Synergistic effect study of g-C3N4 composites for high-performance triboelectric nanogenerators
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Abstract
The energy harvesting crisis has caused great necessity for new energy technologies, among which triboelectric nanogenerators (TENGs) garnered global attention. Based on our previous research on a novel 2D material graphitic carbon nitride (g-C3N4), this work explores the influence of g-C3N4 hybrid dopants with Polydimethylsiloxane (PDMS) on the performance enhancement of TENGs. More specifically, systematic experiments with different ratios of hybrid dopants were conducted, including Ag nanowires with g-C3N4, carbon nanotubes with g-C3N4, and MXene with g-C3N4. The systematic and optimization studies showed that carbon nanotube/g-C3N4 at the optimal ratio of 1:1 in PDMS composite presented an open circuit voltage (Voc) at 122 V, a short circuit current (Isc) at 5.8 μA, and a charge transfer (Qsc) at 105 nC, while Ag/g-C3N4 at the ratio of 3:1 with
Keywords
INTRODUCTION
The world is in constant pursuit of sustainable energy sources. Sustainable and net carbon emission power sources are playing a thriving role due to booming energy consumption in the new era[1]. Promising alternatives for powering wearable devices such as piezoelectric nanogenerators (PENGs), pyroelectric nanogenerators, moisture electric generators, triboelectric nanogenerators (TENGs)[2], tribovoltaic nanogenerators (TVNGs) have presented high output performance, environmental friendliness, self-power capability for various applications, etc. Among these, TENGs are a technology that holds tremendous promise including low cost[3], simple fabrication, high efficiency, versatile structural designs[4], diversity of material selection, sustainability[5], etc.
A TENG is a device that harnesses the triboelectric effect, a phenomenon where a material gains or loses electrons when it contacts a different material, generating a charge difference. By leveraging this effect, TENGs can convert mechanical energy from everyday activities such as walking, running, typing, or natural movement including wind and tide, into electrical energy[6]. This technology is incredibly innovative, highly reliable, and long-lasting, making it ideal for use in wearable devices[7]. The potential applications of TENGs are from powering electronic devices to capturing energy from humans or the environment. Hence, extensive effort has been made to design and fabricate self-powered sensors, sustainable energy sources, and wearable intelligent systems through the approach of nanogenerators.
Polymers usually obtain low dielectric constant and hence possess low capacitance, and low charge abstaining capacity for being addressed as TENGs, especially during application with other electronic devices. Polydimethylsiloxane (PDMS) is a bio-friendly, non-toxic, flexible, highly durable, translucent,
In the context of TENGs, doping is used to enhance the triboelectric properties to generate electrical energy through the triboelectric effect of PDMS. The simplest option is the introduction of high-dielectric ceramic materials such as BaTiO3 or SrTiO3[10] into the polymer matrix which inherently possesses a comparatively low dielectric constant. Also, some other dopants such as MXene, carbon nanotubes (CNTs)[11], metal nanoparticles[12], and two-dimensional (2D) materials[13] have been widely adopted and researched. The goal of doping PDMS in TENGs is to increase its ability to generate electrical energy and improve its other functions such as stability, durability, flexibility, transparency, etc., thereby enhancing its overall performance. By optimizing the doping process and concentration ratio, significant improvements in the efficiency and output of TENGs can be achieved, making them a more practical and feasible solution for energy application[14].
Two-dimensional materials are attractive for fabricating flexible and lightweight or multifunctional TENG devices. The triboelectric properties of graphene or graphene oxide and different transition metal dichalcogenides (TMDs) have been studied previously[15]. As a novel 2D material-graphitic phase carbon nitride which has sp2 hybridized carbon nitrogen bonding similar to graphene, graphitic carbon nitride
Based on our previous work of novel 2D material g-C3N4, we further studied different g-C3N4 composites with various dopants innovatively, such as CNTs, silver metal nanoparticles, MXene, and silver oxide (AgO), at different concentrations and ratios to optimize the electrical output of hybrid dopants and originally summarize the generality with varying combinations of dopants. In this research, we individually co-doped g-C3N4 with four different substances, focused on the characterization of Ag/g-C3N4 PDMS composite and optimized electrical performance at proper ratios for Ag/g-C3N4 PDMS TENG and
RESULTS AND DISCUSSION
Fabrication and characterization
Figure 1A shows the schematic fabrication of TENGs incorporating hybrid dopants. Taking Ag/g-C3N4 PDMS as an example, after adding both silver and g-C3N4 nanoparticles into a PDMS solution, the molecular structure manifests as 2D framework, wherein each hexagonal unit of the g-C3N4 lattice encapsulates a single silver atom, facilitating synergistic interaction with increased conductivity, electron mobility, and more Qsc[17]. Then, the hybrid dopant PDMS composite was prepared using the blade-coating method, as illustrated in Figure 1B. The dopants included g-C3N4 powders combined with one of the following materials: Ag nanoparticles, MXene powders, nickel-coated CNTs, multiwall CNTs, or AgO, at different weight ratios. Figure 1C demonstrated the architecture of basic contact-separation mode TENGs, where the copper-nickel conductive fabric (CNF) acted as both positive dielectric and electrode, along with hybrid dopant/PDMS composite as negative dielectric, and the two dissimilar dielectric films were positioned facing with each other.
