INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 17, No. 4, pp.

1-14 APRIL 2016 / 1

DOI: 10.1007/s12541-016-XXXX-X ISSN 2234-7593 (Print) / ISSN 2005-4602 (Online)

Roll-to-Roll Coating Technology and Its Applications: A

Review

Janghoon Park1, Keehyun Shin1, and Changwoo Lee2,#

1 Department of Mechanical Design and Production Engineering, Konkuk University, 120, Neungdong-ro, Gwangjin-gu, Seoul, 05029, South Korea
2 School of Mechanical Engineering, Changwon National University, 20, Changwondaehak-ro, Uichang-gu, Changwon-si, Gyeongsangnam-do, 51140, South Korea
# Corresponding Author / E-mail: leecw@changwon.ac.kr, TEL: +82-55-213-3618, FAX: +82-55-263-5221

KEYWORDS: Roll-to-roll, Coating, Mass production, Printed electronics

Roll-to-roll (R2R) coating technologies, with their advantages in terms of high throughput and environmental friendliness, are
expected to be used at various industrial sites. Thin-film and thick-film forming can be conducted by various techniques that can be
installed with R2R systems including dip coating, knife-over-edge coating, slot-die coating, direct- and micro-gravure coating, and
spray coating. In this review, coating techniques are introduced from the perspective of process optimization along with examples of
applications. Moreover, R2R web handling is also covered for its relationship with the coating process. Process conditions are
obtained by presenting the mathematical modeling of each process and a real coating window is presented with surveyed data.
Applications of coating technologies focus on printed electronic devices because of their ability to use soluble materials. State-of-art
R2R vacuum coating and lab-scale coating without R2R are not discussed in this review. This summary of R2R coating techniques
and applications aims to give guidelines for operation and long-term prospects for advanced coating manufacturing.

Manuscript received: August XX, 201X / Accepted: August XX, 201X (Invited Paper)

NOMENCLATURE γL = surface tension of liquid

θL = contact angle of liquid
fr = flow rate of liquid εeq = equivalent stain within a web span
u = control input
εeeq = equivalent elastic strain
vref = velocity reference
εtheq = equivalent thermal stain
V = actual line velocity of web/roller
Dd = duration of drying
μE = effective coefficient of web/roller friction
ld = length of drying section
β = wrap angle
T1 = upstream tension twet = wet thickness of the coated layer
T2 = downstream tension μ = viscosity of liquid
h0 = coating gap (distance from the discharger or slot to the ρ l = density of the solid in liquid
substrate) g = acceleration due to gravity (9.80665 m/s2)
H = sum of coating gap and radius of backup roller σ = surface tension of liquid
tw = thickness of the web Ca = capillary number (Ca = μV/σ)
a = centroid of geometric shape in Fig. 2(a) tdry = dry thickness of the coated layer
b = axis of rotation in Fig. 2(a) ρ s = density of the solid in a dried film
Rmean = distance between the web and a n = number of coating stripes
e = distance between a and b w = width of one coating stripe
θ +Φ = angle between a and b Ug = actual line velocity of roller (reverse coating case)
W aSL = surface energy at solid-liquid interfaces Vc = cell volume per unit area of roller surface

