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Solvent-Free Manufacturing of Electrodes for Lithium-Ion

Batteries via Electrostatic Coating
Gerrit Schälicke,* Inga Landwehr,* Alexander Dinter,* Karl-Heinz Pettinger,
Wolfgang Haselrieder, and Arno Kwade

N-Methyl-2-pyrrolidone (NMP) as solvent.

This work demonstrates the feasibility of a novel solvent-free anode production Another oneis the more environmentally
for lithium-ion batteries. It combines a modified dry-mixing procedure with an friendly aqueous-based binder system
innovative electrostatic coating process. The mixing is divided into two steps. At with carboxy-methyl-cellulose (CMC) and
styrene-butadiene-rubber (SBR) dissolved
first, carbon black and binder are deagglomerated and recombined to a matrix
in water, which is today used as standard
structure by intensive mixing. In a second less intensive step, this matrix is
for anodes. For both systems, drying
blended with graphite. The powder mixture is fluidized and then transferred to process of electrodes is the most energy-
the current collector by inducing a high voltage. After a subsequent hot pressing consuming step in the lithium-ion battery
step, the powder coating is permanently fixed on the current collector. This production. The coating and drying pro-
procedure is presented with three different fluorinated binders. Furthermore, cesses of lithium-ion cells with 20.5 Ah
effects of different mixing intensities on the powder and electrode properties are and 3.7 V in a production line with 1 million
cells output per year require about 51% of
examined. The electrodes are investigated in the three-electrode T-cell setup
the total energy consumption.[2] Most of it
versus lithium metal to examine their C-rates and cycle stabilities. The produced is required for heating the large drying units
anodes offer comparable electrochemical performance to conventional wet- and to compensate energy losses.
coated ones on electrode and cell levels. Overall, this new process is a suitable Reduction of investment and operating
alternative to the conventional electrode production techniques. costs is a necessity. This can be realized
by decreasing the amount of solvent in
the slurry and thus shorter drying units.
Unconventional manufacturing methods
1. Introduction such as the use of extruder with less solvents or dry-coating pro-
cesses could be a solution.[3–6] The dry-coating processes known
Commercial lithium-ion battery electrodes are produced by the so far focus on the production of cathodes with lithium cobalt
wet-coating of slurries onto a current collector. The slurry con- oxide (LCO) or lithium nickel cobalt manganese oxide (NCM)
tains active materials (AM), conducting additives, and binder or anodes with lithium titanate (LTO) in combination with
(Bi) dissolved in organic solvent or water depending on the PVDF, a maximum active material content of 98% by weight,
binder system.[1] The most common system for cathodes is and a binder to carbon black (CB) ratio of 1:1. By using electro-
the one with polyvinylidene fluoride (PVDF)-copolymers and static spray guns or pneumatic units, the active material is trans-
ferred to the current collector. The subsequent thermal treatment
is conducted either by a hot rolling process, hot pressing, or by
heating in a convection oven followed by a calendering step at
G. Schälicke, Dr. W. Haselrieder, Prof. A. Kwade
Institute for Particle Technology room temperature (RT) to obtain a stable electrode. All these pro-
Technische Universität Braunschweig cesses seem to be the ideal manufacturing process because they
Volkmaroder Straße 5, 38104 Braunschweig, Germany eliminate the solvents and the corresponding disadvantages.[4–6]
E-mail: g.schaelicke@tu-bs.de Therefore, a new solvent-free dry-coating application for Li-ion
I. Landwehr battery electrodes was developed.[7,8] Here, a gunless electrostatic
Department Coating Systems and Painting Technology deposition and a subsequent hot press unit are used to coat the
Fraunhofer Institute for Manufacturing Engineering and Automation IPA
Nobelstraße 12, 70569 Stuttgart, Germany current collector with anode materials without any solvent. A sig-
E-mail: inga.landwehr@ipa.fraunhofer.de nificant reduction in production costs will be obtained with
A. Dinter, Prof. K.-H. Pettinger respect to lower investment costs, higher throughput speeds dur-
Technology Center for Energy ing the coating, and avoidance of solvents. Further savings result
Landshut University of Applied Sciences from significantly lower energy consumption by eliminating the
Wiesenweg 1, 94099 Ruhstorf an der Rott, Germany dryer stretch, leading to a considerable saving of resources in cell
E-mail: alexander.dinter@haw-landshut.de
production. No emission and explosion-proof thematics are to be
The ORCID identification number(s) for the author(s) of this article discussed with the authorities. This will reduce the environmen-
can be found under https://doi.org/10.1002/ente.201900309. tal impact and simplifies the environmental approval procedures
DOI: 10.1002/ente.201900309 for battery factories.

