Coaxial Triboelectric Nanogenerator and Supercapacitor Fiber-Based

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Coaxial Triboelectric Nanogenerator and Supercapacitor Fiber Based Self-Charging Power Fabric Yanqin Yang, Lingjie Xie, Zhen Wen, Chen Chen, Xiaoping Chen, Aiming Wei, Ping Cheng, Xinkai Xie, and Xuhui Sun ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.8b15104 • Publication Date (Web): 21 Nov 2018 Downloaded from http://pubs.acs.org on November 22, 2018

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ACS Applied Materials & Interfaces

Coaxial Triboelectric Nanogenerator and Supercapacitor Fiber Based Self-Charging Power Fabric

Yanqin Yang†, Lingjie Xie†, Zhen Wen†,*, Chen Chen†, Xiaoping Chen†, Aiming Wei†, Ping Cheng†, Xinkai Xie† and Xuhui Sun†,*

†

Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key

Laboratory

for

Carbon-Based

Functional

Materials

and

Devices,

Soochow

University, Suzhou 215123, China.

*Corresponding Authors E-mail: Z. Wen: [email protected]; X. Sun: [email protected]

ACS Paragon Plus Environment

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ABSTRACT To meet the urgent demand for rapid advancement of wearable electronics, challenges are still remained in developing wearable and sustainable power sources with simple fabrication and low cost. In this work, we demonstrate a flexible

and

coaxial

fiber

by

fabricating

one

dimensional

triboelectric

nanogenerator (TENG) outside and supercapacitor (SC) inside, which can not only harvest mechanical energy but also store energy in all-in-one fiber. In such coaxial fiber, carbon fiber bundles are utilized as the electrode material for TENG as well as the active and electrode material for SC. Meanwhile, silicone rubber is served as the separator between the SC and TENG, the triboelectric material of the TENG, and the encapsulation material for the whole fiber as well. Moreover, both of the SC and TENG exhibit good performance and stability, which ensures its long-term use in daily life. Due to the flexibility and durability of carbon fiber and silicone rubber, the proposed coaxial fibers show great flexibility, which could be further knitted as cloth to sustainably power


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wearable electronic devices. This work presents a promising platform for the wearable electronics as well as smart textile.

KEYWORDS:

coaxial

fiber,

self-charging

power

system,

triboelectric

nanogenerator, supercapacitor, wearable electronics


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INTRODUCTION Wearable electronics such as smart watch, smart glasses, e-skin, etc., have been attracting worldwide interests, which impose the urgent advancement for the matchable power sources.1-6 However, the traditional power sources, e.g. batteries, are relatively difficult to meet the wearable demand because of the hard structure, heavy packaging and possible environmental pollution.7-9 To address this issue, plenty of efforts have been committed into developing wearable power sources, especially textile-like power sources, such as lithiumion batteries and supercapacitors (SCs).10-17 Between the two devices, SCs exhibit distinctive advantages in high charging rate, long cycle life and longterm stability.18-19 Thus, SCs could be a more desirable choice for wearable power sources in daily life. One key challenge in the application of wearable SCs is that they need to be charged sustainably because of their high discharging rate and small capacity.20-22 Therefore, developing a sustainable and wearable energy harvesting device for charging the SCs continuously remains highly desired and challenge.


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Based on the coupling effect of triboelectrification and electrostatic induction, the

recently

developed

triboelectric

nanogenerators

(TENGs)

possess

the

advantages of light-weight, flexibility, simple structure, etc.23-26 Moreover, TENG is aimed at converting low-frequency and irregular mechanical energy into electricity so that a self-charging power system can be built by integrating TENG and SC together, which is very suitable to sustainably drive wearable electronics.27-29 Although some bulk-shaped self-charging power devices have already been reported, the package of them are relatively heavy which may not be compatible to human wearing.30-33 Developing the textile-like self-charging power system that can be fabricated into cloth may provide an ideal and simple strategy for wearable electronics. Nevertheless, the reported textile-like self-charging power systems in present literatures are always fabricated from TENG fibers and SC fibers separately, which to some extent make the fabrication process intricate and limit the application in wearable electronics.34-37 Herein, a self-charging power fiber is demonstrated by fabricating a one dimensional (1D) SC fiber inside and coaxial TENG fiber outside. By this


