Surface Innovations Pages 211–227 http://dx.doi.org/10.1680/si.13.

00017
Review Paper
 Volume 2 Issue SI4
Received 16/07/2013 Accepted 02/10/2013
Physics and applications of superhydrophobic Published online 05/10/2013
and superhydrophilic surfaces and coatings Keywords: contact angle/hydrophilic/hydrophobic/
superhydrophilicity/superhydrophobicity/wetting
Drelich and Marmur

ice | science ICE Publishing: All rights reserved

Physics and applications of superhydrophobic

and superhydrophilic surfaces and coatings
1 Jaroslaw Drelich PhD* 2 Abraham Marmur PhD
Department of Materials Science and Engineering, Michigan Department of Chemical Engineering, Technion – Israel Institute of
Technological University, Houghton, MI, USA Technology, Haifa, Israel

1 2
                 

The terms superhydrophobicity and superhydrophilicity were introduced not very long ago, in 1996 and 2000, respectively.
The former is used to describe exceptionally weak and the latter used to indicate strong interactions of materials and
coatings with bulk water, controlled entirely by surface topography and material chemistry. An explosion of research on
fabrication of superhydrophobic and superhydrophilic surfaces and coatings was noticed almost immediately after the
concepts appeared in the technical literature, with hundreds of reports now published annually. The interest in this new class
of surfaces/coatings is driven by an emerging market for water-repellant, snow- and ice-phobic products and formulations,
water antifogging screens, windows and lenses, antifouling coatings, microfluidic devices, coatings for enhanced boiling
heat transfer, foils for food packaging and many other products. The popularity of this emerging subdiscipline of surface
chemistry can also be attributed to uncomplicated fabrication technologies that can produce superhydrophobic or
superhydrophilic surfaces and coatings, in addition to the simplicity of the testing techniques used, such as contact angle
measurements. In this article, the physics behind superhydrophobic and superhydrophilic effects are reviewed and several
examples of applications of superhydrophobic and superhydrophilic surfaces and coatings are provided.

Notation list θCB Contact angle as per Cassie-Baxter equation: degree

fi Fractional area of a component i of the solid surface θ
W
Contact angle as per Wenzel equation: degree
fs Fraction of the liquid base in contact with solid surface θY Ideal (Young’s) contact angle: degree
r Roughness parameter
rl Roughness ratio of the solid that is in contact with the
1. Introduction
liquid
After more than two centuries of research, capillarity and wetting
SSLV Spreading coefficient: mJ/m2 phenomena still remain popular topics of investigation in many
W Wicking parameter: mJ/m2 modern surface chemistry laboratories. Curiosity and fascination
WS Work of spreading: mJ/m2 with rain droplets splashing in a puddle, water droplets decorating
Τ Adhesion tension: mJ/m2 flowers, leaves of plants and fruits after rain or watering and colorful
γLV Liquid/vapor interfacial tension: mN/m soap bubbles shaped at the end of wheat straw have never been
stronger and go beyond scientific laboratories. Colorful images of
γSL Solid/liquid interfacial tension: mN/m
liquid droplets and puddles, illustrating their behavior on a variety
γSV Solid/vapor interfacial tension: mN/m of surfaces, thrive in professional journals, popular magazines and
ΔGsl Energy of hydration: mJ/m2 Internet. However, terms such as wetting, spreading and contact angle
θ Contact angle: degree are still puzzling to the layman and beginner researcher. To facilitate

This article is dedicated to Professor Emil Chibowski on his 70th birthday.

*Corresponding author e-mail address: jwdrelic@mtu.edu

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 Surface Innovations Physics and applications of
 Volume 2 Issue SI4 superhydrophobic and superhydrophilic
surfaces and coatings
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understanding of these concepts, daily examples of surfaces having 1.3 Example three: to control liquid spreading
controlled or responsive wettability are often much appreciated. by manipulating surface texture
Discussing the varying shapes of water droplets on human skin, on Modern rainwear and umbrellas use a polyester textile for a few
a car windshield and/or on the fabric of an umbrella (or raincoat) is reasons. It is an inexpensive fabric with sufficient mechanical
always helpful to listeners and readers, and these three examples are properties that can be colored and possesses hydrophobic
briefly reviewed as an introduction to the main topics of this review. properties. The water contact angle reported for a smooth surface
of monolithic polyester is about 80°,4 which makes water drops
stick relatively well to the surface. However, on the umbrella
1.1 Example one: introduction to
fabric, most of the droplets roll off easily during rain. A closer
wettability and contact angle
look at the droplet shape suggests a contact angle that appears to be
A drop of water (or any beverage) placed on hand does not spread
>120°, much larger than on a smooth surface of polyester (Figure
spontaneously but forms a lens, such as in Figure 1(a), with a finite
3). This is simply the result of fabric texture. Fibers (threads)
contact angle (roughly defined at this point as the angle that the
of the polymer are knitted together to form a 2D network with
drop makes with the solid surface at their contact point), most often
openings in between the individual strands. The shape of a water
somewhere between 50 and 80°. Skin contains 70–80% of water
drop residing on top of such a textile is affected by the thread
(with proteinaceous structures such as collagen),1 and such high
network density and the size of individual fibers. More openings
contact angle values are rather surprising.2 However, water droplets
in the network and fibers of smaller diameter force the rain drops
normally spread to much smaller contact angles when the same
experiment is repeated on the same hand immediately after it is
washed with soap (Figure 1(b)); washing removes a layer of grease
produced by the skin. This simple experiment implies that the state
of skin is detrimental to the surface’s strength of interaction with
water and demonstrates a close correlation between characteristics
of the surface and water spreading.

