$SSOLHG6XUIDFH6FLHQFH Contents lists available at ScienceDirect Applied Surface Science journal homepage: www.elsevier.com/locate/apsusc Full Length Article High contact surface area enhanced Al/PDMS triboelectric nanogenerator using novel overlapped microneedle arrays and its application to lighting and self-powered devices ⁎ C.K. Chung , K.H. Ke Department of Mechanical Engineering and Center for Micro/Nano Science and Technology, National Cheng Kung University, Tainan 701, Taiwan A R T I C L E I N FO A B S T R A C T Keywords: Triboelectric nanogenerators TENG Mechanical energy CO2 laser Microneedle Morphology One key to enhance the output performance of triboelectric nanogenerators (TENG) is how to increase the effective contact area that strongly depends on the feature morphology and pattern density. Conventional morphologies of TENG including pyramids, cubes, lines, pillars, and domes with insufficient feature surface area are generally fabricated using an expensive-and-time-consuming lithography and etching process. Here, we propose a novel morphology of overlapped microneedles (OL-MN) arrays for high total contact surface area to enhance the output performance of aluminium/polydimethylsiloxane (Al/PDMS) TENG under low operation frequencies using hand tapping. Two kinds of separate low-density and high-density microneedles arrays, namely LD-MN and HD-MN, are comparatively studied. The integrated process of low-cost CO2 laser ablation and PDMS casting is used for rapid prototyping. The OL-MN has the highest total contact surface area compared to the LD-MN and HD-MN at the constant laser power and scanning speed. The output performance of opencircuit voltage (Voc) and short-circuit current (Isc) of OL-MN-TENG are 123 V and 109.7 μA those are 3.66 and 3.71 times the Voc and Isc of LD-MN-TENG, respectively. The excellent OL-MN-TENG can light on 103 LEDs connected in series and store energy in capacitors for application to various self-powered devices. 1. Introduction With the development of global economy, green energy is an essential strategy for all countries in the future because the current fossil fuels have the limitation and shortcomings. The scientists are actively seeking environmentally friendly and sustainable green energy [1–4]. Current advances in various energy harvesters including the thermoelectric, solar, piezoelectric and triboelectric effects are used to store the converted electricity in capacitors for the self-powered electronic devices [5–8]. The triboelectric nanogenerators (TENG) are of sustainable energy, environmentally friendly, and for harvesting pluralistic mechanical energy. It can produce the converted electric performance from a wide range of daily mechanical energy, such as vibration, rolling, and sliding [9–12]. Therefore, the TENG as a new green energy has attracted great attentions because of the simple mechanical-electrical energy conversion for potential applications to commercial products [13–18]. The TENG may harvest the amount of mechanical energy that exists below 5 Hz from the human activities such as walking, shaking and hand tapping. Increasing the output performance of TENG is helpful for enlarging more applications. Different techniques ⁎ including the chemical treatment of surfaces [19,20] physical modification of surface morphology [21–26] are used for improving the performance. The strategy of chemical treatment is to control the chemical composition of material for enhancing the triboelectric polarity difference between two tribo-layers while the physically modified surface morphology is to adjust the contact area and surface roughness of triboelectric layer for generating more triboelectric charge during friction under a constant force and frequency. Moreover, the fabric based surface-embossed polydimethylsiloxane (PDMS) TENG has higher output performance than the flat PDMS one [27]. Therefore one key to enhance the output performance of TENG is to increase the effective contact area that strongly depends on the feature morphology and pattern density. From partial contact to full contact, the featured morphology can increase the effective contact area and triboelectric charge for enhancing output performance [28–33]. Conventional morphologies of TENG such as nano line, cube, pyramid [23], nano pattern [29], nano pillar and dome [25], and micro pillar [22] are operated under low frequencies below 5 Hz and with insufficient feature surface area. For comparison, the output performance of opencircuit voltage (Voc), short-circuit current (Isc), and current density (Jsc) Corresponding author. E-mail address: ckchung@mail.ncku.edu.tw (C.K. Chung). https://doi.org/10.1016/j.apsusc.2020.145310 Received 14 November 