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.

Device design principles and bioelectronic applications for flexible organic electrochemical transistors

Organic electrochemical transistors(OECTs) exhibit significant potential for applications in healthcare and human-machine interfaces, due to their tunable synthesis, facile deposition, and excellent biocompatibility. Expanding OECTs to the fexible devices will significantly facilitate stable contact with the skin and enable more possible bioelectronic applications. In this work,we summarize the device physics of fexible OECTs, aiming to offer a foundational understanding and guidelines for material selection and device architecture. Particular attention is paid to the advanced manufacturing approaches, including photolithography and printing techniques, which establish a robust foundation for the commercialization and large-scale fabrication. And abundantly demonstrated examples ranging from biosensors, artificial synapses/neurons, to bioinspired nervous systems are summarized to highlight the considerable prospects of smart healthcare. In the end, the challenges and opportunities are proposed for fexible OECTs. The purpose of this review is not only to elaborate on the basic design principles of fexible OECTs, but also to act as a roadmap for further exploration of wearable OECTs in advanced bio-applications.

Recent advances and innovations in the design and fabrication of wearable flexible biosensors and human health monitoring systems based on conjugated polymers

Wearable biosensors have received great interest as patient-friendly diagnostic technologies because of their high flexibility and conformability.The growing research and utilization of novel materials in designing wearable biosensors have accelerated the development of point-of-care sensing platforms and implantable biomedical devices in human health care.Among numerous potential materials,conjugated polymers(CPs)are emerging as ideal choices for constructing high-performance wearable biosensors because of their outstanding conductive and mechanical properties.Recently,CPs have been extensively incorporated into various wearable biosensors to monitor a range of target biomolecules.However,fabricating highly reliable CP-based wearable biosensors for practical applications remains a significant challenge,necessitating novel developmental strategies for enhancing the viability of such biosensors.Accordingly,this review aims to provide consolidated scientific evidence by summarizing and evaluating recent studies focused on designing and fabricating CP-based wearable biosensors,thereby facilitating future research.Emphasizing the superior properties and benefits of CPs,this review aims to clarify their potential applicability within this field.Furthermore,the fundamentals and main components of CP-based wearable biosensors and their sensing mechanisms are discussed in detail.The recent advancements in CP nanostructures and hybridizations for improved sensing performance,along with recent innovations in next-generation wearable biosensors are highlighted.CPbased wearable biosensors have been—and will continue to be—an ideal platform for developing effective and user-friendly diagnostic technologies for human health monitoring.

A mixed-coordination electron trapping-enabled high-precision touch-sensitive screen for wearable devices

Touch-sensitive screens are crucial components of wearable devices.Materials such as reduced graphene oxide(rGO),carbon nanotubes(CNTs),and graphene offer promising solutions for flexible touch-sensitive screens.However,when stacked with flexible substrates to form multilayered capacitive touching sensors,these materials often suffer from substrate delamination in response to deformation;this is due to the materials having different Young’s modulus values.Delamination results in failure to offer accurate touch screen recognition.In this work,we demonstrate an induced charge-based mutual capacitive touching sensor capable of high-precision touch sensing.This is enabled by electron trapping and polarization effects related to mixed-coordinated bonding between copper nanoparticles and vertically grown graphene nanosheets.Here,we used an electron cyclotron resonance system to directly fabricate graphene-metal nanofilms(GMNFs)using carbon and copper,which are firmly adhered to flexible substrates.After being subjected to 3000 bending actions,we observed almost no change in touch sensitivity.The screen interaction system,which has a signal-to-noise ratio of 41.16 dB and resolution of 650 dpi,was tested using a handwritten Chinese character recognition trial and achieved an accuracy of 94.82%.Taken together,these results show the promise of touch-sensitive screens that use directly fabricated GMNFs for wearable devices.

Multifunctional Flexible Humidity Sensor Systems Towards Noncontact Wearable Electronics

In the past decade,the global industry and research attentions on intelligent skin-like electronics have boosted their applications in diverse fields including human healthcare,Internet of Things,human–machine interfaces,artificial intelligence and soft robotics.Among them,flexible humidity sensors play a vital role in noncontact measurements relying on the unique property of rapid response to humidity change.This work presents an overview of recent advances in flexible humidity sensors using various active functional materials for contactless monitoring.Four categories of humidity sensors are highlighted based on resistive,capacitive,impedance-type and voltage-type working mechanisms.Furthermore,typical strategies including chemical doping,structural design and Joule heating are introduced to enhance the performance of humidity sensors.Drawing on the noncontact perception capability,human/plant healthcare management,human-machine interactions as well as integrated humidity sensor-based feedback systems are presented.The burgeoning innovations in this research field will benefit human society,especially during the COVID-19 epidemic,where cross-infection should be averted and contactless sensation is highly desired.