1.2 Example two: to control liquid behavior by

adding artificial coating (surface chemistry)
Glass is considered hydrophilic (‘water loving’) material and water
should practically spread spontaneously on its surface.3 However, it
is known that rain droplets do not spread to form a water film on the
windows and windshields, but spread only partially. The contact (a)
angle is typically 10–30° – as a result of surface contamination
with dirt and air-borne organics (Figure 2).

Everyone who owns a car takes it to a carwash for periodic cleaning

and waxing. Waxing of the car windshield is important as it provides
better visibility in the rain. Because of curvature effects, light bends
on rain droplets causing reduction in visibility for the driver and
passengers. During a heavy rain, wavy streams of water are formed
on the windshield of a moving car through which visibility is often
even worse (waving is accelerated by the speed of moving car). A
waxed windshield forces the rain droplets to remain spherical in
shape (large contact angle, ~90° and larger), significantly reducing
the adhesion to the glass. Consequently, droplets easily drift to
the edges of the windshield under the pressure of air produced by
the moving car. These droplets are also more easily removed by
the windshield wipers. Waxing is nothing but coating of the glass
with a hydrophobic (‘water fearing’) material (i.e., hydrocarbons, (b)
fluorinated hydrocarbons or silicone polymer/oil). Coating a Figure 1. Water drop placed on hand (a) before and (b) after soap
surface with hydrophobic films to eliminate or reduce water pick washing. Inserts at the bottoms present water droplets zoomed from
up by hydrophilic materials is not a new idea. In fact, the concept major photographs and additional droplets colored with red dye
dates back to early seafarer’s painting of their wooden boats with captured on separate photographs
tar for waterproofing and resistance to rotting.

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 Surface Innovations
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(a)
Figure 2. (a) Rain droplets on a window. (b) Photo of the outdoor
chair on a porch through window covered by the rain droplets. (c)
Photo of the same outdoor chair through clean window
Figure 3. Water droplets on the fabric of umbrella
to assume a shape close to a perfect sphere when on the surface of
the umbrella. This is an excellent example of the manipulation of
material geometry in the early stages of design and development
of products with enhanced water-resistance. Cassie and Baxter5
are considered the founders of this approach and the authors will
return to their work in the further part of this article.
The three examples briefly discussed above provide a general
introduction to wetting phenomena and surfaces with controlled
wettability. These days, however, the scientific community and
practitioners of wettability, focus their debate on the science and
applications of superhydrophobicity and superhydrophilicity. The
roots of the former term date back to 1996, when Onda et  al.6,7
published two articles on wettability of fractal (rough) surfaces in
which the terms of superhydrophobic and superwetting surfaces
were proposed. The term superhydrophilicity appeared for the first
time in the technical literature in 2000, in four articles published by
three different research groups from Japan.8–11 In 1997, Fujishima
et  al.12 demonstrated the superhydrophilic effect on a glass slide
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Physics and applications of
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Drelich and Marmur
(b) (c)
coated with a thin titanium dioxide polycrystalline film. The
spreading of water was the result of both the hydrophilic properties
of anatase exposed to UV radiation and submicroscopic roughness
of the coating, although the effect of water spreading was entirely
attributed to photoinduced self-cleaning capability of titanium
dioxide at that time, and the term superhydrophilicity was not
used. Why were these new terms introduced and why have they
attracted so much attention in recent years? These questions will
be answered later. Before that, the major terminology and physics
behind wetting phenomena will first be summarized.
2. What is the contact angle and
what does it represent?
Although the ancient civilizations well explored the benefits
of waterproofing coatings and lubricants, the formal scholastic
studies of wetting and capillary phenomena (wetting and capillary
phenomena directly relate to each other in all three-phase systems)
began in the eighteenth century, with the first reports appearing in
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the early nineteenth century. It was Laplace13 and Poisson14 who
established the fundamental background for capillarity. Young15
described the relationship between contact angle and surface
energies for a liquid and a solid surface based on mechanical
considerations. This concept was thermodynamically proven on a
more rigorous basis by Gibbs.16 From that time it has been known
that the behavior of a liquid on a solid surface is controlled by the
competition between the liquid–vapor (γLV), solid–liquid (γSL) and
solid–vapor (γSV) interfacial tensions. A spontaneous and complete
spreading of liquid occurs over the solid surface when the spreading
coefficient (SSLV) is greater than or equal to zero:
1. SSLV = γ SV − γ SL − γ LV
During partial spreading (SSLV  <  0), the liquid forms a lens with
a finite contact angle (θ) at the solid surface. The contact angle is
defined as the angle between the solid surface plane and the tangent
to the liquid surface plotted at the point of contact between three
phases (Figure 4). The contact angle defined by Young’s Equation
2 is referred to as the ideal contact angle (θY where the Y refers to
Young’s contact angle) and is valid only for solids whose surfaces
are homogeneous, isotropic, smooth, rigid and surrounding fluids are
inert to such solid (no chemical reaction or specific adsorption or
dissolution or swelling or rearrangement of phases, molecules and
functional groups):
2. γ SV − γ SL
cos θ Y =
γ LV
3. Typically, the contact angle varies along the three-phase contact
SSLV
cos θ Y = 1 +
γ LV
In the case of microscopic and submicroscopic droplets, a tension
component associated with the three-phase contact line needs to be
added to Young’s equation.17,18
Solids examined in research laboratories that can be described
as ideal solid surfaces, such as required by the Young equation,
are very rare. They are often either rough, at the micro- or nano-
scopic level, or heterogeneous because of multiple phases, different
surface compositions or simple contamination of the surface.19 Most
inorganic solids are anisotropic due to multielemental composition
and crystalline structure. Such surfaces have at least atomic
heterogeneity that can trigger adsorption of constituents from liquid
or gas adding to heterogeneity of the surface and its landscape.3
Some of the solids can also react chemically20,21 or interact
physically with the probing liquid or surrounding gas and promote
surface segregation, reorientation, diffusion or migration.22,23
Dissolution of pharmaceutics, soluble and semisoluble minerals
and many inorganic and organic reagents/products makes the
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wetting characterization of such materials extremely difficult
and sometimes impossible.3 In addition, as spreading is a time-
dependent event, the conditions between solid and spreading liquid
can vary depending on the time of liquid shape observation during
contact angle measurements. Softer materials also deform under
the weight of the probing liquid. Another reason for deformation is
the unsatisfied normal component of the Young’s equation giving
rise to protrusions at the three-phase contact line.24–28 This results in
an increase in the force required to slide a drop on the solid surface
as can be measured using the centrifugal adhesion balance.3,4,26,29
Mutual saturation between phases or preferential adsorption at
interfaces can be very fast, but sometimes, it occurs as a very slow
process and thus exceeds the time of contact angle measurements,
resulting in data measured under non-equilibrium conditions.30
A good protocol requires contact angle measurements in liquid-
saturated gas environment to at least secure equilibrium solid
surface conditions.31 The issues of three-phase system saturation
and equilibration are typically ignored in modern research
laboratories. Although the composition and purity of both the solid
substrate and liquid are often well reported, the gas phase, typically
air, is almost always ill-defined. Each laboratory has a different air
quality, depending on its geographic and urban location, whether
it is purified or not, human traffic in the laboratory and so on.32
Trace quantities, even at a level of parts per billion or even parts
per trillion, of active organic compounds in the gas phase (mostly
exhausted by humans and animals as well as emitted by the
industrial activities) that often adsorb on the solid surface and
change the wetting characteristics of a solid, especially metals and
ceramics.32
line for a liquid drop resting on a rough and/or heterogeneous
solid surface. Local changes in angles of inclination of the rough
surface33 and/or variation in chemistry of a heterogeneous surface34
cause the three-phase contact line to contort. Since the contact
angles are typically measured macroscopically for liquid drops
with a diameter of a few millimeters using low-magnification
optical lenses, the local angles are ignored. Instead, the global
contact angles are measured and are referred to as apparent contact
angles.
A liquid in contact with a rough and/or heterogeneous surface can
have more than one apparent contact angle.33,34 The phenomenon
of multiple liquid–solid metastable configurations can be analyzed
in terms of the Gibbs energy that takes into account the details
of surface geometry, topography and local wettability. Figure 5
shows an imaginary correlation between the Gibbs energy and
apparent contact angle for a liquid on a rough or heterogeneous
solid surface. The Gibbs energy versus contact angle curves
have multiple minima, in contrast to the curve for smooth and
homogeneous solid surface with only single minimum.35,36 Each
energy minimum defines a stable geometry of the liquid, with
 Surface Innovations Physics and applications of
 Volume 2 Issue SI4 superhydrophobic and superhydrophilic
surfaces and coatings
Drelich and Marmur

