Nano Energy 105 (2023) 107997

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Nano Energy
journal homepage: www.elsevier.com/locate/nanoen

Triboelectric nanogenerator with enhanced output and durability based on

Si-DLC films
Mang Gao a, Soo-Bin Kim a, Yahui Li b, c, Shreeharsha H. Ramaswamy a, Junho Choi a, *
a
Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan
b
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Electronic Information and Electrical Engineering, Shanghai Jiao Tong
University, Shanghai 200240, China
c
Department of Micro/Nano Electronics, School of Electronic Information and Electrical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China

A R T I C L E I N F O A B S T R A C T

Keywords: As one of the working modes of triboelectric nanogenerators (TENGs), the sliding-mode TENG has a higher
Si-DLC films charge-transfer efficiency than the contact-separation mode. However, the durability and stability of these de­
Sliding-TENG vices remain challenging for practical applications because most dielectric materials for TENGs are organic
Water lubrication
polymers. This study used Si-incorporated diamond-like carbon (Si-DLC) films as non-polymer dielectric mate­
Durability
Friction coefficient
rials for sliding-TENGs to improve output and durability. Si-DLC films with varying Si contents were prepared
using plasma-based ion implantation and deposition, and their triboelectric and tribological properties were
investigated. The Si-DLC film with a higher Si content exhibited a higher triboelectric output under dry condi­
tions owing to its stronger electron-donating ability. Furthermore, it was found that the output and durability of
the Si-DLC-based sliding-TENG can be further enhanced under unsubmerged water-lubricated conditions
compared with those under dry conditions. This enhanced output is attributed to the more electropositive nature
of water compared with that of the Si-DLC films. Moreover, the enhanced durability and stability of the Si-DLC-
based TENG under water-lubricated conditions are attributed to the anti-abrasion properties of the Si-DLC films,
which prevent the formation of a transferred PTFE layer on the Si-DLC surface. This research proposed an in­
tegrated strategy to enhance output and durability simultaneously, showing great potential for designing durable
self-driving sensing systems in machinery.

1. Introduction materials with robust mechanical durability and stability, such as

The development of Internet of Things (IoT) electronics has
increased the demand for improved power supply units. Traditional
battery-based IoT electronics suffer from many environmental and
economic drawbacks because they are unsustainable and require
recharging or replacement [1]. Since their development in 2012,
triboelectric nanogenerators (TENGs) have attracted significant atten­
tion owing to their self-powering ability, sustainability, low cost, and
easy fabrication [2]. The application of TENG has spurred a wide range
of applications, such as different self-powered sensors [3–6], blue en­
ergy [7–10], and wearable devices [11–13].
Although significant progress has been made over the past decade,
the durability of sliding-mode TENG is still unsatisfactory [14], despite
its high charge transfer efficiency [15–17]. Three strategies are most
commonly used to overcome this limitation. The first involves the use of
diamond-like carbon (DLC) films [18,19]. The use of liquid lubricants on
the sliding interface can also reduce surface wear and extend the lifetime
of sliding-mode TENGs [17,20]. Lastly, durability can be improved by
changing the working modes, such as the noncontact mode [21–23] and
the conjunction of the working modes [24–26]. Ramaswamy et al. re­
ported that DLC films are promising dielectric materials for sliding
TENG [18]. This study provides a valuable introduction towards the
understanding of the triboelectric behavior of DLC films. It aims to
significantly contribute to the design of a highly durable, efficient,
low-friction, and cost-effective sliding-mode TENG. Although DLC films
have been proven to be promising dielectric materials for TENG [18],
their durability and electrical output still require improvement. Wu et al.
proposed a method for improving the durability of TENG by applying
liquid lubricants [20]. The experimental results showed that liquid lu­
bricants could prevent the formation of a transfer film and enhance the

* Corresponding author.
E-mail address: choi@mech.t.u-tokyo.ac.jp (J. Choi).