© KSPE and Springer 2016

 2 / APRIL 2016
α = asymmetry factor of the film-splitting flow
We = Weber number
ρ g = gas density
v = initial relative velocity between the gas and the liquid
D = initial diameter of the drop
σd = surface tension of the drop
1. Introduction
Coating is defined as the process of covering a substrate with a thin
layer by deposition of specific materials in the liquid phase (solution)
or solid phase (powder or nanoparticles).1 Coating techniques can be
adapted to manufacturing in accordance with target specifications such
as coated layer thickness, roughness of the coated surface, rate and
dimension of the coating product, which can be determined by the coating
velocity, width of the coated film and patterning capability (full or striped
coating; here we refer to three-dimensional coating as printing).2,3
The coating process can be conducted in environments of atmospheric
pressure and down to low vacuum.4 It is classified by the choice of
coating materials with regard to solubility. In solution coating, the
target material and a binder are dissolved in a solution that can directly
coat the substrate, and the solution evaporates from the resulting wet
film to obtain a dried film.5,6 In contrast, vacuum deposition such as
chemical vapor deposition,7,8 physical vapor deposition,9,10 atomic layer
deposition,7,11 plasma,12 and sputtering13 are mainly used for thin and
very uniform deposited metallic layers, which are used to conduct heat
or electricity in low- or high-vacuum conditions. In this review, we
only cover solution process examples.
From the viewpoint of production scale, solution coating techniques
can be categorized into lab-scale and large-scale production, which
closely relate to roll-to-roll (R2R) manufacturing.14,15 Drop casting,
spin coating, and bar coating are simple to use, and are used primarily
for small-sized overlays in electronic applications such as flexible
printed circuit boards (FPCB),16 die-sensitized solar cells (DSSC),17
supercapacitors (SC),18 and transparent conducting films (TCF).19,20
These introduced techniques are not compatible with the R2R process
characteristics of large area and high speed. On the other hand, there
are several applicable coating methods for the R2R process; dip coating,
direct gravure coating, micro-gravure coating, knife-over-edge coating,
slot-die coating, spray coating, and liquid flame spray (LFS) coating
are mainly discussed in this paper.2,21-26
Coating technology is used mainly for purposes of decoration,
protection, and functionality.27 Recent studies focused mostly on
functional film coating, which is closely related to printed electronics
applications such as TCF,25 DSSC,21 e-paper,28 radio frequency
identification (RFID),29 organic photovoltaics (OPV),2 batteries,23,30
fuel cells,31 sensors,32-34 microfluidics,34,35 and SC18,25 because of their
needs for thinner layer formations of tens to hundreds of micrometers.25
The above-mentioned coating techniques have process characteristics,
so coating techniques should be selected considering the target device
structures (single- or multi-layer), film thickness ranges (0.01 to 250
μm), and uniformity of coated layers.
INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 17, No. 4
In this paper, a total of seven typical R2R coating techniques are
discussed and a total of 18 applications are introduced. Lab-scale
coating techniques and applications are not discussed, and nor are R2R
vacuum deposition techniques. The purpose of this review is to
introduce the characteristics and process parameters of various R2R-
adapted coating technologies, and to show the state of the art for coating
products reported in previous literature. In particular, web handling is
the core technology of the R2R process, and is also addressed. From
these perspectives, the appropriate guidelines and information are
suggested to readers for consideration relevant to their fields; it is
hoped that this will also give motivation for the development of the
next generation of R2R coating technology.
2. Roll-to-Roll System
The typical R2R system shown in Fig. 16,36 consists of an unwinder,
edge position controller (EPC), dancer roll, infeeder, preheater, dryer
(hot air), outfeeder, and rewinder. Moreover, between the driven rollers
(servo-motor-linked), idle rolls and load cells play roles in web path
changes and tension measurement, respectively. Printing rollers such as
gravure and coating modules like slot-die or knife modules can be
ascribed to the processing zone. The coating or printing process is
performed on a moving substrate in the R2R process rather than glass
substrates on linear stages. In the R2R system, thin and flexible web
materials such as polyethylene terephthalate (PET), polyethylene
naphthalate (PEN), polyimide (PI), metal, paper, and textiles have been
used as substrates.37-42 The web is easy to stretch, and can fluctuate and
break if the web is not precisely transported with appropriate velocity
and tension. Therefore, it is necessary in advance to optimize the
configuration of the R2R system and web controller to achieve a stable
coating process as introduced in the sub-themes in this paper.
2.1 Velocity control
The velocity of the web in the coating process is the most significant
factor affecting the coated layer thickness. It is related to the ratio of
supply liquids to substrate velocity, capillary number, cohesion of the
liquid, shear stress changes of the liquid, and so on.43-46 Therefore,
coating velocity should be controlled precisely in the coating process so
that systemic guidelines can be proposed.
The backup roller has a very important role for precise transportation
in the coating zone, as shown in Fig. 2(a).47 A master speed drive is set
for the backup roller because that roller should not be changed in order
to leave undisturbed the ratio of fr. The coating velocity is controlled by