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strategy, energy harvest and storage can be achieved in just one integrated fiber. Taking advantages of good conductivity, specific capacitance characteristic and great flexibility, carbon fiber bundles are utilized as the electrode and active material of SC as well as the electrode material of TENG. SC and TENG in the fiber are separated by silicone rubber in between so that the mutual interferences are avoided. Silicone rubber also acts as triboelectric material of the TENG and encapsulation material of the coaxial fiber. The performances of the SC and the TENG in the fiber have been investigated independently to evaluate the corresponding capabilities. In addition, due to the flexibility of the whole fiber, a self-charging power textile was proposed by simply weaving the coaxial fibers together, which could sustainably drive the wearable

electronic

devices

easily,

presenting

the

promising

potential

in

wearable power sources and smart textile.

RESULTS AND DISCUSSION The fabrication process and mechanical properties of the coaxial TENG and SC fiber are illustrated in Figure 1. A typical coaxial fiber is fabricated by


6

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coaxially integrating energy storage device and the energy harvesting device in one fiber with supercapacitor inside and TENG outside (Figure 1a). Here, the carbon fiber bundles were utilized as the electrode and active material of supercapacitor due to the high conductivity and high energy storage capability. The inside supercapacitor was assembled in parallel from two electrodes which were pre-coated by H3PO4/PVA electrolyte (state ⅰ and ⅱ). Silicone rubber was employed to package the supercapacitor acting as the separator between supercapacitor and TENG (state ⅲ). Subsequently,


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Figure 1. Schematic diagram and mechanical properties of the coaxial TENG and SC fiber. (a) Fabrication process of the coaxial triboelectric nanogenerator and supercapacitor fiber. (b) Photograph of the prepared coaxial fiber (scale bar 1 cm). (c) Diameter of the single fiber. (d) The cross-sectional microscopy image of the coaxial fiber (scale bar 0.5 mm). (e) The distance between the two carbon fiber bundle electrode in the supercapaitor (scale bar 60 μm). Photograph of the coaxial fiber at (f) bending, (g) knotting, (h) enwinding states. TENG in the coaxial fiber was fabricated by means of winding carbon fiber bundles as electrode material over the supercapacitor fiber and coating silicone rubber outside as triboelectric material (state ⅳ and ⅴ). In consequence, a coaxial SC and TENG fiber can be obtained (Figure 1b). The specific fabrication process is depicted in the Experimental Section. The measured diameter of a typical coaxial fiber is ~2 mm (Figure 1c) which is the thinner compared with other reported TENG fibers listed in Table S1. Correspondingly, the cross-sectional microscopy image (Figure 1d) illustrates this coaxial fiber with the energy storage device (SC) inside and the energy harvesting device (TENG) outside. Figure S1 shows the SEM image of the carbon fiber bundles serving as the electrode of supercapacitor with the radius of about 72.65 μm


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while the single carbon fiber has the radius of about 3.72 μm. Here, silicone rubber layer acts as the separator to prevent the mutual influence between the SC and TENG. The SEM image shows that the carbon fiber bundle electrode is the collection of a large number of carbon fibers and the distance between the two carbon fiber bundles electrodes in the supercapacitor is about 54.23 μm (Figure 1e). To demonstrate the excellent flexibility of the coaxial fiber in complicated application conditions, the coaxial fiber under bending (Figure 1f), knotting (Figure 1g) and enwinding (Figure 1h) deformations are performed, which exhibits great potential in smart textile fabrication and wearable devices applications.


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Figure 2. Electrochemical performance of the SC in the coaxial self-charging power fiber. (a) CV curves of the SC at different scan rates (5-100 mV/s). (b) GCD curves of the SC at different current loadings (1-10 μA). (c) CV curves of the SC under different bending angles (0°-180°). (d) Long-term stability test of the SC for 6000 charging/discharging cycles; GCD curves of the SC during the course of cycling is shown as the inset. (e) Schematic illustration of the seriesconnection of the integrated SCs. (f) Photograph of a green LED lighted up by


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the 2 series-connected SCs. (g) GCD and (h) CV curves of the seriesconnected SCs with various number of single SC (1-4 SCs). The characterizations of the TENG and SC in the coaxial fiber were conducted

individually

to

evaluate

their

performances

respectively.