https://doi.org/10.1016/j.nanoen.2022.107997
Received 6 September 2022; Received in revised form 23 October 2022; Accepted 6 November 2022
Available online 9 November 2022
2211-2855/© 2022 Elsevier Ltd. All rights reserved.
M. Gao et al.
effective solid-solid contact area by squeezing out the air at the inter­
face, thus increasing the triboelectric output. Additionally, sliding-mode
TENG often suffers from output degradation caused by abrasion and
interfacial heat loss [27]. Li et al. [24] developed a device that could
significantly improve the robustness and lifetime of TENGs through an
automatic transition between the contact and noncontact working
states. Despite noncontact mode TENG having high durability and
almost 100% theoretical conversion efficiency, the rapid reduction of
pre-existing charge results in very low output, thus hindering its appli­
cability [22,25,27,28].
Si-incorporated DLC (Si-DLC) films are promising protective coating
materials owing to their excellent tribological and anticorrosion prop­
erties [29–34]. In particular, Si-DLC films exhibit a remarkably low
friction coefficient in the air [31,34]. It is thought that the water mol­
ecules adsorbed on the silanol (Si-OH) groups on the surface of the
Si-DLC film contribute to the low friction of the Si-DLC films [35,36]. It
has also been reported that the friction coefficients of Si-DLC films under
water-lubricated conditions are very low [37,38]. This has been attrib­
uted to the formation of a SiOx(OH)y gel layer on the films, which acts as
a thin lubricant film. Furthermore, because the thickness of DLC films is
on the order of less than a few micrometers, they are suitable for ap­
plications as monitoring sensors or power sources without the need for
changing the original structures of mechanical systems. Besides,
water-solid triboelectric nanogenerators draw a lot of attention due to
the environment-friendly lubrication using water [39], the insensitivity
to ambient humidity, and the easy accessibility of water [40,41].
Additionally, the excellent adhesion of Si-DLC films to steel surfaces
further improves their applicability in these systems. In summary,
research on Si-DLC films as dielectric materials for TENG could be an
essential milestone to enhance the durability of sliding-TENGs further
and extend their engineering applications in real mechanical systems.
In this study, we report Si-DLC films as an abrasion-resistant and
high-output dielectric material for sliding-TENGs, which is promising
for fabricating sensors for mechanical systems. The optimal Si-DLC with
the highest output was obtained by investigating the triboelectric and
tribological properties of Si-DLC films with various Si contents. To
further explore the superiority of the optimal Si-DLC film and under­
stand its performance, experiments were performed under different
water-lubricated conditions. The mechanism behind durability and
output enhancement under water-lubricated conditions was also
explored.
2. Results and discussion
2.1. Physical and tribological properties of Si-DLC films
Si-DLC films were deposited on pure Al and Si substrates using
bipolar-type plasma-based ion implantation and deposition (PBII&D)
[18,42], and a schematic outline of PBII&D is shown in Fig. S1. A gas
mixture of tetramethylsilane (TMS, Si(CH3)4) and toluene (C6H5CH3)
was used as the source gas for the deposition of Si-DLC films. As Si
content has a significant influence on the physical and tribological
properties of Si-DLC films [42,43], Si-DLC films with various Si contents
by changing the TMS ratio of the precursor gas were deposited. The
specific deposition parameters for the Si-DLC are presented in Table S1.
For comparison, hydrogenated DLC (H-DLC) films were also deposited
using toluene as a precursor gas. For simplicity, the deposited Si-DLC
films with different TMS ratios were named TMS 2, TMS 4, TMS 6,
and TMS 8, as shown in Table 1. The thicknesses and Si contents of the
prepared DLC films are also listed in Table 1. A higher TMS ratio in the
source gas equates to a higher Si content in the Si-DLC films. The Si
content gradually increased with the mixing ratio of TMS, and the film
thickness was almost constant at 1.1 µm.
Raman spectroscopy was employed to analyze the microstructures of
the Si-DLC films. In the Raman spectrum of the DLC film, the G band is
attributed to the bond stretching of sp2 sites existing in both ring and
2
Nano Energy 105 (2023) 107997
Table 1
The parameters of deposited Si-DLC and H-DLC films.
Sample Toluene TMS TMS Deposition Si Film
name (sccm) (sccm) Ratio time (min.) contents thickness
(at%) (μm)
H-DLC 10 0 0 76 0 1.05
TMS 2 8 2 20% 90 9.0 1.13
TMS 4 6 4 40% 96 15.0 1.06
TMS 6 4 6 60% 103 17.8 1.08
TMS 8 2 8 80% 114 26.1 1.15
chain structures, while the D band is attributed to the breathing modes
of the sp2 rings [44]. The intensity ratio of the D and G peaks (ID/IG) is
proportional to the sp2/sp3 bond ratio [45]. The measured Raman re­
sults of the Si-DLC films are shown in Fig. 1a,b. It can be seen that both
the ID/IG ratio and G-peak position decrease with increasing Si content.
Si incorporation results in the opening of sp2 rings and a reduction in the
sp2 cluster size because Si cannot form π bonds, leading to a decrease in
the ID/IG ratio with increasing Si content [42]. These behaviors indicate
an increase in sp3 bonds with increasing Si content in the Si-DLC film
[42,46]. The dielectric constants obtained by a spectroscopic ellips­
ometer also show an increasing trend with increasing Si content (Note
S1 and Table S2) [35]. Generally, a high permittivity of contact mate­
rials is known to enhance the output performance of TENG owing to the
increase in charge density [47] and stronger electron-donating capa­
bility [20,48].
The full width at half-maximum of the G peak (FWHM(G)) indicates
structural disorder resulting from bond angle and bond length distor­
tions in the DLC film [46], which increases as the disorder increases [49,
50]. Fig. 1b shows that TMS 6 and TMS 8 exhibit the higher FWHM(G), i.
e., the higher disorder. As the disorder increases in the film, the sp2
cluster size decreases, and the sp2 rings become sparser and more dis­
torted until they begin to open [51]. Choi et al.[42] reported that Si
addition to DLC films can generate a large number of dangling bonds,
indicating an increase in the number of possible electron-donating sites,
which is beneficial for TENG charge accumulation [52,53]. Therefore,
TMS 6 and TMS 8 are expected to have relatively high electron-donating
abilities and high TENG outputs.
The work function reflects the surface electronic polarity of a ma­
terial. A lower work function indicates a stronger electron-donating
ability, and a higher work function indicates a stronger electron-
withdrawing ability [15]. From the aforementioned Raman analysis,
TMS 6 and TMS 8 are more likely to have higher electron-donating
abilities. To further compare the electron-donating capabilities of TMS
6, TMS 8, and H-DLC, the work function and surface potential were
measured by Kelvin probe force microscopy (KPFM). As shown in
Fig. 1c,d, the work functions of TMS 6 and TMS 8 are lower than that of
H-DLC (Fig. S2). In contrast, the surface potential shows an opposite
trend. The work function of TMS 8 is the lowest, indicating that TMS 8
has the strongest electron-donating ability. Ahmed et al. noted that Si
incorporation into DLC films lowered the barrier for electron emission,
resulting in a lower work function [54]. Based on the Raman analysis
results in Fig. 1a,b, it can be inferred that a highly disordered structure
contributes to higher electron emission, resulting in the lower work
function as observed for TMS 8.
The friction properties of the prepared Si-DLC and H-DLC films were
evaluated using a ball-on-disc tribometer (Fig. S3). The specific details