Figure 1. Illustration of fabrication of TENGs with hybrid dopants (taking dopants silver nanoparticle and g-C3N4 powder as an example). (A) Mixing of PDMS, silver nanoparticles, and g-C3N4 powders; (B) Blade coating of the mixture; (C) Structure of TENG; (D) XRD pattern of g-C3N4 powder; (E) FTIR spectra for PDMS composites with different ratios of Ag/g-C3N4; (F) Raman spectra of a sample with 1 wt. % Ag/g-C3N4 dopant at different proportions in PDMS composite; (G) SEM of Ag/g-C3N4 PDMS composite and EDS mapping of elements. TENGs: Triboelectric nanogenerators; PDMS: polydimethylsiloxane; FTIR: fourier transform infrared spectroscopy; EDS: energy dispersive X-ray spectrometry; XRD: X-ray powder diffraction; SEM: scanning electron microscopy.
As CNTs were commonly used and had similar components with g-C3N4, we focused on the characterization of Ag/g-C3N4 PDMS composite. The X-ray diffraction analysis (XRD) of g-C3N4 powder was executed, as shown in Figure 1D, where a significant peak at 28° is indexed to crystalline phase g-C3N4. Surface functional groups were investigated by Fourier transform infrared spectroscopy (FTIR) where PDMS composite with different ratios of silver nanoparticles and g-C3N4 powders showed a similar pattern, as shown in Figure 1E, mainly showing the peaks of PDMS functional groups. Typical peaks of Ag nanoparticles at 2,921 cm-1 and 1,029 cm-1 were marked in the FTIR pattern. Typical peaks of PDMS included ~3,000 cm-1 of CH3, ~1,250 cm-1 of Si-CH3, ~1,000 cm-1 for Si-O-Si, and ~750 cm-1 of Si-CH3. Generally, g-C3N4 showed a sharp absorption at ~807 cm-1 where we could identify a peak around
The Raman spectrum of g-C3N4 typically displayed a peak at around 800-900 cm-1 which was attributed to the in-plane stretching vibration of the carbon-nitrogen bonds, and another peak at around 1,300-1,400 cm-1 which was related to the out-of-plane bending mode of the nitrogen atoms[18]. Additionally, there might be peaks at higher frequencies (above 1,600 cm-1) associated with the stretching modes of the carbon atoms in this material[19]. The Raman spectrum of Ag typically showed several peaks corresponding to different vibrational modes of the Ag atoms or molecules in the sample, which could be divided into two categories. The first one was related to the translational and rotational vibrations of the Ag atoms, which were usually observed in the low-frequency region below 400 cm-1. The second category corresponded to the vibrational modes of the molecules or clusters[20], and typically appeared in the high-frequency region above 400 cm-1. The most prominent peak in the Raman spectrum of Ag was typically associated with the longitudinal optical phonon mode (LO) at around 400 cm-1[21]. It could be seen from Figure 1F that with the rise of Ag concentration, the band in the Raman spectrum had increased significantly. Other notable peaks in the Raman spectrum of Ag included the transverse optical phonon mode (TO) at around 430 cm-1, the
The X-ray Photoelectron Spectroscopy (XPS) analysis [Supplementary Figure 1] was also conducted to observe constituent elements of Ag/g-C3N4 PDMS composite. From XPS spectra, apart from the constituent C and N elements, the presence of Ag could also be observed in the spectrum of the Ag/g-C3N4 PDMS composite[23]. Because of the low concentration of doping, the N and Ag peaks were not significant. The existence of Ag nanoparticles and g-C3N4 nanosheets in PDMS might lead to a strong interaction between two materials due to the intimate attachment of the two materials, and N could donate the lone pair of electrons to the outermost orbital of Ag.
