread all along the slurry after
allowing the slurry to rest for seven days (see Figure 11). It may
be suggested that PVDF distribution is a slow process, and the
polymer actually fails to spread evenly across all powder surface
in the course of mixing and soon after.
Other AM component was employed in the work of Lee
et al.[244]; the authors investigated the influence of the sequence
of slurry preparation steps on the property of LiCoO2/CB/PVDF
– electrode laminates (NMP was used as slurry solvent). Again,
two different sequences of preparation steps were compared:
first sequence comprised of dispersing a dry-premixed AM/CB
powder in PVDF/NMP solution, while the second comprised of
dispersing the same AM/CB mix in a thicker PVDF/NMP solu-
tion (PVDF + 2 of the total NMP volume), followed by a diluting
5
of the resulting slurry with the rest NMP (in three steps, 1 of
5
the total NMP volume in each step). The second method deliv-
ered cathodes with better performance (see Figure 9a). The
authors related the effect to the attaining of more homogeneous
CB distribution by dispersing AM/CB powder in a thicker
PVDF solution first, which resulted in the increase of the elec-
trode conductivity. Similar effect (better electrode laminate per-
formance if slurry preparation starts with thicker solvent, i.e.,
if the binder was added from the very beginning) was reported
in the preparation of other slurry with oxide AM, sp., Li1.2V3O8/
CB/PMMA/[ethyl acetate+ ethylene carbonate] slurry.[250]
It may be concluded that the change in the sequences of the
preparation steps may have different effect depending on the
nature of the components:
• In the case of graphite/CB/PVDF slurry,[248] better binder struc-
ture took place if dispersing in a thinner solvent is using first.
• In the cases of [Li1.2V3O8 or LiCoO2]/CB/[PVDF or PMMA]
slurries, better CB distribution took place, if the starting sol-
vent is thicker.[244]
In both cases, the performance improvements are suggested
to take place because of different morphology changes. In one

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Figure 11.  Energy dispersive spectroscopy mapping of fluorine distribution into the freeze-dried LiCoO2/CB/PVDF slurry samples, a) as prepared,
b) after a 7-day rest; the slurry was prepared by a dry blending of AM and CB powders followed by PVDF addition and dispersing in NMP. Reproduced
and modified with permission.[70] Copyright 2016, Royal Society of Chemistry.

case, the enhancement of the electrode conductivity (because of
better AM/CB intermixing) is assumed to be the cause of the
improvement; the effect, expectably, is the most pronounced
for higher current rates, as it is demonstrated in Figure 9a.
In the other case, the morphology modification was linked to
the improvement of mechanical properties of the electrode,
whereas no significant change in the electrode conductivity
was reported. It may be suggested that both types of electrode
laminate properties alteration, which are caused by variation
of sequence of the preparation steps, as well as the resulting
electrode performance modifications, depend on the particu-
larities of AM CB binder solvent interactions in the
slurry. These aspects may depend not only on the AM, CB and
binder themselves, but also on the particular AM/CB/binder
combination.[208]
Currently, a preliminary dry blending of slurry components
(AM/CB, AM/binder and AM/CB/binder), before dispersing
these precursors into a solvent (or binder solution) is gaining
momentum. A dry blending process, followed by a solvent
(or binder solution) addition and premixed powder dispersing
often has a positive influence on the ultimate electrode perfor-
mance, which was reported in many studies.[54,90,116,251–253] Two
avenues of electrode material modification by preliminary dry
blending of the precursor powder can be taught. First, this is
a dry blending of AM/CB/binder mix; the distinguished fea-
ture of this approach is that the affinity of the PVDF powder
to CB is substantially higher than PVDF affinity to AM, and
thus actually CB/PVDF composite appears first, and then the
AM particles turn to be de-agglomerated and separated with
conductive binder-CB composite (see Figure 12a).[254] It may be
suggested that upon further powder dispersing, the slurry in
some way preserves the structure presented in Figure 12a (i.e.,
the de-agglomerated AM separated with CB/binder composite),
and the morphology persists upon drying. This impels higher
conductivity and better performance to the electrode lami-
nate. Such assumption may be helpful in understanding that
a careful dispersing of the dry AM/CB/binder mix, gives elec-
trode laminates with better performance than high energetic
dispersing (see Figure 12b), which may disrupt the delicate dry
mix configuration.
The second option is a dry blending of AM/CB (without poly-
meric binder) followed by a dispersing of the resulting precursor
mix into a binder solution. The advantageous performance of
electrode laminates prepared in this way is related to an inti-
mate AM and CB intermixing, which increases the electronic
connectivity of AM particles. However, the AM/CB contact

