An Environment‑Tolerant Ion‑Conducting Double‑Network Composite Hydrogel for High‑Performance Flexible Electronic Devices

High-performance ion-conducting hydrogels(ICHs)are vital for developing flexible electronic devices.However,the robustness and ion-conducting behavior of ICHs deteriorate at extreme tempera-tures,hampering their use in soft electronics.To resolve these issues,a method involving freeze–thawing and ionizing radiation technology is reported herein for synthesizing a novel double-network(DN)ICH based on a poly(ionic liquid)/MXene/poly(vinyl alcohol)(PMP DN ICH)system.The well-designed ICH exhibits outstanding ionic conductivity(63.89 mS cm^(-1) at 25℃),excellent temperature resistance(-60–80℃),prolonged stability(30 d at ambient temperature),high oxidation resist-ance,remarkable antibacterial activity,decent mechanical performance,and adhesion.Additionally,the ICH performs effectively in a flexible wireless strain sensor,thermal sensor,all-solid-state supercapacitor,and single-electrode triboelectric nanogenerator,thereby highlighting its viability in constructing soft electronic devices.The highly integrated gel structure endows these flexible electronic devices with stable,reliable signal output performance.In particular,the all-solid-state supercapacitor containing the PMP DN ICH electrolyte exhibits a high areal specific capacitance of 253.38 mF cm^(-2)(current density,1 mA cm^(-2))and excellent environmental adaptability.This study paves the way for the design and fabrication of high-performance mul-tifunctional/flexible ICHs for wearable sensing,energy-storage,and energy-harvesting applications.

Viologen-based flexible electrochromic devices

Electrochromic technology has gained significant attention in various fields such as displays,smart windows,biomedical monitoring,military camouflage,human-machine interaction,and electronic skin due to its ability to provide reversible and fast color changes under applied voltage.With the rapid development and increasing demand for flexible electronics,flexible electrochromic devices(FECDs)that offer smarter and more controllable light modulation hold great promise for practical applications.The electrochromic material(ECM)undergoing color changes during the electrochemical reactions is one of the key components in electrochromic devices.Among the ECMs,viologens,a family of organic small molecules with 1,1'-disubstituted-4,4'-dipyridinium salts,have garnered extensive research interest,due to their well-reversible redox reactions,excellent electron acceptance ability,and the ability to produce multiple colors.Notably,viologen-based FECDs demonstrate color changes in the liquid or semisolid electrolyte layer,eliminating the need for two solid electrodes and thus simplifying the device structure.Consequently,viologens offer significant potential for the development of FECDs with high optical contrast,fast response speed,and excellent stability.This review aims to provide a comprehensive overview of the progress and perspectives of viologen-based FECDs.It begins by summarizing the typical structure and recent exciting developments in viologen-based FECDs,along with their advantages and disadvantages.Furthermore,the review discusses recent advancements in FECDs with additional functionalities such as sensing,photochromism,and energy storage.Finally,the remaining challenges and potential research directions for the future of viologen-based FECDs are addressed.

A review of the scalable nano-manufacturing technology for flexible devices

Recent advances in electronic and photonic devices, such as artificial skin, wearable systems, organic and inorganic light-emitting diodes, have gained consider- able commercial and scientific interest in the academe and in industries. However, low-cost and high-throughput nano-manufacturing is difficult to realize with the use of traditional photolithographic processes. In this review, we summarize the status and the limitations of current nano- patterning techniques for scalable and flexible functional devices in terms of working principle, resolution, and processing speed. Finally, several remaining unsolved problems in nano-manufacturing are discussed, and future research directions are highlighted.

Flexible devices:from materials, architectures to applications

Flexible devices, such as flexible electronic devices and flexible energy storage devices, have attracted a significant amount of attention in recent years for their potential applications in modern human lives. The development of flexible devices is moving forward rapidly, as the innovation of methods and manufacturing processes has greatly encouraged the research of flexible devices. This review focuses on advanced materials, architecture designs and abundant applications of flexible devices, and discusses the problems and challenges in current situations of flexible devices. We summarize the discovery of novel materials and the design of new architectures for improving the performance of flexible devices. Finally, we introduce the applications of flexible devices as key components in real life.