Mechanism
The schematic diagrams manifested the detailed working principle of a triboelectric device using the hybrid doped PDMS composite film as negative and CNF as positive triboelectric materials, respectively. From the first stage [Figure 2AI] where there was no electron transfer and electrode potential, the applied impact force [Figure 2AII] separated the two dielectrics, and then electrification induced the corresponding charges, which caused the charges to transfer from one electrode to another to balance the increased electric potential from decreasing capacity [Figure 2AIII]. While approaching, the charges returned from the positive to the negative electrode for the increasing capacity and form an opposite voltage and displacement current [Figure 2AIV]. The process of repeated contact and separation thus generated continuous alternating current (AC). The electric potential distribution was also simulated using COMSOL software to show the electricity-generating process, as shown in Figure 2B. Figure 2C demonstrated a rectifier as an electronic device that converted AC into direct current (DC) with consistent polarity using one or more
Figure 2. (A) (I-IV) Schematic diagrams of the working principle of contact and separation mode TENG; (B) Simulation results of electrical potential distribution by COMSOL Multiphysics software; (C) Equivalent circuit of a self-powered system TENG, capacitor, another device, and rectifier changing AC to DC; (D) Two opposite electric peaks during a single circle of contact and separation; (E) Schematic structure of dopant/PDMS TENG. TENGs: Triboelectric nanogenerators; AC: alternating current; DC: direct current; PDMS: polydimethylsiloxane.
where σ is the triboelectric charge density on the dopant/PDMS surface, Δσ is the charge density transferred between electrodes, ε0 is the vacuum permittivity, and εdopant/PDMS denotes the relative permittivity of the dopant/PDMS composite, dgap stands for the inter-layer spacing, and ddopant/PDMS is the thickness of dopant/PDMS film. During open circuit conditions, the Qsc is zero, indicating that Voc is maximum when the gap reaches maximum and Voc has no explicit dependency on the properties of triboelectric layers; however, σ surface charge density is related to the dielectric constant of the triboelectric material[26].
Electrical qutput
To evaluate the triboelectric performance, the hybrid dopant/PDMS film was adhered to CNF to form the negative part, and the positive part was only CNF acting as both triboelectric material and electrode, which was then contacted and separated under an impact force of 100 N at a frequency of 3 Hz with an effective area of 4 cm2. The CNF electrodes were connected through copper wire and then to the electrometer to measure and collect signals of Voc, Isc and Qsc. Different ratios of Ag/g-C3N4 PDMS TENG and
Figure 3. Electric performance of TENGs with hybrid dopants. (A) Open circuit voltage; (B) Short circuit current; and (C) Charge transfer of TENG with different ratios of carbon nanotube and g-C3N4 at a total weight proportion of 1 wt. %; (D) Open circuit voltage; (E) Short circuit current; and (F) Charge transfer of TENG with different ratios of Ag nanoparticles and g-C3N4 at a total weight proportion of 1 wt. %. TENGs: Triboelectric nanogenerators.
Based on our preliminary experimental results, the triboelectric performance increased significantly from dopant concentration 5 wt. % to 5 wt. %, so we selected the total doping content at 1 wt. % for practicality and comparability, which was each sample containing 9-gram elastomer, 1-gram curing agent, and 0.1-gram dopants in total.
The group of CNT and g-C3N4 dopants was composed of a different ratio for each sample, which were 0.1 g CNT, 0.075 g CNT+0.025 g g-C3N4 (3:1), 0.05 g CNT+0.05 g g-C3N4 (1:1), 0.025 g CNT+0.075 g g-C3N4 (1:3), and 0.1 g g-C3N4, respectively, with electric performance Voc shown in Figure 3A, Isc in Figure 3B, and Qsc in Figure 3C. The TENGs with hybrid dopants showed higher values of three parameters - Voc, Isc, and
For another group of dopants Ag and g-C3N4, the dopant weight proportions were 0.1 g Ag, 0.09 g Ag+0.01g g-C3N4 (9:1), 0.075 g Ag+0.025 g g-C3N4 (3:1), 0.05 g Ag+0.05 g g-C3N4 (1:1), 0.025 g Ag+0.075 g g-C3N4 (1:3), 0.01 g Ag+0.09 g g-C3N4 (1:9), 0.1g g-C3N4, each for 10 g PDMS mixture, respectively. The optimum concentration ratio of Ag:g-C3N4 was 0.075:0.025 (3:1), resulting in a peak-to-peak Voc of 92 V [Figure 3D], Isc of 4.6 μA [Figure 3E], and Qsc of 49 nC [Figure 3F], which was more than four times higher than that of either pure Ag or pure g-C3N4, approximately. When Ag nanoparticles and g-C3N4 powders were co-doped into PDMS, the doping ratio influenced the permittivity, potential difference, and triboelectric charge. However, an excessive amount of filler might lead to leakage current through the conduction path through the capacitive effect[30]. Therefore, a suitable doping ratio was necessary to achieve optimal TENG performance.