Flexible energy storage devices for wearable bioelectronics

With the growing market of wearable devices for smart sensing and personalized healthcare applications,energy storage devices that ensure stable power supply and can be constructed in flexible platforms have attracted tremendous research interests.A variety of active materials and fabrication strategies of flexible energy storage devices have been intensively studied in recent years,especially for integrated self-powered systems and biosensing.A series of materials and applications for flexible energy storage devices have been studied in recent years.In this review,the commonly adopted fabrication methods of flexible energy storage devices are introduced.Besides,recent advances in integrating these energy devices into flexible self-powered systems are presented.Furthermore,the applications of flexible energy storage devices for biosensing are summarized.Finally,the prospects and challenges of the self-powered sensing system for wearable electronics are discussed.

Rational Design of Cellulosic Triboelectric Materials for Self‑Powered Wearable Electronics

With the rapid development of the Internet of Things and flexible electronic technologies,there is a growing demand for wireless,sustainable,multifunctional,and independently operating self-powered wearable devices.Nevertheless,structural flexibility,long operating time,and wearing comfort have become key requirements for the widespread adoption of wearable electronics.Triboelectric nanogenerators as a distributed energy harvesting technology have great potential for application development in wearable sensing.Compared with rigid electronics,cellulosic self-powered wearable electronics have significant advantages in terms of flexibility,breathability,and functionality.In this paper,the research progress of advanced cellulosic triboelectric materials for self-powered wearable electronics is reviewed.The interfacial characteristics of cellulose are introduced from the top-down,bottom-up,and interfacial characteristics of the composite material preparation process.Meanwhile,the modulation strategies of triboelectric properties of cellulosic triboelectric materials are presented.Furthermore,the design strategies of triboelectric materials such as surface functionalization,interfacial structure design,and vacuum-assisted self-assembly are systematically discussed.In particular,cellulosic self-powered wearable electronics in the fields of human energy harvesting,tactile sensing,health monitoring,human–machine interaction,and intelligent fire warning are outlined in detail.Finally,the current challenges and future development directions of cellulosic triboelectric materials for self-powered wearable electronics are discussed.

Biological Tissue-Inspired Ultrasoft,Ultrathin,and Mechanically Enhanced Microfiber Composite Hydrogel for Flexible Bioelectronics

Hydrogels offer tissue-like softness,stretchability,fracture toughness,ionic conductivity,and compatibility with biological tissues,which make them promising candidates for fabricating flexible bioelectronics.A soft hydrogel film offers an ideal interface to directly bridge thin-film electronics with the soft tissues.However,it remains difficult to fabricate a soft hydrogel film with an ultrathin configuration and excellent mechanical strength.Here we report a biological tissue-inspired ultrasoft microfiber composite ultrathin(<5μm)hydrogel film,which is currently the thinnest hydrogel film as far as we know.The embedded microfibers endow the composite hydrogel with prominent mechanical strength(tensile stress~6 MPa)and anti-tearing property.Moreover,our microfiber composite hydrogel offers the capability of tunable mechanical properties in a broad range,allowing for matching the modulus of most biological tissues and organs.The incorporation of glycerol and salt ions imparts the microfiber composite hydrogel with high ionic conductivity and prominent anti-dehydration behavior.Such microfiber composite hydrogels are promising for constructing attaching-type flexible bioelectronics to monitor biosignals.

Low-temperature metal–oxide thin-film transistor technologies for implementing flexible electronic circuits and systems

Here we review two 300℃metal–oxide(MO)thin-film transistor(TFT)technologies for the implementation of flexible electronic circuits and systems.Fluorination-enhanced TFTs for suppressing the variation and shift of turn-on voltage(VON),and dual-gate TFTs for acquiring sensor signals and modulating VON have been deployed to improve the robustness and performance of the systems in which they are deployed.Digital circuit building blocks based on fluorinated TFTs have been designed,fabricated,and characterized,which demonstrate the utility of the proposed low-temperature TFT technologies for implementing flexible electronic systems.The construction and characterization of an analog front-end system for the acquisition of bio-potential signals and an active-matrix sensor array for the acquisition of tactile images have been reported recently.

