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High Output Polypropylene Nanowire Array Triboelectric Nanogenerator Through Surface Structural Control and Chemical Modi Fication
High Output Polypropylene Nanowire Array Triboelectric Nanogenerator Through Surface Structural Control and Chemical Modi Fication
RAPID COMMUNICATION
a
State Key Laboratory of Solid Lubrication, Lanzhou Institute of Chemical Physics, Chinese Academy of
Sciences, Lanzhou 730000, China
b
University of Chinese Academy of Sciences, Beijing 100049, China
c
Institute of Nanoscience and Nanotechnology, School of Physical Science and Technology, Lanzhou
University, Lanzhou 730000, China
Received 20 September 2015; received in revised form 12 November 2015; accepted 14 November 2015
Available online 24 November 2015
KEYWORDS Abstract
Polypropylene; We report a new method to fabricate a polypropylene (PP) nanowire array based triboelectric
Nanowire; nanogenerator (TENG) with high output through structural control and surface functionalization for
Surface modification; harvesting friction mechanical energy. Compared with the smooth PP film based TENG, the short
Triboelectric nano- circuit current (Isc) and open circuit voltage (Voc) of the PP nanowire based TENGs with the nanowire
generator;
diameter of about 100 nm and length of about 14 μm increase by more than 4 times. More
Mechanical energy
importantly, after surface functionalization with a modifier of 1H,1H,2H,2H-perfluorooctyltrichlor-
harvesting
osilane, the output of the PP nanowire based TENG is further increased to a maximum Voc of 1900 V
and a short circuit current density of 19 mA/m2, increased by more than 100 times than that of the
flat PP film based TENG. This TENG can light up 372 commercial LEDs. Furthermore, a self-powered
temperature sensor is designed, which shows great potential application in daily life. By taking this
simple and effective surface modification strategy, we believe various materials could be used for
energy harvesting by TENGs and other devices with high performance.
& 2015 Elsevier Ltd. All rights reserved.
n
Corresponding authors. Tel.: +86 931 4968169.
E-mail addresses: wangda@licp.cas.cn (D. Wang), wmliu@licp.cas.cn (W. Liu).
http://dx.doi.org/10.1016/j.nanoen.2015.11.017
2211-2855/& 2015 Elsevier Ltd. All rights reserved.
High output polypropylene nanowire array triboelectric nanogenerator 49
Figure 1 (a) Schematic depiction of the fabrication process of PP nanowires prepared by hot processing technique and post surface
modification with fluorinated compounds. (b) Schematic diagram and photo of PP nanowire based TENG.
Figure 3 FESEM images of PP nanowires of (a) Top view and cross-sectional with lengths of (b) 2.4 μm, (c) 4.0 μm, (d) 6.2 μm,
(e) 14 μm, (f) 20 μm.
Figure 4 The performance of PP based TENGs with different nanowire length from 0 to 20 mm. (a) Short circuit current, (b) short
circuit current density, (c) open circuit voltage, and (d) comparation by histogram of Isc and Voc of the PP based TENG with different
nanowire length.
To simplify and study of the electrostatic generation stuck onto the copper tape surface as a lead wire. Then,
process, a piece of aluminum foil (16 cm2) was chosen as both of the PP film and Al electrode were stuck onto a piece
the matched friction and electrode material with PP film. of polyethylene terephthalate (PET) sheet and sealed with a
First, a copper foil tape was firstly stuck onto the backside PET tape to form an arch structure to make it able to
of PP nanowire film layer (16 cm2), and then a Cu lead was automatically restore without external force after pressing.
52 Y. Feng et al.
Figure 5 Schematic diagram of synthesis of Pdop-F (a) and PFTS (b) on the surface of PP nanowire.
Figure 6 (a) XPS spectrum of PP friction layer before and after surface functionalization. Water contact angle on (b) flat PP film,
(c) PP nanowire film, (d) Pdop-F modified nanostructure PP nanowire, and (e) PFTS modified nanostructure PP nanowire.