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In the mixing step, various challenges arise, which have to be
solved to obtain an end product comparable with conventional
wet manufactured electrodes. On the one hand, there is the ten-
dency of the CB to form larger clusters due to its primary particle
size of less than 100 nm.[9] To support the anode active material
creating electron conducting paths and to keep the internal
electrical resistance of the electrode, small, parallel particle-
particle-contacts (P2P) must be generated. Therefore, the CB
should be finely distributed and stable in small agglomerates and
aggregates in the composite, without reacting.[10] On the other
hand, to maintain the integrity of the electrode, it is important
to distribute the binder in the dry mixing process so that it is uni-
formly, finely distributed everywhere.[11,12] The subsequent coat-
ing must bond to the current collector (adhesion) and the layer
itself must also be stable (cohesion) for handling during cell
manufacturing and electrochemical cycling, causing mechanical
stress during lithium intercalation and deintercalation.[13]
Finally, the required fine distribution of the material creates the
necessity to operate with relatively high mixing intensities. In this
study, battery anode materials with different fluorinated thermo-
plastics were pretreated via a high intensive mixing processes. For
the powder treatment, we choose a two-step process: In the first
step, the target is to disperse the carbon black particles and the
binder homogenously without fragile active material particles.
In the second mixing step, the active material was mixed homo-
geneously with the carbon black-binder-mixture at constant speed
and duration. For characterization of the powder mixtures, electri-
cal powder conductivity was measured. The intensively pretreated
and mixed powder formulations were applied to the current col-
lector by high-voltage electrostatic charge. The adhesion strength
of the coating toward the current collector was characterized to
compare the mechanical strength of the anodes. Scanning electron
microscopy with energy dispersive X-ray spectroscopy (SEM/EDX)
images were taken to show fluorine distribution exemplarily.
Finally, the electrochemical performance of the dry-coated anodes
was determined in three-electrode T-cells versus lithium metal.
2. Results and Discussion
2.1. Powder Formulation
Preliminary tests have shown that graphite is delaminated and
destructed by high mixing intensities as shown in Figure 1.
Figure 1. a) Low intensively mixed material, vc ¼ 10 m s
1; b) same material high intensively mixed and destructured, vc ¼ 40 m s
1.
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At low mixing intensities, no destruction of the active material
particles is optically discernible compared with high mixing
intensities at which destruction occurs by using a Nobilta powder
processor (HOSOKAWA ALPINE AG).
It has also turned out that stabilized, nonreagglomerating dry
CB grinding within a mixture consisting of CB and binder is pos-
sible. Due to the sensitivity of the active material particles and the
described successful deagglomeration of CB, a two-stage mixing
process was developed. In the first step, the carbon black and the
binder are granulated with high intensity at 10–40 m s
1, and
in the second step, the active material is mixed with the CB-
binder-composite at 5 m s–1 of circumferential speed. Table 1
summarizes further properties of the used materials and the
formulation strategies.
2.2. Powder and Electrode Level
2.2.1. Specific Electrical Powder Conductivity
The conductivity of the dry mixed powders was investigated
before coating them onto copper foil. These measurements show
quite good carbon black deaglommeration and the mixing qual-
ity. Figure 2 depicts the specific electrical powder conductivities
for tetrafluoroethylene, hexafluoropropylene, and vinylidene
fluoride (THV) and fluorinated ethylene propylene (FEP) binder
in a mixture with carbon black after the first mixing step. The
conductivity decreases on average with increasing mixer circum-
ferential speed and longer mixing duration. The THV binder has
an overall lower specific conductivity than the FEP binder. THV
has the lower melting point, hence local melting of the binder is
expected during mixing leading to an insulating layer that covers
the conductive particles. Thus, longer and more intensive mixing
has a negative effect on the electrical conductivity.
Figure 2 shows the specific electrical powder conductivities for
the composites of active material, the different binder systems,
and carbon black (after second mixing step). Because of the high
amount of active material, the overall conductivity of the mixture
increases in both cases by a factor of about 3. This is due to the
fact that the graphite active material has a high conductivity, and
thus, the electrons can flow far through the particles without fur-
ther transition resistances. However, the tests were extended to
include circumferential speeds of 10 and 20 m s
1. Compared
with pure carbon black-binder-mixtures, THV has the higher
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Table 1. Formulation strategies and material properties.