2019; Received in revised form 23 December 2019; Accepted 6 January 2020 $YDLODEOHRQOLQH-DQXDU\ (OVHYLHU%9$OOULJKWVUHVHUYHG $SSOLHG6XUIDFH6FLHQFH C.K. Chung and K.H. Ke Table 1 Comparison of surface morphology, materials, fabrication methods, operation condition, and electrical characteristics. Morphology Materials Fabrication method Operation condition Electrical characteristics Voc (V) Pyramid Line Cube Nano pattern Textile Nano-pillar Nano-Dome Micro pillars Isc (μA) Lighting (LEDs) J (μA/cm ) ITO/PET-PDMS/ PET/ITO Photolithography, etching Linear motor 18 0.7 0.13 Pyramid > Cube > line > flat film Ag/PDMS-ZnO/Ag [23] Mechanical force stimulator (10 kgf) 130 N 3 Hz 10 N 5 Hz Hand tapping, 3 Hz Hand tapping, 3 Hz 120 65 – 60 83 72 2.5 3.2 8.3 – 102.8 33.6 43.1 29.5 1.5 0.98 53 18 Microneedle LD-MN Al/PDMS/Al Al/PDMS/Al Chemical treatment, dipcoating ICP etcher, Thermal oxidation Soft lithography plasma treated CO2 laser ablation CO2 laser ablation HD-MN Al/PDMS/Al CO2 laser ablation Hand tapping, 3 Hz 110.4 62.7 2.09 91 OL-MN Al/PDMS/Al CO2 laser ablation Hand tapping, 3 Hz 123 109.7 3.6 103 Au/PDMS/Au Al/PDMS/Al of TENG follows the ascending order of flat film < line < cube < pyramid [23]. For instance, the voltage and the current of the pyramid TENG forced by a linear motor are 18 V and 0.7 μA, and corresponding to the Jsc of 0.13 μA cm−2, which is almost 5–6 times enhancement compared with the flat film [23]. Besides, the Voc and Isc of the nano dome TENG are 83 V and 3.2 μA, while the Voc and Isc of the nano pillar are 60 V and 2.5 μA, using a force of 130 N at 3 Hz [25]. The Voc and Isc of the micropillar aluminium (Al)/PDMS TENG increases from 42 V to 72 V and 4.2 μA to 8.3 μA, respectively, after the argon plasma treatment, using 10 N at 5 Hz [22]. Table 1 lists the comparison of TENGs with various feature-morphology structures. In brief, most structures of lines, cubes, pyramids, pillars, domes and various micro-nano patterns generally have some fabrication limitations including complicated, time-consuming, and high-cost lithography and etching process. Also, the materials of high-cost Au and Ag, and brittle ITO are highly selected as the electrode layer. Recently, Trinh and Chung proposed a unique microneedles (MN) array introduced into TENG [30] as MN-TENG to enhance performance through a bending–friction–deformation (BFD) behavior in the contacting and friction. The Al-PDMS MN-TENG can easily generate the bending, friction and deformation between the microneedles and Al under the applied force. It occurs not only between top Al electrode and PDMS MN but also more strongly between the MN and MN together with the MN and PDMS substrate during pressing state for enhancing effective contact surface area and performance. The BFD behavior is related to the density and total contact surface area of MN morphology to influence the output performance of Al/PDMS TENG. The separated microneedles array in [30] with low-to-medium pattern density of 159–388 MN/cm2 has a maximum output performance of 102.8 V (Voc) and 43.1 μA (Isc). Comprehensive research on promoting the output performance of the separated pattern array is lacking. It is of thus interest to study if there is some MN pattern array for more effective contact area to benefit the output performance. In this article, we propose a simple and innovative overlapped MN array method to increase the total effective contact surface area of TENG for enhancing output performance under low operation frequency using hand tapping. Moreover, the integrated process of lowcost CO2 laser ablation and PDMS casting is used for rapid prototyping. Two separated array types of the microneedle density with low density (LD-MN, 229 MN/cm2) and high density (HD-MN, 433 MN/cm2) are used as references for comparison with the overlapped microneedle density (OL-MN, 654 MN/cm2) fabricated at the constant laser power and scanning speed. The feature density of OL-MN is 2.85 time LD-MN and 1.51 time HD-MN, respectively. The total surface area calculated is 17.6 × 103, 19.94 × 103 and 22.91 × 103 mm2, respectively, for the LD-MN, HD-MN, and OL-MN as listed in Table 2. The OL-MN-TENG Ref 2 [29] 75 – [25] [22] [30] This article This article This article exhibits the best performance of Voc and Isc for 123 V and 109.7 μA, respectively, those are 3.66 and 3.71 times the Voc and Isc of LD-MNTENG, respectively. The OL-MN-TENG can light on 103 LEDs connected in series and charge a 0.47 μF capacitor above 2.0 V in 3.6 sec. The OLMN-TENG merits with good mobility and sustainability that is suitable for self-powered devices. Various self-powered devices are demonstrated including the self-powered e-watch for portable electronic devices, the self-powered buzzer as a safety sound for seeking help in emergency, the ME-NCKU LEDs flickering as an advertising board for communication and the self-powered humidity sensor for potential environmental Internet of Things (IoT) sensors network which is estimated that in 2020, there will be trillions of sensor units distributed on the earth [31]. 