Cyclic

voltammetry (CV) and galvanostatic charging/discharging (GCD) techniques were employed to measure the electrochemical performance of the SC in the coaxial self-charging power fiber, as shown in Figure 2. The CV curves of a single SC are shown close to rectangular shape when examined at different scan rates ranging from 5 to 100 mV/s, and there is no significant distortion in the rectangular curves even at the high scan rate of 100 mV/s, which reflect great capacitive property and high-rate charging capability of the SC in the coaxial fiber (Figure 2a). Meanwhile, examined in the potential window from 0 to 0.8 V, the GCD curves of the SC are close to symmetrical triangle shape under the current load of 1-10 μA. It is observed that no evident ohm-drop happened in the GCD curves even when the discharging rate is 10 μA, which further reflects the excellent capacitance behavior and great conductivity of the carbon


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fiber electrode. When the current load is 5 μA, the discharging capacitance of the SC in the GCD analysis is about 62.5 μF, and the corresponding massspecific capacitance can be ~31.25 mF/g (Figure 2b). In order to apply such SC in the smart textile fabrication, the flexibility become an important concern. The CV curves of the SC bending at different angles from 0° to 180° show exactly same, indicating the excellent flexibility and stability of the SC in the coaxial fiber (Figure 2c). Figure S2 also illustrates the CV curves of the SC when knotting and enwinding where the curves match well with each other, further exhibiting the stability of the SC. Moreover, the cycling performance test has been conducted to further investigate the long-term durability of the SC. The capacitance still can maintain about 80% after charging and discharging for 6000 cycles at the current load of 5 μA (Figure 2d). Because of the low-current output of TENG in practical application, several SCs are connected in series (Figure 2e). The two series-connected SCs can easily light up a commercial LED after charging (Figure 2f and Movie S1), revealing the good performance of series-connected SCs. The CV and GCD curves of the series-connected SC


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with different number of units show that the voltage of the series-connected SCs increases almost linearly with the increasing units so that the wearable electronics with different required voltage can be driven accordingly, which indicates the adaptability of the SC in practical application (Figure 2g and h).

Figure 3. Electric performance of the TENG in coaxial self-charging power fiber for harvesting mechanical energy. (a) Working mechanism of the TENG in single-electrode mode. (b) Simulation result of the potential distribution of the TENG under open circuit condition using COMSOL software. Electrical output performance of single fiber of TENG including (c) transferred charge (Qtr), (d) open-circuit voltage (Voc) and (e) short-circuit current (I

sc).

(f) Output power of

the single fiber of TENG under different operation frequencies.


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The electric performance of the TENG in the coaxial self-charging power fiber for harvesting mechanical energy is shown in Figure 3. Such TENG works in single-electrode

mode

and

the

working

mechanism

is

based

upon

the

combination of triboelectrification and electrostatic induction effect (Figure 3a).3841

When the moving object (skin) touches the silicone rubber, because of the

diverse triboelectric polarities of these two materials, negative charges would be generated on the surface of silicone rubber while positive charges on the surface of the skin (ⅰ). Once the skin starts moving away from the silicone rubber, positive charges would be induced in the carbon fiber electrode due to the electrostatic induction effect. Thus, electrons would transfer from the carbon fiber bundle electrode to the ground, resulting in the current output (ⅱ). The electrons would stop flowing until a new electrical balance is established when the skin is separated far away enough from the silicone rubber (ⅲ). When the skin approaches the silicone rubber again, electrons would transfer in the opposite direction, generating a reverse current signal (ⅳ). Cycling contact and separation

would

generate

the

alternating

current


signals

continuously.

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Moreover,

to

more

quantitatively

understand

the

process

of

electricity

generation, COMSOL software was utilized to simulate potential distribution of the TENG under each motion step (Figure 3b). The basic electrical output performance of a typical TENG in the coaxial fiber under various motions frequencies (1-2.5 Hz) are shown in Figure 3c-e. Nylon film was utilized as the moving object with the surface area much larger than the TENG fiber so that the TENG fiber can be fully touched by the film. The short-circuit transferred charge (Qtr) and open-circuit voltage (Voc) of the device maintain at ~15.1 nC and ~42.9 V, respectively, almost unchanged under various motion frequencies. Meanwhile, the short-circuit current (Isc) of the device increases with the increasing frequencies with 0.19 μA at 1 Hz and 0.51 μA at 2.5 Hz. Compared with previous reported TENG fibers, the output performance of the coaxial is also comparable as shown in Table S1. Furthermore, the output power of the TENG is evaluated with the connection of different external load resistances ranging from 10-10000 MΩ (Figure 3f). Here, the output power P generated per cycle is obtained via V-Q test and the result can be calculated as


