Article

www.acsnano.org

Highly Efficient Light-Driven TiO2−Au Janus

Micromotors
Renfeng Dong,† Qilu Zhang,† Wei Gao,‡,§ Allen Pei,‡,∥ and Biye Ren*,†
†
Research Institute of Materials Science, South China University of Technology, Guangzhou 510640, China
‡
Department of Nanoengineering, University of California San Diego, La Jolla, California 92093, United States
*
S Supporting Information
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ABSTRACT: A highly efficient light-driven photocatalytic TiO2−Au

Janus micromotor with wireless steering and velocity control is
described. Unlike chemically propelled micromotors which com-
Downloaded via SHENZHEN UNIV on December 26, 2020 at 16:21:30 (UTC).

monly require the addition of surfactants or toxic chemical fuels, the

fuel-free Janus micromotor (diameter ∼1.0 μm) can be powered in
pure water under an extremely low ultraviolet light intensity (2.5 ×
10−3 W/cm2), and with 40 × 10−3 W/cm2, they can reach a high
speed of 25 body length/s, which is comparable to common Pt-based
chemically induced self-electrophoretic Janus micromotors. The
photocatalytic propulsion can be switched on and off by incident
light modulation. In addition, the speed of the photocatalytic TiO2−
Au Janus micromotor can be accelerated by increasing the light
intensity or by adding low concentrations of chemical fuel H2O2 (i.e.,
0.1%). The attractive fuel-free propulsion performance, fast movement triggering response, low light energy requirement,
and precise motion control of the TiO2−Au Janus photocatalytic micromotor hold considerable promise for diverse
practical applications.
KEYWORDS: Janus micormotors, self-electrophoresis, TiO2, light driven, fuel free

T he autonomous motion of nano/microscale objects has

stimulated considerable research efforts over the past
decade.1−9 Particular attention has been given to
chemically powered micromotors which include bimetallic
catalytic nanowires,10,11 microtubular microrockets,12,13 and
Janus microspheres.14,15 However, they mostly exhibit auton-
omous self-propulsion in the presence of hydrogen peroxide
fuel10,11,14 or hydrazine15 which greatly hinders the practical
utility of chemically powered nanomotors. Therefore, efforts
toward the fuel-free nanomotors powered by external stimuli
such as magnetic fields,16,17 electrical fields,18,19 ultrasound,20,21
and light22,23 are particularly exciting and considerably
promising toward practical applications. In particular, light is
one of the most important and versatile physical stimuli to
facilitate and regulate the propulsion of micro/nanomotors.24,25
However, the major challenge of light-driven micromotors is to
achieve the high propulsion speed and precise motion
control.26,27
Here, we demonstrate light-driven TiO2−Au Janus micro-
motors (∼1.0 μm diameter) based on light induced self-
electrophoresis mechanism which display efficient propulsion
(over 25 body length/s) under an extremely low UV light
intensity (40 × 10−3 W/cm2) in the presence of pure water
without adding any extra fuel. The light-driven Janus motors
reach a fast speed which is comparable to common Pt-based
chemically induced self-electrophoretic Janus micromotors. The
propulsion of Janus micromotor can be conveniently triggered
even at extremely low ultraviolet (UV) light intensity (2.5 ×
10−3 W/cm2) with high repeatability and accelerated by
increasing the light intensity or by adding low concentrations
of chemical fuel H2O2. As illustrated in Figure 1A, the Janus
micromotors consist of plain TiO2 particles (∼1.0 μm mean
diameter) with one hemisphere coated with Au metal. On the
one hand, anatase TiO2 is widely studied due to its interesting
properties, including photocatalytic activity, biocompatibility,
high chemical stability, and low costs;28,29 it is commonly used
for decontamination purposes due to the high photoactivity of
TiO2.30,31 On the other hand, it is well-established that Au-
doped TiO2 or the TiO2−Au system has a greatly enhanced
catalytic performance compared to that of bulk TiO2.32−34 In
light of these advantages, we designed catalytic TiO2−Au Janus
micromotors by coating a thin film of gold (gold film thickness:
40 nm) on TiO2 particles (Figure 1B). When the TiO2 surface
is exposed to UV light, the self-electrophoretic propulsion
mechanism is immediately triggered and efficiently propels the
micromotor in pure water.
Received: September 21, 2015
Accepted: November 23, 2015
Published: November 23, 2015