2. Experimental procedures 2.1. Design and fabrication of the separated and overlapped microneedle array Fig. 1 shows the schematic diagram of the separated and overlapped master mold of polymethyl methacrylate (PMMA) fabricated by CO2 laser ablation. The low-cost commercial CO2 laser (VL-200, Universal Laser System Inc., USA) of 10.6 μm in wavelength has a maximum power of 30 W and a maximum scanning speed of 1140 mm/s. The integrated system with the CorelDraw software was used for controlling CO2 laser parameters. The linear separated and overlapped array of PMMA master mold was related to the ablated spacing (Fig. 1(a)). The spacing (S) is dependent on pulse per inch (PPI) under the relationship of S = 25,400 (μm)/PPI. Because of the same power and speed, the spot radius (R) is the same. When the spacing is greater than the sum of the two radius (S > 2R), it will be separated; and if S < 2R it will overlap, as shown in Fig. 1(a1–a2). The interspacing between rows and rows is non-overlapped (Fig. 1(a3–a4)) while the cross section of the separated and overlapped ones is shown in Fig. 1(b). Fig. 2 shows the schematic fabrication flow of the overlapped microneedles arrayed PDMS and the assembly of Al/PDMS MN-TENG. The completed female PMMA master mold (Fig. 2(a)) is used for the casting of PDMS with the solution (Sylgard 184, Dow Corning) containing both the elastomer and curing agent in a mass ratio of 10:1 and then degassed the air bubbles of PDMS via a vacuum about 1 h; and followed by curing in the oven at 85 °C for 1 h as shown in Fig. 2(b). The size of PDMS is 6 cm × 5 cm and the thickness is about 300 μm by a scraper. Finally, the cured PDMS was placed at room temperature for cooling, and peeled out of the female mold to form OL-MN arrays (Fig. 2(c)) for the assembly of Al/PDMS TENG (Fig. 2(d)). $SSOLHG6XUIDFH6FLHQFH C.K. Chung and K.H. Ke Table 2 Separated array microneedle and overlapped array microneedle related parameters and overlap estimation at the constant laser power of 6.9 W and a scanning speed of 22.8 mm/s. Samples Ablated spacing (μm) LD-MN 716 HD-MN 394 OL-MN 245 Average Height and Width (μm) H: 2171 W: 358 H: 1431 W: 301 H: 1311 W: 268 Surface area (mm2) Density (MN/ cm2) Junction area overlapped parameter calculated Single ablation area (μm2) Appraised the ablation area between two folded OL-MN (μm2) Estimated percentage of one overlapped area between two circles (% μm2) 17604.8 229 100659.7 Non overlap Non overlap 19945.6 433 71157.8 Non overlap Non overlap 22916.8 654 56410.4 1680.2 1.51% characterization of the surface morphology of PDMS was recorded by optical microscopy (OM, Olympus BX 51M, Japan). The Voc and Isc signal generated by the TENG were recorded by an oscilloscope (HIOKI Memory HiCorder MR8870-20, Japan), the electric signals of Voc and Isc are generated due to the externally applied force using a hand tapping. 3. Results and discussions 3.1. The separated and overlapped microneedles array The PMMA mother molds of three types of microneedles array namely separated LD-MN, HD-MN and overlapped OL-MN are ablated by the CO2 laser processing at a constant power of 6.9 W, a constant scanning speed of 22.8 mm/s, and the different ablated spacing of 716 μm, 394 μm and 245 μm, respectively, as shown in the top three optical micrographs of Fig. 3(a–c). The corresponding cast PDMS microneedles are shown in the bottom three optical micrographs of Fig. 3(a–c). The height and width of LD-MN are 2171 μm and 358 μm, respectively, while the HD-MN are 1431 μm and 301 μm. However, the height and width of OL-MN can have two types of expressions as shown in Fig. 4(a), that is, the conical tip area above the overlapped bottom area denoted as HT and WT, and the other is the height and width of single microneedle as H and W. The measured HT and WT of the conical tip area are 1080 μm and 235 μm, respectively, while the H and W of the OL-MN are 1311 μm and 268 μm. The cross-sectional OM clearly exhibits the difference between the separated and the overlapped MN arrays. The overlapped area A0 (μm2) in the geometrical relationship of Fig. 4(b) can be estimated by formula (1): Ao = 1 ⎛ πθ 2 πθ 2 R1 − R12sinθ + R2 − R22sinθ⎞ 2 ⎝ 180 180 ⎠ (1) where R1 and R2 are the radius of the ablated holes in an unit of μm, respectively, and θ (°) the corresponding overlapped angle in an unit of degree. Here, R1 