Figure 12.  Electrode laminates with AM/CB/binder dry pre-blended precursor; a) the morphology before dispersing in a solvent. Reproduced and
modified with permission.[254] Copyright 2016, Nature Publishing Group. b) the performance of the electrode with AM/CB/binder dry pre-blended pre-
cursor prepared with differently dispersed slurries. AM is LiMn2O4/LiNi0,80Co0,15Al0,05O2 mix, CB is super P-Li, binder is PVDF, slurry solvent is NMP.
Reproduced and modified with permission.[116] Copyright 2016, Elsevier.

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Figure 13.  a) Schematics of AM and CA dry mixing; AM stands for Li[Ni1/3Mn1/3Co1/3]O2 with mean particle size 8.9 μm, CA stands for carbon black with
mean particle size 35 nm, binder – PVDF, blender – Nobilta.[259] Reproduced and modified with permission 2016, Elsevier.[54] b) TEM of the Si/Al2O3
nano-particles ball-milled with carbon black. Indeed, ball-milling with CB may result in a thin carbon coating of a treated material. Reproduced and
modified with permission.[262] Copyright 2016, Elsevier.

modification may have a complicated character. It was reported to[264]), but the ultimate cathode performance of the electrode
that in the course of an intensive blending of AM/CB mix, AM laminate prepared with the more conductive AM/CB powder
particles are covered with a thin carbon layer,[54,255] similar to a mixed on highly intensive Nobita blender is noticeably lower
carbon coating, resulting from a chemical type carbon plating; than the performance of the electrode laminate prepared with
the morphology of such mix is exemplified in Figure 13. Gen- the less conductive AM/CB powder treated on low intensity
erally, such plating substantially improves the cathode perfor- rotary drum blender (Figure 15). One more aspect is that a
mance (most of the cathode AM have a low conductivity).[255–258] dry pre-treatment helps to gain a better CA distribution and
It was found, though, that in case of inadequate amount of CB, electrode performance enhancements only if the employed
the conductivity of the ultimate electrode laminate may be sub- blending process fits the properties of the specific AM’s/CA’s;
stantially low, because of the development of a layered structure otherwise, the preliminary dry blending may even compromise
AM/[CB layer]/[binder layer], schematically shown in Figure 13; the ultimate electrode performance.[265]
importantly, an additional CB improves the
laminate conductivity.
The improvement in the electrode lami-
nate performance upon dry mixing is sug-
gested to be related with the increase of
the AM – connectivity, due to a better AM/
CA intermixing,[260] which provides an even
distribution of smaller CA particles around
larger AM particles.[54,261–263] This improve-
ment of connectivity is related to the blending
procedure mode, but this relation has a com-
plicated character. Whereas, an effect of a
low energy blending frequently is insignifi-
cant (e.g., intensive ball-milling blender was
reported to be substantially more effective
than manual mortar-and-pestle mixing[263]),
the extra-intensive blending often also has a
negative influence on the electrode laminate
performance;[252] this fact was explained by
CB aggregation in the slurry prepared from
the raw AM/CB powder, and AM aggregation
in the slurry prepared from an “over-blended”
AM/CB powder (see Figure 14).
Worth noting, the increase in the AM/
BC powder conductivity is not a warranty
of improved performance of the ultimate Figure 14.  Morphology and performance of the cathodes prepared from AM/CB mix without
electrode; a high-energy powder blender a dry blending, AM/CB dry blended at moderate conditions (ball-milled at 200 rpm) and inten-
sively blended AM/CB powder (ball-milled at 600 rpm); AM – LiCoO , CB – acetylene black
(Nobilta[259]) delivered AM/CA powder mix (average particle size 48 nm), binder and solvent for ultimate slurry2 preparation are PVDF
with a substantially better conductivity than a and NMP respectively. Reproduced and modified with permission.[252] Copyright 2016, The
low energy rotary drum type blender (similar Electrochemical Society.

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Figure 15.  Power test performance of the pouch cells with electrodes prepared from differently processed AM/CB powders and (b) powder conductivity
of the corresponding dry AM/CB cathode powders processed with the rotary drum mixer, the Nobilta and the Eirich intensive mixers, and the planetary
mixer (PMH10); cathode materials: AM – LiNi1/3Co1/3Mn1/3O2, binder PVDF CB – Super P-Li; anode materials: AM – MCMB, binder PVDF, CB – Super
P-Li and TIMREX SFG6L mix. Reproduced and modified with permission.[90] Copyright 2016, The Electrochemical Society.