Influence of external factors
The performance of TENGs can be influenced by frequency or external force, so we have evaluated the
Figure 4. (A) Open circuit voltage; (B) Short circuit current; (C) Charge transfer at different frequencies from 1 Hz to 6 Hz; and (D) Open circuit voltage; (E) Short circuit current; (F) Charge transfer at different impact forces of 10 N, 50 N, 100 N, and 200 N, respectively.
As discussed above, when the frequency increased, the current of TENGs also increased while the charge and voltage changes were relatively small. This phenomenon could be mainly due to the capacitive nature of TENGs, where the electric charge stored on the TENG surface increased with the frequency but the voltage across the TENG remained relatively constant[31]. As a result, the current generated by the TENG increased with frequency, leading to an enhancement in its electrical output. Moreover, the overall performance of the TENG also depended on other factors, such as material properties, surface roughness, operating conditions, and surrounding environment parameters including temperature, humidity, etc.
Applications
The output power density was evaluated by connecting with different external load resistances from 1 Ω to 500 MΩ at a working frequency of 3 Hz and force impact of 100 N. It can be noted that the current decreased as the resistance increased. Then, the instantaneous peak power density of TENGs can be calculated by P=I2R/S, where P, I, R, and S denoted power density, output current, resistance, and size. The peak power density achieved maximum of 1.45 W/m2 for Ag/g-C3N4 PDMS TENGs at the resistance of
Figure 5. The instantaneous peak power density of (A) Ag/g-C3N4 PDMS TENG (B) CNT/g-C3N4 PDMS TENG at a series of external resistance loadings and the corresponding current output; (C) The equivalent circuit of charging capacitance and photographic demonstration; (D) Durability study for Ag/g-C3N4 PDMS TENG after (1) 100, 500, 1,000, 5,000, 10,000, and 20,000 cycles, respectively, as well as (2) 0 h, 1 h, 5 h, 1 day, 2 days, 10 days, respectively; (E) Applications of Ag/g-C3N4 PDMS TENG as self-powered wearable sensors. TENGs: Triboelectric nanogenerators; PDMS: polydimethylsiloxane; CNT: carbon nanotubes.
Subsequently, with a multichannel data acquisition system, the self-powered electric output via touch could recognize the tactile trajectory and detect the pressure distribution. A circular PDMS film was divided into eight equal segments with alternating conductive foil 1-4 to four channels for independent signal capture. Touching these sections activated a single electrode TENG, which could generate a voltage pulse (> 60 mV) in the corresponding channel while producing negligible signals in non-contacted channels [Figure 6A], enabling real-time touch localization through electronic signal tracking [Figure 6B]. Two round TENGs were also integrated into an insole at the front and back to monitor the center of gravity and analyze gait for posture correction using multichannel signal acquisition and processing. Voltage outputs, as depicted in Figure 6C, indicated a higher peak at the front TENG when weight was forward, and conversely, a higher rear TENG signal when weight shifted backward, as shown in Figure 6D. Balanced weight distribution resulted in nearly equal TENG signals, with average values and the insole's structure [Figure 6E]. Based on a digital multimeter with Bluetooth module and filter circuit module, the real-time signal generated by our TENG can be transferred wirelessly to personal mobile devices and displayed on software application functional interface [Supplementary Video 2].
Figure 6. (A) Bar chart comparison of average sensing signals for a four-channel pressure sensing system, inset is the pattern illustration and real picture; (B) Sensing signal patterns by the sequence of pressing channels 1, 2, 3, and 4 in succession sequentially; (C) Signal pattern of the two-TENG insole while walking with the center of gravity at the front; (D) Signal pattern of the two-TENG insole while walking with the center of gravity at the back; (E) Bar chart comparison of average sensing signals while walking with center at the front, center at the back, and center at the middle, respectively, inset is the photo of the double-TENG insole. TENGs: Triboelectric nanogenerators.