Vapor γLV

Liquid No spreading Complete spreading

θ
γSV
Partial spreading

γSL (c)
Solid
γSV << γLV θ >> 90°
(a)

θ γSV = γLV θ == 90°

θmin
γSV > γLV θ << 90°
θmax
θ

(b) (d)

Figure 4. (a) A sessile drop on an ideal solid surface. Vectors represent three interfacial tensions and θ is the contact angle. (b) A shape of a liquid
drop on a horizontal and tilted solid surface (α represent the tilting angle of the solid surface). θmax and θmin are the maximum and minimum
contact angles, respectively. (c) Three cases of a liquid behavior on a solid surface: during non-wetting, complete wetting and partial wetting. (d)
Liquid drops on surface of different wetting characteristics

unique equilibrium or quasi-equilibrium contact angle that can be
measured experimentally, especially if sufficient times for transition
between states and equilibration are allowed. Often external energy
needs to be provided to drive transitions between metastable states
and overcome the energetic barriers.37,38 Equilibration time can
vary from seconds to hours to days to weeks and, unfortunately,
such measurements are scarce in the technical literature. It should
be recognized however, that only some of these equilibrium contact
angles have practical meaning and special protocols need to be
followed to measure them.
(Young’s) contact angle that would be measured on a flat surface
of the same solid. This equation describes the most stable contact
angle when the liquid completely penetrates into the roughness
grooves (‘homogeneous wetting’ regime).
The Cassie equation for a chemically heterogeneous (two-
component) surfaces is as follows41:
5. cosθ C  f1 cosθ Y1  f 2 cosθ Y2

The most stable equilibrium state is associated with the lowest
Gibbs energy value and corresponds to either Wenzel’s state on a
rough surface or Cassie’s state on a heterogeneous surface.39 The
Wenzel equation is as follows:40
4. cos θ W = r cos θ Y
where f is the fractional area of a component of the solid
surface; f1 + f2 = 1; and θ1Y and θ2Y are Young’s contact angles
corresponding to the two components. Both the Wenzel and
Cassie equations apply to surfaces whose protrusions and/or
heterogeneities are small in comparison with the size of liquid/
vapor interface.36,42

where r is the roughness parameter that expresses the ratio of the If liquid does not penetrate into surface protrusions and is present
true the solid surface to its horizontal projection, and θY is the ideal on the air pockets or placed over a porous material such as fabric,

