Paper-based Triboelectric Nanogenerators And Their .

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Paper-based triboelectric nanogenerators and theirapplications: a reviewJing Han‡1,2, Nuo Xu‡1,3, Yuchen Liang1,4, Mei Ding5, Junyi Zhai1,2,3, Qijun Sun*1,2,3and Zhong Lin Wang*1,2,6ReviewOpen AccessAddress:1Beijing Institute of Nanoenergy and Nanosystems, Chinese Academyof Sciences, Beijing, 101400, P. R. China, 2School of Nanoscienceand Technology, University of Chinese Academy of Sciences, Beijing,100049, P. R. China, 3Center on Nanoenergy Research, School ofPhysical Science and Technology, Guangxi University, Nanning,530004, P. R. China, 4Qichen (Shanghai) Medical Co., Ltd., Shanghai201319, P. R. China, 5College of Materials Science and Engineering,Changsha University of Science & Technology, Changsha, 410114,P. R. China and 6School of Materials Science and Engineering,Georgia Institute of Technology, Atlanta, Georgia 30332-0245, UnitedStatesEmail:Qijun Sun* -;Zhong Lin Wang* -* Corresponding authorBeilstein J. Nanotechnol. 2021, 12, ived: 29 October 2020Accepted: 30 December 2020Published: 01 February 2021This article is part of the thematic issue "Nanogenerators and flexibleelectronics".Guest Editor: Y. Mao 2021 Han et al.; licensee Beilstein-Institut.License and terms: see end of document.‡ Equal contributorsKeywords:energy harvesting; interaction; Internet of Things (IoT); paper-basedsensors; self-powered devices; P-TENGs; triboelectric nanogeneratorAbstractThe development of industry and of the Internet of Things (IoTs) have brought energy issues and huge challenges to the environment. The emergence of triboelectric nanogenerators (TENGs) has attracted wide attention due to their advantages, such as selfpowering, lightweight, and facile fabrication. Similarly to paper and other fiber-based materials, which are biocompatible,biodegradable, environmentally friendly, and are everywhere in daily life, paper-based TENGs (P-TENGs) have shown great potential for various energy harvesting and interactive applications. Here, a detailed summary of P-TENGs with two-dimensionalpatterns and three-dimensional structures is reported. P-TENGs have the potential to be used in many practical applications, including self-powered sensing devices, human–machine interaction, electrochemistry, and highly efficient energy harvesting devices.This leads to a simple yet effective way for the next generation of energy devices and paper electronics.IntroductionEnvironmental pollution is an undeniable fact in our daily lives.The air pollution caused by industrial waste generation (gases/toxins) and by the combustion of fossil fuels is getting more andmore serious [1,2]. Meanwhile, with the rapid growth of theInternet of Things (IoTs), the explosive growth of sensors hasled to the massive use of batteries, which have also resulted insevere environmental issues in virtue of their short lifetime. Inthis regard, renewable energy sources, such as wind, wave, and151