Last, the TENGs were moved to a oven and dried at 80 1C for was collected through LabVIEW Base Development System
2 h to dry the TENG thoroughly before the output (National Instruments).
measurements.
The morphologies and composition of PP nanowire before Figure 1a shows the schematic illustration of the fabrication
and after chemical modification were tested on a field process of PP nanowire and its surface functionization by
emission scanning electron microscopy (FESEM, JSM-6701F, chemical modification method. First, the AAO templates are
JEOL Inc., Japan) and an X-ray photoelectron spectroscopy prepared by a two-step anodization on pure Al substrate in
(XPS, ESCALAB 250xi). Contact angle (CA) was tested via oxalic acid solution. Then, the PP nanowire arrays are
DSA-100 optical contact angle meter (Kruss Company, Ltd., fabricated by a hot processing technique using AAO as hard
Germany) at ambient temperature (20 1C). The short circuit template. By pressing the PP film into the AAO pores at a
current (Isc) and open circuit voltage (Voc) were tested via high temperature, the PP nanowire/AAO coaxial nanoarray
SR570 Low Noise Current Preamplifier (Stanford Research structure is formed. After removing the AAO template in a
Systems) and NI-PCI6259 (National Instruments), the data hot NaOH solution, the PP nanowire array is obtained. Last,
High output polypropylene nanowire array triboelectric nanogenerator 53
Figure 7 The performance of PP based TENGs before and after surface chemical modification with Pdop-F and PFTS. (a) Short-
circuit current, (b) short circuit current density, (c) open circuit voltage, and (d) charge density. Photographs of PFTS modified PP
nanowire based TENG for (e) pressing and (f) releasing to can instantaneously light up 372 LEDs.
Figure 8 (a) Schematic images of self-powered temperature sensor, (b) linear paragraph of voltage signals at different
temperature, (c) voltage obtained under different temperature.
the PP nanowire arrays are modified with fluorinated coupling effect of contact charging and electrostatic induc-
compounds to obtain the fluoro-terminated PP nanowire tion during the contact or friction process [13,14]. While
materials, which are used as the friction layers of TENGs. two materials with different triboelectric polarities come
The contact electrification process between PP nanowire into mechanical contact, charges occur at their surfaces.
and Al film and the working mechanism of PP-Al based TENG When they are separated, electrostatic potential difference
are illustrated in Figure 2. Generally, the generation of between the two materials results in the current flowing
electric charge of TENG is attributed to the result of the through external circuit. As shown in Figure 2a, before PP
54 Y. Feng et al.
contacting with Al, no charge transfer occurred. When the the lowest output of both short circuit current and open circuit
PP nanowires and Al electrode are pressed to contact, the voltage, which is in consistent with the fact that nanostructure
positive charges generate on Al foil and the negative is a key factor that greatly influences the output value of TENG.
charges generate on PP surface (Figure 2b) [30]. Due to Meanwhile, the length of the PP nanowire has importance
the electrostatic induction effect, the conducting layer of influence on the electric output. From Figure 4a–c, both short
Cu tape generates the opposite charges to the PP friction circuit current and open circuit voltage firstly increases and
layer, resulting in the formation of a current flows from Al reaches the largest value at 14 μm, and then decreases after
electrode to Cu electrode during the releasing process that point. This tendency is much more clearly and the tendency
(Figure 2c). Once the charges reach the balance state, no of open-circuit voltage is consistent with short circuit current as
current flows in the circuit (Figure 2d). Similarly, during the shown in Figure 4d. The peak values of the open-circuit voltage
pressing process, a reverse current is detected from Cu and the short circuit current can reach 157 V and 1.36 μA with
electrode to Al electrode (Figure 2e). Thus, coupling the the PP nanowire length of 14 μm, corresponding to a current
contact electrification with electrostatic induction effects, density of 0.85 mA/m2 (Figure 4b) and charge density of 3.3 μC/
the alternative electricity generates while the TENG experi- m2 (Figure 7d). Compared with the flat PP film based TENG, the
ences a pressing-releasing process. output of PP nanowire based TENG is enhanced by more than
four times. The diameter of the PP nanowire can also influence
the electric output of the TENGs as shown in Figure S2. The
Enhancing the output of TENG by structural control assembled TENGs reach the peak values with the PP diameter of
100 nm. Therefore, the optimal length and diameter of PP
The morphology and nanostructure of the friction electrode nanowire for TENGs are 14 μm and 100 nm, indicating an
play key roles in the output of TENG. For example, important designing principle of triboelectric elecreode for
compared with the smooth surface, the nanowire structure enhancing TENG’s output performance by structural control.