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Advancing CA
Receding CA
∗ Metastable states
Gibbs energy
Energy barrier
Most stable CA
Apparent contact angle
Figure 5. The Gibbs energy for a liquid on a rough or heterogeneous
solid surface
screen, membrane and so on (see Section 1.3), then the Cassie
equation is modified to become the Cassie-Baxter equation5:
6. cos θ CB = rl fS cos θ − (1 − fS )
where fs is the fraction of the liquid base in contact with solid
surface (fs  <  1), and (1  −  fs) is the fraction of the liquid base in
contact with air pockets and rl is the roughness ratio of the solid
that is in contact with the liquid. Air is not wetted by water and,
therefore, the water/air contact angle is equal to 180°. The cosine
of 180° is equal to −1, leading to the minus sign in the second term
of Equation 6.
This equation predicts an apparent contact angle for any geometry
and structure of the surface, the topography of which is not fully
penetrated by the liquid, also known as ‘heterogeneous wetting’. A
practical challenge for such systems is always to define and quantify
the value of fs. In addition, the portion of a liquid in contact with the
solid is often contorted due to the solid’s topography that adds to
the complexity of contact angle analysis.
Going back to the Gibbs energy curve in Figure 5, the Wenzel or
Cassie-Baxter contact angle is associated with the total minimum,
respectively.43,44 Whether the system remains in the Cassie-
Baxter or Wenzel wetting state depends on which of them has the
lower energy, as well as on the way the liquid is introduced into
contact with the solid surface (deposition, immersion, spreading
or vapor condensation). Transitions between these two states can
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be triggered by external stimuli including pressure, mechanical
vibrations and temperature gradient. Recent experimental and
computer simulation studies suggest that a transition from the
Wenzel state to the stable and robust Cassie–Baxter state is only
possible on hierarchical superhydrophobic surfaces.45
Della Volpe demonstrated that equilibrium or quasi-equilibrium
(metastable) contact angles can be measured for almost any
imperfect solid.38 Such measurements are still not very popular
because the conventional instruments require considerable
modification to accommodate speakers or other vibration-
inducing devices.38,46 Nevertheless, the advancing contact angle
and receding contact angle are easily measureable on solids.31
These two angles are well defined and should always be
reported. Advancing contact angle is the maximum metastable
contact angle measured for the liquid that advances or recently
advanced over unwetted solid surface.31 On the Gibbs energy
against contact angle curve in Figure 5, it corresponds to the
metastable state located at the far right side of the curve (as long
as the energy barrier preventing the system from moving to the
second metastable state is larger than the intrinsic thermal energy).
Receding contact angle is the minimum metastable contact angle
measured for the liquid receding or recently retreated from the
wetted solid. It corresponds to the contact angle associated with
the first metastable state in Figure 5. The experimental protocol for
measurements of advancing and receding (static) contact angles
was recently published.47
The difference between advancing and receding contact angles is
called contact angle hysteresis, and its value provides insights into
quality of the solid surface and strength of adhesion to liquid.48 The
wetting characterization and, consequently, understanding of solid
surfaces are limited if only advancing contact angles are measured.
Unfortunately, receding contact angle measurements have not been
commonly reported.
3. Some controversies and
recent developments
The contact angle measurements using the sessile-drop and
captive-bubble techniques are among the simplest surface
characterization methods.31 Researchers with diverse
backgrounds representing almost all fields of science and
engineering use these methods, not always with sufficient
training in preparation of surfaces and measurements of
advancing, receding and equilibrium contact angles, and their
interpretation. As a result, the modern literature is flooded
with contact angles that are in between advancing and receding
and are not equilibrium contact angles. Reproduction of these
experimental ‘intermediate’ contact angles, if pursued, becomes
a challenge to other laboratories. The problem of questionable
contact angle measurement methodologies was raised in an
earlier publication, and recommendations on sample preparation
 Surface Innovations
 Volume 2 Issue SI4
and contact angle measurements protocols were made;31 these
will not be repeated here. In short, the question, ‘What does
measured contact angle represent?’ (addressed in Section 2)
cannot be answered without proper measurements of contact
angles and understanding three-phase conditions during these
measurements. Simply, many experimental contact angle data
cannot be analyzed using the Young, Wenzel, Cassie or Cassie-
Baxter thermodynamic equations.
Validity of the Wenzel, Cassie and Cassie-Baxter equations
has been questioned in recent years in many publications, as
discussed in more detail in the previous review.3 For example,
Gao and McCarthy49 doubted the validity of both the Wenzel
and Cassie-Baxter approaches and argued that contact line,
and not the contact area, is important in interpretation of the
contact angles. A similar conclusion was also drawn earlier for
chemically heterogeneous surfaces.50 Already in early reports,19,51
the importance of understanding surface characteristics in the
vicinity of the three-phase contact line to explain the experimental
contact angles was discussed. It needs to be recognized, however,
that thermodynamic relationships such as Young, Wenzel, Cassie
and Cassie-Baxter equations, discussed in Section 2, were
derived for equilibrium contact angles at non-deformable and
non-reactive solids based on the assumption of reproducible
surface characteristics at submillimeter/microscopic dimensions.
Derivations of these equations also rely on the assumption of
small displacements made by a liquid. These displacements must
be much larger than dimensions of surface pattern or topography
variation; in practice, it translates to the size of a liquid drop being
orders of magnitude larger than any heterogeneity or asperity. For
large surface chemical heterogeneities19 or roughness features,52
there is a need to analyze the shape and contortion of the three-
phase contact line instead of measuring one global contact angle.
In fact, local considerations of the shape and length of the contact
line and global considerations involving interfacial area within
the contact line do not contradict but complement each other.53
Measurement of meaningful contact angles is especially
challenging on rough and structured surfaces. Experimentally
measured advancing and receding contact angles are generally
not representative of what thermodynamic relationships predict,
a fact that is often not well recognized by the critics of contact
angles and their validities in Wenzel and Cassie-Baxter regimes.
Here, additional effects such as line pinning, capillarity, porosity
pressure buildup, surface curvature and so on, might contribute
to the observed contact angles, which are not always accounted
for by the thermodynamic relationships. The pinning of the
contact line on surface defects such as edges of asperities is a
well known phenomenon that causes departure from the Wenzel
assumptions – whether in terms of surface area or contact line
length.54,55 Both the shape and sharpness of roughness features
and their edges affect pinning of the contact line.56 A small