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P = V × Q × f (1)

where V is the voltage across the external load, Q is the transferred charge across the external load per cycle and f is the motion frequency. The output power increases with the increasing motion frequency and the maximum output power (~ 1.12 μW) can be achieved at 2.5 Hz. In addition, it can be observed that the optimum resistance decreases when the motion frequency increases, which is attributed to the decrease of the TENG impedance with the increase of the motion speed. Furthermore, for long-term application, we conducted the stability test for over 8000 cycles. As shown in Figure S3, the output performance of the TENG does not decrease significantly during the continuous contact and separation process which exhibits excellent stability resulting from closely-coating of silicone rubber with good durability and flexibility.


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Figure 4. Demonstration of coaxial TENG and SC fiber based self-charging power fabric in practical wearable electronics. (a) Photograph of the fabricated textile into cloth (scale bar 5 mm). (b) GCD curves of the SC in the coaxial fiber before and after washing for 3 times. (c) Transferred charge of the TENG in the coaxial fiber before and after washing for 3 times at operation frequency of 1.5 Hz. (d) Circuit diagram of the self-charging power system containing TENG, SC, rectifier and load. (e) Charging and working curve of two pairs of 4-series connected SCs by manually patting the coaxial TENG textile and (f) powering an electronic watch. To make effective use of this coaxial self-charging power fiber, several units were knitted together to make the fabric, as demonstrated in Figure 4a. In


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practical application of cloth, the launderability is a critical parameter for daily wearing so that washing test was conducted firstly in this work (Figure S4). The coaxial fiber was immersed in the water and we used a magnetic stirrer to simulate the washing process. It can be observed that there is no obvious change in the GCD curves of the SC part after washing for 3 times (Figure 4b) and the Qtr of the TENG part could remain relatively stable as well (Figure 4c), which ensures its longterm capability when woven into cloth. Figure 4d illustrates the working circuit diagram of the coaxial fiber. Here, TENG in this coaxial fiber would harvest mechanical energy from hand patting and generate alternating current signal while the SC acts as the energy storage unit. However, the alternating current (AC) generated by TENG cannot be directly stored in SC. So, before charging the SC, the rectifier was utilized here to convert AC into direct current (DC). The rectifier is commercially bought and is in relatively small size which could be designed into a logo in the cloth. Meanwhile, the flexible and transparent diode has been reported already.42 It is highly possible that flexible rectified could be fabricated and applied in wearable devices. Charging and discharging processes are controlled by the switches. When S1 is off and S2 is on, the SC would be charged by the TENG. When S1 is on and


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S2 is off, the electronic devices would be driven by the SC. Figure 4e shows the working curve of the fabric knitted from 8 coaxial fibers with two pairs of 4series-connected SCs. SCs could be charged when patting the fibers, however, when stop patting, a plateau of the voltage would be kept without the leakage, indicating the excellent performance and stability of the SCs. After charged to 2 V, the series-connected SCs can drive an electronic watch working, as demonstrated in Figure 4f and Movie S2. The charging efficiency of the SC from TENG in this self-charging power fabric is calculated in Note S1. Moreover, the charging efficiency of the SC from TENG could be greatly enhanced by introducing the reported power management units to the self-charging power system43-45.

CONCLUSION In summary, a coaxial fiber integrating SC and TENG has been successfully proposed for harvesting body motion energy and sustainably powering electronic devices. The diameter of the coaxial fiber is about 2 mm, and the SC with specific capacitance of 31.25 mF/g is fabricated inside the fiber, which shows


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excellent capacitive behavior and stability to be an energy storage device in the self-charging power system. Meanwhile, the TENG outside the fiber was fabricated with Voc of 42.9 V, Qtr of 15.1 nC, maximum Isc of 0.51 μA and maximum output power of 1.12 μW. Based on the coaxial fiber, the fabric can be simply woven as the power source of wearable electronics. By continuously patting the outside TENGs, the SCs inside can be charged and then drive the electronic devices. The single coaxial self-charging power fiber with the facile fabrication process presented in this work provides a simple and effective strategy for textile-like self-charging power system and exhibits the promising potential in application of smart textile and wearable electronics.