© 2015 American Chemical Society 839 DOI: 10.1021/acsnano.5b05940

ACS Nano 2016, 10, 839−844
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Figure 1. (A) Schematic of catalytic TiO2−Au Janus micromotors
powered by UV light in water. (B) Scanning electron microscope
(SEM) image of a spherical TiO2−Au micromotor, and (C−E) the
corresponding Energy Dispersive X-ray (EDX) images for Ti, Au,
O, respectively. Scale bar, 0.5 μm. (F) Tracking lines (taken from
Supporting Information Video S1) illustrating the distances
traveled by three micromotors in pure water over 1 s. Scale bar,
10 μm.
RESULTS AND DISCUSSION
The propulsion of the TiO2−Au micromotors dominantly
originates from the light induced self-electrophoresis.35
Compared to Pt−Au Janus motors which require H2O2 for
self-electrophoresis, the light-driven TiO2−Au system can
generate a self-induced electric field in pure water and the
motion can be controlled by light. Upon UV irradiation of the
Janus micromotors, charge separation occurs within the TiO2
and electrons are injected from the TiO2 conduction band into
the Au hemisphere. Protons are produced from the oxidation of
water at TiO2 and the resulting electrons are consumed during
the reduction of protons at Au. The resulting flux of H+
generates a fluid flow toward the Au hemisphere, generating a
slip velocity and propelling the micromotors with the TiO2
hemisphere forward (Supporting Information Video S2 shows
that the TiO2−Au Janus motors are moving toward TiO2 side
under an extremely low UV intensity, 2.5 × 10−3 W/cm2). In
contrast, plain TiO2 microspheres without Au layer only display
Brownian motion even upon exposure to 40 × 10−3 W/cm2 UV
light (Supporting Information Video S1). Previous reports have
demonstrated thermophoretic micromotor propulsion from
infrared irradiation of Au.36 However, to validate which is the
dominant mechanism resulting in the propulsion of the TiO2−
Au micromotors, photoinduced self-electrophoresis or thermo-
phoresis, control experiments were conducted using poly-
styrene (PS)−Au Janus particles (1.0 μm diameter). Under 40
× 10−3 W/cm2 intensity light, no obvious directional
movement was observed for PS−Au Janus particles, while the
TiO2−Au micromotors were moving pretty fast (Supporting
Information Video S1). The control experiments of the
micromotors in salt rich environment (NaCl solution) have
been investigated. The speed of TiO2−Au Janus motor in 1.0
mM NaCl solution is obviously smaller than that in pure water
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Article
(Supporting Information Video S3). The micromotor stops
moving in the presence of 10.0 mM salt. These results further
confirm the self-electrophoresis mechanism. We also examined
the mixed potentials of Au and TiO2 electrodes with and
without illumination (Figure 2). It is clear from the Figure 2
Figure 2. A Tafel plot of Au, Ni, and TiO2 with and without
illumination (0.5 × 10−3 W/cm2).
that the potential difference between the Au electrode and
illuminated TiO2 (ΔETiO2(light)−Au = 307 mV) electrode is larger
than that between Au electrode and TiO2 electrode without
illumination (ΔETiO2(dark)−Au = 237 mV). As reported previously
by Nakato and Tsubomura, the height of the Schottky barrier at
the Au/TiO2 contact is considerably increased by illumination,
and the photovoltage obtained is much larger than that
expected from the barrier height in the dark.37 These findings
are consistent with the obtained results. The motion of such
light-driven Janus micromotor is strongly dependent on the
coated layer due to the self-electrophoresis mechanism. We
tried TiO2−nickel (Ni) Janus micromotors as control, as
illustrated in the Supporting Information Video S4, and the
speed of TiO2−Ni Janus micromotor (8 μm/s under 40 × 10−3
W/cm2 UV light intensity) is much lower than that of TiO2−
Au Janus micromotors (25 μm/s). The Tafel plot of Au, Ni,
and TiO2 with and without illumination (0.5 × 10−3 W/cm2)
(shown in Figure 2) clearly indicates that the potential
difference between Ni and illuminated TiO2 electrode
(ΔETiO2(light)−Ni = 150 mV) is significantly smaller than that
between Au and illuminated TiO2 electrodes (ΔETiO2(light)−Au =
307 mV). This finding is consistent with the propulsion
behavior of the corresponding micromotors and further
confirms the self-electrophoresis mechanism of the light-driven
metal-TiO2 micromotors. Regarding the insulation layer,
aluminum oxide (Al2O3)−TiO2 Janus microsphere was chosen
as the control. As illustrated from Supporting Information
Video S4, Al2O3−TiO2 Janus microsphere does not display
directional motion under 40 × 10−3 W/cm2 UV light intensity.
Such phenomenon can be attributed to the greatly hindered
electrophoresis between the insulation layer and TiO2.
As indicated from Figure 1A, the photoactivity of TiO2
comes from its hole−electron separation triggered by photons
of energy equal to or higher than its bandgap. The conduction
band of Au lies below that of TiO2, and as a result, the Au
hemisphere acts as a sink for electrons, increasing electron−
hole pair lifetime and recombination times which result in
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Figure 3. (A−D) Tracklines of micromotors (Supporting Information Video S5) with UV intensities of (A) 2.5, (B) 5, (C) 10, and (D) 40 ×
10−3 W/cm2, over 1 s. Scale bar, 10 μm. (E) The influence of the UV light intensity on the speed of Janus micromotors in pure water. (F)
Average MSD versus time interval (Δt) analyzed from tracking trajectories. (G) Diffusion coefficient of TiO2−Au Janus micromotor under
different UV light intensity, the values determined from the MSD plots (20 micromotors were analyzed).