related to the friction experiment were illustrated in Note S2. The co­
efficients of friction (COF) of the TMS 8 and H-DLC films and wear scars
of the PTFE balls are shown in Fig. 1e,h, respectively. It was found that
the COF of TMS 8 was the lowest among the DLC films. The wear scars of
the PTFE balls sliding against TMS 8 were smaller and smoother than
those of H-DLC. The COF and specific wear rates are shown in Fig. 1f,g
(The calculation method of specific wear rates is given in Note S2). The
COFs of the DLC films were obtained by averaging the values of the last
600 s in Fig. 1e, and the wear rates were calculated according to the
M. Gao et al.
Fig. 1. (a) Raman spectra of Si-DLC and H-DLC films. (b) ID/IG ratio, G-peak position, and FWHM(G) obtained from the Raman spectra. (c) Work function and (d)
surface potential of H-DLC, TMS 6, and TMS 8. (e) Coefficients of friction obtained from ball-on-disc tribotests. (f) COF and (g) wear rate of Si-DLC films. (h) Wear
scar of PTFE balls after the tribotests.
equations in Note S2. Both the COF and wear rate decreased as the TMS
ratio increased. It is apparent that TMS 8 exhibited the best tribological
properties among the prepared DLC films.
2.2. Improved output of TENG based on Si-DLC films
A series of triboelectric experiments were conducted to investigate
the performance of Si-DLC-based TENGs under dry conditions. The
freestanding mode as shown in Fig. S4 was used for the experiments, and
PTFE was used as the counter dielectric pair. The experimental results
under an applied load of 3 N, working frequency of 1 Hz, and the stroke
of reciprocating motion of 20 mm are shown in Fig. 2a-c. The short-
circuit current (ISC), open-circuit voltage (VOC), and short-circuit trans­
ferred charge (Q) increased with the increasing TMS ratio. The VOC of
TMS 8 was approximately twice those of H-DLC. TMS 8 showed the best
performance when compared with other DLC films, and a possible
reason for this result is that TMS 8 has a stronger electron-donating
ability compared to other DLC films, as indicated by the Raman anal­
ysis and KPFM measurements.
The triboelectric properties of TMS 8 were further investigated under
various working frequencies and loads. The experimental setup is the
same as shown in Fig. S4, and the basic working principle is displayed in
Fig. 2d, which is working in freestanding mode (The detailed
3
Nano Energy 105 (2023) 107997
introduction of the working principle is provided in Note S3). Aiming to
study the working mechanism of TENG based on TMS 8, the COMSOL
simulation software was used for finite element analysis of the potential
distribution during a complete working cycle, as shown in Fig. 2e.
As displayed in Fig. 3a-c, both VOC and ISC increase with load. The
increase of output with load is because the contact area enlarges with
the increase of load. As shown in Fig. 3d-f, VOC shows an almost constant
value with increasing working frequency, and ISC increases linearly with
the working frequency. This is because that VOC is only related to the
number of transferred charges, whereas ISC reflects the speed of charge
transfer so that ISC shows a larger value at a higher frequency.
The power density of the Si-DLC-based (TMS 8) TENG was obtained
by measuring the output voltage and current with external loads ranging
from 0.01 to 1000 MΩ. The results are shown in Fig. 3g,h. The output
voltage increased with the increasing resistance, whereas the current
density decreased from 10 MΩ. As a result, the maximum power density
reached 0.773 mW⋅m− 2 at an external load of 400 MΩ, as presented in
Fig. 3h.
2.3. Enhanced output of Si-DLC-based TENG under water-lubricated
conditions
Several studies have explored water as a promising triboelectric layer
M. Gao et al.
Fig. 2. Electrical characteristics of the DLC films: (a) Open-circuit voltage, (b) short-circuit current, and (c) short-circuit transferred charge measured at an applied
load of 3 N and a working frequency of 1 Hz. (d) Working principle of TMS 8-based TENG in free-standing mode. (e) Simulated potential distribution of TMS 8-based
TENG during the reciprocating motion.
to scavenge abundant, clean, and renewable water-based energy
[55–59]. Chung et al. [57] reported that water becomes charged when it
comes into contact with the air or water pipe, and the maximum charge
density can reach 4.5 μC/m2. When water comes into contact with the
PTFE film, positive charges are induced [60]. Therefore, when water is
paved between PTFE and the Si-DLC film, part of PTFE contacts with
water, and the rest of PTFE contacts with Si-DLC film so that the positive
triboelectric layer comprises both a water layer and a Si-DLC layer.
Because water has a relatively low viscosity, the water layer would not
be retained in the sliding interface when PTFE and Si-DLC move relative
to each other.
The triboelectric properties of the TMS 8 and H-DLC coatings were
investigated under dry and water-lubricated conditions with an exper­
imental setup, as shown in Fig. S5. The results are shown in Fig. 4a, b
(Original electrical output signal under dry and water-lubricated con­
ditions are presented in Fig. S6). The working frequency, applied load,
stroke, and gap distance between two PTFE surfaces were 1 Hz, 2 N,
12.8 mm, and 4 mm, respectively. Water (150 μl) was introduced be­
tween the TMS 8 and PTFE as a lubricant (The reason for the water
amount selection was illustrated in Note S4 and Fig. S7). From Fig. 4a, b,
it is clear that both the open-circuit voltage and short-circuit current
increase dramatically after applying the water lubricant (The compari­
son of outputs for TMS 8 under dry and water conditions was presented
in Video S1).
Supplementary material related to this article can be found online at
doi:10.1016/j.nanoen.2022.107997.
Under water-lubricated conditions, the contact surface becomes a
partial solid-solid contact and partial liquid-solid contact. Because TMS
4
Nano Energy 105 (2023) 107997
8 has a stronger electron-donating capability than H-DLC, TMS 8 can
produce a higher output for solid-solid contact. Meanwhile, the effect of
the liquid-solid contact between PTFE and water is almost the same for
the H-DLC- and TMS 8-based TENG. However, the effects of the liquid-
solid contact of H-DLC and TMS 8 with water on the output are unclear.
Therefore, to understand the whole mechanism of output increase, more
experiments need to be conducted.
To understand the characteristic behavior of the Si-DLC-based TENG
under water-lubricated conditions, a series of experiments were con­
ducted under four different lubrication conditions, as shown in Fig. 4c:
(i) dry condition; (ii) water-unsubmerged, non-grooved condition; (iii)
water-unsubmerged, grooved condition; and (iv) water-submerged,
grooved condition. Water (150 μl) was introduced into the sliding
interface as a lubricant for experiments under unsubmerged conditions.
As shown in Fig. 4d, e, the output of the water-unsubmerged, non-
grooved condition (Fig. 4c-ii) was approximately double that of the dry
condition (Fig. 4c-i). Furthermore, the output of the water-
unsubmerged, grooved condition (Fig. 4c-iii) was higher still (Original
electrical output signals are presented in Fig. S8). Because water is an
electropositive material [57,61] and PTFE is a strong electronegative
material, positive charges are induced in the water layer when contact is
made. Under the water-unsubmerged, grooved condition (Fig. 4c-iii),
water entrapped in the groove can reflow into the sliding interface be­
tween TMS 8 and PTFE, which is similar to the groove bearing [62].
More water can induce more charges on the PTFE surface. When there is
no groove in the middle of the PTFE, as illustrated in Fig. 4c-ii, water is
squeezed out from the sliding interface due to its low viscosity. In this
case, the solid-solid contact between TMS 8 and PTFE becomes more
M. Gao et al. Nano Energy 105 (2023) 107997