can greatly enhance the Voc and Isc of TENG [31,32], while According to Figure S1, the hole diameter become lager with
there are still the optimized size and morphology of the longer etching time. The nanowires with 80 nm diameter
nanowire. PP nanowire arrays with different length and stacked together which result in a small nanowires density
diameter were designed on the surface of the PP friction while the nanowires density of 135 nm diameter is too big,
material, which can be demonstrated by the FESEM images which will result in a lower contact area. Both of the two has a
of the top and cross-sectional views as shown in Figure 3 and lower output due to the nanowires are not thoroughly con-
Figure S1 in the supporting information. The PP nanowires tacted. The morphology of 100 nm and 120 nm is similar but the
with different lengths were fabricated via controlling the nanowires of 100 nm diameter has a tilt angle, which can lead
thickness of the AAO template, which can be controlled by to a larger output according to the paper published before.
adjusting the Al anodization time from 20 min to 2 h. The [33]. For the length, if the length of PP nanowires is too short,
diameter of PP nanowire is controlled by the pore size of the contact area will not be big enough to obtain good output.
the AAO template, which can be adjusted by controlling the If the nanowires are too long, once the nanowires are pressed
pore widening time in 5 wt% H3PO4 from 3 to 10 min (Figure to bent they may not be able to recovery to the original state
S1a–d). After the same hot pressing process, the PP nano- due to permanent deformation at the root. Thus their con-
wires with different length and diameter were prepare by tribution to friction is very limited. If the nanowires have
using the AAO templates with different thickness and pore optimal length, they are able to revert to original orientation
size. Figure 3a–f show the top view and the cross-sectional when bent due to bending stiffness, which is expected to
views of the PP nanowire with the diameter of 100 nm and provide addition friction area to obtain the biggest output [34].
the length from 2.4 to 20 μm, and Figure S1e–i show the of
PP nanowire with differnert diameter 80–135 nm. According
to these images, the PP film has uniform nanowire array Enhancing the output of TENG by surface chemical
structure in a large area, and the nanowires have smooth modification
surface and uniform diameter from top to bottoms, which is
beneficial to produce triboelectricity. The surface composition of the friction material is another
We measured the electrical output of the PP based TENG key factor to influence the performance of TENG. The
through the contact electrification between the PP nanowire greater difference of the triboelectric polarity of the
array friction layer and Al electrode, as shown in Figure 1b and friction materials, the higher output of the TENGs. It has
Figure 4. The TENG was mechanically triggered by a linear been proven that fluoropolymer, for instance, polytetra-
motor that provides dynamic impact with controlled force at a fluoroethylene (PTFE) and polyvinylidene fluoride (PVDF)
frequency of 5 Hz. All of these PP films with or without nanowire are two of the most suitable triboelectric negative friction
structures were assembled with Al films to fabricate TENGs in materials for TENG till now, since fluorine is the most
the same condition. To proceed more detailed study about these electronegative element of all. However, the high cost
TENGs based on PP nanowires with different length, Voc and Isc and rare types usually restrict the application of fluorinated
were tested separately and the results were shown in Figure 4. composite materials in TENG. Is there a simple and low cost
From the working principle, the charges transferred between Al method to change the triboelectric polarity of the normal
electrode and Cu tape electrode in the external circuit during friction material for TENG? For this, we introduced a surface
the contact and separation process instantaneously generated chemical modification method to adjust the surface compo-
positive and negative currents. Accordingly, an alternative Voc sition of friction material for TENG. The modifiers are
appeared during the pressing-releasing process of the TENGs. It fluorine-containing polymer and small molecule which can
can be seen from Figure 4 that the flat PP film based TENG has adjust the surface triboelectric polarity to increase the
High output polypropylene nanowire array triboelectric nanogenerator 55