u and feedback from an encoder (V) by comparing with vref. Most
backup rollers are linked to servo motors, but the wrap angle becomes
involved when a backup roller is constructed as an idle roller. The belt
friction can be expressed as in Eq. (1),48
1 T
μE = --- ln ⎛ ----2-⎞ (1)
β ⎝ T1 ⎠
If is 180°, the air entrainment and slippage between the web and the
backup roller can be minimized by maximizing the traction forces as
increments of μE. As a result, the velocity of the backup roller can be
stabilized.47
 INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 17, No. 4
Fig. 1 Configuration of a general R2R printing and coating system (Adapted from Ref. 6 with permission)
Fig. 2 Importance of coating speed: (a) a schematic of the slot-die
coating process (Adapted from Ref. 47 with permission) and (b) flow
rate setup with coating velocity increments (Adapted from Ref. 6 with
permission)
From the viewpoint of roller eccentricity and roundness, the coating
velocity is related to roller machining and machine setup, and the
coating gap considering the roller eccentricity model can be expressed
as in Eq. (2),47,49
h0 = H – [tw + Rmean + e sin (θ + φ )] (2)
The h0 can be changed periodically by eccentricity of the roller,
APRIL 2016 / 3
which affects coating phenomena,50 tension control, and the constant
value of V. Moreover, the roundness of the backup roller is also related
to Eq. (2) from the viewpoint of the relationship between angular
velocity and V,37 so a pretest of roundness and eccentricity should be
measured.
After the velocity of the backup roller is stabilized, the flow rate
should be precisely controlled in the accordance with velocity changes,
as shown in Fig. 2(b).6 For fixed velocity, the deposition rate of the
liquid can be different for various coating techniques; this can involve
varying the flow rate in spray24 and slot-die coating,50 the depth in knife-
over-edge coating,2 and the transfer ratio from the solution bath in
gravure and micro-gravure coating.22,51
These settings are also related to the precision of the pump (whether
screw, gear, or syringe) and stage alignment; but viscosity and the roller
velocity are dependent in transfer coating cases based on transfer by
shearing of a liquid onto the roller.52
2.2 Tension control
Tension control is a very important issue in the R2R process. Various
studies on tension control have been conducted based on tension
modeling,53 experimental verification,54 and controller design.55,56 All of
these efforts are focused on the minimization of tension disturbances
such as elongation of the web, flutter, and positioning;48 but surface
tension is also significant.57
The relationship between surface energy of the web substrate and
surface tension of the liquid is shown in Eq. (3),58
a
WSL = γ L ( 1 + cos θL ) (3)
Droplet testing was carried out on a tensioned web as shown in the
a
inset of Fig. 3(a).57 Fig. 3(a) shows that θ L was varied and WSL changed
when dropping 1-bromonaphthalene, glycerol, and ethylene glycol on a
PET substrate with tension applied from 2 to 7 N/mm2.
Furthermore, the thicknesses of printed layers were changed in the
case of gravure printing using Ag ink in the range of 100~150 mPa·s,
as shown in Fig. 3(b). The change was small, about 70 nm; but this
 4 / APRIL 2016 INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 17, No. 4
Fig. 3 The effect of surface tension on printability: (a) surface tension
of a substrate (inset: contact angle measurement) and (b) thickness of a
printed layer (Adapted from Ref. 57 with permission)
would make an enormous difference in the coating process.
There are other ways to change the surface tension of liquids and
substrates by solvent tuning59 and plasma treatment.60 Material tuning
and substrate treatment can be useful for changing coating ability, but
surface tension control is also too important to be ignored.
2.3 Temperature Control
A solution process coating layer requires a drying process to
evaporate the solvent. The temperature of the drying section has an
influence on plastic substrates such as PET, PEN, and PI because of
thermal deformation.54 Among them, PET is most widely used as a
substrate, but it expands and shrinks at or above 75°C.36 Tension of the
web can be varied according to the temperature, which can be expressed
as in Eq. (4),61
e th
ε eq ( t) = ε eq ( t ) + ε eq (4)
In the drying section, there is an effect of thermal strain change
th e
represented as ε eq (this is not limited to the effect of ε eq within the
span). The stress of the substrate due to temperature changes increases
by about 4 times when the temperature is varied from 30 to 100°C.61
The change is also attended by a conductivity change of the Ag printed
layer, as shown in Fig. 4(a).62 The tension increase is inversely
proportional to the conductivity and temperature variations in the
Fig. 4 Drying effects on the coated layer and the web substrate: (a)
conductivity change as tension changes at different temperature
conditions (Adapted from Ref. 62 with permission) and (b) coffee ring
effect of an inkjet-printed layer (Adapted from Ref. 63 with
permission)
experimental results.
The effective drying time can be expressed as in Eq. (5),
l
Dd = ---d (5)
V
In the fixed temperature condition, Dd was determined by layer
characteristics and ld and V changed with the design of the dryer zone
and process speed changes. Firstly, the solvent should evaporate and,
secondly, the functionality of the layer (such as its conductivity) should
be considered. However, effective drying and sintering methods have
been investigated in recent studies, including the use of infrared, lasers,
intense pulsed light, ultraviolet, and microwaves.64
These methods focused on the reduction of time and not only on
substrate damage. Thus, Dd can be minimized not only by ld and V but
also by controlling sintering power and temperature within the limit of