curvature of the fiber or post can also change wetting behavior
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of the liquid.32 Pressure buildup in porosity or in between short-
distanced posts can prevent the liquid from penetrating into the
porous structure.57–59
Furthermore, the contact angles are often measured to access
indirectly either adhesion or solid surface energy, important
quantities in formulation of coatings, painting, printing, de-icing,
biocompatibility and so on. The correlations between the
advancing and receding contact angles and solid–liquid adhesion
for solids with imperfect surfaces (having a certain degree of
roughness and/or heterogeneity) are not straightforward, and at
present are poorly understood. Measured advancing and receding
contact angles represent a combination of the effects associated
with not only the solid surface tension but also sample geometry,
size, shape and distribution of the roughness/heterogeneity
features. For this reason, some recent attempts concentrated on
direct measurements of liquid–solid interactions, initiated by a
design of two apparatuses. The centrifugal adhesion balance,
introduced in 2009, uses centrifugal and gravitational forces to
induce different normal and lateral force combinations for direct
adhesion measurements between a liquid drop and a solid surface.29
Then in 2011, Samuel et al.60 introduced a microbalance with a
specially designed hydrophobic loop to hold a liquid drop capable
of measuring the liquid–solid surface interactions on drop-surface
approach (snap-in force) and pull-off force (adhesion) during
liquid drop detachment. The authors found for a large number
of samples having various surface characteristics that advancing
contact angles correlate better with the snap-in force whereas
receding contact angle with the pull-off force. Extension of this
work to equilibrium contact angles could probably help to justify
thermodynamic relationships and pinpoint to their limitations for
particular surface structures.
4. Defining hydrophobic and hydrophilic
surfaces using contact angle criterion
A variety of different definitions and techniques have been
used in the literature to describe/measure the hydrophobic and
hydrophilic (homogeneous and smooth) surfaces as discussed in
detail in the previous contribution3 (the authors will not repeat the
discussion in this article). In general, a hydrophilic surface has
strong affinity for water as compared with nonpolar fluid such as
air or oil whereas a hydrophobic surface repels water. The term
hydrophobicity originates from two ancient Greek words: hydro
for water and phobos for fear. The Greek word philic means love,
therefore hydrophilicity stands for ‘loving water’. On the basis of
the dependence on capillary penetration of the water contact angle,
and on the sign of the nominator in Equation 2, it is natural to draw
the line between hydrophilicity and hydrophobicity at a Young
contact angle of 90° (Figure 4).61 It is expected that a hydrophobic
smooth surface has a weak affinity for water, as it interacts with
water exclusively through van der Waals forces.62 Although the van
der Waals attraction of a hydrophobic solid with water is commonly
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 Surface Innovations
 Volume 2 Issue SI4
stronger than with vapor, it is weaker than water–water cohesive
forces involving additional polar and hydrogen interactions.63
The definitions of hydrophobicity and hydrophilicity can be
generalized to define hygrophobic and hygrophilic surfaces,
respectively (i.e. a surface which a liquid fears or likes, as shown
in the first row of Table 1).61,64 It is, however, too general for the
classification of a variety of different solids having different
contact angles, especially those used in technological operations.
Therefore, the classifications of hydrophilic and hydrophobic
surfaces based on contact angle, work of spreading, free energy
of hydration and water adhesion tension were proposed in the
past as shown in Table 2 (the reader should return to the original
publication3 for the source of the numerical limits used in this
classification). Hydrophilic surfaces are those on which water
spreads completely, visually ‘zero contact angle’. Partially
hydrophilic and hydrophobic solids – classes which encompass
a vast majority of materials – called here weakly hydrophilic
and weakly hydrophobic, are those on which macroscopic water
films are unstable and bead up to lenses with contact angle
smaller than 90° (Figure 4). Hydrophobic surfaces are those
commonly recognized having water contact angles of at least
90°. Superhydrophilic and superhydrophobic surfaces are also
included in Table 2, but they will be discussed Section 5.
Examples of hydrophilic and hydrophobic materials were provided
in the earlier publication and will not be repeated here.3 Hydrophilic
surfaces according to the above definition are more abundant in
nature than hydrophobic ones, but they become contaminated very
quickly and surfaces lose their natural strong affinity for water. As
of today, only organics that are hydrophobic are known; there is no
reported inorganic for which the water contact angle of the clean
surface is 90° or larger. Among these organics, fluorine-containing
Wettability
Morphology of surface
classification
Smooth Hydrophilic
Hygrophilic
Hydrophobic
Rough/porous Parahydrophilic
Parahygrophilic
Parahydrophobic
Very rough/very porous Superhydrophilic
Superhygrophilic
Superhydrophobic
Superhygrophobic
Data adapted from Ref. 61.
Table 1. Terminology for wettability classification
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polymers and molecules are the most hydrophobic, with water
contact angle near 120°. It seems that the natural substances have
been surpassed by man-made ones in terms of hydrophobicity, as
organic fluorine-based molecules have not yet been reported in
biological systems and they are more hydrophobic than any natural
hydrocarbons.
5. Defining superhydrophobicity
and superhydrophilicity
In spite of success in manufacturing hydrophobic (organic)
materials and broad availability of hydrophilic materials, many
applications benefit from surfaces and coatings that enhance
spreading of water (or other liquid) or reduce it, beyond what
natural or synthetic materials with smooth surfaces demonstrate.
Surface roughening is necessary to enhance or reduce the spreading
of liquid on a solid. The principles of this fabrication were founded
several decades ago by Wenzel40 and Cassie and Baxter5 who
described contact angles and different mechanisms of wetting on
rough surfaces. The detailed analysis of these two equations, 4 and
6, is commonly presented in the literature and will not repeated
here beyond what was discussed in Section 2.
It follows from Equation 4 that any surface roughening (expressed
in term of r roughness factor) will reduce the contact angle on
hydrophilic material, and can lead to the complete spreading of
water or another liquid. Roughening of a hydrophobic surface, on
the other hand, will increase the contact angle. In such a system, a
large water drop will remain suspended on the tops of asperities or
other roughness features, thus requiring the use of Equation 6 to
predict the contact angle. Liquid drops can also remain suspended
on many rough and textured surfaces of hydrophilic materials
if the three-phase system is trapped in a metastable state (see
Contact angle (θ)
θsmooth < 90°
θsmooth ≥ 90°
θ < θsmooth < 90°
θ ≥ θsmooth ≥ 90°
θ ~0° < θsmooth
θ > θsmooth ≥ 150°, very low hysteresis (a few degrees)
θ > θsmooth > 90°, very low hysteresis (a few degrees)
 Surface Innovations Physics and applications of
 Volume 2 Issue SI4 superhydrophobic and superhydrophilic
surfaces and coatings
Drelich and Marmur