enhanced reactivity on the micromotors surfaces.35 Therefore,
such structure makes the TiO2−Au Janus micromotor much
more efficient than the reported plain TiO2 micromotor whose
average speed is around 10 μm/s under 2.5 W/cm2 UV light
intensity.27 Compositional analysis using SEM and EDX
mapping indicates that the Au coating only covers half of the
TiO2 spherical particle (Figure 1B−E, the relative EDX pattern
in Supporting Information Figure S1 also illustrating the
composition of the TiO2−Au Janus micromotor), generating
the asymmetry necessary for directional motion. The micro-
motor tracklines in Figure 1F show that the new TiO2−Au
Janus motors move immediately at a speed of around 25 μm/s
in pure water upon UV light irradiation.
As photocatalysis primarily drives the TiO2−Au micromotor
propulsion, the motion speed of the micromotors is able to be
precisely controlled by adjusting the UV irradiation intensity
(I). The highly efficient TiO2−Au Janus micromotors can be
propelled by super low UV light intensity. Figure 3A reveals
pretty slow but directional motion when I is 2.5 × 10−3 W/cm2.
When increasing I from 5- to 10 × 10−3 W/cm2, the speed of
the micromotors increases from 5.6 to 11.2 μm/s (Figure
3B,C). The micromotors can move at a speed of over 25 μm/s
corresponding to a relative speed of 25 body lengths/s under a
light intensity of 40 × 10−3 W/cm2 (Figure 3D). Such efficient
speed is almost 2 times faster than reported speed of light
driven TiO2 micromotors in pure water;27 however, over 60
times lower UV light power is needed. Also, such efficient
speed is comparable to that of the catalytic micro/nanomotors,
and significantly larger than the speed of previously reported
841
photothermally propelled motors.26 Figure 3E illustrates the
diagram of the influence of light intensity (I) on the speed of
TiO2−Au Janus micromotor. To clearly indicate the directional
movement of the Janus motors at extremely low UV light
intensity, we experimentally estimated the enhanced diffusion
coefficients of the motors. The motors (number of motors n =
20) were tracked over 10 s, the mean squared displacement
(MSD) was calculated at different UV light intensity (0, 2.5 ×
10−3, 5 × 10−3 W/cm2) and the diffusion coefficient (D) was
calculated by the equation D = MSD/iΔt, where Δt is the time
interval. Here, for the case of two-dimensional analysis from the
recorded video, i is equal to 4 (Figure 3F,G, respectively). It
can be clearly observed that although the speed under 2.5 ×
10−3 W/cm2 UV light is almost the same as that without UV
light, the MSD of Janus motor under 2.5 × 10−3 W/cm2 UV
light is significantly higher than that without UV light. These
results demonstrated that the UV light with extremely low
intensities still has obvious influence on the propulsion of the
Au−TiO2 micromotors. In general, the relationship of incident
light (I) and the flux (Φ, the number of incident photons per
unit area per second) can be described as equation 1.24
hc
I=Φ
λ (1)
−34
Here, h, c, and λ represent Planck’s constant (6.626 × 10 J·
s), speed of light (3 × 108 m/s), and wavelength of the UV light
(330−380 nm in this case), respectively. As a result, the flux Φ
of photons of wavelength λ increases with increasing I on the
micromotor, and thus, the number of the photogenerated holes
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Figure 4. Cyclic “On” and “Off” UV light activation of the TiO2−Au Janus micromotor. (A) Schematic and time-lapse images illustration of
TiO2−Au Janus micromotor moving status in pure water with UV light and without UV light, respectively. (B) Corresponding speed/time
dependence illustrating the UV light triggered “On/Off” motion control of the TiO2−Au Janus micromotor in pure water without any
additional chemicals. The images were taken at 1-s intervals from Video S6. Scale Bar, 10 μm. UV light intensity, 40 × 10−3 W/cm2.