EXPERIMENTAL METHODS Fabrication of the coaxial TENG and SC fiber. The H3PO4/PVA gel electrolyte was first prepared by mixing 3 mL H3PO4 with 27 mL deionized water and then adding 3 g PVA powder into the solution. The mixture was kept stirring at 85 ℃ for about 6 h until the solution became clear. The prepared carbon fiber bundles with the weight of 2 mg and the length of 10 cm was


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immersed into 0.1 mL H3PO4/PVA electrolyte with one end of the bundles kept above the solution. After the solution became solid state (~ 12 h), another 0.1 mL H3PO4/PVA electrolyte solution was added onto the carbon fiber bundles and then solidified at room temperature. Since the shape of the carbon fiber bundles are closely to a cylindrical, after solidifying, the excrescent parts of the electrolyte were trimmed so as to keep the cylindrical shape. Subsequently, with two prepared fibers assembling in parallel, the fiber-shaped solid-state supercapacitor in the coaxial fiber was obtained. Silicone rubber (Smooth-on, Ecoflex 00-10, two components in a 1:1 weight ratio) was used for the package of supercapacitor. By pouring the liquid silicone rubber over the supercapacitor which was hung vertically, a uniform and thin film would be formed over the supercapacitor after solidifying in room temperature. Carbon fiber bundles (~ 20 mg) were winded over the silicone rubber-coated supercapacitor fiber tightly and uniformly. By coating the winded carbon fiber bundles with liquid silicone rubber, the TENG in coaxial fiber can be obtained after solidifying.


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Characterization and Measurement. A scanning electron microscope (SEM, Carl Zeiss Supra 55) was employed to investigate the morphology of carbon fiber. An optical microscope was employed to measure the cross-sectional view of the coaxial SC and TENG fiber. Electrochemical performance of SC including CV and GCD were measured by electrochemical workstation (CHI 760E) at room temperature. For electrical output performance of TENG, a linear motor was used to simulate human motions, providing contact and separation movement. A programmable electrometer (Keithley 6514) was adopted to test the open-circuit voltage, short-circuit current and transferred charge, respectively. The software platform (LabVIEW) was utilized for real-time data acquisition control and analysis. ASSOCIATED CONTENT Supporting Information The Supporting Information is available free of charge via the Internet at http://pubs.acs.org. Figure S1. a) SEM image of the carbon fiber bundle serving as the electrode of the supercapacitor. b) SEM image of a single carbon fiber.


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Figure S2. CV curves of the SC when (a) knotting and (b) enwinding. Figure S3. Short-circuit transferred charge of the coaxial fiber cycling for over 8000 cycles at the working frequency of 1.5 Hz. Figure S4. Photograph of washing test of the multifunctional coaxial selfcharging power fiber. Figure S5. The curve of accumulated charges generated by TENG after rectified. Table S1. Comparision of the coaxial fiber with other TENG fibers. Note S1. Efficiency calculation of the supercapacitor from TENG Movie S1. Lighting up a LED light using 2 series-connected SCs. Movie S2. Driving an electronic watch working using the self-charging power fabric.

AUTHOR INFORMATION Corresponding Author *Zhen Wen ([email protected]) *Xuhui Sun ([email protected]) Author Contributions Yanqin Yang and Lingjie Xie contributed equally to this work. The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript.


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Notes The authors declare no competing financial interest. Acknowledgement The work was supported by National Natural Science Foundation of China (NSFC) (No. U1432249, No. 61804103), National Key R&D Program of China (No. 2017YFA0205002), Natural Science Foundation of the Jiangsu Higher Education Institutions of China (No. 18KJA535001, No. 14KJB150020), Natural Science Foundation of Jiangsu Province of China (No. BK20170343), China Postdoctoral Science Foundation (No. 2017M610346), State Key Laboratory of Silicon Materials, Zhejiang University (No. SKL2018-03) and Nantong Municipal Science and Technology Program (No. GY12017001). This work was also supported by the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), the 111 Project and Joint International Research Laboratory of Carbon-Based Functional Materials and Devices. A patent has been filed based on the research results presented in this manuscript.


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Coaxial Triboelectric Nanogenerator and Supercapacitor Fiber-Based

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