TENG output. Herein, Pdop-F and PFTS were selected as the TENG, and 25 time than that of PP nanowire based TENG
surface modifiers to functionalize the PP nanowires and the without PTFS modification. The PFTS modified PP nanowire
flat PP films. The synthesis of Pdop-F was carried out as based TENG can instantaneously light up 372 commercial LEDs
described in our previous work [27–29] and the molecular as shown in Figure 7(e,f) and the supplementary video. There-
structure and preparation process are shown in Figure 5a. fore, the surface modification of fluoropolymers or fluorochem-
Particularly, the prepared Pdop-F molecule has a phenolic icals can significantly enhance the output performance of
hydroxyl group which can absorb tightly on the surface of PP TENGs. Fluoropolymer or fluorochemicals with higher fluorine
nanowire by the intermolecular forces, such as hydrogen- content will generate a higher output. Moreover, the chemical
bond interaction. For the modification with PFTS, we chose modification and nanostructure have a synergistic effect for
a simple and modified physical vapor deposition method enhancing the output performance of TENGs. A durability test
which can form a thin and uniform PFTS layer on the surface has also been proceeded under 5 Hz contact frequency with the
of PP nanowires. The PFTS molecule can form a chemical TENG continuously working for about 37,000 recycles. The
bond with the surface of PP nanowires, resulting in the good result is shown in Figure S4. The nanowire appears little wear
stability of the composite friction layer (Figure 5b). but the output the Isc keeps a steady state and hardly decreases
We verified the surface composition of the functionalized during the test. It can be concluded that the PFTS modified
PP by XPS analysis. As shown in Figure 6a, there is no F1s TENG can work for a long time without the output performance
peak in the spectrum of the as-prepared flat and nanos- having a significant decrease. The high effective and simple
tructured PP film. While after modification with Pdop-F and surface modification strategy provides a new way to change
PFTS, strong F1s signals appear. The PFTS modified samples some normal nonpolar materials into suitable friction materials
have obviously stronger F1s signal, indicating more fluoride for TENG use.
on the surface of PP from the chemical bond of PFTS. Supplementary material related to this article can be
Another reason could be the fluorine content in PFTS found online at http://dx.doi.org/10.1016/j.nanoen.2015.
(48.6 wt%) is much higher than Pdop-F(23.8 wt%). Moreover, 11.017.
the nanowire structure on the surface of PP could also
enlarge the surface area to self-assemble more chemical Application on self-powered temperature sensor
molecule than the flat PP film, which could be also proved
by the XPS result in Figure 6a. The water contact angle
It is very important to give an actual application rather than
measurement was also used to verify the functionalized PP
merely demonstration of LEDs since it is worthy if TENGs can
surfaces. As shown in Figure 6b, when a water droplet
be utilized in daily life. Herein, we design a simple tempera-
dropped on the flat PP surface, a small contact angle of
ture sensor powered by our TENG. The schematic image is
about 921 was observed. After the fabrication of PP
shown in Figure 8a. It can be seen from the image that a
nanowire, the water contact angle increased to 1281,
negative temperature coefficient(NTC) resistor is in series
indicating the nanostructure is an important factor to
with TENG. In this system, the voltage ranges with the
create hydrophobic or super hydrophobic surface. After
change of temperature from room temperature (23 1C) to
modification with Pdop-F and PFTS, the water contact angle
100 1C and the results are shown in Figure 8(b,c). It can be
was further increased to 1421 and 1551, owing to the
concluded from the image that the sensor is sensitive from
contribution of nonpolar (-CF3) end groups in the modifiers
room temperature to 100 1C. Moreover, it seems that the line
with low surface energy. The surface modification has little
presents a liner relationship and the linear formula is fitted
impact on surface morphology of PP nanowires, which could
and given in Figure 8b. As a result, this temperature sensor is
be demonstrated by the FESEM images in Figure S3.
more suitable for temperature from room temperature to
Figure 7 shows the performance of the flat PP and PP
100 1C. It indicates that the FTFS functionalized PP TENG has
nanowire based TENGs before and after modification with
a great application prospect in practical use.
