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Nano Research
Nano Res
DOI
10.1007/s12274-014-0698-2
Chinese Brushes: From Controllable Liquid
Manipulation to Template-Free Printing Microlines
Qianbin Wang1, Qingan Meng1, Huan Liu1 (), and Lei Jiang1,2
Nano Res., Just Accepted Manuscript • DOI: 10.1007/s12274-014-0698-2
http://www.thenanoresearch.com on December 16 2014
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TABLE OF CONTENTS (TOC)
Chinese
Brushes:
From
Controllable
Liquid
Manipulation to Template-Free Printing Microlines
Qianbin Wang1, Qingan Meng1, Huan Liu1*, and Lei
Jiang1,2
1 Key Laboratory of Bio-Inspired Smart Interfacial
Science and Technology of Ministry of Education, Beijing
Key Laboratory of Bio-inspired Energy Materials and
Devices, School of Chemistry and Environment, Beihang
University, Beijing, 100191, P. R. China.
2 Beijing National Laboratory for Molecular Sciences
(BNLMS), Key Laboratory of Organic Solids, Institute of
Chemistry, Chinese Academy of Sciences, Beijing,
100190, P. R. China.
In this mini-review, we discussed that the essence of the Chinese brush
in controllable liquid transfer lie in the anisotropic multi-scale
Page Numbers.
structural feature of the fresh emergent hairs. Drawing inspirations, its
applications in controllable liquid pumping, highly efficient liquid
transfer and template-free printing microlines were addressed
respectively.
1
Nano Res
DOI (automatically inserted by the publisher)
Review Article
Chinese Brushes: From Controllable Liquid Manipulation to
Template-Free Printing Microlines
Qianbin Wang1, Qingan Meng1, Huan Liu1 (), and Lei Jiang1,2
1
Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education, Beijing Key Laboratory of
Bio-inspired Energy Materials and Devices, School of Chemistry and Environment, Beihang University, Beijing, 100191, P. R.
China.
2 Beijing National Laboratory for Molecular Sciences (BNLMS), Key Laboratory of Organic Solids, Institute of Chemistry, Chinese
Academy of Sciences, Beijing, 100190, P. R. China.
Received: day month year / Revised: day month year / Accepted: day month year (automatically inserted by the publisher)
© Tsinghua University Press and Springer-Verlag Berlin Heidelberg 2011
ABSTRACT
As a traditional writing instrument for calligraphy and painting, the Chinese brush enjoys a high reputation
over the last 5000 years due to its distinguishable ability in controllable handling ink liquid, which therefore be
widely used to deposit ink into certain characters or figures during culture communication. In this mini-review,
we firstly discussed that the essence of the Chinese brush in controllable liquid transfer lie in the anisotropic
multi-scale structural feature of the fresh emergent hairs. Then, drawing inspirations, its applications in
controllable liquid pumping, highly efficient liquid transfer and template-free printing microlines were
addressed respectively. We envision that the fundamental of Chinese brushes and its applications in liquid
manipulation mentioned in this review may also be extended to other liquid phase functional material systems.
KEYWORDS
Chinese brushes, dynamic wetting, multi-scale structures, liquid transfer, direct printing
1. Introduction
As an important writing tool, the Chinese brush
plays a crucial role in the process of the oriental
civilization development over the past five thousand
years [1]. The distinguishable feature of the Chinese
brush over other writing tools is that it enables
controllable transfer of low viscosity ink liquid onto
papers or other substrates [2-3]. Therefore,
understanding the mechanism of liquid transfer of
the Chinese brush is not only scientifically important
for the deep knowing the fundamental of wetting in
open fibrous systems, but also practically
meaningful for manipulate liquid in versatile fields,
especially those in microscopic scale. So far, attempts
on the topic of wetting on fibers have been mostly
focused in the area of efficient water collection, the
directional water transport, and self-assembly into
micro-patterns on both natural and synthetic fibers,
as has been reviewed recently [4-5]. However,
manipulating liquid in more sophisticated and
well-controlled way by structured conical fibers
remains challenge, and the Chinese brush offers a
solution in this aspect.
This mini-review is focused on the fundamental
of controllable liquid transfer of the Chinese brush,
and its applications in liquid manipulation ranging
from the liquid pumping, highly efficient liquid
————————————
Address correspondence to Huan Liu, [email protected]
2
transfer to template-free printing of microlines.