Fig. 3. (a) Open-circuit voltage, (b) short-circuit current, and (c) trend of them under loads of 1–5 N for TMS 8-based TENG. (d) Open-circuit voltage, (e) short-circuit
current, and (f) trend of them under working frequencies of 1–3 Hz for TMS 8-based TENG. (g) The output voltage and current density, and (h) the power density
under different external load resistances at an applied load of 2 N and a working frequency of 1 Hz.

dominant (i.e., the sliding condition approaches the dry condition),
resulting in a lower output. In the case of water-submerged conditions,
because all the charges at the sliding interface dissipate into the water,
which in turn screens the PTFE (Fig. 4c-iv), the output approaches zero
[63].
2.4. Mechanism of output enhancement of Si-DLC-based TENG under
water-lubricated conditions
To further understand the mechanism that the output of TMS 8 is
enhanced under unsubmerged water-lubricated conditions, three
different counter materials — Al, nylon, and steel — were applied
against PTFE. The output performance is shown in Fig. 5a, b (The
electrical signals are presented in Fig. S9). It can be observed that the
output of Al and steel increased with water lubrication, whereas the
output of nylon decreased. These results can be explained by the charge-
transfer mechanism. Sun et al. demonstrated that the charge transfer
phenomenon of contact electrification could occur at the liquid-solid
interface by a tiny droplet on the solid surface at the atomic level [64].
Under unsubmerged water-lubricated conditions, the solid-solid
contact area between the nylon and PTFE was partially substituted by
water [65]. Because water is less electropositive than nylon, the charges
produced by nylon outweigh those produced by water (Fig. 5c-ii),
leading to an output decrease. Furthermore, the fluidability of water
confined between nylon and PTFE further contributed to the reduction
in output (Fig. 5c-iii). The negatively charged water in contact with
nylon flows onto the PTFE surface when nylon and PTFE move relative
to each other owing to the fluidability of water. The negatively charged
water induces positive charges on the PTFE surface when in contact,
generating negative charges on the Al electrode through electrostatic
induction after the contact (Fig. 5c-iii). The negative charges can
neutralize the positive charge induced by nylon on the Al electrode [20],
resulting in a further decrease in output.
In contrast, Al and steel (Fig. 5d) are electropositive compared with
PTFE, but less electropositive than water [66]. When Al or steel is used
as the counter dielectric surface of PTFE, both water and Al (or steel) in
contact with PTFE generate negative charges on the PTFE surface.
Because water is the most electropositive, more negative charges are
generated on the PTFE surface compared with the dry condition,
resulting in output enhancement, as shown in Fig. 5d-i–ii. However,
because water is more electropositive than Al (or steel), negative charges
are not generated on the water surface. Therefore, the positive charges