substrate damage sensitivity. If the temperature is too high or the
duration of drying time is not suitable, the coated layer can present a
non-uniform surface in the inkjet printing case called the “coffee ring
effect” and the “Malangoni effect”, as shown in Fig. 4(b).63
In the large-area coating case, the increment of thickness on the edge
of a coated surface is the problem, so it has been improved by changing
the coating method65 or by process optimization experimentally.43
 INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 17, No. 4
Fig. 5 R2R-based coating techniques: (a) dip coating (Adapted from Ref. 66 with permission); (b) knife-over-edge coating (Adapted from Ref. 2
with permission); (c) slot-die coating (Adapted from Ref. 76 with permission); (d) direct gravure coating (Adapted from Ref. 52 with permission);
(e) micro-gravure coating (Adapted from Ref. 32 with permission); and (f) spray coating (Adapted from Ref. 67 with permission)
3. Roll-to-Roll Coating Processes
The appropriate coating operating conditions, which are called the
coating window, can be selected to obtain the target thickness of a layer
by mathematical and experimental approaches. Coating flows have been
analyzed by mathematical prediction based on the governing equation1,50
using computational fluid dynamics68,69 for visualization. No genuinely
predictive modeling for the coating process has been investigated
because of the complexity of coating flow and the variety of coating
liquids.1 The computational approach can offer more accurate dynamics
of flow in small regions, but demands a substantial amount of time for
analysis and encounters problems when extended to large-area processes
like the R2R process. Therefore, it is advantageous to screen the most
effective coating parameters to achieve desired coating results based on
knowledge and skill rather than analytical modeling.
The coating processes can be categorized into self-metered and pre-
metered types.70 Self-metered coating determines the coating thickness
through combined effects of coating parameters such as liquid properties,
web velocity, and geometry of coater shapes. On the other hand,
premetered coating involves coating parameters that independently
affect the coating thickness, and is therefore more sensitive.1 In this
section, we combine and summarize R2R-adaptable coating techniques
as shown in Fig. 5, including the self-metered dip and knife-over-edge
techniques and the pre-metered slot-die, direct gravure, micro-gravure,
APRIL 2016 / 5
and spray coating techniques along with their main coating parameters
in order to offer a guideline and perspective for industry.
3.1 Dip coating
Dip coating is the simplest method for film fabrication and is
normally used in the lab-scale step of very advanced TCF structures
before scale-up.71 It can also be adapted to the R2R process21,66 with
immersed roller modules in the reservoir, as shown in Fig. 5(a). The
bare film is driven from an upstream span and soaked in the liquid first.
The coating process is performed when the web moves out to the
outside of the reservoir. The coated layer thickness twet formulated on
the web by withdrawal relative to various parameters of μ, V, ρ l, and
g can be expressed as in Eq. (6),66
μV
twet = 0.8 ------
- (6)
ρl g
The coefficient of 0.8 is the constant for Newtonian liquids, and not
for low-Ca cases less than 0.01.72 As a result, liquid characteristics and
coating velocity are dependent on formulation of the liquid in the dip
coating process. To obtain the good coating products in the dip coating
process, high-viscosity liquids with high surface tension are suitable in
order to maximize the drag force of the liquid on the substrate.66 For
more detailed information on modeling, see the previous work of
Scriven et al.66
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3.2 Knife-over-edge coating
R2R knife-over-edge coating was used in the fabrication of layers of
OPVs, batteries, e-paper, and fuel cells.2,23,28,31 Knife-over-edge coating
is simply classified as one of the blade coating methods, as shown in
Fig. 5(b). A knife is vertically positioned over the roller at a distance
of h0, wiping away excess liquid and formulating a coating layer when
substrate moves past with a specific velocity. The mathematical
estimation of the coated layer can be expressed as Eq. (7),2
1 ρ
tdry = --- ⎛ h0 -----l⎞ (7)
2 ⎝ ρs ⎠
tdry can be varied by changing h0 and the liquid concentration (such
as by varying ρ l and ρ s). The density terms belong to material and
solution properties but only the process condition of h0 can control the
thickness of the coated layer in the case of a fixed solution. As mentioned
in Eq. (2), h0 can become unstable due to the eccentricity and roundness
of the roller,47 so a knife should be fixed accurately to the coating zone
to obtain a uniform coating. Moreover, the knife must be arranged
parallel to the web’s motion direction. The coating velocity is not
related to coating thickness control but is closely related to the leakage
of coated liquid. The leakage and overflow of the liquid is a critical
problem in knife-over-edge coating. This problem has been handled by
changing the knife length and shape and installing a solution bath for
high-viscosity solutions.2
3.3 Slot-die coating
Slot-die coating [Fig. 5(c)] is the typical R2R-adapted method used
widely in various coating products such as OPVs,73 TCF,74,75 pressure-
sensitive adhesives (PSA),43 and has been especially easily demonstrated
for multi-layer and stripe coating.76 In contrast with self-metered coating,
it is a pre-metered coating technique in which tdry can be estimated and
controlled by tuning coating conditions and liquid properties such as h0,
V, fr, μ, σ, and ρ l. Without considering the concentration of the solution,
twet can be determined by combining the process parameters as presented