Material Binder Carbon black Active material

Designation PVDF FEP-copolymer THV-copolymer Super C65 Artificial graphite

a) a) a) [14]
d50/μm 85 5 5 0.040 19b)
Tmelt/ C 160–168 a)
252 a)
165 a)
– –

First step Mass fraction carbon black, binder 50 50 –

mixture/%
Mixing speed vc/time tm 10, 20, 30, and 40 m s
1 for 10/20 min

Second step Mass fraction carbon black, binder, active 7 7 86

material mixture/%
Mixing speed vc/time tm 5 m s
1 for 10 min

a) b)
Material data sheet; Laser diffraction measurement.

powder conductivity through sufficient parallel connection of

650 P2P contacts and a sink in transfer resistance.
600
2.2.2. Electrode Adhesion Strength and SEM Characterization
550
S m-1

500 Figure 3 shows an exemplary impression of the structure of the

P/

AM-CB-Bi-mixtures: electrostatically dry-coated anodes. Directly after the electrostatic

450 FEP, t m =10 min coating, the applied powder has only a loose and temporally lim-
specific electrical conductivity

400 THV, t m =10 min ited bond (a). After hot pressing at about 200 kN (40 MPa), the
material is permanently and stably bonded (b) resulting in a
350 coating density of 1.70 g cm
3. A surface analysis using field-
emission scanning electron microscopy (FE-SEM) shows a some-
150 CB-Bi-mixtures:
what nonuniform surface (c). However, compared with a
FEP, t m =10 min
125 wet-processed and calendered anode shown in Figure 4 with a
FEP, t m =20 min
coating density of 1.77 g cm
3, the surface roughness of the
100 THV, t m =10 min dry-processed electrode is higher, due to area instead of line
75 THV, t m =20 min pressure.
50
In addition, cross sections were prepared, and the fluorine was
made visible in EDX as shown in Figure 3d. The images were
10 20 30 40 taken as an example from a THV system processed at 30 m s–1.
Circumferential speed vc / m s -1 The electrode shows no binder gradients, but an even distri-
bution over the entire electrode height. This is a great advantage
Figure 2. Specific electrical powder conductivity of carbon black, binder
mixtures, and active material, carbon black, binder mixtures at different of this method compared with wet coating because even a rapid
mixing speed and duration. hot process cannot lead to an internal segregation.[15]
However, the binder is not finely distributed, but there are
local accumulations. Both for a speed of 30 and 40 m s
1, the
binder is particulate and punctual and not as finely distributed
conductivities by adding the active material, except at a peripheral as initially assumed.
speed of 40 m s
1. Both curves for the different binders show a The adhesive strength of the dry-powder-coated anodes is
maximum of specific electrical powder conductivity at 30 m s
1. shown in Figure 5. It should be noted that the standard deviation
Low intensities provide “unclosed” percolation for electrons is a measure of the coating homogeneity, which has to be
within the mixture; the carbon black is still present in coarser improved in the future process development. Nevertheless,
agglomerates. Therefore, the existence of only a few single con- the dry-powder-coated anodes have an average adhesive strength
tacts increases the transfer resistance. The high stress at 40 m s
1 of over 200 kPa. That is clearly below the value of conventional
probably makes the carbon black too small, which leads to a wet-processed anodes (2500 kPa, by own wet process and same
higher number of P2P contacts. Too many of these contacts measurement, 1000 kPa[17]), but in the range of other results of
increase not only the parallel connection of the carbon black dry-coated electrodes.[6]
but also the contact resistance due to the newly created interfaces, The highest average adhesive strength with 450 kPa provides
which leads to a lower powder conductivity at high mixer inten- the anode with FEP mixed at 30 m s
1. For the coarse PVDF,
sities. Moreover, the very high speed may create a dense carbon whole binder particles are present both in the powder mixture
black coating of the graphite particles resulting in an optimum in (Figure 6a) and in the hot-pressed coating (Figure 6b). This