and R2 are the same, so formula (1) is simplified as formula (2): Fig. 1. Schematic illustration of the CO2 laser fabrication process of the separated and overlapped PMMA master mold: (a) The separated and overlapped with the defined inter-hole spacing; (a1–a2) The spacing of single row is controlled by the pulse per inch of CO2 laser parameter; (a3–a4) The interspacing between rows and rows is non-overlapped; (b) The cross-sectional view of the ablated process for the separated or overlapped ones. Ao = πθ 2 R − R2sinθ 180 (2) The Ao of OL-MN calculated is 1680.2 μm , and the overlap ratio is 1.5%. The density (MN/cm2) of the separated and overlapped microneedles is defined as formula (3) and can be calculated by the OM images in Fig. 3: 2 2.2. The material selection, assembly and electrical measurements The Al foil and flexible PDMS are selected as the electrode and the friction materials for a sizeable triboelectric charge affinity difference. In addition, Al is low-cost and easy to access while PDMS is of good elastomer for reversible large deformation. The assembled Al/PDMS MN-TENG contains an separated or overlapped MN-PDMS film, two Al electrodes at the top and bottom attached to two PMMA plates, respectively, and four springs that are fixed at four corners for two PMMA separation distance of about 10 mm, as shown in Fig. 2(d). The Density = N A (3) where N is the total number of microneedles related to ablated spacing, and A is the total area of the MN-PDMS specimen in an unit of cm2. The density of LD-MN and HD-MN are 229 MN/cm2 and 433 MN/cm2, respectively. Moreover, the density of OL-MN is raised to 654 MN/cm2, which is 2.8 times and 1.5 times that of LD-MN and HD-MN, respectively. The increased MN density benefits for enhancing the contact $SSOLHG6XUIDFH6FLHQFH C.K. Chung and K.H. Ke Fig. 2. Schematic diagrams of microneedle PDMS casting and assembly of Al/PMDS TENG: (a) the illustrated PMMA master mold substrate, (b) the casting PDMS solution on PMMA master mold and curing in oven, (c) the cured PDMS was placed at room temperature for cooling and peeled out of female mold, and (d) the schematic image of the assembled Al/PDMS TENG. area during the contact deformation [30]. It is highly significant in the OL-MN as the comparison in Fig. 4(c) and (d). In addition, we estimate the surface area of three samples of LD-MN, HD-MN and OL-MN by 3D parametric Solidworks software. The calculated surface area of OL-MN is 22.91 × 103 mm2, the HD-MN is 19.94 × 103 mm2, and LD-MN is 17.6 × 103 mm2 as listed in Table 2. Fig. 5(a) and (b) show the OM micrographs of the ablated PMMA and the merged cast three kinds of MN-PDMS i.e. LD-MN, HD-MN and OL-MN at the same laser power and scanning speed for comparing the physical geometry and the measured average dimensions of microneedles, respectively. Decreasing the ablated spacing from LD-MN to HD-MN to OL-MN increases the pattern density but reduces the average MN height (H) and width (W) as shown in Fig. 5(c)–(d) and Table 2. This is attributed to the contributed laser energy per spot that decreases at a shorter ablation spacing. The output of the laser energy per spot during the laser ablation is expressed by formula (4): Energy per Spot = Linear Energy Density Pulses Per Inch number of PPI and the energy per spot is dependent on a linear energy density divided by the number of pulses. The magnitude of energy per spot in order is LD-MN > HD-MN > OL-MN. So the evolution of the ablated H and W of single MN in order is the same as listed in Table 2. However, the total contact surface area is multiplied by total MN number. It results in the result that OL-MN has the highest total contact surface area, the HD-MN the second and the LD-MN the lowest. It is noted that the highest pattern density in OL-MN combined with the appropriate height and width can contribute to the highest total contact surface area at the constant force. 3.2. Working mechanism of the OL-MN-TENG Fig. 6 shows the basic contact-separation operation mechanism of the OL-MN-TENG. In the initial position, the upper electrode (Al) and the friction layer PDMS are electrically neutral without any charge transfer as shown in Fig. 6(a). When a mechanical force is continuously downward applied to the TENG, a higher degree of deformation occurs. The contact surface area of the two materials increases with deformation to enhance the triboelectric effect. According to the polarity difference order of the triboelectric series, the maximum transfer of electrons from the Al surface to PDMS with a microstructured surface at (4) where the linear energy density (P/S) is derived from the ratio of laser power (P: Watt) to scanning speed (S: mm/s). The P/S is equal at