7. Peculiarities of Slurries Containing Nanosized de-bundling,[303] the implementation of water-based slurries

Carbon – Graphene and CNT (Carbon Nano-Tube)
Materials
The implementation of graphene – based and carbon nano-
tube – based (CNT) materials has been growing within
recent years[266–273]; the materials are used as conductive addi-
tives,[274–279] as anode active materials[280–287] and as cathode
substrates for Li-air cells.[288] Progress in the field implies the
addressing of the features of nano-CCM slurries and the devel-
opment of the adequate dispersing techniques.
7.1. CNT
CNT’s are mostly used as conductive additives; basically, the
larger is the aspect ratio of the conductive particles the smaller
conductive additive volume fraction needs for maintaining
percolation (and conductivity) of the composite comprised of
insulating matrix and these conductive particles.[29,289,290] This
circumstance suggests that CNT’s and carbon nano-fibers
(CNF’s) CA’s are beneficial for electrode formulations because
the smaller is CA fraction the larger is the AM fraction, and
the higher is the electrode energy density. Many studies were
inspired with this consideration, and were dedicated to the
implementation of these high aspect ratio CA’s in the electrode
formulations.[291] CNT and/or CNF–based CA’s were success-
fully used as conductive additives being combined with var-
ious cathodic and anodic materials (LiFePO4,[274] LiCoO2,[292]
LiNi0.7Co0.3O2,[293] CFx,[294] LiMn0.8Fe0.2PO4,[295] LiMn2O4,[296]
TiO2,[297] SnO2,[298] Li4Ti5O12,[299] Si[300,301]), and the superiority
of CNT/CNF – based CA’s over the common low aspect ratio
CCM’s was demonstrated. The quality of CNT – material dis-
persing strongly affects the conductivity of the electrodes.[302]
The preparation of the slurries with high-aspect ratio CCM’s
presents some challenges, because these CCM’s are prone to
the bundle forming. Whereas the most common NMP/PVDF
slurry solvent is generally favorable for CNT – dispersing and
requires special approaches.
First, the CNT’s sides easily adhere to one another due to
the strong van der Waals interaction[304]; second, in the course
of hydrodynamic shear flow mixing inter-fiber friction alone
causes CNT agglomeration even aside from the inter-particles
attractive forces,[305,306] which suggests that the mixing approach
has a strong impact on the ultimate CNT-containing slurry
quality. The ultrasonic mixing is considered as an advantageous
and it is often applied for CNT dispersing.[307–310] It should be
taken into consideration, though, that CNT’s may undergo scis-
sion on prolonged sonication, and hence the optimal mixing
time and power are to be carefully determined for the best
results.[311–313] It also may be advantageous to apply special
mixing modes; e.g., it was demonstrated that the combination
of high-energy and low-energy sonication is advantageous.[314]
Whereas CNT bundling is compromising the slurry proper-
ties, the parallel orientation of CNT’s is advantageous for the
conductivity of the CNT composites[315]; this circumstance
suggests that the slurry mixing process is to combine CNT
de-bundling with overall “next-level” orientation of the de-
bundled CNT; e.g., the mixing process, which comprised of a
high-energy shear mixing followed by a low-energy shear stir-
ring, delivers CNT-epoxy composites with better conductivity
than the composites prepared by a sole prolonged high-energy
mixing.[316] The preparation of CNTs – containing slurries may
be assisted by surfactants; surfactants are particularly often
used for preparation of aqueous CNT- containing slurries.[317]
Whereas surfactant action is similar in the case of CNT dis-
persing and in the case of the common CCM dispersing,[318]
the distinct feature of the CNTs dispersing process is that de-
bundling is required. For this end, surfactants with long hydro-
philic sections have a more favorable CNT-repulsion action
(i.e., repulsion forces act over a longer distance and are also
more potent).[319] On the contrary, surfactants with too long
hydrophobic sections are disadvantageous, as they tend to
interact with two CNT-particles at once; this results in overall
CNT-attraction. Because of this, many common surfactants may