in Eq. (8),50
h0
twet = --------------------------------
–2/3
- (8)
1 + 1.49Ca
This equation is called the viscocapillary model, which was derived
by Carvalho and Kheshgi, and this equation is only valid at low Ca
numbers below 0.02.50 From Eq. (8), it is clear that, in the slot-die
coating process, coating properties affect the coating thickness.
Furthermore V and h0 have an impact as R2R process parameters. V is
easier to set in the R2R process, and has been identified as the most
significant parameter in the R2R slot-die coating process.6,76
In high-Ca cases, the coating window is changed and is not
appropriate for use of the viscocapillary model. Apart from Eq. (8), the
thickness of the coated layer can be derived as in Eq. (9), which is more
suitable for high-Ca coatings:2,43
fr ρ l
tdry = ----------
- ⋅ ----- (9)
nwV ρs
It has been verified that the proposed Eq. (9) predicts the actual
coating thickness when using high-viscosity solutions.43 Moreover, Eq.
(8) does not consider fr, which is a very significant term in the coating
process, because the meniscus downstream is considered as having a
cylindrical shape. Thus, fr should be controlled along with V; these
factors are dependent on each other in a relationship of proportionality
for a stable meniscus.6 To conclude, slot-die coating is a sensitive process
depending on various parameters suited to producing high-precision
layers.
3.4 Gravure coating
Gravure coating is the only method of using a coater as a backup
roller itself. Using the engraving style on the roller, a gravure roller can
implement a complex line patterning and not only a coating layer.36,77
The gravure printing method is a rapid process with high-resolution
printed lines compared with other printing processes such as inkjetting,78
offset printing,79,80 screen printing,81 and transfer printing.82 In the
patterning process, the gravure roller and a nip roll rotate differently to
transport the web substrate at a specific velocity.
In contrast, using a gravure roller as a coating process, the pattern
is engraved all over the surface and the gravure roller’s rotation direction
can be changed to contrast with the web’s driving direction. Direct and
offset coatings mean that the gravure roller directly touches the web
and that a coating layer is transferred by an offset roller, respectively.
In addition forward coating in the same direction as the web’s driving
direction, reverse coating can be done in the opposite direction to web’s
motion. This is classified under the category of nip rolling.52
Figs. 5(d) and (e) illustrate forward gravure coating with a nip roll
and micro-gravure coating, respectively. Micro-gravure coating is defined
where the diameter of the coating roller is very small compared with its
width. Micro-gravure coating can obtain thin layers as in slot-die
coating.51 Benkreira et al. theoretically established the film thickness in
reverse gravure coating as shown in Eq. (10),52,83
U 1
twet = -----g- ⋅ ------------------------------ ⋅ Vc (10)
V ⎛ Ug ⎞ 1.65
α ------ +1
⎝V⎠
twet in gravure coating is determined by the velocity ratio Ug/V and
Vc. Vc is related to the machining of the roller and the doctoring pressure
depth and pressure fixed in the coating process.
The velocity ratio Ug/V is the main experimental parameter in gravure
coating. It is the origin of the drag force on the substrate from the roller.
It is realized that the same velocity between the roller and the web is
the condition for the lowest twet.32 twet increases proportionally to the
velocity ratio Ug/V, which can be used to increase the flow ratio
(withdrawal).52
Gravure coating is a pre-metered technique, but has limitations with
respect to the surface energies of the liquid and the substrate. The
aggregation of liquid itself and interaction between the liquid and the
substrate can determine the liquid transfer ratio, so these must also be
considered.84
3.5 Spray coating
Fig. 5(f) depicts spray coating on an R2R-transported web substrate.
Spray coating has been conducted where liquid was forced by gas flow
and discharged through a nozzle. Spray coating is known not to be
compatible with the R2R process and is complex because it handles
droplets.2 R2R spray coating has been introduced for fabrication of SC
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Table 1 Previous research on implemented R2R coating techniques, operating conditions, and products (D: dip coating, DG: direct gravure coating,
K: knife-over-edge coating, MG: micro-gravure coating, SD: slot-die coating, LFS: liquid flame spray coating, S: spray coating)
Solid
Method App. Material μ V h0 fr Temp. w twet/dry
contents
D21 DSSC TiO2 10wt% - 1 - - 120-140 - 10 (wet)
22 992-
DG - - 1-4 19.8-210 - - - 100 1-10 (dry)
1088 kg/m3
28
K e-paper TiO2 - - 9.14 - - 179-192 - 12-40 (dry)
K87 OPV ZnO 50 mg/ml - 0.8 300 - 125-130 250 0.02 (dry)
K/MG23 Battery (Li) Carbon - - 0.25-10 25 (K) - - 875-1185 2-200 (dry)
K/SD31 Fuel cell PBI 9wt% - 0.20 400 - 140 250 40 (dry)
Paper
LFS24 TiO2 50 mg/ml - 150 105-25·104 23 75-110 50 1 (dry)
(coated)
MG32 Sensor (flex) Carbon 1120 kg/m3 20 0.3 (web) - - 130 150 4.31 (dry)
MG51 TCF PEDOT:PSS - 1-1000 0.18 - - - - 0.02 (dry)
SD6 AR Si 1.5-5 3.3 1.6-4.4 100 2-13 140 100 0.06-0.13 (dry)
SD73 OPV P3HT:PCBM 13.5 mg/ml - 2 - 1.7 140 <305 0.129 (dry)
P3HT:PCBM/
SD88 OPV 60 mg/ml 25 240 - - 140 - 100 (wet)
PEDOT:PSS
Sensor
SD33 Ag - - 1.2-2.4 100 2-7 - 250 0.67-0.252 (dry)
(piezo)
43
SD PSA PSA 20wt% 1800 2-10 100-400 10.65-53.74 120 150 4.5-5 (dry)
74 AgNW/
SD TCF 0.5wt% - 2.7 100 3-25 150 260 -
PEDOT:PSS
PEDOT:PSS/ 10-20wt%
SD75 TCF - 2-10 40-60 16.2-54 130 500 5-60 (wet)
AgNW (AgNW)
47
SD TCF CNT/AgNW/Si - 2.12-8.68 1-2 30-50 3-9 110 250 1-26 (wet)
S25 SC CNT 1 mg/ml - 4 cm2/s - - - - 4 (dry)
Units: μ (mPa·s), V (m/min), h0 (μm), fr (ml/min), Temp. (°C), w (mm), and twet/dry (μm).