the same P and S, therefore the pattern density is proportional to the Fig. 3. Optical micrographs (OM) of the master mold PMMA (top three) and cast PDMS (bottom three) microstructure: (a) LD-MN, (b) HD-MN, and (c) OL-MN to compare the variation of three morphologies. $SSOLHG6XUIDFH6FLHQFH C.K. Chung and K.H. Ke Fig. 4. Schematic diagram of an overlapped array compared with a separated array: (a) The overlapped microneedle has the conical tip area above the overlapped bottom area denoted as HT and WT, and the other is the total average height and width of single microneedle as H and W; (b) An illustrated diagram of estimating the overlap area; (c1–c4) Separated arrays and (d1–d4) overlapped arrays in (1) front view, (2) side view, (3) top view, (4) an isometric view, respectively. Fig. 5. The merged OM micrographs of (a) the ablated holes of PMMA and (b) the cast MN-PDMS of three ablation spacing at the same linear energy density for comparing the physical geometry; the relationship of the ablated spacing with the measured: (c) average height and (d) average width of MNs. $SSOLHG6XUIDFH6FLHQFH C.K. Chung and K.H. Ke Fig. 6. The working principle of the OL-MN-TENG with cross-sectional optical micrographs under cycled pressing–releasing operation: (a) the initial position of OL-MN-TENG between Al and PDMS are electrically neutral without any charge transfer, (b) the complete contact of the Al and OL-MN leads to a high degree of triboelectric charge transfer through the Al friction with the greatest MN deformation, (c) the restoring of two contact surfaces generates a current through the external circuit when the force is releasing, (d) the complete separation results in a new electrical equilibrium, and (e) the electrostatic induction again drives the electrons to flow in the opposite direction when pressing again. a complete contact produces a greatest triboelectric charge as shown in Fig. 6(b). The two contact surfaces starts to separate by spring when the force is releasing. Since the triboelectric charge creates a potential difference between the two electrodes, in order to balance the potential difference, the electrostatic induction drives the electrons of the bottom electrode, flowing to the top electrode through the external loop to maintain an electrical equilibrium state as shown in Fig. 6(c). The generated electricity continues until the complete separation and the open-circuit voltage reaches its maximum value as shown in Fig. 6(d). Subsequently, when pressing downward again, the electrostatic induction drives the electrons to flow in the opposite direction as shown in Fig. 6(e) and reach a maximum deformation at a full contact (Fig. 6(b)). The cycling contact-separation operation generates an alternating current. during the contact-separation is shown in Fig. 6. Fig. 6(b–e) shows the OL-MN subjected to a cycled force produced a wide range of contact areas and deformation behavior, at partial contact. In addition, Fig. 6(b) with full contact shows all vacancies between the OL-MNs and Al electrode are filled with the largest area. The Voc of TENG is proportional to the triboelectric charge density (σ) at a constant initial position was given by formula (5): Voc = σ·x (t ) ε0 (5) where x(t), σ, and ε0 represent the distance between the upper and lower friction layers at a time t, the triboelectric charge density of PDMS surface, and vacuum permittivity, respectively [34]. Fig. 8 shows the conceptual illustration of the induced charge density of the separated and overlapped array with the deformed contact area. Increasing the total contact-surface-area from the deformation and pattern density can induce more contact charge transfer to enhance triboelectric charge density as well as triboelectric performance [35,36]. 3.3. The performance of OL-MN-TENG To evaluate the effect of the separated and overlapped MN-PDMS films on the output performance of the MN-TENG, the three kinds of the density MN-TENG consisting of LD-MN, HD-MN, and OL-MN PDMS films were used for the electrical test. All sample size of MN-PDMS is 6.0 cm × 5.0 cm, and the test condition of initial position between the upper and lower friction layers was set about 10 mm at a difference of pattern density. Fig. 7 shows the electrical signals of the Voc and Isc of the separated array (LD-MN, HD-MN) and overlapped array (OL-MN). The Voc of HD-MN is 110.4 V and the Isc is 62.7 μA, corresponding to Jsc of 2.09 μA/cm2, while the Voc of LD-MN is 33.6 V, and Isc is 29.5 μA, corresponding to Jsc is 0.98 μA/cm2. Moreover, the OL-MN has the best performance characteristics, the peak Voc of 123 V, Isc of 109.7 μA and Jsc of 3.6 μA/cm2. In comparison, the Voc and Isc of OL-MN are 3.66 times and 3.71 