Beilstein J. Nanotechnol. 2021, 12, 151– power, appear to be the most efficient and effective solutions [3-10]. However, the infrastructure constructions for harvesting energy from renewable sources (e.g., wind powerstations and solar photovoltaic energy systems) are huge,expensive, and take a long time to be built. Even worse, harvested wind and solar energy cannot be incorporated into thepower grid, which inevitably calls for additional energy storagefacilities [11-13]. Therefore, there are still increasing demandsfor the development of power sources which are highly efficient, clean, and sustainable.In recent years, the triboelectric nanogenerator (TENG), firstinvented by the Wang group in 2012 [14], has been quickly developed to be a revolutionary breakthrough in the energy harvesting [15-21] and self-powered systems [22-27]. Based onelectrostatic induction and triboelectrification [28], the novelTENG can utilize the Maxwell’s displacement current to readilydrive electrons to flow through an external circuit and powerportable electronic devices. To harvest the ubiquitous mechanical energy from its surroundings, TENGs need to have a simpledevice design and to be low cost and lightweight. TENGs havealso shown the pivotal ability to convert low-frequency mechanical energy from walking, waving, and eye-blinking intoelectricity. TENGs can readily serve as a sustainable powersupply based on four basic operation modes [29], includingvertical contact–separation mode [30-32], lateral-sliding mode[33-35], single-electrode mode [36,37], and freestanding triboelectric-layer mode [38]. As an advanced and durable energysource, TENGs have shown promising and significant featuresthat are applied to power units in the micro- and nanoscale [3944], high-voltage sources [45], self-powered systems [46-50],and blue energy harvesting devices [51-56].Paper, by far one of the most inexpensive and flexible materialswidely used in daily life, was developed more than 2000 yearsago in China. Paper and other fiber-based materials are integralcomponents of many objects that are used on a regular basis bythe population, which are also available in different compositions, thickness and surface roughness. Most importantly, paperis biocompatible, biodegradable, and environmentally friendly,and has tremendous advantages over the majority of other materials (e.g., it is lightweight, renewable, and air-permeable).Besides, paper is flexible and can be easily folded or bent into3D structures without causing structural damage.In the last decades, paper-based electronic devices, such asmicrofluidic paper-based analytical devices (µPADs) [57-60]and thin-film transistors (TFTs) [61-65] have been widely investigated. Recently, they have also been applied in variousenergy-related devices [66-68]. Although paper is intrinsicallyinsulating, conductive materials (e.g., metal nanowires, con-ducting polymers, carbon nanotube (CNT) inks, multiwall carbon nanotube (MWCNT) inks, and reduced graphene oxide)[69-82], can be easily absorbed or used as a coating layer on thesurface of the paper due to its wettability and moisture-retention capacity. This provides an efficient method to preparepaper electrodes for TENGs. Paper has also been proven to be anatural TENG friction layer. Due to that, it shows a tendency ofeasily losing electrons (i.e., electropositive) when contacting amaterial that can easily gain electrons (i.e., electronegative).Furthermore, due to the high roughness and porous nanofiberstructure it can lead to enhanced TENG output performancesowing to improved charge-trapping abilities.Based on the above advantages and conveniences, paper-basedTENGs (P-TENGs) have exhibited great potential for manypractical applications, leading to a simple yet effective way forthe next generation of energy devices and paper electronics. Inthis review, we try to look back and summarize the latest developments in the field of P-TENGs. Figure 1 schematically showsthe theme of this review article and several typical examples inwhich P-TENGs are used. This paper starts with an overview ofTENGs and the corresponding working mechanism of fourbasic working modes based on charge transfer and on theelectron-cloud potential-well model. Regarding surface modification and fabrication methods involving paper, we then highlight the strategies to improve the output performance ofP-TENGs. In another section, we give a detailed review on theapplication of P-TENGs, with two-dimensional patterns andthree-dimensional structures, on self-powered sensing devices,human–machine interaction, electrochemistry and highly efficient energy-harvesting systems. To conclude the review,perspectives and proposals regarding future potential applications and research directions are discussed.ReviewFour working modes of TENGs andcharge-transfer mechanismsTENGs, which are emerging and efficient apparatus for energyconversion, have been attracting significant attention from thefields of energy harvesting and self-powered systems. Thetriboelectric effect [83-85], a type of contact-induced electrification, is the basis of TENGs. It was found that when two different materials are in physical contact, their interfaces becomeelectrically charged. Due to contact electrification (CE, or triboelectrification) [86], opposite charges will be induced when thetwo materials are separated by a mechanical force, which willcorrespondingly generate a potential difference between the twomaterials due to electrostatic induction. If an electrical load isconnected through an external circuit, the previously inducedpotential difference will drive the electrons to flow between152

Beilstein J. Nanotechnol. 2021, 12, 151–171.Figure 1: P-TENGs and their applications.the two materials (through the electrodes and the externalcircuit). Depending on the circuit configurations and on thevariations in the polarization direction, TENGs can have fourworking modes [87], including vertical contact–separation (CS)mode, in-plane lateral-sliding (LS) mode, single-electrode (SE)mode, and freestanding triboelectric-layer (FT) mode, as shownin Figure 2a.In the vertical CS mode, a stack of two dielectric films is platedwith a metal electrode at the back surface of each layer. Whenthe two dielectric films are vertically separated and periodicallycontacted due to the application of external forces, a small airgap is formed in the middle and a potential difference is induced between the two electrodes, which can drive the forward/reverse flow of charges via the external circuit. The in-plane LSFigure 2: (a) Four working modes of TENGs [87]. Copyright 2018 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim. Adapted with permissionfrom Changsheng Wu et al., “Triboelectric Nanogenerator: A Foundation of the Energy for the New Era”, Advanced Energy Materials, John Wiley andSons. (b) Working mechanism of a TENG based on the vertical contact–separation mode.153