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Figure 3. a) Images of just coated powder and b) heat treated electrode, c) FE-SEM top-view and d) cross sections from electrode (THV @ 30 m s
1);
pressed coating density: 1.70 g cm
3; yellow: EDX detected fluorine.

Figure 4. Calendered wet-processed anode; material mass fraction: 85%

graphite, 5% conductive carbon, 10% binder; coating density:
1.77 g cm
3.[16]

results in such a low adhesive strength to the substrate for this

binder system. The adhesive strengths of the electrodes whose
carbon black binder mixture has been mixed at 30 m s
1 tend
to be slightly more adhesive than those mixed at 40 m s
1. In
addition, the adhesive strength of FEP is higher than that of
THV. This is because higher intensities produce locally higher
temperatures and the binder begins to melt. This binder can then
be absorbed more by the carbon black and is no longer available Figure 5. Adhesion strength of dry-processed anodes.

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Figure 6. a) PVDF binder particles in powder mixture with anode active material and carbon black; b) molten PVDF (circle) within the hot-pressed anode
coating.

100

99
AM
Discharge capacity / mAh·g-1

400
98

Coul. efficiency / %
97

350 96

95

FEP 30 m·s -1 , ~2.7 mAh·cm-2 FEP 30 m·s-1 94

300 FEP 40 m·s -1 , ~2.7 mAh·cm-2 FEP 40 m·s-1
93
THV 30 m·s -1 , ~3.5 mAh·cm-2 THV 30 m·s-1
(1) (2)
THV 40 m·s -1 , ~3.6 mAh·cm-2 THV 40 m·s-1 92

5 10 15 20 25 30 35 40 45 50
Cycle number / -

Figure 7. Discharge capacity (▴) and coul. efficiency (▪) curves for dry-powder-coated graphite anodes with different powder pretreatment and binder
in lithium half cells. 1) two cycles at 0.1 C (CC) charge (CCCV)/0.1 C discharge. 2) 50 cycles of cyclization stability test at 0.2 C charge (CCCV)/0.5 C
discharge (CC).