times LD-MN, respectively, while the Voc and Isc of HDMN are 3.2 times and 2.12 times LD-MN. It is noted that the magnitude of H and W of MN in order is LD-MN > HD-MN > OL-MN but the pattern density of OL-MN (654 MN/cm2) is 2.8 times LD-MN (229 MN/ cm2) and 1.5 times HD-MN (433 MN/cm2), respectively. The pattern density has a higher influence than H and W for the total contact surface area that is the featured surface area multiplied by the total MN number. In addition, more MN number may enhance the output performance for more triboelectric charge density because of the more deformed effective contact area that is the key to performance enhancement [25,32,33]. The real deformation process of the OL-MN 3.4. OL-MN-TENG: energy storage, lighting emission, and self-power application The ability to store energy is important for the real application. Fig. 9(a) uses a bridge rectifier circuit design to convert AC power to DC power for charging capacitors and lighting LEDs. Fig. 9(b) shows the charging behavior of LD-MN, HD-MN and OL-MN on a 0.47 μF capacitor. The charging voltage (Vc) of OL-MN-TENG comes to 2 V in 3.6 s. Furthermore, the OL-MN-TENG has a stable Vc of about 2.2 V while the average Vc of HD-MN is 1.8 V, and the LD-MN-TENG is 1.2 V. The higher charging voltage of the OL-MN-TENG indicates that the capacitor stores a higher amount of charge than the separated LD-MN and HD-MN. The stored charge in a capacitor can be calculated by the capacitance formula (6): C= Q V (6) The amount of stored charge is proportional to the magnitude of charged voltage at the same capacitor. The charge stored on a 0.47 μF via the OL-MN-TENG is 1.03 μC compared with the HD-MN-TENG of 0.84 μC, and LD-MN-TENG of 0.56 μC. The stored charge of OL-MNTENG and HD-MN-TENG is 1.83 and 1.5 times higher than LD-MN $SSOLHG6XUIDFH6FLHQFH C.K. Chung and K.H. Ke Fig. 7. Measurement of open-circuit voltage and short-circuit current of separated and overlapped arrays: (a) voltage and (b) current was measured during the realtime using hand tapping (LD-MN, OL-MN), (c) peak voltage and (d) peak current comparing the separated arrays (LD-MN, HD-MN) and overlapped arrays (OL-MN) performance. TENG, respectively. Fig. 9(c) shows the lighting emission application of OL-MN-TENG, HD-MN-TENG, and LD-MN-TENG by the colored LEDs connected in series. The OL-MN-TENG, HD-MN-TENG, and LD-MNTENG drove 103, 91, and 18 bright LEDs, respectively, by hand tapping as shown in Fig. 9(c1–c3). The lighting behavior of OL-MN-TENG is shown in the supporting information Video S1. Fig. 10(a) demonstrated the all-blue LEDs arranged in the ME-NCKU advertising board for flickering communication application as the supporting information Video S2. Moreover, Fig. 10(b) shows the circuit design for self-powered e-watch using three capacitors in parallel for the total capacitance of over 10 μF. The OL-MN-TENG realizes the ability of mechanicalelectrical energy conversion and stored energy in the capacitors for applications to the self-powered e-watch, buzzer, and humidity sensor at a low frequency using hand-tapping as shown in Fig. 10(c), (d) and (e), respectively. We not only let the e-watch start working, and the ewatch will be gradually extinguished after stop pressing the OL-MNTENG; then we restart hand-pressing the OL-MN-TENG to make the ewatch restart normally working in a short time of about 10 s as the supporting information Video S3. We also demonstrated a self-powered buzzer via OL-MN-TENG to store energy in a 47 μF capacitor, and when pressing the button to drive the buzzer to make sound sirens attracting attention for seeking help in emergency as shown in Fig. 10(d) as the supporting information Video S4. Furthermore, the IoT network sensors like people’s five senses can detect information received from the surrounding environment information. We successfully demonstrate the self-powered humidity sensor by two capacitors in parallel for the total capacitance of 80 μF to supply the power for triggering the humidity sensor with displaying an environment humidity (53%), as shown in Fig. 10(e) as the supporting information Video S5. In brief, we successfully demonstrate various applications of the self-powered devices using the OL-MN-TENG including the LED lighting, communication with the advertising board, the portable e-watch, the buzzer of alarm sound for seeking help, and the driven humidity sensor to detect the humidity for potential environment IoT. 4. Conclusion The performance of TENG is dependent on the featured morphology that is related to total contact area. The conventional morphology such as pyramids, cubes, lines, pillars, and domes generally uses an expensive, complicated, and time-consuming fabrication