5
M. Gao et al. Nano Energy 105 (2023) 107997

Fig. 4. (a) Open-circuit voltage and (b) short-circuit current comparison between H-DLC and TMS 8 under dry and water-lubricated conditions. (c) Schematics of Si-
DLC-based TENG under dry and three different water-lubricated conditions: (i) dry condition, (ii) unsubmerged and non-grooved condition, (iii) unsubmerged and
grooved condition, and (iv) submerged and grooved condition. (d) Open-circuit voltage, and (e) short-circuit current of TMS 8 under different water-
lubricated conditions.

on the Al electrode are not neutralized when the positively charged
water flows onto the PTFE surfaces (Fig. 5d- ii–iii), resulting in output
enhancement. The TMS 8 case is similar to that of Al (or steel); therefore,
the output of TMS 8 can be enhanced under unsubmerged
water-lubricated conditions.
TMS 8 shows a higher output than H-DLC (Fig. 4a,b) under a water-
unsubmerged grooved condition because water is more electropositive
than H-DLC and TMS 8. The totally induced charges on the Al electrode
originate from two areas: solid-solid contact and solid-liquid contact. In
the solid-solid contact area, the TMS 8/PTFE pair can induce more
charge than the H-DLC/PTFE pair because TMS 8 is more electropositive
than H-DLC. For the solid-liquid contact (Fig. 5D-ii–iii), the H-DLC/water
pair can induce more charges than the TMS 8/water pair on the contact
surfaces because TMS 8 is more electropositive than H-DLC (H-DLC is
less electropositive than TMS 8, and TMS 8 is less electropositive than
water in the triboelectric series). This results in higher output for H-DLC
than for TMS 8. However, it should be noted that the overall charges
induced from the solid-solid contact and solid-liquid contact of TMS 8
were higher than those of H-DLC as shown in Fig. 4a,b, indicating that
the output under unsubmerged water conditions is mainly dominated by
the solid-solid contact, i.e., the unsubmerged water lubrication is in the
boundary lubrication regime.
2.5. Durability of Si-DLC-based TENG
The durability of the Si-DLC (TMS 8)-based TENG under dry and
water-lubricated (unsubmerged and grooved) conditions was investi­
gated and compared with that of H-DLC-based TENG. The applied load,
working frequency, and reciprocating stroke length were 2 N, 4 Hz, and
12.8 mm, respectively. Water (150 μl) was applied to the sliding inter­
face for lubrication. Under dry conditions, the outputs for both Si-DLC
and H-DLC gradually decrease, as shown in Fig. 6a. It was found that
Si-DLC under water-lubricated conditions maintained a stable output
(Fig. 6b), dropping by only 20.96% from its maximum value after 3 h of
sliding. In contrast, there was 34.73% reduction of the output for H-DLC
compared with its maximum value after 3 h of sliding. Original elec­
trical output signals of durability tests are presented in Fig. S10. As the
test time goes on, the water volume will decrease, which will affect the
output. Therefore, to further demonstrate the durability of Si-DLC-based
TENG, 150 μl water was initially used to verify the durability and 25 μl
water was added to the friction interface every hour (Fig. S11). Fig. S11
shows that the maximum output can be maintained even after 200 min,
and 68.75% of the maximum output can be remained after the 360 min
(86,400 cycles) test.
To investigate the reason why Si-DLC under water-lubricated