There are four main sections. First, the importancy of
the Chinese brush as a writing tool was briefly
introduced, as well as its basic physicochemical
nature. Then, the representative behavior of the
Chinese Brush in controllable liquid manipulation
was described, followed by the mechanism analysis.
The third section presents the applications of
Chinese brushes inspired devices in liquid
manipulation and template-free printing. In the last
section, we make a conclusion and present our own
thoughts about the future development of this area.
Figure 1 The fundamental of the controllable liquid transfer of the Chinese brush and its applications in liquid
manipulation and template-free printing. (a) The Chinese brush is a traditional writing tool for calligraphy and
painting, and often used to deposit ink onto certain substrates as various characters and figures, which then as
a carrier to deliver emotions or convey knowledge from one generation to another. Recreation from internet
3
raw materials, and the horse was painted by Xu Beihong. (b) The optical picture of the freshly emergent hair
(FE-hair) and its schematic illustration reveal the unique anisotropic microstructures featured by tapered
architecture with oriented squamae. (c) When drop was released on the surface of FE-hairs, driving force Fl
arising from Laplace pressure difference, gravitational force Fg, and the asymmetric retention force Fa arising
from anisotropic arranged squamae would working on it. And the conical feature of FE-hairs can induce a
Laplace pressure difference to propel the droplet move to the low curvature area. (d) The oriented squamae
may generate a retention force to control the liquid unidirectional spreading or moving along the oriented
squamae [2]. Copyright 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (e-g) the applications of the
Chinese brush inspired device in various fields: (e) Controllable liquid pumping. Left: Silicon oil droplet would
present self-propelled movement behavior and be balanced at the same position for a fixed volume no matter
where it was released on the surface of FE-hairs array. Right: The balance position show linearly inversely
proportional to Ω1/3 (Ω is the drop volume) [2]; (f) Highly efficient liquid transfer. Left: The design of the
bio-inspired highly efficient liquid transfer system. When a drop was hold at the tip region, the bio-inspired
multi-scale structured conical fiber exhibit highest efficiency in liquid manipulation. Right: Change the apex
angles and tilt angles could significantly alter the maximum liquid capacity of the bio-inspired conical fibers,
and the maximum liquid capacity is 428 times greater than its own volume was realized [6]. Copyright 2014
American Chemical Society. (g) Template-free printing of microlines. Left: Schematic illustration of
template-free printing device with two parallel FE-hairs and an artificial liquid reservoir. Right: the microlines
generated by direct writing ink liquid (surface tension of 45 mN/m) on glass surface by using the model
bio-inspired device, exhibiting tunable width range from 10 μm to ca. 130 μm [2].
2. General knowledge of Chinese brushes
Among all the writing tools, the Chinese brush, alias
ink brush or writing brush, is a unique writing
instrument that is peculiar to China. It is titled the
most ancient one among Four Treasures of Chinese
traditional Study [1]. As an important writing
instrument for calligraphy and painting, the Chinese
brush have played a distinctive and irreplaceable
role in the culture exchange and heritage for its
ability in deposit liquid ink onto papers in various
patterns and characters [3]. By using brush in cursive
and fast way with varying posture, speed and
pressure, eastern artists renders each ink stroke in a
continuous and harmonious rhythm to deliver their
emotions or convey knowledge [1, 7], as shown in
Figure 1a. Thanks to the Chinese brush, Chinese
culture have spread to neighboring countries and
then to all over the world.
Been a traditional tool for calligraphy and
painting, the Chinese brush has been existed more
than five thousand years. The archaeological
discoveries demonstrated that the inscriptions on
painted pottery and shell-and-bone writing indicated
the use of Chinese brushes in the Neolithic Age [7].
Today’s brushes, as has been documented [8], were
developed in Qin Dynasty (221-206 BC) by using the
hairs of rabbit, under the inspiration that the tail of
an injured rabbit could leave a long and continuous
blood trace behind. Since then, Chinese brushes have
been used as a main tool to record people’s thinking
and feeling by various characters and figures, which
facilitate the culture spreading and transmission
from one generation to another.
Normally, qualified Chinese brushes are made of
a bundle of quasi-parallel freshly emergent hairs
(FE-hairs) of animals such as hare, goat, horse, rabbit,
mouse, wolf, fox, gorilla, swam, pig, badger, or even
the virgin hairs of human babies. Each type of hair
has a different elasticity or even ink capacity, which
in turn results in a different appearance of ink stroke.