EXPERIMENTAL
Materials
The silicone elastomer base and related curing agent for PDMS (SYLGARD® 184) were bought from Dow Chemical Company (USA). PDMS was fabricated by elastomer and curing agent with a ratio of 10:1. Stainless steel yarns (SSYs, Bekinox AISI 316L) were purchased from Bekaert (Belgium). CNF was purchased from 3M. CNTs, MXene, Ag, and AgO nanoparticles were from Dieckmann Company, and
Fabrication of g-C3N4 hybrid PDMS composite
Taking Ag nanoparticles and g-C3N4 powders as an example, two dopants were mixed at a certain ratio and added into the PDMS liquid homogeneously; after thorough ultrasonication for more than 12 h, 1 gram of curing agent, and 9 grams of PDMS liquid were added into the mixture and stirred for 20 min. Subsequently, the mixture was transferred to a mold and spread evenly across the blade surface to avoid air bubbles into the mixture, and then kept in a desiccator under a vacuum oven at 80 °C for 12 h to form a
Assembly of PDMS TENG
PDMS was adhered to CNF to form the negative part and further cut into a square of 4 cm2, and another piece of CNF was cut into the same size square as the counterpart acting as both tribomaterial and electrode, which was then contacted and separated. Finally, they adhered separately to two pieces of acrylic substrates for the triboelectric performance tests. The CNF electrodes were connected through copper wire and then to the electrometer to measure and collect signals of Voc, Isc and Qsc.
Characterization and measurement
Fourier transforms infrared (FTIR) absorption spectra were recorded on a spectrometer (Spectrum 100, Perkin Elmer). The Raman spectra were acquired using a NomadicTM Raman 3-in-1 microscope with 532 nm lasers. The XRD patterns were recorded on an X-ray diffractometer (D8 Advance, Bruker) with Cu Kα radiation to identify the crystalline phase. A Field Emission Scanning Electron Microscope (SEM, Tescan MIRA) was used to characterize the morphology and Energy Disperse Spectroscopy (EDS) data was acquired simultaneously. XPS spectra were investigated on an ESCALAB210 spectrometer. The output performance under impacting/releasing cycles was evaluated by utilizing a button/key durability life test machine (ZX-A03, Zhongxingda, Shenzhen) equipped with a self-configuring digital indicator (Interface 9860) to control the applied force at the precision of 0.1 N and range of 999 N. The output voltage signal was collected by Keysight DSO-X3014A oscilloscope and N2790A high voltage probe with 8 MΩ internal resistance. Voc and Isc were measured using an electrometer system Keithley 6514.
CONCLUSIONS
In summary, the hybrid dopants/PDMS composites were designed and prepared by embedding nanoparticles into the PDMS matrix, and experiments on ratio optimization with different hybrid dopants were carried out. Ag/g-C3N4 at the ratio of 3:1 at 1 wt % in PDMS composite manifested the best electrical properties with Voc of 92 V, Isc of 4.6 μA, Qsc of 49 nC, under 100 N and 3 Hz, and the optimized composite TENG reached output power density of 1.45 W/m2. Similar to that of Ag/g-C3N4, CNT/g-C3N4 PDMS TENG presented the optimal mixture ratio at 1:1 to achieve the best electric performance of Voc at 122 V, Isc at 5.8 μA, and Qsc at 105 nC. Other groups of hybrid dopants including AgO/g-C3N4 and MXene/g-C3N4 were also evaluated. TENGs made from PDMS were flexible, resistant, and durable, which could be applied in wearable electronics and positioned at various joint parts of the human body. When connected to multichannel acquisition and signal processing devices, we designed a novel disc device that detected pressure at different locations and an insole that tracks the center of gravity of the gait to correct the walking posture. Our TENG could convert mechanical energy from human motion into electrical energy, providing energy sources and self-powered sensors for wearable devices. This work provided insights and a promising avenue for boosting the electrical output and practical applications of TENGs.
DECLARATIONS
Acknowledgments
The first author would like to acknowledge The Hong Kong Polytechnic University for providing postgraduate scholarship.
Authors’ contributions
Substantial contributions to conceptualization, methodology, investigation, experimentation, data analysis and interpretation, and writing of the original draft: Xiao, Y.
Resources, methodology: Lu, J.
Supervision, writing review and editing: Xu, B.
Availability of data and materials
The data of the findings in this study are available from the corresponding author upon reasonable request.
Financial support and sponsorship
None.
Conflict of interest
All authors declared that there are no conflicts of interest.
Ethical approval and consent to participate
Not applicable.
Consent for publication
Not applicable.
Copyright
© The Author(s) 2025.
Supplementary Materials
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Xiao, Y.; Lu, J.; Xu, B. Synergistic effect study of g-C3N4 composites for high-performance triboelectric nanogenerators. Energy Mater. 2025, 5, 500057. http://dx.doi.org/10.20517/energymater.2024.155
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