devices.25 There have been many studies of spraying and evaporation
of spray-coated layers.67 Firstly, atomization is the key issue in spray
coating, and can be expressed as in Eq. (11),67
2 phenyl-C61-butyric acid methyl ester [P3HT:PCBM] and poly(3,4-
ρg v D
We = --------------
- (11)
σd
By changing We, the breakup of drops for atomization is classified
into three regimes: bagging, stripping, and catastrophic breakup.85 From
this equation, we can see that the liquid properties and gas flow can be
determined for a uniform layer. This has been determined for uniform
atomization. Nevertheless, there is no mathematical model of spray-
coated thickness relating to the coating conditions in the R2R process.
Moreover, the flight of droplets and their landing on the substrate with
splashing must also be considered in obtaining a uniform layer.86
However, LFS coating in the next section is worthy of notice because
of its rapid and thick-layer coating ability.24
4. Roll-to-Roll Coating Applications
Research mentioned in this section shows R2R transportation
performed for coating examples and applications. There have been many
studies on various coatings that have the potential to be realized in R2R
processes, but only the implemented cases were surveyed. In Table 1,
the coating methods, applications, main coating materials, solid contents,
viscosity, coating conditions such as V, h0, fr, and drying temperature,
and coating output such as w and twet/dry are summarized.
Slot-die coating was shown as the most used technique for R2R
coating applications in the survey data listed in Table 1. OPV fabrication
was actively researched using stripe coating of poly(3-hexylthiophene):
ethylenedioxythiophene)-poly(styrenesulfonate) [PEDOT:PSS] on PET
film coated by indium tin oxide (ITO).73,88 The shim plate makes it
possible to coat stripes. The fabricated module shows working IV
curves, as shown in Fig. 6(a), which play a role in large-area modules
as shown in the inset of Fig. 6(a). There has been research on anti-
reflection (AR) coatings on PET films where Si material was used,
indicating R2R compatibility.6 Not only polymer material, but also Ag
has been coated in R2R slot-die coating systems, forming a large-area
conductive layer which was then patterned to ablate the unnecessary
area by laser writing,89 as shown in Fig. 6(b).33 The fully coated and
written Ag layer was used for piezoresistive sensors. Moreover, a PSA
solution of high-viscosity liquid was fully coated on a PET substrate,
as shown in Fig. 6(c). A PSA film product showed a uniformly coated
layer that can be used in display and protective films.43 Lastly, TCF was
conducted many times47,74,75 in previous works based on R2R slot-die
coating. Fig. 6(d) shows one example of fully R2R-slot-die-coated
silver nanowire (AgNW)/PEDOT:PSS hybrid film.74 The inset of Fig.
6(d) shows a scanning electron microscope (SEM) image of a AgNWs
network and PEDOT:PSS-covered surface that can enhance electrical
properties. TCF has been widely adopted in electronics applications such
as touch screens and OPVs.3
R2R gravure coating has been used for industrial applications, but
has been more closely adapted to printing techniques.36,77 In recent
 8 / APRIL 2016 INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 17, No. 4