for bonding to the substrate. This effect is further enhanced by
the low melting temperature of THV. The depicted result of
PVDF, in this case a binder with large particle sizes in relation
to the active material, is not suitable for the dry mixing and coat-
ing process. The retention of large binder particles in the mixture
results in an unstable electrode coating which makes subsequent
cell preparation impossible.
2.3. Cell Level
A direct comparison of electrochemical characteristics between
dry-processed graphite anodes containing FEP and THV as
binder with different carbon black-binder pretreatment has been
performed by cycling and charge/discharge rate performance
tests. All measurements were conducted in three-electrode
T-cells with lithium as counter and reference electrodes. The
cycling performance of the dry-processed-coated anodes is
shown by the discharge capacity and coulomb efficiency of the
various dry-processed-coated anodes depicted in Figure 7 as
the function of cycle number at RT.
To analyze the cycling stability, constant current (CC) and con-
stant voltage (CV) cycling was conducted directly after two forma-
tion cycles at 0.1 C. The electrochemical functionality was tested
with low charging rate at 0.2 C and a discharge rate of 0.5 C. All
dry-powder-coated anodes reach in the first two cycles
370 mAh g
1 (99% of the theoretical capacity). After 50 cycles
at 0.5 C, the anodes delivered more than 345 mAh g
1. The dry-
powder-coated anode with FEP mixed at 30 m s
1 has the highest
cycling and efficiency stability. The retention capacity concerns
97% of the theoretical capacity after 50 cycles.
Figure 8 shows the discharge C-rate tests of the dry-processed
anodes with FEP (2.7 mAh cm
2) and THV (3.5 mAh cm
2) in
T-cells versus Li/Liþ at RT. The charging rate was kept constant
at 0.2 C during changing the discharge rate from 0.1 to 5 C after
three cycles. Despite the fact that the process parameters are kept
constant, there are significantly different loads of material on the

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FEP 30 m·s -1, 2.7 mAh·cm-2 THV 30 m·s-1, 3.5 mAh·cm-2

450 FEP 40 m·s -1, 2.7 mAh·cm-2 450 THV 40 m·s-1, 3.5 mAh·cm-2
conv. wet anode, 3.0 mAh·cm-2 conv. wet anode, 3.0 mAh·cm-2
400 400
AM

AM
Discharge capacity / mAh·g -1

Discharge capacity / mAh·g -1

350 350

300 300

250 250

200 200

150 150

100 100

50 50
0.1C 0.2C 0.5C 1C 2C 3C 5C 1C 0.2C 0.1C 0.2C 0.5C 1C 2C 3C 5C 1C 0.2C

1 4 7 10 13 16 19 22 25 1 4 7 10 13 16 19 22 25
Cycle number / - Cycle number / -

Figure 8. Discharge capacity at various C-rates for wet-processed anodes (blue circles) compared with dry-powder-coated anodes with different powder
pretreatment and FEP binder (left) and THV binder (right) in lithium half cells cycled between 0.02 and 1.5 V; average of three measurements.

electrodes when changing the binder system, which makes a compared. Powder mixing experiments were conducted at differ-
direct comparison of FEP and THV difficult and the higher ent durations within a two-step process, in which the first step
charged electrodes get lower capacity values at higher rates. serves the production of a carbon black-binder-matrix and the
Within the systems, the electrodes from different mixing speeds second step serves the gentle homogenization with the active
achieve relatively similar capacities, with FEP 30 m s
1 at a C-rate material. The mixing process results in higher electrical powder
of 1 C, from cycle 22, being about 30 mAh g
1 higher than the conductivities for shorter mixing times. A maximum conductiv-
more intensively mixed ones. For THV, the more intensively ity was found for a mixer circumferential speed of about
mixed materials result in slightly higher capacities at lower C-rates 30 m s
1. Low stress on the carbon black binder mixture produ-
of the more intensively mixed materials. Then, the capacities equal ces insufficient percolation for the flowing electrons; high inten-
at higher C-rates and the same behavior is achieved at the repeated sities lead to increased transfer resistances due to strongly
decrease to 1 C. There is a tendency to recognize that the grinded carbon black agglomerates. In the case of the investi-
long-term cyclization correlates with the conductivity of the pow- gated PVDF, binders with large particle sizes in relation to
der mixture of carbon black and binder. Due to the higher propor- the active material are not suitable for the dry mixing process,
tions of binder and especially carbon black till date, the and the retention of large binder particles in the mixture results
pretreatment of the composite materials has only a minor influ- in an unstable electrode coating. The binders FEP and THV with
ence on the subsequent performance and reduces expected dif- significantly smaller particles could be processed into stable
ferences in C-rate and cycling performance. There is a electrodes. The binder is distributed relatively homogeneously
correlation between the cycle performance and the C-rate test. over the entire electrode but is still enriched at certain locations.
The mixture with FEP shows that the less intensively mixed This leads to the lower adhesion to the current collector
composites are electrochemically more efficient and stable as compared with wet-processed electrodes.
well as achieve higher discharge capacities. In the case of The choice of the binder and its processing in the mixing phase
THV, the reverse occurs; higher stress during mixing leads has an effect on the durability and later performance. The current
to higher capacities. process with focus on short process times makes binder, like the
In comparison with the conventionally wet-coated anodes, the investigated PVDF, not processable due to its particle size.
FEP system reaches very similar discharge capacities even at The electrochemical results show with regard to the coulomb
high C-rates. For the THV system at C-rates above 1 C, the efficiency that high mass-loaded electrodes with comparable per-
dry-coated electrodes deviate significantly from wet-processed formance can be produced with this method, and it is a suitable
ones. The different binder systems influence the area loading alternative to commonly used wet-coating process of anodes
because the electrodes are manufactured with the same process for lithium-ion batteries. Future investigations target higher
parameters and presumable the internal structure. Due to the amounts of active materials in the electrodes, reduction of bind-
calendering of the wet-coated electrode, there are further struc- ers, and conducting additives, maintaining the adhesion and fur-
tural effects, like the surface roughness (cf. Figure 3 and 4), ther processability of the manufactured electrodes. Cathode
which also influence the capacities at higher C-rates. materials such as NCM are also under examination.