Pdop-F and PFTS. Excitingly, after the surface functionalization,
the output of Isc and Voc have largely increase, either the PP
nanowire based TENG or the flat PP film based TENG. And the Conclusions
output performance has an obvious tendency that the PP
nanowire based TENGs have higher output values than that of In summary, we have demonstrated a new way to fabricate PP
flat PP film based TENGs, indicating the importance of nanowire based TENGs with high output by structural control
structural design. Moreover, the PTFS modified TENGs exhibit and surface functionalization. The PP nanowire arrays are
higher output performance contrast to Pdop-F modified ones, prepared by a facile hot processing technique using porous
which is consistent with the fluorine content proved by XPS anodic aluminum oxide as template, followed by modifying
results in Figure 6a. Combining the nanostructure and chemical with fluorinated compounds to adjust the surface composition
modification, the PTFS modified PP nanowire based TENG got of PP nanowire. Compared with the smooth PP film based
the highest output due to the synergy of the two effect factors. TENG, the fluorinated PP nanowire based TENG shows a
The PP nanowire structure increases the frictional contact area, significant improvement of the output to light up 372 commer-
and the post chemical modification with PFTS improves the cial LEDs, indicating both the nanowire structures and the
triboelectric polarity of PP nanomaterial, resulting the high surface composites of the friction material play important roles
output performance of TENG. The open circuit voltage of PFTS in the output of TENG. The nanowire structure increases the
modified PP nanowire based TENG reaches the highest Voc of effective contact area to generate more triboelectric charges,
1900 V and the Isc of 30 μA, corresponding to the current density and the post chemical modification with fluorinated compounds
of 19 mA/m2 and charge density of 65 μC/m2 (Figure 7d). The Isc adjusts the polarity of PP nanomaterial to improve the genera-
increased by more than 100 times than that of the flat PP based tion efficiency of triboelectric charges, resulting in a high
56 Y. Feng et al.
output performance of TENG. Moreover, the TENG can power a [24] A.M. Md Jani, D. Losic, N.H. Voelcker, Prog. Mater. Sci. 58
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Supplementary material associated with this article can be
[34] G. Zhu, C.F. Pan, W.X. Guo, C.Y. Chen, Y.S. Zhou, R.M. Yu,
found in the online version at http://dx.doi.org/10.1016/j. Z.L. Wang, ACS Nano 12 (2015) 4960.
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Yange Feng received his B.S. in Chemistry
from Qingdao University of Science and
References Technology, China in 2013. He is currently
study in State Key Laboratory of Solid
Lubrication, Lanzhou Institute of Chemical
[1] J. Zhong, Y. Zhang, Q. Zhong, Q. Hu, B. Hu, Z.L. Wang, Physics (LICP), Chinese Academy of Sciences
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[6] Z.L. Wang, G. Zhu, Y. Yang, S. Wang, C. Pan, Mater. Today 15 and Ph.D. (2015) in Material Physics and
(2012) 532. Chemistry from Lanzhou University. He is
[7] Z.H. Lin, G. Cheng, S. Lee, K.C. Pradel, Z.L. Wang, Adv. Mater. currently a research assistant at LICP, CAS.
26 (2014) 4690. His research mainly focuses on designing
[8] Y. Yang, H. Zhang, Y. Liu, Z.-H. Lin, S. Lee, Z. Lin, C.P. Wong, and fabrication of triboelectric generators
Z.L. Wang, ACS nano 7 (2013) 2808. that harvest and convert ambient friction
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Mater. Interfaces 6 (2014) 3031.