Beilstein J. Nanotechnol. 2021, 12, 151–171.mode relies on the relative slippage between the two materialsin a horizontal direction parallel to the surface. An alternatingcurrent output can be produced during the sliding motions between the top and the bottom layers. This kind of slippage isalso common in a variety of rotation-induced sliding modes,which exhibit huge potential for application in high-outputTENG devices. Compared with the vertical CS mode and thein-plane LS mode, the SE mode has only one electrode at thebottom, which is connected to ground and taken as the reference electrode. The direction of the induced electric field can bereversely changed during the approximation or separation between the bottom electrode and the upper dielectric materials.The charge exchange will occur between the bottom electrodeand ground to balance the induced potential variation. The application scenarios of TENGs with an SE mode are broad, including direct finger/hand/skin touch or body motions. The FTmode uses two unconnected symmetrical electrodes as the reference electrodes. When the top free-standing (i.e., noncontact)dielectric layer moves from one electrode to the other, electrostatic charges will be induced on the two electrodes in sequence. Similar to the SE mode, if one takes one electrode asthe reference electrode, the induced charges will flow from thereference electrode to the other electrode through the externalload. Thus, the electrical output is induced by the asymmetriccharge distribution during the suspending (forward/backward)movements.Based on the combination effect of triboelectrification and electrostatic induction, the working mechanisms of the four operational modes of TENGs are similar. Taking P-TENGs in the CSmode (most common design in previous works) as a typical representative example, we further systematically analyze theworking mechanism of the detailed charge-transfer process.Figure 2b elucidates the charge generation and the electrontransfer process at the friction interfaces (paper/the other dielectric layer) and electrodes (upper/bottom electrode) during onecontact–separation cycle of P-TENGs. The electrificationoccurs at the interfaces between the paper and the other dielectric layer owing to different electronegativities when they comeinto contact. Different triboelectric charges (positive and negative charges) are induced by the same amount on the surfaces ofthe friction layers. As there is no electric potential at this stage,there is no electron transfer between the two conductive layers(Figure 2b-I). When the two friction layers start to separatealong the vertical direction, opposite charges are induced in theupper and lower conductive electrodes owing to electrostaticinduction (Figure 2b-II). As the distance between the two layersincreases, the electric potential difference between the twolayers enhances, driving the electrons to flow through theexternal load which generates an instantaneous current. Whenthe two layers are separated by a maximum distance, thepositive and negative triboelectric charges become fullyequilibrated, resulting in no current flow through the load(Figure 2b-III). When the two layers approach each other, theelectrostatic charges are induced and accumulate again, drivingthe electrons to flow through the load between the two conductive layers in a reverse direction (Figure 2b-IV). Finally, the twofriction layers become fully in contact and the whole systemreturns to the initial state. At this stage, the triboelectric chargesare completely balanced and there is no output current.Although the origin of the contact electrification has been amatter of debate for a long time, no conclusive model to explainthis phenomenon has been proposed. Previous studies investigated whether the electron or ion transfer were dominant in thecontact-electrification phenomenon. However, the results werehighly controversial [88,89]. Xu et al. [90] have proposed thatthe quantification of the surface charge density at different temperature values is a critical method for investigating this phenomenon. This can be readily explored as an effective tool toidentify the transferred charges and the corresponding CEmechanism in TENGs. The results shown in [90] suggest thatthe electron transfer dominates the CE process. The chargeretention ability is attributed to the intrinsic potential barrierheights of the different materials, which can prevent the chargedissipation. As the CE behavior is dependent on the surrounding temperature, Xu et al. [91] have further explored the operation of TENGs at high temperature values. Their results revealthat the thermionic emission of electrons is the main reason forCE and the atomic thermal vibrations strongly influence the CEat increased temperature values.To better demonstrate the electron-transfer mechanism,which is dominant in CE, Xu et al. have proposed an electroncloud potential-well model (Figure 3). At the initial state, sincethe highest occupied energy levels of the two materials (A andB) are different and the individual electron clouds of the materials are separated by a distance d, the electrons cannot be transferred between material A and material B. The trapping effectof the potential wells prevents the electrons from escaping(Figure 3-i). Once the material A comes into contact with thematerial B, their electron clouds collide with one another toform ionic or covalent bonds. The overlap between the electronclouds enable the electrons to spontaneously flow from material A to material B (Figure 3-ii). The majority of the transferredelectrons will remain in B even if the material A is separatedfrom the material B by an enlarged energy barrier. This leads toA and B being positively and negatively charged, respectively(Figure 3-iii). As the temperature rises, the transferred electrons in B tend to more easily escape from the potential welland to be thermionically emitted into the air, leading to agradual decay of the surface charges (Figure 3-iv).154