Nanomaterials based flexible devices for monitoring and treatment of cardiovascular diseases(CVDs)

Cardiovascular diseases(CVDs)are one of the most serious diseases threatening human health in the world.Therefore,effective monitoring and treatment of CVDs are urgently needed.Compared with traditional rigid devices,nanomaterials based flexible devices open up new opportunities for further development beneficial from the unique properties of nanomaterials which contribute to excellent performance to better prevent and treat CVDs.This review summarizes recent advances of nanomaterials based flexible devices for the monitoring and treatment of CVDs.First,we review the outstanding characteristics of nanomaterials.Next,we introduce flexible devices based on nanomaterials for practical use in CVDs including in vivo,ex vivo,and in vitro methods.At last,we make a conclusion and discuss the further development needed for nanomaterials and monitoring and treatment devices to better care CVDs.

Polymer nanocomposite dielectrics with high electrocaloric effect for flexible solid-state cooling devices

Nanocomposite dielectrics show great promising application in developing next generation wearable all-solidstate cooling devices owing to the possessed advantages of high cooling efficiency, light-weight and small volume without the induced greenhouse effect or serious harm to ozone layer in the exploited refrigerants. However, low electrocaloric strength in nanocomposite dielectric is severely restricting its wide-spread application because of high applied operating voltage to improve electrocaloric effect. After addressing the chosen optimized ferroelectric ceramic and ferroelectric polymer matrix in conjunction with the analysis of crucial parameters, recent progress of electrocaloric effect(ECE) in polymer nanocomposites has been considerably reviewed. Subsequently, prior to proposing the conceptual design and devices/systems in electrocaloric nanocomposites, the existing developed devices/systems are reviewed. Finally, conclusions and prospects are conducted, including the aspects of materials chosen, structural design and key issues to be considered in improving electrocaloric effect of polymer nanocomposite dielectrics for flexible solidstate cooling devices.

Graphene-based materials for flexible energy storage devices

The booming developments in portable and wearable electronics promote the design of flexible energy storage systems. Flexible supercapacitors and batteries as promising energy storage devices have attracted tremendous attention. As the key component of both supercapacitors and batteries, electrode materials with excellent flexibility should be considered to match with highly flexible energy storage devices. Owing to large surface area, good thermal and chemical stability, high conductivity and mechanical flexibility,graphene-based materials have been widely employed to serve as promising electrodes of flexible energy storage devices. Considerable efforts have been devoted to the fabrication of flexible graphene-based electrodes through a variety of strategies. Moreover, different configurations of energy storage devices based on these active materials are designed. This review highlights flexible graphene-based two-dimensional film and one-dimensional fiber supercapacitors and various batteries including lithium-ion, lithium–sulfur and other batteries. The challenges and promising perspectives of the graphene-based materials for flexible energy storage devices are also discussed.

Layered double hydroxides as electrode materials for flexible energy storage devices

To prevent and mitigate environmental degradation,high-performance and cost-effective electrochemical flexible energy storage systems need to be urgently developed.This demand has led to an increase in research on electrode materials for high-capacity flexible supercapacitors and secondary batteries,which have greatly aided the development of contemporary digital communications and electric vehicles.The use of layered double hydroxides(LDHs)as electrode materials has shown productive results over the last decade,owing to their easy production,versatile composition,low cost,and excellent physicochemical features.This review highlights the distinctive 2D sheet-like structures and electrochemical characteristics of LDH materials,as well as current developments in their fabrication strategies for expanding the application scope of LDHs as electrode materials for flexible supercapacitors and alkali metal(Li,Na,K)ion batteries.

An overview of recent progress in the development of flexible electrochromic devices

Electrochromic materials are capable of reversibly switching their colors or optical properties through redox reactions under applied voltages,which have shown great potential applications including smart windows,nonemissive displays,optical filters,among others.Although the current rigid electrochromic devices have shown emerging interest and developed rapidly,many applications(e.g.,wearable/deformable optoelectronics)are blocked due to their inflexible features.Herein,the adaption of rigid electrochromic devices to flexible ones is of particular interest for the new era of smart optoelectronics.In this review,the current state-of-the-art achievements of flexible electrochromic devices(FECDs)are highlighted,along with their design strategies and the choice of electrochromic materials.The recent research progress of FECDs is reviewed in detail,and the challenges and corresponding solutions for real-world applications of FECDs are discussed.Furthermore,we summarize the basic fabrication strategies of FECDs and their potential applications.In addition,the development trend,the perspectives,and the outlook of FECDs are discussed at the end of this Review,which may provide recommendations and potential directions to advance the practical applications of FECDs.