The most notable feature of the Chinese brush is its
ability in large-mass ink loading and the continuous
and uniform ink delivery onto the paper with
well-controlled manner, despite different brushes are
used for different styles of calligraphy and writing.
Worth noting is that only the FE-hairs render the
Chinese brush the excellent ability in liquid
manipulation, which will be addressed in detail in
this mini-review.
3. Large-mass ink holding by Chinese
brushes
4
The first step of traditional Chinese calligraphy or
painting is dipping the Chinese brush into the
low-viscosity ink, by which step the ink was
transferred into the brush. Upon this ink loading
operation, the naturally dispersed FE-hairs in the
brush would re-shape into a bundle with a tapered
topological architecture under the interaction
between the capillary forces and the elasticity of the
hairs [9-10], and presents an obvious expanded
appearance on a certain position. We quantitatively
demonstrated that over 2 times greater than its own
weight of ink could be stored within the spaces
between FE-hairs in the Chinese brush [2], which
renders the brush an adaptable “ink reservoir”. To
better visualize the ink loading process, we
constructed a two parallel hairs model system to
explore the liquid transfer behavior of the Chinese
brush. When a silicon oil droplet (surface tension of
20 mN m–1) was released on the surface of two
parallel hairs, it could exhibit different self-propelled
movement behaviors along the FE-hairs at different
regions. And for a fixed volume of droplet, it would
always stop and be balanced at the same position
despite the place it was released. This behavior was
also shared by other particles-based suspensions, for
example, ink liquid with surface tension = 45 mN
m–1. [2]
Why the silicon oil droplet can be dynamically
balanced within the two parallel hairs system? The
mechanical analysis revealed that the unique
anisotropic multi-scale structures of the FE-hairs,
featured by tapered architecture with oriented
squamae (Figure 1b), is the key [2]. It is well known
that for a droplet held at a conical fiber, the curvature
gradient of a conical fiber would arouse a Laplace
pressure difference (P), driving the drop move from
the tip to the top of the conical fiber [2, 11-13], as
presented in Figure 1c. The Force arise from the
Laplace pressure difference can be obtained by
integrating P times the area around the entire liquid
surface, express as,
4 tan 
(1)
Fl ~

(rf  R0 )2
where  is the surface tension of the liquid,  is the
half apex angle of the conical fiber, rf is the radius of
the fiber, R0 is maximum radius of the drop, and  is
the volume of the liquid. For a droplet on the tip
region (high curvature site) of the conical fiber, the
Laplace pressure that acts on it is much larger than
that acts on the top region (low curvature site),
because the local curvature variation at the tip region
is much bigger than that at the top region [2, 13].
Thus, the P can generate a large force to propel the
drop move upwards apart from the tip, until it was
balanced by the anisotropic force that generated
from the oriented squamae and the gravity.
Another possible force favorable for the liquid
transfer of the Chinese brush is assignable to the
unique oriented squamae of the FE-hairs [14-15],
which could generate anisotropic wetting behavior
[16-17]. For a drop on the asymmetric structures of
oriented squamae, 2 and 1, the anisotropic
retention force arising from the oriented squamae
will induce a special retention force differential
(Figure 1d) could be express as [18],
1
Fa  f d  fu  2w sin[ r 0  a 0 ] 
2
(2)
1
1
[sin( 2   )  sin( 1   )]
2
2
where is the solid–liquid contact width, θa and θr is
the apparent advancing and receding contact angles,
and   a0 r 0 (θa0 and θr0 are the true advancing
and receding contact angles). When 2 > 1, the
retention force differential is Fa > 0, which can
therefore generate an anisotropic hysteresis, leading
to the liquid unidirectional spreading or moving
along the oriented squamae [19-20].
The cooperative effect of P that aroused from
the conical feature of the FE-hairs, the asymmetrical
retention force that generated by the oriented
squamae and the gravity make large mass of liquid
dynamically balanced within the brush, empowering
the Chinese brush the unique liquid controlling and
holding capacity, and consequently its versatile
applications in controllable manipulating functional
liquid phase materials.
4 Applications of the Chinese brush and
bio-inspired devices
Differ from the other reported fibers systems where
the driving force normally was one-directional, the
Chinese brush offer a multiple driving forces to
make possible the liquid could be continuously
stabilized/hold within it. It thus provides solutions in
controllable manipulating liquid in various ways.