Mass-producible low-cost flexible electronic fabrics for azo dye wastewater treatment by electrocoagulation

Electrocoagulation is progressively becoming an ecologically friendly water treatment method owing to its lack of secondary pollution,high active ingredient concentration,high treatment effectiveness,simple equipment,and simplicity of automated control implementation.Herein,electrocoagulation is offered as a method for treating wastewater containing azo dyes using a revolutionary flexible electronic fabric that can be mass-producible at a reasonable price.A computer-controlled machine embroiders 316L stainless steel fiber(316L SSF)onto an insulating fabric to manufacture a flexible electronic device of cathode and anode with a monopolar arrangement on the fabric surface.Using methyl orange(MO)solution to simulate azo dye wastewater,the decolorization rate of 500 ml MO reached 99.25% under the conditions of 50 mg·L^(-1)initial mass concentration,120 min electrolysis time,15 mA·g^(-1)current density,1 cm electrode spacing,0.1 mol·L^(-1)NaCl,pH 7.6,200 r·min^(-1)rotational speed of the stirrer,and 22-25℃ room temperature.In addition,it is feasible to embroider flexible electronic fabrics with varied sizes and numbers of electrodes based on the amount of treated sewage to increase the degradation rate,which has significant practical application value.

Artificial Intelligence Meets Flexible Sensors:Emerging Smart Flexible Sensing Systems Driven by Machine Learning and Artificial Synapses

The recent wave of the artificial intelligence(AI)revolution has aroused unprecedented interest in the intelligentialize of human society.As an essential component that bridges the physical world and digital signals,flexible sensors are evolving from a single sensing element to a smarter system,which is capable of highly efficient acquisition,analysis,and even perception of vast,multifaceted data.While challenging from a manual perspective,the development of intelligent flexible sensing has been remarkably facilitated owing to the rapid advances of brain-inspired AI innovations from both the algorithm(machine learning)and the framework(artificial synapses)level.This review presents the recent progress of the emerging AI-driven,intelligent flexible sensing systems.The basic concept of machine learning and artificial synapses are introduced.The new enabling features induced by the fusion of AI and flexible sensing are comprehensively reviewed,which significantly advances the applications such as flexible sensory systems,soft/humanoid robotics,and human activity monitoring.As two of the most profound innovations in the twenty-first century,the deep incorporation of flexible sensing and AI technology holds tremendous potential for creating a smarter world for human beings.

Progress of Proximity Sensors for Potential Applications in Electronic Skins

Recently,electronic skins and fl exible wearable devices have been developed for widespread applications in medical monitoring,artifi cial intelligence,human–machine interaction,and artifi cial prosthetics.Flexible proximity sensors can accurately perceive external objects without contact,introducing a new way to achieve an ultrasensitive perception of objects.This article reviews the progress of fl exible capacitive proximity sensors,fl exible triboelectric proximity sensors,and fl exible gate-enhanced proximity sensors,focusing on their applications in the electronic skin fi eld.Herein,their working mechanism,materials,preparation methods,and research progress are discussed in detail.Finally,we summarize the future challenges in developing fl exible proximity sensors.

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.

Wearable multilead ECG sensing systems using on-skin stretchable and breathable dry adhesives

Electrocardiogram(ECG)monitoring is used to diagnose cardiovascular diseases,for which wearable electronics have attracted much attention due to their lightweight,comfort,and long-term use.This study developed a wearablemultilead ECG sensing system with on-skin stretchable and conductive silver(Ag)-coated fiber/silicone(AgCF-S)dry adhesives.Tangential and normal adhesion to pigskin(0.43 and 0.20 N/cm2,respectively)was optimized by the active control of fiber density and mixing ratio,resulting in close contact in the electrode–skin interface.The breathableAgCF-S dry electrodewas nonallergenic after continuous fit for 24 h and can be reused/cleaned(>100 times)without loss of adhesion.The AgCF encapsulated inside silicone elastomers was overlapped to construct a dynamic network under repeated stretching(10%strain)and bending(90°)deformations,enabling small intrinsic impedance(0.3,0.1 Hz)and contact impedance variation(0.7 k)in high-frequency vibration(70 Hz).All hard/soft modules of the multilead ECG system were integrated into lightweight clothing and equipped with wireless transmission for signal visualization.By synchronous acquisition of I–III,aVR,aVL,aVF,and V4 lead data,the multilead ECG sensing system was suitable for various scenarios,such as exercise,rest,and sleep,with extremely high signal-to-noise ratios.

Inducing Fe 3d Electron Delocalization and Spin‑State Transition of FeN_(4) Species Boosts Oxygen Reduction Reaction for Wearable Zinc–Air Battery