process as well as insufficient feature surface area. Here, we demonstrate the novel OLMN-TENG for improving the total contact surface area via the featured surface area of single high-aspect-ratio microneedle multiplied by the total MN number during deformation of the MN-PDMS and Al friction layers. Moreover, the OL-MN-TENG is fabricated by a low-cost CO2 laser and PDMS casting process for rapid production. The Voc (123 V) and Isc (109.7 μA) of OL-MN-TENG are 3.6 times and 3.7 times that of LD-MN-TENG (Voc of 33.6 V, Isc of 29.5 μA), respectively. The OL-MNTENG can light up the ME-NCKU advertising board and 103 LEDs $SSOLHG6XUIDFH6FLHQFH C.K. Chung and K.H. Ke Fig. 8. Conceptual illustration of contact area and deformation behavior expected effects of the separated (left) and the overlapped microneedle array (right) on the friction layer. Fig. 9. Energy storage and lighting application: (a) the circuit diagram design: (a1) capacitor charging and (a2) LED, (b) the charging voltage curve on a 0.47 μF capacitor of LD-MN, HD-MN, and OL-MN (c) LED lighting situation: (c1) OL-MN-TENG drove 103 LED images; (c2) HD-MN-TENG drove 91 LEDs; (c3) LD-MN-TENG drove 18 LEDs. $SSOLHG6XUIDFH6FLHQFH C.K. Chung and K.H. Ke Fig. 10. Applications of OL-MN-TENG to: (a) ME-NCKU logo on the advertising board (supporting information Video S2), (b) the circuit design using 2.2, 3.3, and 4.7 μF capacitors in parallel for charging e-watch, (c) the OL-MN-TENG driven self-powered e-watch. (c1–c2) the electronic watch from start work to normally work process (supporting information Video S3). (d) The OL-MN-TENG driven self-powered buzzer (supporting information Video S4), and (e) self-powered humidity sensor (supporting information Video S5). Acknowledgement connected in series as well as the self-powered e-watch, buzzer, and humidity sensor for various successfully practical applications through harvesting mechanical energy in the living environment. This work is partially sponsored by the Ministry of Science and Technology (MOST), Taiwan, under contract No MOST 108-2221-E006-187. CRediT authorship contribution statement Appendix A. Supplementary material C.K. Chung: Conceptualization, Supervision, Validation, Writing review & editing, Investigation, Methodology. K.H. Ke: Conceptualization, Investigation, Methodology, Data curation, Formal analysis, Writing - original draft. Supplementary data to this article can be found online at https:// doi.org/10.1016/j.apsusc.2020.145310. References Declaration of Competing Interest [1] Q. Zhang, Z. Zhang, Q. Liang, F. Gao, F. Yi, M. Ma, Q. Liao, Z. Kang, Y. Zhang, Green hybrid power system based on triboelectric nanogenerator for wearable/portable electronics, Nano Energy 55 (2019) 151–163. [2] H.J. Yoon, H. Ryu, S.W. Kim, Sustainable powering triboelectric nanogenerators: approaches and the path towards efficient use, Nano Energy 51 (2018) 270–285. [3] V.L. Trinh, C.K. Chung, Harvesting mechanical energy, storage, and lighting using a novel PDMS based triboelectric generator with inclined wall arrays and microtopping structure, Appl. Energy 213 (2018) 353–365. 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. $SSOLHG6XUIDFH6FLHQFH C.K. Chung and K.H. Ke [4] M. Hook, X. Tang, Depletion of fossil fuels and anthropogenic climate change – a review, Energy Policy 52 (2013) 797–809. [5] C. Wu, A.C. Wang, W. Ding, H. Guo, Z.L. Wang, Triboelectric nanogenerator: a foundation of the energy for the new era, Adv. Energy Mater. 9 (2019) 1802906. [6] J.-H. Lee, J. Kim, T.Y. Kim, M.S. Al Hossain, S.-W. Kim, J.H. Kim, All-in-one energy harvesting and storage devices, J. Mater. Chem. A 4 (2016) 7983–7999. [7] X.S. Zhang, M.D. Han, B. Kim, J.F. Bao, J. Brugger, H.X. Zhang, All-in-one selfpowered flexible microsystems based on triboelectric nanogenerators, Nano Energy 47 (2018) 410–426. [8] W. He, H. Van Ngoc, Y.T. Qian, J.S. Hwang, Y.P. Yan, H. Choi, D.J. Kang, Synthesis of ultra-thin tellurium nanoflakes on textiles for high-performance flexible and wearable nanogenerators, Appl. Surf. Sci. 392 (2017) 1055–1061. [9] M. Ma, Z. Kang, Q. Liao, Q. Zhang, F. Gao, X. Zhao, Z. Zhang, Y. Zhang, Development, applications, and future directions of triboelectric nanogenerators, Nano Res. 11 (2018) 2951–2969. [10] L. Lin, Y.N. Xie, S.M. Niu, S.H. Wang, P.K. Yang, Z.L. Wang, Robust triboelectric nanogenerator based on rolling electrification and electrostatic induction at an instantaneous energy conversion efficiency of similar to 55%, ACS Nano 9 (2015) 922–930. [11] W. Kim, D. Bhatia, S. Jeong, D. Choi, Mechanical energy conversion systems for triboelectric nanogenerators: kinematic and vibrational designs, Nano Energy 56 (2019) 307–321. [12] H. Askari, E. Hashemi, A. Khajepour, M.B. Khamesee, Z.L. Wang, Tire condition monitoring and intelligent tires using nanogenerators based on piezoelectric, electromagnetic, and triboelectric effects, Adv. Mater. Technol. (2018) 1800105. [13] H. Zhang, Y. Yang, T.