5
4.1 Controllable liquid pumping
Directional driving of liquid droplets on solid
surfaces has attracted much attention in many fields,
such as microfluidic devices [21-23] and lab-on-chip
architectures [24-26]. Until now, great progress has
been made to control the motion of a liquid droplet
on a solid surface by introducing energy gradients
such as chemical [27-28], thermal [29-30], shape
[31-32] or wetability gradients on surfaces [33-34] or
using external driving forces [35-36] such as gravity,
electric or magnetic fields. Besides, surfaces with
anisotropic
chemical,
mechanical,
physical,
morphological, and topological properties have been
engineered for transporting drops [37-39], and may
offer new approaches to propel liquid droplets in the
demand direction. For example, we recently reported
that spider silks with unique periodic knot/joints and
cacti with conical spines are capable of collecting tiny
water droplets from humid air. [11, 13] We also
demonstrated that water droplets could move in a
controllable demand direction under the action of
surface roughness gradient or stimuli-responsive
wettability. [40-42]
However, the directional liquid motion via an
open fibrous media, especially those with anisotropic
arranged microstructures, is rarely reported so far.
Chinese brushes here provide one alternative
solution. We recently demonstrated that the FE-hair
enables liquid pumping, even in a controllable
manner. [2], as shown in Figure 1e. It is illustrated
that
silicon
oil
droplets
would
present
position-dependent self-propelled movement when
released at the surface of parallel FE-hairs. For detail,
the drop would spontaneously move from the tip to
the region of larger radius when released at the tip of
the hairs since the conicity of the tip region is the
most remarkable. While when released at the top of
the conical structure, the liquid would automatically
move downward to the region of higher curvature,
because the local conicity is too small to generate
enough driven force to overcome the retention force
that acted oppositely. Most importantly, all the
droplets would stop and be balanced at certain
position where the P was balanced by the gravity
and anisotropic retention force. We also
demonstrated that the balance position of droplets
on the surface of the FE-hairs would show significant
dependence on the volume of liquid, presenting a
well-controlled manner. Although liquid pumping
by fibrous media have been recently suggested as a
feasible strategy in applications as liquid transport
[43], water collection [5, 11, 13, 44-45] and water–oil
separation [46], none of them proceed in a
controllable manner. The controllable liquid
pumping on the FE-hairs give our new insight in
transporting liquid with controllable direction,
location and even speed.
4.2 Highly Efficient Liquid Transfer
Highly efficient liquid transfer is significantly
important in chemical reactions [47-48], printing or
patterning [49-52] and biological assays [53-54]. So
far, many bio-inspired artificial liquid transfer
systems were developed, and could be divided into
three main categories. The first is the drop on the
functional surface. For example, superhydrophobic
surfaces with high adhesion could provide particular
advantages in lossless liquid droplet transporting.
[55]. The second is drop in the enclosed channel
system. Such as, a synthetic microfluidic system
could realize water transport at large negative
pressures, which provide an approach for
technological uses of water under tension [56]. The
last is the drop on the open fibrous system. For
instance, bio-inspired thin fibers with unique spindle
knot and the joint structures could hang a large
volume of water droplet between spindle knots [45].
Although dynamic wetting in these systems offers
benefits in many practical applications, the efficiency
of liquid transfer system is far away from the
requirements of engineering applications.
The great ink loading ability of the Chinese brush
allows us to design and fabricate bio-inspired
materials that could be applied in highly efficient
liquid transfer [2, 6], as presented in Figure 1f.
Recently, drawing inspiration from the controllable
liquid transfer in ratchet conical hairs, a dynamic
electrochemical method was develop to fabricate an
anisotropic multiscale structured conical copper wire
(SCCW) with controllable conicity and surface
morphology that mimic the structural feature of
FE-hairs in Chinese brushes. The conicity of the
copper wire was controlled by length of the wire
immersed into the electrolyte, while the surface
morphology could be accurately controlled by
6
reciprocating the working electrode at a small
velocity (v < 0.02 mm/s). The SCCW exhibit the
similar behavior with that of the Chinese brush: the
water droplet with fixed volume could be balanced
at certain position dynamically under the
cooperative effect of P, the asymmetrical retention
force, and the gravity. Here, due to the physical
rigidity of the SCCW, the effect of the way it interacts
with liquid on the liquid amount could be
investigated. It is found that the highly efficient
liquid manipulation ability was realized by using the
boundary condition of the dynamic liquid balance
behavior at the tip region of the SCCW. When
cooperatively controlling the tilt angle and apex
angle of the SCCW, a large mass of liquid can be
manipulated in a well controllable manner, and over
428 times greater than its own volume of liquid
could be operated, presenting a highly efficient
liquid transfer system. This bio-inspired SCCW
could provide new insight in designing novel
materials and devices to manipulate liquid in a more
controllable way and with high efficiency.