Fig. 6 R2R slot-die coating applications (a) IV curve for 16 serially connected OPVs 35.5 cm2 in size [inset: photograph of OPV module of 79×84
mm] (Adapted from Ref. 73 with permission); (b) Slot-die-coated Ag layer and ablated line by laser writing (Adapted from Ref. 33 on the basis of
OA); (c) R2R slot-die coating process of a PSA solution (Adapted from Ref. 43 with permission); (d) Photograph of AgNW/PEDOT:PSS film [inset:
SEM image of AgNW/PEDOT:PSS film] (Adapted from Ref. 74 with permission)

studies, micro-gravure coating was further investigated for advanced
electronics applications, as shown in Fig. 7. A carbon-material-based
solution was synthesized as a mixture of carbon powder, toluene solvent,
and binder, and deposited on PET film as shown in Fig. 7(a). The
carbon-coated layer was obtained with 4.31-μm layer thickness for a
flex sensor.32 Moreover, a PEDOT:PSS layer was coated on a PET
substrate by using a R2R micro-gravure coating technique that achieved
a 20-nm-level thickness layer, as shown in Fig. 7(b).51
The introduced techniques and applications are the major examples
highlighted at present. These use the pre-metered type of coating
methods that encompass various coating products by tuning various
significant process conditions as introduced in section 3. On the other
hand, there are self-metered coating techniques used in some examples,
such as knife-over-edge and dip coating, as shown in Fig. 8. In Fig.
8(a), OPVs are fabricated by three main techniques; slot-die coating for
PEDOT:PSS and P3HT:PCBM, knife-over-edge coating for ZnO, and
screen printing for Ag electrode patterning.87
Slot-die coating is mainly used for OPV coating because of its
possibility for stripe coating. In this case, a ZnO layer covers the whole
substrate after knife-over-edge coating because that layer is necessary
for stripe shapes. The ZnO layer obtained is a very thin layer of only 20-
nm thickness. An example of dip coating is presented in Fig. 8(b) via
the SEM image of TiO2 particles. For DSSC, an ITO-coated PET was
dip coated in a TiO2 solution to obtain a 10-μm wet thickness (1~2-μm
dry thickness).21 This was conducted at a low temperature condition of
120~140°C, but could not obtain better performance than at 400°C
because of plastic substrate use.
Lastly, R2R spray coating applications are presented. A solution
based on a combination of carbon nanotubes (CNTs) and isopropanol
was coated on Al foil for SC devices.25 The CNT solution was coated
at a speed of 4 cm2/s, which means that all of the covered layer needs
time to coat as the substrate is moving. The coated product indicates a
4-μm-thickness of CNTs on the Al foil, as shown in the SEM image in
Fig. 9(a). In contrast with general spray coating, the LFS process shows
a special mechanism in the atomization of droplets, as shown in Fig.
9(b). LFS is specialized for metallic material coating as a kind of
thermal spraying method.24 A liquid with metal is fed to the nozzle and
gas is combusted at high temperature to obtain small droplets. The
example of LFS in Fig. 9(b) focuses on increasing the hydrophobicity90
of paperboard. This was conducted at the very high speed of 150 m/min
for 1-μm-thickness, but the temperature near the nozzle was very high,
so distance between the nozzle (h0) and the substrate should be
maintained to minimize the deformation of the substrate.91
Based on the information in Table 1, the coating window in
previous works from the viewpoint of productivity and precision for V
and tdry of the layer can be introduced as in Fig. 10. The points on the
figure indicate the maximum and minimum values of tdry and V for
each coating method. The lowest tdry value was obtained for micro-
gravure and knife-over-edge coating cases of 20 nm thickness.51,87 The
maximum possible tdry was obtained as 40 μm in the case of knife-over-
edge coating for TiO2 powder deposition.28 Furthermore, the lowest V
and highest V were confirmed for micro-gravure, LFS, direct gravure,
and slot-die coating techniques as 0.18, 150, 210, and 240 m/min,
respectively.22,24,32,88 Self-metered coating techniques tended to distribute
 INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 17, No. 4
Fig. 7 R2R micro-gravure technique coating products: (a) large-area
coated carbon composite on PET substrate with copper contacts
(Adapted from Ref. 32 with permission) (b) SEM image of a PEDOT:
PSS-coated layer on PET film (Adapted from Ref. 51 with permission)
to the narrow region of V, but covered a wide tdry range. Because of
that, these techniques influence the coating results through the natural
properties of the liquids used. On the other hand, the pre-metered coating
methods covered a wide range of process conditions and thickness range
because of their various other possible tuning parameters in the coating
process, such as μ, σ, h0, and fr.
The introduced coating window cannot assure that all practical