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favor CNT – bundling.[320] These circumstances suggest that the
Review
choice of surfactants for CNT dispersing needs a special care.
Generally, best fit surfactants hold molecules having relatively
short, flat and rigid chains and possessing distinct hydrophilic
and hydrophobic ends.[321]
Another way to facilitate CNT dispersing is the CNT surface
modification; the modification may consist a covalent attach-
ment of different groups and/or molecules to the sides and/
or to the ends of CNT’s.[322] It may also consist a reductive
treatment, which imparts negative charge to the treated CNT’s
(turning them into “nanotubides”).[323] Such nanotubides are
surrounded with cations and thus mimic polyelectrolytes.
These approaches impart high dispersibility to CNT/CNF. At
the same time, the CNT-modifying molecules may hinder the
Li+ and electron transfer into ultimate LIB-electrodes,[324] and
may enhance electrolyte decomposition (leading to overall LIB
degradation).[325] These instances suggest careful choice of the
specific type of CNT – modification.
It worth noting, though, that all of the above matter is mostly
related to the CNTs, whereas CNF’s are usually used as the plat-
form for AM/CNF composite material formation so that AM and
CNF intimate mixing takes place before the slurry preparation
stage; moreover, often AM/CNF – composite based LIB-electrodes
may be prepared without binder and thus the slurry fabrication
stage may be bypassed. This is particularly the case for LIB-anodes
(CNF often serve as CA and also as anode AM).[326–328]
7.2. Graphene
Graphene is a 2D – carbon material; it was employed as LIB-
anode active material and also as a conductive additive for
LIB-cathodes.[270,329–333] Anodes were often prepared solely
from graphene and a binder[334,335] or from graphene, a binder
and 3D nano-sized carbon additives.[281,336–340] The reason for
3D-carbon admixing is that graphene being a planar issue with
relatively large sizes impedes Li+ ion transport to some extent;
this steric effect may be tackled by introducing 3D nano-sized
carbon black and 1D CNT’s, which serves as spacers between
graphene platelets offering Li+-diffusion pathways.[331]
The other type of graphene-based LIB-anodes are the anodes,
in which graphene is combined with other anode materials.
Figure 16. a) The coating stability window for slot-die coating machine. Reproduced and modified with permission from Marcel Dekker Inc.[366]
b) barring-type coating defects. Reproduced with permission.[50] Copyright 2016, Elsevier.
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First, graphene is often used as the platform for AM/graphene
composite preparation.[341–344] In this case, AM and graphene
intimate intermixing takes place before the slurry formation
stage. Second, graphene may be also employed in the same way
as common conductive additives are using, i.e., as a component
of AM/CCM/binder slurry.[345,346]
Regarding LIB-cathodes, most of the studies were focused on
AM/(graphene composite) systems providing AM and graphene
properly arranged morphologically before slurry preparation
step.[341,342,347–349] Graphene was also employed as the cathode
conductive additive[350–352] being added at the slurry preparation
stage. The above development poses an issue of graphene and
graphene-based nano-composite slurry preparation; re-stacking
of the graphene platelets in the course of slurry preparation may
take place and this process is damaging for the electrode perfor-
mance.[353,354] Similarly to CNT’s, graphene may be properly dis-
persed into the common NMP/PVDF solvent-binder combina-
tion by ultrasound or by high shear hydrodynamic mixing[355,356];
this approach is frequently used in the art.[273,333,349,357–359] The
dispersing of graphene and/or graphene-based materials into
water-based slurry is a more challenging task; it is often car-
rying out employing surfactants[360,361] and/or graphene platelet
surface modifications.[362–364]
8. The Relation Between Slurry Properties and
Technological Manufacturing Process Aspects
Industrial electrode production involves the coating of the cur-
rent collector foil with a wet slurry layer of the predetermined
thickness followed by drying. Slot die high speed coaters are
the equipment of choice for such processing.[48] As shown in
Figure  16, the resulting electrode should have an even thick-
ness and should be free of coating defects; the coating process
should be highly productive (i.e., the coating speed should
be high). To this end, the hydrodynamic parameters of the
applying LIB-electrode slurry (which is generally behaving as
non-Newtonian liquid)[53] should comply with some conditions
for obtaining an even and defect free coatings onto the sub-
strate foil.
First, the slurry should have properties, which provide
an option of small wet layer thickness variations leveling
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(such variations appear as the result of unavoidable disturbances
of the slot coating flow[365]), and the leveling should be fast enough
for keeping pace with the coating rate; a low slurry viscosity favors
fast leveling.[366] Second, with a reference to Figure 13a, the
coating process is stable and results in a defect-free coating only
if the capillary number values (capillary number, Ca = (μV)/σ, is a