4.3 Template-Free Printing Microlines
As a maskless, non-lithographic route, direct-write
technologies offer the ability to rapidly fabricate
one-dimensional (1D) structured materials for
photonic [57-60], electrical [61-62] and biomaterial
applications [63]. Different from traditional
approaches, such as ink-jet printing, screen printing
or micro-contact printing, direct-writing technologies
required neither costly and complicated equipment
nor complex fabrication processes [64-66], which
would therefore be beneficial for direct patterning
1D structured materials with a low cost and high
yield. For example, Lewis et al used rollerball pens
with conductive silver inks to direct print electrodes
on paper, offering a low-cost, portable fabrication
route for printed electronic and optoelectronic
devices [61]. Mirkin et al fabricated a polymer pen
lithography, which could be employed to direct write
protein
nanoarrays
in
a
low-cost
and
high-throughput manner [67].
Recently, inspired by the fascinating ability of
FE-hairs in manipulating low viscosity liquid, a facile
direct printing device with two parallel FE-hairs was
designed and fabricated, as presented in Figure 1g
[2]. To supply a continual liquid, a man-made liquid
reservoir was equipped and connected to the parallel
FE-hairs. When such model device was contacted
with the high adhesive substrate, such as paper, glass
slide and silicon wafer, liquid materials in the
reservoir could steadily, uniformly and continuously
transferred onto the substrate, leaving a microline on
the surface of substrate. This direct printing device
enables preparing 1D microlines with well-defined
profile on various smooth substrates through direct
writing liquid phase materials. To be noticed, the
resolution could be down to 10 m. This bio-inspired
direct printing device provides a new simple
alternative for preparation microlines that could be
applied for easy printing micro-patterned optical,
electric, as well as sensing devices. We envision this
technique is applicable for versatile functional liquid
phase material with inherit or better performances.
5. Conclusion and perspectives
As one of the most ancient writing tools, the Chinese
brush provides a powerful and efficient approach to
control liquid transfer. By analyzing the
structure-function relationship in the Chinese
brushes, we conclude that the cooperative effect of
P that aroused from conical architecture, the
asymmetrical retention force arising from oriented
micro-meter scaled squamae and the gravity is
responsible for the controllable liquid manipulation.
Understanding the mechanism of the hairs structures
in ink holding of the Chinese brush system inspired
us to develop novel bio-inspired devices that could
manipulate liquid materials, especially in microscale,
as liquid pumping for transporting liquid with
controllable direction, location and speed; high
efficiency liquid transfer for chemical reactions or
biological assays; and template-free printing for easy
printing micro-patterned optical, electric, as well as
sensing devices.
Utilizing natural product of the animal hair to
record the thinking and living experiences onto some
medium, is always beneficial for the development of
civilization in the human history, although the
mechanism has far from being discussed. Realizing
such ancient wisdom is of paramount importance
even to modern science and technology, since it
provides versatile promising applications in field of
the modern science. Here, we envision that the
7
Chinese brush and the bio-inspired devices will shed
new lights on developing 1D fibrous materials that
enables manipulate liquid phase material, as
polymer, nano-particle suspension and small
molecule solution, in well-controlled manner, which
is meaningful in various fields as optical and electric
devices and bio-sensing and diagnosis.
[8] Sima, Q., Records of the grand historian: The
Biography of Meng Tian. Zhonghua Book Company:
1967.
[9] Bico, J.; Roman, B.; Moulin, L.; Boudaoud, A.,
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2004, 432 (7018), 690-690.
[10] Py, C.; Bastien, R.; Bico, J.; Roman, B.; Boudaoud,
A., 3D aggregation of wet fibers. EPL (Europhysics
Acknowledgements
Letters) 2007, 77 (4), 44005.
The authors thank the financial support by National
Research Fund for Fundamental Key Projects
(2013CB933000), Program for New Century Excellent
Talents in University (NCET-13-0024), National
Natural Science Foundation (61227902, 21121001,
91127025,), Fok Ying Tong Education Foundation
(132008), and the Fundamental Research Funds for
the Central Universities.
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