and electrons in TiO2 increases. Therefore, there will be a Video S7). Such directional control could offer more possibility
proton gradient enhancement and corresponding fluid shear for the light-driven micromotor applying in variety of practical
velocity resulting from increased irradiation intensity. Accord- applications.
ingly, the speed of the micromotors can be modulated by Interestingly, low concentrations of H2O2 can also improve
incident light intensity. the motion of the TiO2−Au micromotors. The micromotors
Compared to catalytic micromotors which consume chemical can be accelerated gradually by increasing the concentration of
fuels, the as-developed light-driven TiO2−Au micromotors H2O2 under 40 × 10−3 W/cm2 UV light. The TiO2−Au
have the impressive advantages of highly repeatable simple micromotors display Brownian motion (Figure 6A) in 0.1%
motion control. As Figure 4 illustrates, the repeated on/off
cycling of UV light illumination induces the activation and
inactivation of the movement of micromotors reflecting the fast
response rate of the micromotors upon the UV irradiation. The
speed of the micromotors is around 25 μm/s under 40 × 10−3
W/cm2 UV light exposure, but stop moving immediately when
the UV light is off. This “stop/go” propulsion behavior
indicates that high reversibility and controllable micromotor
motion can be achieved by switching the UV irradiation on or
off (as shown in Supporting Information Video S6). Even after
30 cycles of such on and off control, the micromotors still show
highly repeatability.
Directional control of micromotor is also a critical perform-
ance for diverse practical applications. The deposition of a
paramagnetic Ni layer between Au layer and TiO2 can be easily
realize magnetic control of the directionality of the light-driven
TiO2−Au Janus micromotor.38−40 Figure 5A illustrates the
structure of such magnetic guided Janus micromotors. With the
use of an external magnetic field, Au−Ni−TiO2 Janus Figure 6. Tracklines for TiO2−Au micromotors under three
micromotors can be precisely navigated following predeter- conditions: (A) with H2O2 without UV, (B) without H2O2 with
mined trajectories (Figure 5B and Supporting Information UV, and (C) with both H2O2 and UV, over 1 s. Scale bar, 10 μm
(taken from Supporting Information Video S8). (D) Schematic of
catalytic TiO2−Au Janus micromotors powered by UV light in low
concentration of H2O2.