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M. Gao et al. Nano Energy 105 (2023) 107997

Fig. 5. (a) Open-circuit voltage and (b) short-circuit current for different dielectric materials under water-lubricated conditions. The counter dielectric material was
PTFE. For Al and Nylon, the working conditions were a working frequency of 1 Hz, a working load of 2 N, and a stroke of 12.8 mm. Thicknesses of Al and Nylon are
1 mm and 0.3 mm, respectively. The dimensions of the materials were 20 mm × 30 mm. For steel, the stroke was 20 mm and other working conditions were the same
as Al and Nylon. Charge interactions between (c) Nylon and PTFE and (d) Al (or Steel) and PTFE under unsubmerged water-lubricated conditions.

conditions can maintain a stable output and show better anti-abrasive
capability, the COFs of TMS 8 and H-DLC under water-lubricated con­
ditions were measured simultaneously during TENG measurements. As
shown in Fig. 6c, the COF of TMS 8 was lower than that of H-DLC under
water-lubricated conditions.
These results indicate that water can effectively function as a
boundary lubricant, particularly for Si-DLC; that is, the anti-abrasion
properties of Si-DLC against PTFE are better than those of H-DLC
(Fig. 6d-g). A white transferred layer of PTFE was observed on the Si-
DLC film as well as on the H-DLC film tested under dry conditions,
which reduced the TENG output. Transferred layers of TMS 8 and H-DLC
on Al substrates under water-lubricated conditions were observed with
scanning electron microscope (SEM) (Fig. S12), and the composition of
the transferred layers was further identified with energy-dispersive X-
ray spectroscopy (EDS) (Fig. S13). It was confirmed that transferred
layers were originated from PTFE debris. Si-DLC can effectively reduce
the formation of PTFE transferred film on its surface under the water-
lubricated condition, as shown in Fig. 6e, thus maintaining a stable
and high output. The PTFE surfaces before and after durability tests
under water-lubricated conditions were compared as displayed in
Fig. 6h-j and Fig. S14. As shown in Fig. S14, the PTFE surface remained
much less PTFE debris after durability tests by the TMS 8 than that by H-
DLC. In the comparison of the SEM image at the contact area, the PTFE
surface after durability tests against H-DLC (Fig. 6j) shows an obvious
scratch which is similar to the morphology of H-DLC before the
durability test as shown in Fig. S12c. However, the PTFE surface after
durability tests against TMS 8 (Fig. 6i) does not show apparent scratches
and was more similar to the PTFE surface before the durability test
(Fig. 6h).
It was reported that adsorbed water molecules exist on the surface of
Si-DLC film as a SiOx(OH)y gel layer [35]. It is considered that the gel
layer can effectively reduce the friction and wear of Si-DLC film and
PTFE. In addition, it was found that the water contact angle of the
Si-DLC film (64.94º) was smaller than that of the H-DLC film (69.75º)
(Fig. S15). The more hydrophilic nature of the Si-DLC film results in
easier adsorption of water molecules onto its surface. These reasons
possibly contribute to the stable output and anti-abrasion properties of
Si-DLC-based TENG under water-lubricated conditions.
Both PTFE [67,68] and Si-DLC [69,70] have been applied to sliding
bearings and shown good thermal and tribological performance. A
thrust bearing equipped with self-driving speed sensing ability based on
Si-DLC-based TENG was fabricated to demonstrate the feasibility of
making durable self-driving sensing systems in machinery. The experi­
mental setup and specific structures are shown in Fig. S16 (detailed
fabrication methods are explained in Note S5). Firstly, the output cur­
rents of the device under dry and water-lubricated conditions were
compared, as displayed in Fig. S16c and d (Video S2). Apparently, the
output increased dramatically (approximately 3 times) under
water-lubricated condition. Then, the output under water-lubricated
condition for different speeds were obtained and the speed was