-C. Hou, Y. Su, C. Hu, Z.L. Wang, Triboelectric nanogenerator built inside clothes for self-powered glucose biosensors, Nano Energy 2 (2013) 1019–1024. [14] J. Yang, J. Chen, Y. Su, Q. Jing, Z. Li, F. Yi, X. Wen, Z. Wang, Z.L. Wang, Eardruminspired active sensors for self-powered cardiovascular system characterization and throat-attached anti-interference voice recognition, Adv. Mater. 27 (2015) 1316–1326. [15] S. Wang, L. Lin, Z.L. Wang, Triboelectric nanogenerators as self-powered active sensors, Nano Energy 11 (2015) 436–462. [16] Z.L. Wang, On Maxwell's displacement current for energy and sensors: the origin of nanogenerators, Mater. Today 20 (2017) 74–82. [17] A. Chandrasekhar, G. Khandelwal, N.R. Alluri, V. Vivekananthan, S.J. Kim, Batteryfree electronic smart toys: a step toward the commercialization of sustainable triboelectric nanogenerators, ACS Sustain. Chem. Eng. 6 (2018) 6110–6116. [18] M. Taghavi, A. Sadeghi, B. Mazzolai, L. Beccai, V. Mattoli, Triboelectric-based harvesting of gas flow energy and powerless sensing applications, Appl. Surf. Sci. 323 (2014) 82–87. [19] C. Yao, X. Yin, Y. Yu, Z. Cai, X. Wang, Chemically functionalized natural cellulose materials for effective triboelectric nanogenerator development, Adv. Funct. Mater. 27 (2017) 1700794. [20] B.K. Yun, J.W. Kim, H.S. Kim, K.W. Jung, Y. Yi, M.S. Jeong, J.H. Ko, J.H. Jung, Base-treated polydimethylsiloxane surfaces as enhanced triboelectric nanogenerators, Nano Energy 15 (2015) 523–529. [21] Y.P. Jeon, J.H. Park, T.W. Kim, Highly-enhanced triboelectric nanogenerators based on zinc-oxide nanoripples acting as a triboelectric layer, Appl. Surf. Sci. 445 (2018) 50–55. [22] G.G. Cheng, S.Y. Jiang, K. Li, Z.Q. Zhang, Y. Wang, N.Y. Yuan, J.N. Ding, W. Zhang, Effect of argon plasma treatment on the output performance of triboelectric nanogenerator, Appl. Surf. Sci. 412 (2017) 350–356. [23] F.R. Fan, L. Lin, G. Zhu, W. Wu, R. Zhang, Z.L. Wang, Transparent triboelectric nanogenerators and self-powered pressure sensors based on micropatterned plastic films, Nano Lett 12 (2012) 3109–3114. [24] J. Chen, Z.L. Wang, Reviving vibration energy harvesting and self-powered sensing by a triboelectric nanogenerator, Joule 1 (2017) 480–521. [25] I.W. Tcho, W.G. Kim, S.B. Jeon, S.J. Park, B.J. Lee, H.K. Bae, D. Kim, Y.K. Choi, Surface structural analysis of a friction layer for a triboelectric nanogenerator, Nano Energy 42 (2017) 34–42. [26] Y.P. Jeon, J.H. Park, T.W. Kim, Highly flexible triboelectric nanogenerators fabricated utilizing active layers with a ZnO nanostructure on polyethylene naphthalate substrates, Appl. Surf. Sci. 466 (2019) 210–214. [27] D. Choi, S. Yang, C. Lee, W. Kim, J. Kim, J. Hong, Highly surface-embossed polydimethylsiloxane-based triboelectric nanogenerators with hierarchically nanostructured conductive Ni–Cu fabrics, ACS Appl. Mater. Interfaces 10 (2018) 33221–33229. [28] M.L. Seol, S.H. Lee, J.W. Han, D. Kim, G.H. Cho, Y.K. Choi, Impact of contact pressure on output voltage of triboelectric nanogenerator based on deformation of interfacial structures, Nano Energy 17 (2015) 63–71. [29] W. Seung, M.K. Gupta, K.Y. Lee, K.S. Shin, J.H. Lee, T.Y. Kim, S. Kim, J. Lin, J.H. Kim, S.W. Kim, Nanopatterned textile-based wearable triboelectric nanogenerator, ACS Nano 9 (2015) 3501–3509. [30] V.L. Trinh, C.K. Chung, A facile method and novel mechanism using microneedlestructured PDMS for triboelectric generator applications, Small 13 (2017) 11. [31] F. Wortmann, K. Flüchter, Internet of things, Bus. Inform. Syst. Eng. 57 (2015) 221–224. [32] W. Yang, X. Wang, H. Li, J. Wu, Y. Hu, Comprehensive contact analysis for verticalcontact-mode triboelectric nanogenerators with micro-/nano-textured surfaces, Nano Energy 51 (2018) 241–249. [33] W. Yang, X. Wang, H. Li, J. Wu, Y. Hu, Z. Li, H. Liu, Fundamental research on the effective contact area of micro-/nano-textured surface in triboelectric nanogenerator, Nano Energy 57 (2019) 41–47. [34] S. Niu, S. Wang, L. Lin, Y. Liu, Y.S. Zhou, Y. Hu, Z.L. Wang, Theoretical study of contact-mode triboelectric nanogenerators as an effective power source, Energy Environ. Sci. 6 (2013) 3576–3583. [35] B.A. Grzybowski, M. Fialkowski, J.A. Wiles, Kinetics of contact electrification between metals and polymers, J. Phys. Chem. B 109 (2005) 20511–20515. [36] H.T. Baytekin, A.Z. Patashinski, M. Branicki, B. Baytekin, S. Soh, B.A. Grzybowski, The mosaic of surface charge in contact electrification, Science 333 (2011) 308–312.