H2O2 without UV light exposure; however, the speed of such

Figure 5. (A) Schematic of the magnetic control of multilayer Au−
Ni−TiO2 Janus micromotors. (B) Time-lapse images (taken from
Supporting Information Video S7) showing the magnetically
guided propulsion of an Au−Ni−TiO2 micromotor under 40 ×
10−3 W/cm2 UV light. Scale bar, 10 μm.
842
light-driven Janus motor can reach 42 μm/s (Figure 6C) with
additional 0.1% H2O2, which is almost 2 times compared to the
one in pure water (Figure 6B). Such fast speed of TiO2−Au
Janus motors in 0.1% H2O2 is almost 20 times faster than the
common Pt based Janus motors in 0.2% H2O2 at room
temperature,14,41 which is the lowest H2O2 concentration
requirement with high speed for Janus motors so far. The
acceleration of TiO 2 −Au Janus motors in low H 2 O 2
concentrations with UV light is due to the enhanced self-
electrophoretic effects in H2O2 compared to pure water (Figure
6D).42,43
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CONCLUSIONS
In conclusion, we described light-driven TiO2−Au Janus
micromotors which can be powered efficiently by extremely
low UV light energy in pure water. In addition, the light
induced self-electrophoresis mechanism has been demonstrated
in detail also. This study showed that photocatalytic micro-
motors can be accelerated by increasing the light power
intensity or addition of low concentrations of extra chemical
fuels H2O2. Furthermore, such light-driven, TiO2-based micro-
motors can be driven in a precisely controlled manner,
involving controllable activation, acceleration, deceleration,
stop and directional control. In addition, the gold hemisphere
in TiO2−Au Janus micromotors can be easily modified with
diverse functional groups offering various possibilities to
challenging complicate tasks. The fuel-free property of these
light-driven micromotors combined with the decontaminative
capabilities of TiO2 should naturally lead to useful applications
in environmental remediation.31,44 These light-driven, precisely
controllable, and highly efficient TiO2-based phtotocatalytic
Janus micromotors hold considerable promise for the design of
practical light-driven nanomachines toward a wide range of
important future applications ranging from nanofabrication45 to
environmental remediation.3
EXPERIMENTAL SECTION
Synthesis of Janus Micromotors. TiO2 microspheres were
prepared by the solvent extraction/evaporation method using
tetrabutyl titanate as a precursor.46 Briefly, 1.0 mL of tetrabutyl
titanate (Sigma #244112) was dissolved in 40.0 mL of ethanol and
incubatde at room temperature for 3 h; then, TiO2 microspheres were
collected by centrifugation at 7000 rpm for 5 min and washed
repeatedly with ethanol (Guangzhou Chemical Reagent Co.) and
ultrapure water (18.2 MΩ·cm), three times each, then dried in air at
room temperature. TiO2 (anatase) microsphere is obtained after
annealing for 2 h at 400 °C. The X-ray diffraction (XRD) pattern
(Supporting Information Figure S2) reveals that the TiO2 micrspheres
have a good anatase phase. For the TiO2−Au light-driven Janus
micromotor, TiO2 microspheres (1.0 μm mean diameter) are used as
the base particles. TiO2 particles (10.0 μg) were first dispersed in
150.0 μL of ethanol. The sample was then spread onto glass slides and
dried uniformly to form particle monolayers. The particles were
sputter coated with a thin gold and nickel layer using a Quorum Q
150T ES Sputter Coater for 3 cycles with 60 s per cycle. The metal