Beilstein J. Nanotechnol. 2021, 12, 151–171.Figure 3: The proposed electron-cloud potential-well model for electron transfer, which is the dominant mechanism of contact electrification [90].Copyright 2018 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim. Adapted with permission from Cheng Xu et al., “On the Electron‐TransferMechanism in the Contact‐Electrification Effect”, Advanced Materials, John Wiley and Sons.Treatment methods for paper and P-TENGsThe electrical properties of paper are critical determinants of theperformance of P-TENGs. The original paper structure usuallydoes not meet all the requirements for the desired applicationson P-TENG devices. Therefore, corresponding treatment processes (e.g., deposition of conductive materials by laser patterning, screen printing, spray coating, thermal deposition, surfacemorphology engineering, and chemical modification [46,9298]) are often applied to convert paper into a conductive electrode or into a charge-enriched friction layer to improveP-TENG output performances. As the TENG output performance closely depends on the triboelectric polarity of the friction layer, the engineering of friction layers with more chargeswith an opposite polarity induces a larger triboelectric chargedensity. Since paper is mainly composed of cellulose, whichgenerally shows a tendency of losing electrons (electropositive),it is preferred to pair paper with a friction material that caneasily gain electrons (electronegative) according to the triboelectric series [83,99,100].Figure 4 depicts a paper-based 3D foldable device submitted toa direct laser patterning method, which can convert ink-soakedpaper substrates to multifunctional carbide/graphene (MCG)composites [92]. The composites have shown good conductivity even after repeated mechanical bending and folding tests.Moreover, the laser pattering process results in porous MCGstructures (with pore sizes ranging from hundreds of nanometers to several microns), which can be used in various applications, such as mechanical energy harvesting devices, chemicalsensors, and electrochemical supercapacitors.Screen printing is a facile, efficient, high-throughput andlow-cost printing method [101]. A layer of ink is scraped acrossthe screen surface and, then, extruded through the open poresof a patterned mesh into the substrate. The printing resolutionand the pattern thickness depend on the density of the mesh andon the properties of the ink, respectively. Screen printing hasbeen widely used for fabricating conductive electrodes, semiconducting layers of solar cells, and active materials in field-155

Beilstein J. Nanotechnol. 2021, 12, 151–171.Figure 4: Treatment methods for paper and P-TENGs. Schematic illustration of a simplified MCG composite obtained by a direct laser-writing MCGpatterning process. An SEM image of a paper depicting three regions (from left to right): paper, paper soaked with a Mo–gelatin ink, and paper withconverted MCG composites [92]. Copyright 2018 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim. Adapted with permission from Xining Zang etal., “Laser‐Induced Molybdenum Carbide–Graphene Composites for 3D Foldable Paper Electronics”, Advanced Materials, John Wiley and Sons.effect transistors (FETs). It is commonly used as a planarprinting technique for batch processing. It is also further adaptable to a roll-to-roll process or to rotary screen printing, whichenables a facile and high-throughput printing on curved surfaces. The deposition process assisted with soft stencils isanother “bottom-up” method for the preparation of functionalmaterials on flexible and irregular surfaces. Even thoughP-TENGs require flexible conductive materials, metallic materials (e.g., copper, zinc, silver, and gold) are still frequently usedas electrodes for flexible electronics due to their excellentelectrical conductivity. By using the Kapton tape to attach softstencils to paper, various metals can be deposited through thestencils by thermal/e-beam evaporation, sputter depos

201319, P. R. China, 5College of Materials Science and Engineering, Changsha University of Science & Technology, Changsha, 410114, P. R. China and 6School of Materials Science and . electrochemistry, and highly efficient energy harvesting devices. This leads to a simple yet effective way for the next generation of energy devices and paper .

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