Measure of hydrophilicity/hydrophobicity (20°C)

Type of surface Contact angle: Water adhesion Work of spreading: Energy of
degree tension: mJ/m2 mJ/m2 hydration: mJ/m2
Supehydrophilic (r > 1) ~0a ≥73 ≥0 ≤−146
Hydrophilic ~0 ≥73 ≥0 ≤−146
Weakly hydrophilic (56–65°) > θ > 0 73> τ > (30–40) 0 > Ws > −(32–42) −113 > ΔGsl > −146
Weakly hydrophobic 90° > θ > (56–65°) (30–40) > τ > 0 –(32–42) > Ws > −73 −73 > ΔGsl > −113
Hydrophobic 120° > θ ≥ 90° 0 ≥ τ > −36 −73 > Ws > −109 −36 > ΔGsl > –73
Supehydrophobic (r > 1) θ > 150° a
τ ≤ −63 Ws ≤ −136 ΔGsl ≥ −10
a
Apparent contact angle.
See Ref. 3 for the source of the numerical limits.

Table 2. Proposed measures of hydrophilicity and hydrophobicity of solid surfaces

Figure 5).64,65 The invasion of liquid can be inhibited on material
surfaces through careful selection of the design, geometry, size
and contour of surface features and protrusions.64,66–68 An energy
barrier unfavorable to liquid wicking may be maximized in this
manner.59,69–73 This energetic barrier, if it is larger than the inherent
thermal energy7 needs to be overcome by mechanical means such
as vibrations,74,75 impact76,77 or load imposed on the drop.73,78
(superwetting) surfaces cannot be achieved without manipulating
the roughness of hydrophilic materials, on flat surfaces of which
water (liquid) droplets do not spread completely and remain as
lenses with contact angle smaller than 90°. In terms of a wicking
parameter, W:
7. W = γ sv − γ sl = γ l cos θ > 0

The term of superhydrophobicity was introduced in 1996 by Onda A minimum roughness of the surface necessary to initiate liquid
et al.6,7 to describe unusually high water contact angles, observed wicking that results in zero apparent contact angle is commonly
on fractal hydrophobic coatings, although the foundation to this predictable through the Wenzel equation:
discipline can be dated back a few decades.79 The now commonly
accepted meaning of a superhydrophobic surface is a surface on 1
which the water (advancing) contact angle is at least 150°, and 8. r≥
cos θ
the contact angle hysteresis as well as the sliding (or rolling off)
angle (sliding/rolling angle is the minimum angle of sloped solid
Obviously, roughening of the surface or change in a coating texture
at which water (liquid) drop rolls off the surface) do not exceed
do not necessarily lead to superhydrophobic or superhydrophilic
5–10° (Table 2). Although currently superhydrophobic surfaces are
systems. Weak or moderate changes in surface topography can
inspired by biological specimens,80–97 the early research was inspired
produce surfaces or coatings that do not comply with the definitions
by the practical need to enhance coating repellency of water and
of superhydrophobic or superhydrophilic. For that reason, Marmur
snow.98,99 These days, superhydrophobic coatings are manufactured
recently proposed terms of parahydrophobic and parahydrophilic
by chemical, physical and/or mechanical modifications of both
(Table 1).61
organic and inorganic materials.69,100–113

The opposite term of superhydrophobic is superhydrophilic, 6. How superhydrophobic

defined in the previous contribution.114 This type of surface is also
of great interest at this time, although still some questions regarding
its definition remain open.113 It is generally accepted that the first
prerequisite for a surface to be superhydrophilic (superwetting) is
that its apparent contact angle with water is less than 5°. In the
previously published note,114 the authors suggested that the term
superhydrophilic (or superwetting) only refers to a textured and/
or structured surface (rough and/or porous) possessing roughness
factor (r = ratio of real surface area to projected surface area)
defined by Wenzel equation40 larger than 1, on which water (liquid)
spreads completely (Table 2). Therefore, again, superhydrophilic
surfaces are designed?
The essence of superhydrophobicity is the easy removal of a drop
from the solid surface.115 For achieving this goal, a small external
force should be able to get the drop out of equilibrium, and the motion
of the drop should be relatively rapid. A small external force could
be, for example, the component of the drop weight along the surface
when the latter is slightly tilted. The reaction of the drop to this force
depends on contact angle hysteresis. When the solid surface is, for
example, tilted (Figure 4(b)), the shape of the drop may transform
into another equilibrium shape. This will be the case if the new
shape may be such that the local contact angles along the contact