3. Conclusions 4. Experimental Section

This work demonstrates the feasibility of solvent-free electrode
production via electrostatic deposition for anodes in lithium-
ion batteries. Fluorinated thermoplastic binders with different
physicochemical properties and particle sizes have been
Material Description: Anode material for lithium-ion rechargeable battery
(Artificial graphite), FEP (3M Dyneon), terpolymer of THV (3M
Dyneon), carbon black (Super C65, Timcal), and copper foil with double-
sided Cu-treatment (Schlenk) was used as received. Ethylene carbonate
(EC), ethylmethyl carbonate (EMC), vinylencarbonate (VC), and lithium

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Figure 9. Schema of the electrostatic dry-powder coating process for electrodes.
(hexafluoro)phosphate (LiPF6) composition were used as received
(Selectilyte LP57, EC:EMC (3:7) 1 m LiPF6 þ2% VC, BASF) and stored
under Argon in a glovebox. Glass fiber membrane (SART13440-130-K,
Sartorius) and Li-foil (99.9%, GelonLIB) were used as received.
Mixture Preparation: The investigated formulations contained a mass
fraction of 86% active materials, 7% binder, and 7% carbon black.
Mixtures containing carbon black and binder were treated with different
intensities by varying the circumferential speed of the used mixer, a pico-
bond mixing reactor on a picoline platform (HOSOKAWA ALPINE). The
various weighed powdery components (binder and carbon black) were pre-
homogenized in a beaker by stirring with a spatula for 20 s. From this mix-
ture, 10 g were added to the mixer to reach a filling degree of about 30%.
The carbon black binder (THV, FEP) powder was mixed for 10 min, carbon
black and PVDF for 20 min at the relevant circumferential speed of 10, 20,
30, and 40 m s
1 as depicted in Table 1. Afterward, the sample was
weighed together with the active material to obtain the selected ratio
of active material, carbon black, and binder. Depending on the formula-
tion, a total of 25 g of material was produced for this purpose. The mixing
of the active material with the carbon black-binder-matrix was conducted
for 10 min at 5 m s
1.
Electrode Preparation: The anodes had been produced by using a novel
two-stage process: In the first step, a modified fluidized bed system was
used for the electrostatic coating followed by a hot pressing in the second
step (Figure 9).
The dry-blend anode mixture was transferred directly on the current
collector foil. To do so, the material was fluidized by using compressed
air combined with mechanical vibration. By applying high voltage (HV)
on the internal electrode system (10 to 25 kV; depending on the properties
of the mixture), the particles were charged and transferred to the grounded
copper foil. The foil was moved with a constant velocity (up to 2 m min
1)
and a constant distance above the fluidized bed. The loading of the elec-
trode was controlled by varying the distance between electrode and
counter electrode in combination with the substrate velocity and high volt-
age. The right combination of these parameters also avoided the unde-
sired separation of the different components in the mixture during the
application process. The retention time in the high-voltage field was
approximately 2 s and enabled an average loading of 11 mg cm
2, which
corresponded to a capacity of about 3.5 mAh cm
2. The dry-coated electro-
des were treated in a hot press for 2 to 5 min by a constant pressure
(200 kN). The temperature of the pressing jaws depended on the melting