[11] H. Zhang, Y. Yang, X. Zhong, Y. Su, Y. Zhou, C. Hu, Z.L. Wang, Shuanhong Ma received his B.S. (2011) from
ACS nano 8 (2013) 680. Tianshui Normal Univesity. He is currently a
[12] F.R. Fan, Z.Q. Tian, Z.L. Wang, Nano Energy 1 (2012) 328. Ph.D student in professor Zhou's Group in
[13] H.T. Baytekin, A.Z. Patashinski, M. Branicki, B. Baytekin, Lanzhou Institute of Chemical Physics, CAS.
S. Soh, B.A. Grzybowski, Science 333 (2011) 308. His research mainly focuses on biotribology,
[14] B.A. Grzybowski, A. Winkleman, J.A. Wiles, Y. Brumer, bionic-tribology.
G.M. Whitesides, Nat. Mater. 2 (2003) 241.
[15] G. Zhu, B. Peng, J. Chen, Q. Jing, Z. Lin Wang, Nano Energy 14
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[16] K. Autumn, M. Sitti, Y.A. Liang, A.M. Peattie, W.R. Hansen,
S. Sponberg, T.W. Kenny, R. Fearing, J.N. Israelachvili,
R.J. Full, Proc. Natl. Acad. Sci. USA 99 (2002) 12252. Daoai Wang received his Ph.D. in Lanzhou
[17] L. Heepe, A.E. Kovalev, A.E. Filippov, S.N. Gorb, Phys. Rev. Institute of Chemical Physics, CAS. From 2009
Lett. 111 (2013) 104301. to 2010, he worked as a Postdoc in Max Planck
[18] G. Huber, H. Mantz, R. Spolenak, K. Mecke, K. Jacobs, Institute of Microstructure Physics. From 2010
S.N. Gorb, E. Arzt, Proc. Natl. Acad. Sci. S. A 102 (2005) 16293. to 2013, he worked as a JSPS researcher in the
[19] W.R. Hansen, K. Autumn, Proc. Natl. Acad. Sci. USA 102 (2005) University of Tokyo. And he is now a professor
385. in Lanzhou Institute of Chemical Physics sup-
[20] A.G. Gillies, R.S. Fearing, Langmuir 27 (2011) 11278. ported by ‘‘Top Hundred Talents’’ Program of
[21] J. Lee, R.S. Fearing, Langmuir 24 (2008) 10587. Chinese Academy of Sciences. His research
[22] J. Lee, C. Majidi, B. Schubert, R.S. Fearing, J. R. Soc. interests include mnanoenergy technology,
Interface 5 (2008) 835. photoelectrochemistry, and marine tribology.
[23] S.H. Shin, Y.H. Kwon, Y.H. Kim, J.Y. Jung, M.H. Lee, J. Nah,
ACS nano 9 (2015) 4621.
High output polypropylene nanowire array triboelectric nanogenerator 57
Feng Zhou got his PhD in 2004 in Lanzhou Weimin Liu got his PhD in Lanzhou Institute
Institute of Chemical Physics. He spent of Chemical Physics in 1990 and spent a year
three years (2005–2008) in the department (1993–1994) in department of Chemistry,
of Chemistry, University of Cambridge as a Penn State University, USA. Currently, he is
postdoctoral research associate. And he is a full Professor and the director in the State
currently a professor and deputy director in Key Laboratory of Solid Lubrication. He was
State Key Lab of Solid Lubrication, LICP, elected as Academicians of CAS in 2013. His
CAS. His research interests are the micro/ research interests cover tribology of poly-
nanostructured surfaces for lubrication, mer composites, organic and nanoparticular
drag/noise reduction and anti-biofouling lubricating oil additives, ultra-thin lubricat-
applications, high performance lubricants. Details can be found ing films, and particularly in space tribology.
at: http://www.licp.cas.cn/zfz/