219

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 Surface Innovations
 Volume 2 Issue SI4
line match both the geometry of the drop required by the Young-
Laplace equation and the local Young contact angles. On a tilted
solid surface, the drop is not axisymmetric; therefore, for geometric
reasons, its local contact angle must vary along the contact line (it is
highest at the lower end). Thus, a drop can be at equilibrium only if
the hysteresis range is sufficiently wide to account for the geometric
requirements of the drop shape. Consequently, easy removal of a
drop from a surface requires minimization of hysteresis. In addition,
it is reasonable to assume44,116,117 that the drop will quickly react
to the removing force if its actual contact area with the solid (the
‘wetted area’) is as small as possible.
Thus, the main design consideration is the minimization of contact
angle hysteresis as well as of the wetted area. This can be achieved,
as in nature, by making the drop settle at the Cassie-Baxter state.
In this state, the contact with the solid is minimal (if properly
designed), so most of the drop base is in contact with air. Now, air
is very uniform, thus hysteresis is minimized. In addition, air is
very hydrophobic, therefore the contact angle in the Cassie-Baxter
state is high, a fact that contributes to minimizing the wetted area.
It turns out then that a suitable roughness that leads to the drop
being in the Cassie-Baxter state answers both the need for minimal
wetted area and minimal hysteresis.115
The Cassie-Baxter state may be thermodynamically stable,
metastable or unstable in comparison with the Wenzel state. It
is stable if the Gibbs energy of the Cassie-Baxter state is smaller
than that of the Wenzel state (this is easily indicated by the
contact angle: the lower contact angle corresponds to the lower
energy). To find out whether the drop is unstable, a ‘feasibility
condition’ that depends on the specific roughness details was
developed.44 Mathematically, this condition indicates when
the Gibbs energy function has a saddle point. The ‘feasibility
condition’, for example, implies that convex-type protrusions
may allow the Cassie-Baxter state, but concave dents will not.
If the drop is neither stable nor unstable, it is in the metastable
state. The latter could be practically applied, if necessary, and
if the energy barrier between the Cassie-Baxter state and the
Wenzel one is high enough.
The main question now is how to optimize the roughness in
order to get the best possible superhydrophobic surface? To
answer this question, the parameters to be optimized need to
be defined. In principle, these are the chemistry of the surface,
its morphology, and the cost. The latter is not discussed
here, however, it should be remembered that the cost may be
detrimental to any suggested superhydrophobic product. As far as
the chemistry of the surface is concerned – it simply should be as
hydrophobic as possible. The problem of the optimal roughness
is more complicated. Some theoretical simulations indicated44,117
that rounded-top protrusions appear to be better than flat-top
ones with sharp edges. This seems to be in agreement with
220
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Drelich and Marmur
designs by nature itself. Another question is whether fractal or
multiscale roughness, which is ubiquitous in nature, is essential
for superhydrophobicity. The researchers agree that multiscale
roughness is helpful.118 A recent, relatively detailed study44 of
three types of roughness geometries with up to four roughness
levels showed that the main effect of this type of roughness is in
reducing the sizes of the roughness protrusions that are necessary
for stable superhydrophobicity. Thus, it may be assumed, until
further studied, that multiscale roughness helps in making the
surface more stable from a mechanical point of view.
7. Applications of superhydrophobic,
oleophobic, superhydrophilic
and superwetting surfaces
Hundreds of scientific reports on formulation of superhydrophobic,
superhydrophilic, oleophilic and so on, appear every year in the
literature since the beginning of the twenty-first century, including
several published in the previous issues of this journal.68,119–129
Review of all the literature and possible applications targeted by
the authors exceeds the scope of this review. Only a few examples
of commercial products that authors are either aware of or found
through the Internet are provided.
7.1 Self-cleaning (superhydrophobic) paints
A self-cleaning paint has been marketed by the Sto AG company,
Germany,130 and is probably the first commercial self-cleaning paint
introduced on the market (Figure 6). Polysiloxane emulsion with
particles of titanium dioxide and silicon dioxide is used as an exterior
paint and can be used on mineral (concrete) and organic (non-elastic
such as shielding) substrates. Dirt particles have a reduced adhesion
to the painted surface and are easily cleaned off by the rain.
7.2 Self-cleaning (superhydrophobic)
product coatings
Several different companies have made self-cleaning superhydro­
phobic coatings available on the market, although many of the
small spin-off nanotechnology-based companies are still searching
for a specific application of their coating product. One of the first
companies, if not the first one, working on commercial super­
hydrophobic coatings was NTT in Japan, where one of us had the
privilege to work with in the middle of 1990s.98,99 Their spray
that contained polytetrafluroethylene particles and a binder was
specifically designed for antennas and other transmission systems,
particularly located at a high elevation, to reduce the accumulation
of snow (Figure 7).
Hypho Technology Pte Ltd. (Singapore) introduced the Uri-pel coating
specifically designed for the spray coating of toilet urinals to eliminate
the need for flushing water (flushless urinals).131 This company is
trying to introduce their coating to other products such as shower
screens, solar cells and panels, automobile windshields and others.
 Surface Innovations
 Volume 2 Issue SI4
7.3 Self-cleaning (superhydrophilic)
paints and product coatings
Haruna Singapore Pte Ltd. offers self-cleaning paints (HP
Tiocoat),132 which are based on photocatalytic titanium
dioxide nanoparticles, patented by the Singapore Institute
of Manufacturing Technology, a research institute under the
(a) (c)
(b) (d)
Figure 6. (a) Lotus leave, (b) self-cleaning of the lotus leave with a water
droplet, (c) Painting with the Lotusan paint and (d) self-cleaning of the
Lotusan coating with water droplets. All images are courtesy of Sto Corp
Uncoated
antenna
(a)
Figure 7. HIREC superhydrophobic and antisnow coating offered
by NTT-AT in Japan. (a) Optical image of a water drop on top of the
coating and (b) picture of the coated and uncoated satellite dishes
during winter. All images are courtesy of NTT-AT
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Singapore Agency for Science, Technology and Research
(A*STAR). Titanium dioxide decomposes organic substances
including mold, mildew, fungi and other microorganisms
through photocatalytic reaction using ultraviolet radiation
from sunlight or artificial light sources. This company also
offers similar titanium dioxide nanoparticle-based coatings
for windows and other glasses. Such coatings can also be
used on ceramics in bathrooms and kitchens to fight bacteria
attached to the tiles, counters, glass walls or oxidize/remove
foul smell from stains in the toilet (e.g. titanium dioxide–coated
tile and glass are commercially available – see Section 7.4).
Superhydrophilicity accelerates washing dirt and stain with
the stream of water or by rainfall. Photoreactivity of titanium
dioxide coating is strong enough to attack an organic paint
surface, causing the so-called paint-chalking phenomenon. To
prevent the direct contact of titanium dioxide particles with
organic paint, an inorganic–organic layer is used to prevent
substrate-damage from the photocatalytic reaction. Additional
benefits of using paints and coatings with anatase, titanium
dioxide, include the decomposition of other organic pollutants
(e.g. car exhausts NOx, formaldehyde, benzene, volatile orgainc
compounds), and protecting the surface from UV damage. It
has also been suggested that a titanium dioxide–based coating
reduces the energy consumption needed for cooling buildings
in the summer.
7.4 Self-cleaning (superhydrophilic) windows/glass
As early as in 2001, self-cleaning windows were introduced on the
market by Pilkington Glass under the brand name of Pilkington
Activ (Figure 8). Soon after that, several other major glass
companies released similar products including PPG Industries
(SunClean),133 Cardinal Glass Industries (Neat Glass) and134 Saint-
Gobain (Aquaclean and Bioclean).135 The products rely on a similar
invention to that discussed in Section 7.3. Glass for windows
(typically soda lime silicate float glass) are coated with a thin (from
Coated
antenna
(b)
221
 Surface Innovations Physics and applications of
 Volume 2 Issue SI4 superhydrophobic and superhydrophilic
surfaces and coatings
Drelich and Marmur