Flexible organic photovoltaic devices based on oligothiophene derivatives

For the purpose of developing flexible organic photovoltaic devices, we have fabricated two flexible devices using 5-formyl- 2,2′：5′,2″：5″,2′″-quaterthiophene （4T-CHO）, 5-formyl-2,2′：5′, 2″：5″,2′″：5′″,2″″-quinquethiophene （5T-CHO） and 3,4,9,10-perylenetertracarboxylic dianhydride （PTCDA）. The PET-ITO/4T-CHO/PTCDA/A1 device has an open circuit voltage （Voc） of 1.56 V, photoelectric conversion efficiency of 0.77%. The PET-ITO/5T-CHO/PTCDA/A1 device has a Voc of 1.70 V, photoelectric conversion efficiency of 0.84%. The two flexible devices have high Voc （1.56 and 1.70 V）. It is possible that intermolecular hydrogen bonding between -CHO group of nT-CHO and carboxylic dianhydride of PTCDA contributes to enhancing the efficiency by promoting interfacial electron transfer and eliminating the subconducting band trap sites.

Flexible biomimetic olfactory neurons based on organic heterojunction

Simulating the human olfactory nervous system is one of the key issues in the field of neuromorphic computing.Olfac-tory neurons interact with gas molecules,transmitting and storing odor information to the olfactory center of the brain.In order to emulate the complex functionalities of olfactory neurons,this study presents a flexible olfactory synapse transistor(OST)based on pentacene/C8-BTBT organic heterojunction.By modulating the interface between the energy bands of the organic semiconductor layers,this device demonstrates high sensitivity(ppb level)and memory function for NH3 sensing.Typi-cal synaptic behaviors triggered by NH_(3) pulses have been successfully demonstrated,such as inhibitory postsynaptic currents(IPSC),paired-pulse depression(PPD),long-term potentiation/depression(LTP/LTD),and transition from short-term depression(STD)to long-term depression(LTD).Furthermore,this device maintains stable olfactory synaptic functions even under differ-ent bending conditions,which can present new insights and possibilities for flexible synaptic systems and bio-inspired elec-tronic products.

Carbon-Based Flexible and All-Solid-State Micro-supercapacitors Fabricated by Inkjet Printing with Enhanced Performance

By means of inkjet printing technique, flexible and all-solid-state micro-supercapacitors(MSCs) were fabricated with carbon-based hybrid ink composed of graphene oxide(GO,98.0vol.%) ink and commercial pen ink(2.0vol.%). A small amount of commercial pen ink was added to effectively reduce the agglomeration of theGO sheets during solvent evaporation and the following reduction processes in which the presence of graphite carbon nanoparticles served as nano-spacer to separate GO sheets. The printed device fabricated using the hybrid ink,combined with the binder-free microelectrodes and interdigital microelectrode configuration, exhibits nearly 780%enhancement in areal capacitance compared with that of pure GO ink. It also shows excellent flexibility and cycling stability with nearly 100% retention of the areal capacitance after 10,000 cycles. The all-solid-state device can be optionally connected in series or in parallel to meet the voltage and capacity requirements for a given application.This work demonstrates a promising future of the carbonbased hybrid ink for directly large-scale inkjet printing MSCs for disposable energy storage devices.

Flexible Zn-ion batteries based on manganese oxides: Progress and prospect

The ever-growing market of wearable electronic devices has greatly stimulated the rapid development of flexible Zn-ion batteries(ZIBs).Manganese oxides are one of the most commonly used hosts for zinc ion accommodation and thus receive particular research interest for high-performance flexible ZIB constructions.In this review,a comprehensive summary of the recent development of flexible ZIBs with manganese oxides as cathode materials is presented.Apart from the brief introduction of flexible electronic devices and ZIBs,the charge storage mechanisms and crystal structures of various manganese oxides are summarized.Modifications of the cathode materials in terms of morphology,conductivity,structures,and flexibilities are illustrated in detail,together with the demonstration of structure-performance relationships and applications in flexible ZIBs.Finally,limitations to be overcome are indicated and the future work directions are proposed.