7
M. Gao et al. Nano Energy 105 (2023) 107997

Fig. 6. The durability tests of TENG under (a) dry and (b) water-lubricated conditions. (c) The COFs of TMS 8 and H-DLC-based TENG under unsubmerged water-
lubricated conditions. Observation of the surfaces of (d, e) TMS 8 films and (f, g) H-DLC films after being tested under (d, f) dry and (e, g) water-lubricated conditions.
(h) PTFE surface before durability test. PTFE surfaces after durability tests under water-lubricated conditions against (i) TMS 8 and (j) H-DLC.

measured by the peak number method and frequency method, respec­
tively [71]. From Fig. S16f-h, it can be found that both methods can
accurately measure the speed. This work presents a thrust bearing
equipped with self-sensing capability with Si-DLC-based TENG, and
shows application prospects in machinery.
Supplementary material related to this article can be found online at
doi:10.1016/j.nanoen.2022.107997.
3. Conclusion
In this study, an abrasion-resistant and high output Si-DLC-based
sliding-mode TENG was presented. Triboelectric experiments demon­
strated that the Si-DLC prepared with a source gas with an 80% TMS
ratio (TMS 8) had the greatest output. Raman analysis indicated that
TMS 8 had a more disordered structure and a higher sp3 bond ratio. The
permittivity of the film was found to increase with an increase in Si
content, which was beneficial for charge storage. Additionally, the
disordered structure of Si-DLC films provided more electron emission
sites, resulting in an enhanced electron-donating ability. The KFPM re­
sults also indicated that TMS 8 showed the lowest work function, which
evidenced the stronger electron-donating ability of TMS 8. Subsequent
triboelectric experiments under dry conditions agreed with the Raman
analysis and KFPM results. The optimal Si-DLC film also exhibited su­
perior tribological properties to other DLC films.
The experimental results under water-lubricated conditions indi­
cated that the Si-DLC-based TENG exhibited an enhanced output as well
as a lower COF. The reduction in COF is attributed to the formation of a
SiOx(OH)y gel layer on the surface of the Si-DLC films, as reported in
previous studies, which greatly improves the anti-abrasion performance
and, thus the durability and stability of the TENG by preventing the
transfer of a PTFE layer onto the Si-DLC surface.
The output voltage under unsubmerged water-lubricated conditions
was improved by a factor of more than 2.5 compared with that under dry
conditions. The experimental results obtained using different dielectric
materials under unsubmerged conditions revealed that the output
enhancement of the Si-DLC-based TENG is a result of the stronger
electropositivity of water.
Considering their advantageous mechanical properties of low fric­
tion, high durability, and ease of application to a mechanical system
without any structural change, Si-DLC films are very promising