less than 10–30 nm, depending on the technology) transparent layer
of photocatalytic (hydrophilic) nanocrystalline anatase (TiO2).
7.5 Antifogging (superhydrophilic) mirrors
The antifog mirrors are now offered in Asia and Pacific Region
including Japan, China, Singapore, South Korea and other
countries. For example, Shanghai Divas Glass Co. Ltd. offers
variety of antifog mirrors for bathrooms.136 The Blackwood-Eddy
Pty. Ltd. (Australia) is offering fogless shaving mirrors.137
7.6 Antifogging (superhydrophilic) shields,
goggles and eyeglasses/sunglasses
When the temperature changes and the humidity is high or goes
up lens fogging can become a major problem because of reduced
visibility. A wide variety of antifog safety glasses and antifog
safety goggles are offered by manufacturers. Antifog sunglasses
and goggles, including swimming goggles, are also broadly spread
and offered. Also, motorcycle, safety and surgical face shields are
available from several manufacturers. Although details about antifog

The window is exposed

to daylight

Daylight triggers the

Pilkington Activ
coating

Reaction loosens dirt

Rain water hits window

and sheets down glass

Dirt is washed away by

rain

Window is left clean

Figure 8. Self-cleaning windows produced by Pilkington Glass and

images illustrating their performance. All images are courtesy of
Pilkington United Kingdom Ltd

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 Surface Innovations
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coatings are typically not publicized, many of the products most
likely rely on either silicone- or titanium dioxide–based coatings.
7.7 Antifogging (superhydrophilic)
bags and packaging films
Food bags and packaging films made of polymer with antifog
surfaces are offered broadly. Details of this technology are
unknown, but, most likely, the surfaces of polymers, such as
polyethylene terephthalate (PET), are oxidized and/or roughened
to enhance water ability to spread.
7.8 Self-cleaning and stain-resistant
(superhydrophobic) fabrics/clothes
Dickson in Germany fabricated Orchestra Max fabric, made
of UV-resistant acrylic resin, with superhydrophobic and self-
cleaning characteristics, designed primarily for retail, hotels and
catering outfits.138
7.9 Other applications
It should be mentioned at the end that new products with either
superhydrophobic or superhydrophilic, or related coatings, are
currently booming on the market and many of them can already be
found on the shelves of stores. For example, frying pans used a rough
Teflon coating for many years now, although at the time of invention
this coating was not called superhydrophobic or superoleophobic
but could be grouped into these categories these days.
Quite recently, Apple introduced a fingerprint-resistant oleophobic
coating present on the glass screen of Apple iPhone 3GS. It does
not eliminate grease from the screen but make its cleaning much
easier and more efficient by simply wiping the screen with a soft,
lint-free cloth to remove oily fingerprints.139
8. Conclusion
The research on superhydrophobicity and superhydrophilicity
dates back to the second half of the 1990s, although the solid
foundation for this new subdiscipline was established in eighteenth
to middle of twentieth centuries. It has exploded at the beginning
of the twenty-first century and will certainly attract attention
of many research groups in the years to come. The progress
on fabrication and characterization of superhydrophobic and
superhydrophilic surfaces and coatings, along with understanding
of a liquid spreading and adhesion on such materials, is driven by
a broad application of superhydrophobic and superhydrophilic
surfaces in products with antifogging screens, windows and lenses,
antifouling coatings, microfluidic devices, biocompatible implant
devices, coatings for enhanced boiling heat transfer, foils for food
packaging and many others. There is already a wide spectrum of
products available on market whose design was inspired by the
superhydrophobic and superhydrophilic phenomena.
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Acknowledgements
The authors express deep appreciation to Michelle Leader of Sto
Corp. (Germany), Julia Berkin of Pilkington United Kingdom
Ltd. (Great Britain) and Yoko Katsuyama of NTT-AT (Japan)
for providing images for this publication. Jaroslaw Drelich
acknowledges Patrick Bowen for his corrections to the manuscript.
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