examples are reflected but shows the actual used operating ranges in
recent works. There is more information about coating conditions given
in Table 1. The μ range used in coating was distributed from about 1
to 1800 mPa·s. Most research did not mention μ, but it is important
when considering the rheology of liquids. Moreover, h0 was hundreds
of micrometers, but in the LFS case took values from 100 to 250 mm,
so droplets flying from the nozzle would not be easy to control at the
highest V.24 fr was controlled by changing V from 1.7 to 53.7 mL/min.
In the case of high μ, a solution was selected for high fr, and LFS was
also promising for the fast transfer of droplets. The drying temperature
was set to below 200°C to prevent plastic deformation because web
substrates in the coating examples were PETs.92 The highest temperature
of near 200°C was for the TiO2 coating case in which there was
appreciable solid in the liquid, requiring high temperature conditions
for solubility. Moreover, even the temperature was low, it is possible to
compensate by longer drying time with longer distances in the drying
zone.36 Drying and sintering issues are very critical in R2R processes
because the web is always moving; so, in recent study, there have been
APRIL 2016 / 9
Fig. 8 Examples of self-metered coating: (a) R2R slot-die coating,
knife-over-edge coating, and screen printing techniques use OPV film
at a rewinding zone (Adapted from Ref. 87 with permission) (b) SEM
image of the surface after R2R dip coating using a TiO2 film for a
DSSC application (white bar: 100 nm) (Adapted from Ref. 21 with
permission)
many works on alternative drying methods. The reader is referred to
the work of Wünscher et al. for drying and sintering trends in the
present day.64 The w in the results ranged over 50~1185 mm, with an
average of 300 mm, demonstrating R2R works based on wide, large-
area web substrates.
In addition, important standards of evaluating coating results are
mentioned in previous work such as operating tension, roughness of the
coated layer, and waviness of the coated layer.43 Some research
suggested operating tension of 19.6 N to 250 N. In the general coating
case, the operating tension is very low but the self-metered coating
techniques set a high value of operating tension.22,87 As mentioned
above, tension control has an impact in high-precision layer coating.
Most importantly, the coated layer should be evaluated in longitudinal
and lateral directions relative to the web, but this was not considered.
Only the PSA case, in which significant waviness of the layer occurred,
concentrated on the profile of uniformity.43 In large-area coating, the
roughness of small parts is also important, but the large-area thickness
distribution is very critical as coating technology moves into multi-
layer coating production. In the R2R lamination process, the film
should be uniform to prevent outgassing and bubble formation in the
multi-layer structure.93 Moreover, a uniform coating surface is critical
in optically significant coating products because of scattering on the
surface.94
 10 / APRIL 2016
Fig. 9 R2R Spray coating examples: (a) schematic of R2R spray coating
and an SEM image of a CNT layer on Al foil (Adapted from Ref. 25
with permission); (b) schematic of the LFS coating process on R2R-
transported paperboard (Adapted from Ref. 24 with permission)
Fig. 10 Operation window of R2R coating processes (and coating
materials) based on the references in Table 1
5. Conclusion
In this review, R2R-adapted coating technologies have been
introduced. The guidelines and the key points of R2R transportation
were explained in terms of control of coating velocity, operating tension,
and temperature. Various coating techniques exist, but not every method
is suited to the R2R process. Dip, direct gravure, knife-over-edge, liquid
flame spray, micro-gravure, and slot-die coating techniques are the
representative processes for R2R production. A mathematical model of
their coating processes was introduced from the viewpoint of mass
INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 17, No. 4
production. The proposed modeling offers physical sight for
understanding the relationship between coating results and operating
conditions. Process applications were reviewed specifically for each
coating method, material, coating condition, and product output. All
coating techniques have advantages and disadvantages in terms of their
operating windows and characteristics for products. Most applications
in R2R coating focus on electronic devices and single-layer film
products. There are many materials and a wide range of material
conditions, so coating techniques and operating ranges can be determined
by considering their importance for each coating product.
ACKNOWLEDGEMENT
This research was supported by National Research Foundation of
Korea (NRF-2014R1A1A1003477).
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