Swift Assembly of Adaptive Thermocell Arrays for Device‑Level Healable and Energy‑Autonomous Motion Sensors

The evolution of wearable technology has prompted the need for adaptive,self-healable,and energy-autonomous energy devices.This study innovatively addresses this challenge by introducing an MXene-boosted hydrogel electrolyte,which expedites the assembly process of flexible thermocell(TEC)arrays and thus circumvents the complicated fabrication of typical wearable electronics.Our findings underscore the hydrogel electrolyte’s superior thermoelectrochemical performance under substantial deformations and repeated self-healing cycles.The resulting hydrogel-based TEC yields a maximum power output of 1032.1 nW under theΔT of 20 K when being stretched to 500%for 1000 cycles,corresponding to 80%of its initial state;meanwhile,it sustains 1179.1 nW under theΔT of 20 K even after 60 cuthealing cycles,approximately 92%of its initial state.The as-assembled TEC array exhibits device-level self-healing capability and high adaptability to human body.It is readily applied for touch-based encrypted communication where distinct voltage signals can be converted into alphabet letters;it is also employed as a self-powered sensor to in-situ monitor a variety of body motions for complex human actions.The swift assembly approach,combined with the versatile functionality of the TEC device,paves the way for future advancements in wearable electronics targeting at fitness monitoring and human–machine interfaces.

Flexible Nanocomposite Conductors for Electromagnetic Interference Shielding

With the extensive use of electronic communication technology in integrated circuit systems and wearable devices, electromagnetic interference(EMI) has increased dramatically. The shortcomings of conventional rigid EMI shielding materials include high brittleness, poor comfort, and unsuitability for conforming and deformable applications. Hitherto, flexible(particularly elastic) nanocomposites have attracted enormous interest due to their excellent deformability. However, the current flexible shielding nanocomposites present low mechanical stability and resilience, relatively poor EMI shielding performance, and limited multifunctionality. Herein, the advances in low-dimensional EMI shielding nanomaterials-based elastomers are outlined and a selection of the most remarkable examples is discussed. And the corresponding modification strategies and deformability performance are summarized. Finally, expectations for this quickly increasing sector are discussed, as well as future challenges.

A review of neutral pH polymer electrolytes for electrochemical capacitors:Transitioning from liquid to solid devices

The development of neutral pH polymer electrolytes has enabled high-performance solid-state,thin,and flexible electrochemical capacitors(ECs)to provide power for future consumer electronics and Internet-of-Thing devices.Notwithstanding their promising prospect,there is still some lack of understandings or disconnections from fundamental science to practical applications of these electrolytes.In this review,we provide an overview of stateof-the-art studies on ECs with neutral pH electrolytes in both liquid and solid configurations.Starting from the fundamental studies on the voltage window and ion conduction of salt species in liquid solution to polymer electrolytes,key considerations in developing neutral pH polymer electrolytes are discussed.The performance of the polymer electrolytes along with their enabled solid symmetric and asymmetric EC devices,as well as some enhanced functionalities are presented.The future directions for research on neutral pH polymer electrolytes are proposed,expected to provide reference for further enriching the fundamental knowledge and improving the device performances.

Regulating Thermogalvanic Effect and Mechanical Robustness via Redox Ions for Flexible Quasi‑Solid‑State Thermocells

The design of power supply systems for wearable applications requires both flexibility and durability.Thermoelectrochemical cells(TECs)with large Seebeck coefficient can efficiently convert lowgrade heat into electricity,thus having attracted considerable attention in recent years.Utilizing hydrogel electrolyte essentially addresses the electrolyte leakage and complicated packaging issues existing in conventional liquid-based TECs,which well satisfies the need for flexibility.Whereas,the concern of mechanical robustness to ensure stable energy output remains yet to be addressed.Herein,a flexible quasisolid-state TEC is proposed based on the rational design of a hydrogel electrolyte,of which the thermogalvanic effect and mechanical robustness are simultaneously regulated via the multivalent ions of a redox couple.The introduced redox ions not only endow the hydrogel with excellent heat-to-electricity conversion capability,but also act as ionic crosslinks to afford a dual-crosslinked structure,resulting in reversible bonds for effective energy dissipation.The optimized TEC exhibits a high Seebeck coefficient of 1.43 mV K−1 and a significantly improved fracture toughness of 3555 J m^(−2),thereby can maintain a stable thermoelectrochemical performance against various harsh mechanical stimuli.This study reveals the high potential of the quasi-solid-state TEC as a flexible and durable energy supply system for wearable applications.