8
M. Gao et al.
dielectric materials for sliding-TENGs. In particular, the Si-DLC-based
TENG under water-lubricated conditions shows a dramatic improve­
ment in durability and electrical output; hence, the Si-DLC-based TENG
has broad applicability as self-powered monitoring sensors in real me­
chanical systems.
4. Experimental section
4.1. Preparation of Si-DLC films
Si-DLC films were deposited using PBII&D on Al and Si plates with
thicknesses of 1 mm and 600 µm, respectively. A schematic diagram of
PBII&D is shown in Fig. S1. A gaseous mixture of TMS and toluene was
used as the source gas for the deposition of the Si-DLC film. The sub­
strates were ultrasonically cleaned with petroleum benzene, ethanol,
and acetone before film deposition. For comparison, H-DLC films were
also prepared using toluene as the source gas. According to deposition
parameters presented in Table S1, Si-DLC and H-DLC films used in this
study were prepared.
4.2. Experimental setup
The fabricated sliding-mode TENG is shown in Fig. S4. A commercial
reciprocating friction tester (FPR-2100, Rhesca) was used for the ex­
periments. An acrylic plate was used as the substrate, and thin Al tape
was pasted onto the acrylic plate (thickness is 1 mm) as an electrode.
Two pieces of polytetrafluoroethylene (PTFE) tape were paved onto the
Al electrodes. The thicknesses of PTFE and Al tapes are 90 µm. The H-
DLC and Si-DLC films were deposited on the upper Al electrode, which
was attached to an acrylic plate. The areas of the PTFE and DLC films
were 35 × 40 mm2 and 30 × 20 mm2, respectively. The reciprocating
stroke was 20 mm, and the gap between the two PTFE films was 4 mm.
The surface charge of the PTFE was reduced by rinsing the surface with
ethanol after each test [72].
A high-speed reciprocating friction tester (MFT5000, Rtec) was used
to simultaneously measure the friction coefficients and triboelectric
properties under water-lubricated conditions. Schematic diagrams of the
tests are shown in Fig. S5. The TENG output under dry conditions was
measured for comparison.
4.3. Characterization of materials
The thickness of H-DLC and Si-DLC films was measured by a surface
profilometer (SE500, Kosaka Laboratory), and their thickness was
1.1 µm. The roughness (Ra) of different H-DLC and Si-DLC films
deposited on Al was also measured with a surface profilometer, and they
were approximately 0.12 µm, which is the same as the roughness of the
Al substrate. The microstructure of the H-DLC and Si-DLC films was
analyzed using Raman spectroscopy (inVia Raman Microscope,
Renishaw). The surface morphologies of H-DLC and Si-DLC film after the
durability tests were observed by SEM (JSM-7800 F Prime, JEOL), and
the elemental information was surveyed by EDS, confirming the ele­
ments. KPFM (Park XE-7, Park Systems) was used to measure the surface
potential distribution and work function of Si-DLC films. The element
composition ratio of H-DLC and Si-DLC films was measured using
energy-dispersive X-ray spectroscopy (EDS, TM3030Plus Miniscope,
Hitachi High-Tech). A commercial spectroscopic ellipsometer (Five Lab,
MARY 102) was used to obtain the complex dielectric constant.
4.4. Electrical measurements
The short-circuit current, open-circuit voltage, and transfer charge
were recorded through an electrometer (6514, Keithley), and an oscil­
loscope (DSOX2014A, Keysight) was used to store the data measured
from the 6514 electrometer. Electrical current behavior at different
external loading resistances was measured by the SR 560 low noise
9
Nano Energy 105 (2023) 107997
current preamplifier.
CRediT authorship contribution statement
Mang Gao: Investigation, Conceptualization, Experimental conduc­
tion, Data curation, Formal analysis, Validation, Writing – original draft.
Soo-Bin Kim: Analysis, Validation, Writing – review & editing. Yahui
Li: Analysis, Validation, Writing – review & editing. Shreeharsha H.
Ramaswamy: Experimental guiding. Junho Choi: Conceptualization,
Methodology, Funding acquisition, Project administration, Resources,
Supervision, Writing – review & editing.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data Availability
Data will be made available on request.
Acknowledgments
This work was partially supported by JKA and its promotional funds
from KEIRIN RACE (Grant ID is 2021Ｍ－211). Gao was supported by
the Chinese Scholarship Council (CSC) for his doctoral program at the
University of Tokyo.
Appendix A. Supporting information
Supplementary data associated with this article can be found in the
online version at doi:10.1016/j.nanoen.2022.107997.
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M. Gao et al. Nano Energy 105 (2023) 107997

Mang Gao, received the B.S. degree in Petroleum Engineering Shreeharsha H. Ramaswamy obtained his Ph.D. degree in the
from Yangtze University (Jinzhou), China, in 2012. He ob­ department of Mechanical Engineering in 2021, The University
tained his master’s degree from Harbin Institute of Technology, of Tokyo, Tokyo, Japan. His research interests include
Shenzhen, China at the major of Mechatronic Engineering, and Tribology, Plasma coating, Thin films, Semiconductor Process,
currently he is pursuing the Ph.D. degree in the University of Triboelectric Nanogenerator.
Tokyo, Tokyo, Japan at the major of Mechanical Engineering.
His research interests include thin films, plasma coating, en­
ergy harvesting, durable Triboelectric Nanogenerator,
Diamond-Like Carbons, self-powered sensors and smart con­
dition monitoring system.

Soo-bin Kim, received Bachelor’s degree in 2018 and Master’s
degree in 2021 from the department of Mechanical Engineer­
ing, Korea University, Seoul, Korea. Currently, he is a Ph.D.
candidate in Choi’s laboratory, the Department of Mechanical
Engineering, the University of Tokyo, Tokyo, Japan. His
research interests include tribology, thin films, energy har­
vesting, renewable energy, and computational analysis.
Junho Choi, received Bachelor’s degree in 1994 and Master’s
degree in 1996 from Dept. of Metallurgical Engineering, Korea
University, Seoul, Korea. He obtained Ph.D. degree from Dept.
of Mechanical Engineering, The University of Tokyo in 2000.
Since 2010, he has been Associate Professor, Dept. of Me­
chanical Engineering, The University of Tokyo. His research
interests are surface engineering and tribology, including
plasma coating, triboelectric nanogenerator, diamond-like
carbon films, nano-carbon materials, and self-assembled
monolayers.

Yahui Li, received his M.S. degree in materials physics and

chemistry from Harbin Institute of Technology, and is currently
a Ph.D. candidate of electronic science and technology at
Shanghai Jiao Tong University. His research interests focus on
the energy harvesting and MEMS sensors.

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