Transition metal-nitrogen-carbon materials(M-N-Cs),particularly Fe-N-Cs,have been found to be electroactive for accelerating oxygen reduction reaction(ORR)kinetics.Although substantial efforts have been devoted to design Fe-N-Cs with increased active species content,surface area,and electronic conductivity,their performance is still far from satisfactory.Hitherto,there is limited research about regulation on the electronic spin states of Fe centers for Fe-N-Cs electrocatalysts to improve their catalytic performance.Here,we introduce Ti_(3)C_(2) MXene with sulfur terminals to regulate the electronic configuration of FeN_(4) species and dramatically enhance catalytic activity toward ORR.The MXene with sulfur terminals induce the spin-state transition of FeN_(4) species and Fe 3d electron delocalization with d band center upshift,enabling the Fe(II)ions to bind oxygen in the end-on adsorption mode favorable to initiate the reduction of oxygen and boosting oxygen-containing groups adsorption on FeN_(4) species and ORR kinetics.The resulting FeN_(4)-Ti_(3)C_(2)Sx exhibits comparable catalytic performance to those of commercial Pt-C.The developed wearable ZABs using FeN_(4)-Ti_(3)C_(2)Sx also exhibit fast kinetics and excellent stability.This study confirms that regulation of the electronic structure of active species via coupling with their support can be a major contributor to enhance their catalytic activity.

Cross-linked polyelectrolyte reinforced SnO_(2)electron transport layer for robust flexible perovskite solar cells

SnO_(2)electron transport layer(ETL)is a vital component in perovskite solar cells(PSCs),due to its excellent photoelectric properties and facile fabrication process.In this study,we synthesized a water-soluble and adhesive polyelectrolyte with ethanolamine(EA)and poly-acrylic acid(PAA).The linear PAA was crosslinked by EA,forming a 3D network that stabilized the SnO_(2)nanoparticle dispersion.An organic–inorganic hybrid ETL is developed by introducing the cross-linked PAA-EA into SnO_(2)ETL,which prevents nano particle agglomeration and facilitates uniform SnO_(2)film formation with fewer defects.Additionally,the PAA-EA-modified SnO_(2)facilitated a uniform and compact perovskite film,enhancing the interface contact and carrier transport.Consequently,the PAA-EA-modified PSCs exhibited excellent PCE of 24.34%and 22.88%with high reproducibility for areas of 0.045 and 1.00 cm~2,respectively.Notably,owing to structure reinforce effect of PAA-EA in SnO_(2)ETL,flexible device demonstrated an impressive PCE of 23.34%while maintaining 90.1%of the initial PCE after 10,000 bending cycles with a bending radius of 5 mm.This successful approach of polyelectrolyte reinforced hybrid organic–inorganic ETL displays great potential for flexible,large-area PSCs application.

Flexible Tactile Electronic Skin Sensor with 3D Force Detection Based on Porous CNTs/PDMS Nanocomposites

Flexible tactile sensors have broad applications in human physiological monitoring,robotic operation and human-machine interaction.However,the research of wearable and flexible tactile sensors with high sensitivity,wide sensing range and ability to detect three-dimensional(3D)force is still very challenging.Herein,a flexible tactile electronic skin sensor based on carbon nanotubes(CNTs)/polydimethylsiloxane(PDMS)nanocomposites is presented for 3D contact force detection.The 3D forces were acquired from combination of four specially designed cells in a sensing element.Contributed from the double-sided rough porous structure and specific surface morphology of nanocomposites,the piezoresistive sensor possesses high sensitivity of 12.1 kPa?1 within the range of 600 Pa and 0.68 kPa?1 in the regime exceeding 1 kPa for normal pressure,as well as 59.9 N?1 in the scope of<0.05 N and>2.3 N?1 in the region of<0.6 N for tangential force with ultra-low response time of 3.1 ms.In addition,multi-functional detection in human body monitoring was employed with single sensing cell and the sensor array was integrated into a robotic arm for objects grasping control,indicating the capacities in intelligent robot applications.

Functionalized Fiber-Based Strain Sensors:Pathway to Next-Generation Wearable Electronics

Wearable strain sensors are arousing increasing research interests in recent years on account of their potentials in motion detection,personal and public healthcare,future entertainment,man-machine interaction,artificial intelligence,and so forth.Much research has focused on fiber-based sensors due to the appealing performance of fibers,including processing flexibility,wearing comfortability,outstanding lifetime and serviceability,low-cost and large-scale capacity.Herein,we review the latest advances in functionalization and device fabrication of fiber materials toward applications in fiber-based wearable strain sensors.We describe the approaches for preparing conductive fibers such as spinning,surface modification,and structural transformation.We also introduce the fabrication and sensing mechanisms of state-of-the-art sensors and analyze their merits and demerits.The applications toward motion detection,healthcare,man-machine interaction,future entertainment,and multifunctional sensing are summarized with typical examples.We finally critically analyze tough challenges and future remarks of fiber-based strain sensors,aiming to implement them in real applications.

Recent Progress of MXene-Based Nanomaterials in Flexible Energy Storage and Electronic Devices

The increasing demands for wearable electronics have stimulated the rapid development of flexible energy storage devices.MXenes are considered as promising flexible electrodes due to the ultrahigh volumetric specific capacitance,metallic conductivity,superior hydrophily,and rich surface chemistry.