Recent advances in nanofiber-based flexible transparent electrodes

Flexible and stretchable transparent electrodes are widely used in smart display,energy,wearable devices and other fields.Due to the limitations of flexibility and stretchability of indium tin oxide electrodes,alternative electrodes have appeared,such as metal films,metal nanowires,and conductive meshes.However,few of the above electrodes can simultaneously have excellent flexibility,stretchability,and optoelectronic properties.Nanofiber(NF),a continuous ultra-long one-dimensional conductive material,is considered to be one of the ideal materials for high-performance transparent electrodes with excellent properties due to its unique structure.This paper summarizes the important research progress of NF flexible transparent electrodes(FTEs)in recent years from the aspects of NF electrode materials,preparation technology and application.First,the unique advantages and limitations of various NF materials are systematically discussed.Then,we summarize the preparation technology of various advanced NF FTEs,and point out the future development trend.We also discuss the application of NFs in solar cells,supercapacitors,electric heating equipments,sensors,etc,and analyze its development potential in flexible electronic equipment,as well as problems that need to be solved.Finally,the challenges and future development trends are proposed in the wide application of NF FTEs in the field of flexible optoelectronics.

Recent progress in graphene-based wearable piezoresistive sensors:From 1D to 3D device geometries

Electronic skin and flexible wearable devices have attracted tremendous attention in the fields of human-machine interaction,energy storage,and intelligent robots.As a prevailing flexible pressure sensor with high performance,the piezoresistive sensor is believed to be one of the fundamental components of intelligent tactile skin.Furthermore,graphene can be used as a building block for highly flexible and wearable piezoresistive sensors owing to its light weight,high electrical conductivity,and excellent mechanical.This review provides a comprehensive summary of recent advances in graphene-based piezoresistive sensors,which we systematically classify as various configurations including one-dimensional fiber,two-dimensional thin film,and threedimensional foam geometries,followed by examples of practical applications for health monitoring,human motion sensing,multifunctional sensing,and system integration.We also present the sensing mechanisms and evaluation parameters of piezoresistive sensors.This review delivers broad insights on existing graphene-based piezoresistive sensors and challenges for the future generation of high-performance,multifunctional sensors in various applications.

In-situ-selective-UV crosslinking fabrication of solid liquid host guest electrolyte: A facile one-step method realizing highly flexible electrochromic device

Flexible electrochromic devices (FECDs) are promising candidates for the next generation of wearable electronics due to their low operating voltage and energy consumption. For the flexible electrochromic devices, the electrolyte is an important component. Typically, the electrolyte needs to be formulated according to the device structure and usage scenario. A high-performance electrolyte involves consideration of many factors, including choosing the right polymer, solvent, curing agent, and ion type to satisfy particular device specifications. In this work, a ultraviolet-curable solid–liquid host–guest (UV-SLHG) electrolyte is developed. Several aspects of performance are improved by introducing the solid–liquid coexisting microstructure without changing the electrolyte formulation, including excellent adhesion, a 30% increase in tensile characteristics, and a seven-fold increase in ionic conductivity when compared to a fully cured solid-state electrolyte. More importantly, the unique advantage of SLHG electrolytes lies that the thickness will not change significantly during bending. The FECD made by using the UV-SLHG-based electrolyte sustained 10,000 bending cycles at the bending radius of 2.5 mm while maintaining outstanding optical modulation. A wearable ring-type ECD and a battery-free FECD wine label were made as demonstrators. The UV-SLHG strategy is not only suitable for the FECDs but also universally applicable to other electrolyte-based of flexible electronics such as flexible capacitors and batteries.