layer thickness was found to be 40 nm, as measured by the Veeco
DEKTAK 150 Profilometer. For the TiO2−Ni−Au magnetic Janus
motors, TiO2 particle monolayers were prepared as in the method
above. A 40 nm layer of Au followed by a 10 nm layer of Ni were
sequentially deposited on half of the particles by Quorum Q 150T ES
Sputter Coater. The TiO2 microspheres were coated with Al2O3 layer
using ultrahigh Vacuum Magnetron Sputter Coater JPG 560. The
micromotors were subsequently released from the glass slides via pipet
pumping and dispersed into double distilled water. The polystyrene−
Au Janus microsphere as a control was fabricated with the same
method using polystyrene microsphere (Baseline #6-1-0100).
Speed Calibration Experiments. To determine the relationship
between the TiO2−Au, TiO2−Ni, and TiO2−Al2O3 motor speed and
light intensity, the light intensity ranged from 2.5 × 10−3 to 40 × 10−3
W/cm2. Sodium chloride (NaCl) solutions (0.2−200.0 mM) were
prepared for testing salt rich environment control experiment. A 0.2%
aqueous hydrogen peroxide (Alfa Aesar #33323) solution was
prepared and directly mixed with the motor droplets. The propulsion
calibration experiments were performed by mixing 1.0 μL of the motor
and hydrogen peroxide solutions each.
Electrochemical Potential Measurements. Tafel plot is used to
obtain the potential established at different segment of different Janus
micromotors (Au, Ni, and TiO2) with and without illumination (0.5 ×
10−3 W/cm2 UV light intensity, λ = 330−380 nm) in a pure water
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environment. Gold, nickel, and TiO2 films (all the films’ thicknesses,
100 nm) on ITO glass disc (diameter, 1.0 cm) were used as the
working electrode in the electrochemical potential measurements,
respectively. We use the CH Instrument Model CHI600C to test the
potential at a scan rate of 5 mV/s and over a potential range of −0.2 to
0.3 V (vs Ag/AgCl, 3 M KCl reference).
Equipment. SEM and EDX pictures were obtained by Zeiss VEO
18; XRD pattern was obtained by X-ray Diffractomer (Panlytical, Inc.
X′ Pert Pro). UV light was generated by Mercury lamp sockets,
dichroic mirror DM 400 and barrier filter BA420, intensity controlled
by ND filters (4×, 8×, 16×) (all from Nikon), and light intensity was
measured by UV radiometer UV-A (Videos were captured by an
inverted optical microscope (Nikon In-strument, Inc. Ti−S), coupled
with 40× objectives, and a Zyla scmos digital camera (ANDOR) using
the NIS-Elements AR 4.3 software.
ASSOCIATED CONTENT
*
S Supporting Information
The Supporting Information is available free of charge on the
ACS Publications website at DOI: 10.1021/acsnano.5b05940.
Supporting videos description, supporting figures (PDF)
Supporting videos (ZIP
AUTHOR INFORMATION
Corresponding Author
*E-mail: mcbyren@scut.edu.cn.
Present Addresses
§
Wei Gao, Electrical Engineering and Computer Sciences,
University of California, Berkeley, California 94720, United
States.
∥
Allen Pei, Department of Materials Science & Engineering,
Stanford University, Stanford, California 94305, United States.
Notes
The authors declare no competing financial interest.
ACKNOWLEDGMENTS
The financial support from the NSFC (21274047) and the
Specialized Research Fund for the Doctoral Program of the
Education Ministry (20120172110005) is gratefully acknowl-
edged.
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DOI: 10.1021/acsnano.5b05940
ACS Nano 2016, 10, 839−844