temperature of thermoplastic binder in the mixture and ranged from
170 to 300  C.
Electrical Powder Conductivity: The specific electrical powder conductiv-
ity κP was measured using the Zwick020 materials testing machine
(ZwickRoell GmbH). For this, 1.0 g mixed powder was weighed and filled
into a cylindrical measuring cell (diameter of 12 mm). Within this cell, the
powder was pressed successively up to 400 N by a stamp with 2.5 mm
min
1. The stamp and the base plate of the cell were electrically contacted
via a CC source and a current of 10 mA was applied. According to Ohm’s
law, the specific electrical conductivity was determined by the voltage drop
across the sample at a normal force of 100 N, according to
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I  δB
κP ¼ (1)
U  AS
where I is the electrical current, δB is the powder bulk height, U is the
voltage drop, and AS is the stamp area.
Adhesion Strength: For determining the coating adhesion strength of
the anodes, a recently described improved method was used.[13] It was
measured using the Zwick020 materials’ testing machine (ZwickRoell
GmbH) at constant conditions within a drying room at 20  C and a
dew point of
30  C. For this purpose, punched samples of 12 mm diam-
eter were prepared and applied to a sample carrier with double-sided
adhesive tape (Tesa SE). On the opposite side, there was also a stamp
with double-sided adhesive tape. During the measuring procedure, the
two stamps were moved together with the sample in between. A contact
pressure of 0.6 MPa was applied for 30 s. The sample was moved apart
with 100 mm min
1 and the occurring forces were scanned with 2000 Hz
and thus recorded the necessary force to cause sample breakdown. The
adhesion strength was calculated according to
jF p, max j
σn ¼ (2)
A
where Fp,max is the maximum pull-off normal-force and A is the sample
area.
Electrochemical Characterization: Electrochemical characterization of
the prepared dry-coated anodes was conducted by charge/discharge rate
performance and cycling tests. All measurements were determined in
three-electrode T-cells using lithium metal as counter and reference elec-
trodes. The T-cells were assembled with 1.13 cm2 anode, separator, and
electrolyte under argon atmosphere in a glovebox (H2O content
< 0.1 ppm). The cells were controlled by a battery test system (CTS
LAB, BaSyTec) and cycled between 0.02 and 1.5 V versus Li/Liþ at RT,
using CV at 0.02 V until the current dropped below C/20.
Supporting Information
Supporting Information is available from the Wiley Online Library or from
the author.
Acknowledgements
The authors acknowledge the German Federal Ministry of Education and
Research (BMBF) for funding within the project “LoCoTroP” (03XP0079).
The authors like to thank the German Research Foundation (DFG) for
sponsoring the FE-SEM (Merlin Compact, Zeiss). The authors also
acknowledge the Center for Solar Energy and Hydrogen Research
Baden Wuerttemberg (ZSW) for supplying the calendered wet-processed
reference anode and Chris Meyer for providing the SEM image of the
calendered wet-processed anode.
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Conflict of Interest [5] D.-W. Park, N. A. Cañas, N. Wagner, K. A. Friedrich, J. Power Sources
2016, 306, 758.
The authors declare no conflict of interest. [6] B. Ludwig, Z. Zheng, W. Shou, Y. Wang, H. Pan, Sci. Rep. 2016,
6, 515.
[7] M. Cudazzo, A. Lenz, I. Landwehr, DE102016212610A1, 2018.
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