combination of the slurry viscosity μ, slurry surface tension σ and
substrate speed V) are all located inside the stability area, below
the border line, as shown in Figure 16a.[367] Since the substrate
speed V, determines the coater productivity, the slurry viscosity is
to be as low as possible, as the expression for Ca hints.
Bottom line, the production considerations are in favor of
the slurries with low viscosities; it stands to reason though, that
the means of slurry viscosity control should not compromise
the ultimate LIB-electrode performance. Even such extensive
slurry parameter, as slurry solid fraction content (slurry vis-
cosity, expectably, depends on solid fraction content[233]) should
be used with caution for viscosity adjustment since the elec-
trode performance may substantially depend on the solid frac-
tion content in the electrode slurry,[88] seemingly because of the
AM/CA separation in the course of drying.
Another approach to adjust the slurry viscosity is to employ
surfactants; this method should also be used with care, though.
On one hand, the optimal concentration of surfactant often
exists, and the addition of an extra surfactant may decrease the
viscosity[233]; on the other hand, an optimal value of surfactant
content may be also related to the electrode performance, i.e., the
extra amount of surfactant may decrease the slurry viscosity, but
in doing so, it may compromise the electrode performance.[199]
9. Conclusion, Summary and Outlook
This contribution outlines and discusses the current techniques
of AM/CA/binder slurry preparation and their possible future
development. The numerous examples of slurry preparation
techniques are reviewed; their advantages and drawbacks were
considered in connection with the ultimate LIB-electrode prop-
erties. The work shows the capabilities and potentials of var-
ious mixing techniques, and emphasizes the differences in the
resulting electrode morphology and performance depending
on the precursor slurry properties. Besides of the influence on
the electrodes morphology (i.e., AM/CA/binder distribution
and electrode porosity), a special attention is being paid to the
reality that the specific dispersion processes are able to modify
the structure of the electrode components (AM, CA and the
binder). These processes also substantially change the interac-
tion of the binder and AM/CA surfaces; all of these are particu-
larly related to ball-milling and ultrasonic methods of slurry
preparation.
A proper preparation of LIB-electrode slurries assumes the
attainment of the homogeneity along with appropriate distribu-
tion of the slurry components; only an adequate combination of
these slurry parameters offers the correct approach to improve
the electrode morphology and hence, to increase the specific
capacity and cycle life, and also minimize manufacturing cost.
This is because of diminishing slurry preparation and elec-
trode drying times, saving expensive battery-grade materials,
and because of substitution of the expensive and hazardous
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www.advenergymat.de
processing materials (solvents and dispersing aids). Despite
Review
of the great body of works in the literature, extensively being
reviewed here, a detailed understanding of the relation between
the mixing process parameters (type of mixing, transferring
energy, dispersing aids, etc.), the resulting slurry properties
and the ultimate electrode structure is not gained up to now,
and it is clear that the ambitious task of the preparation of the
slurry with a fully adequate properties cannot be solved without
an extensive research in the field of different mixing and dis-
persing techniques in application to LIB-electrode slurries.
The reviewed bulk of literature implies that whereas slurry
requirements seem considerably straightforward (AM, CA and
a binder are to be intimately and evenly intermixed, and slurry
viscosity is to be low), it worth to focus on a careful choice
of the best mixing process for each specific electrode slurry
(taking into consideration properties of the particular AM, CA
and the specific binder) rather than a search for “the best way
of slurry preparation”, in general. This conclusion is based on
the works reporting that often the processes, which deliver an
excellent intermixing of some systems, may be less efficient
in the case of some other systems (the mixing procedure may
damage some AM and CA components, may damage binder,
surfactant leftovers may compromise performance, etc.).
The fundamental and basic knowledge of the complex mul-
ticomponent slurry preparation processes is also applicable in
other technological fields, where such slurries are used, such
as composite material preparation, or medicine/pharmacy,
offering great opportunities in designing and preparation of
new products.
Acknowledgements
The study was financially supported by the Israeli Science Foundation
via The Israeli National Research Center for Electrochemical Propulsion
(INREP) and by the Nancy and Stephen Grand Technion Energy Program
(GTEP). The authors thank Dr. Moran Balaish (Technion) for her
assistance in the TOC graphic preparation and Mr. Jess Levinson (MA,
USA) for his proof reading and kind editing efforts.
Received: March 27, 2016
Revised: May 19, 2016
Published online:
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