Wearable and stretchable conductive polymer composites for strain sensors:How to design a superior one?

Wearable and stretchable strain sensors have potential values in the fields of human motion and health monitoring,flexible electronics,and soft robotic skin.The wearable and stretchable strain sensors can be directly attached to human skin,providing visualized detection for human motions and personal healthcare.Conductive polymer composites(CPC)composed of conductive fillers and flexible polymers have the advantages of high stretchability,good flexibility,superior durability,which can be used to prepare flexible strain sensors with large working strain and outstanding sensitivity.This review has put forward a comprehensive summary on the fabrication methods,advanced mechanisms and strain sensing abilities of CPC strain sensors reported in recent years,especially the sensors with superior performance.Finally,the structural design,bionic function,integration technology and further application of CPC strain sensors are prospected.

High energy density in ultra-thick and flexible electrodes enabled by designed conductive agent/binder composite

Thick electrodes can increase incorporation of active electrode materials by diminishing the proportion of inactive constituents,improving the overall energy density of batteries.However,thick electrodes fabricated using the conventional slurry casting approach frequently exhibit an exacerbated accumulation of carbon additives and binders on their surfaces,invariably leading to compromised electrochemical properties.In this study,we introduce a designed conductive agent/binder composite synthesized from carbon nanotube and polytetrafluoroethylene.This agent/binder composite facilitates production of dry-process-prepared ultra-thick electrodes endowed with a three-dimensional and uniformly distributed percolative architecture,ensuring superior electronic conductivity and remarkable mechanical resilience.Using this approach,ultra-thick LiCoO_(2)(LCO) electrodes demonstrated superior cycling performance and rate capabilities,registering an impressive loading capacity of up to 101.4 mg/cm^(2),signifying a 242% increase in battery energy density.In another analytical endeavor,time-of-flight secondary ion mass spectroscopy was used to clarify the distribution of cathode electrolyte interphase(CEI) in cycled LCO electrodes.The results provide unprecedented evidence explaining the intricate correlation between CEI generation and carbon distribution,highlighting the intrinsic advantages of the proposed dry-process approach in fine-tu ning the CEI,with excellent cycling performance in batteries equipped with ultra-thick electrodes.

Breaking Through Bottlenecks for Thermally Conductive Polymer Composites:A Perspective for Intrinsic Thermal Conductivity,Interfacial Thermal Resistance and Theoretics

Rapid development of energy,electrical and electronic technologies has put forward higher requirements for the thermal conductivities of polymers and their composites.However,the thermal conductivity coefficient(λ)values of prepared thermally conductive polymer composites are still difficult to achieve expectations,which has become the bottleneck in the fields of thermally conductive polymer composites.Aimed at that,based on the accumulation of the previous research works by related researchers and our research group,this paper proposes three possible directions for breaking through the bottlenecks:(1)preparing and synthesizing intrinsically thermally conductive polymers,(2)reducing the interfacial thermal resistance in thermally conductive polymer composites,and(3)establishing suitable thermal conduction models and studying inner thermal conduction mechanism to guide experimental optimization.Also,the future development trends of the three above-mentioned directions are foreseen,hoping to provide certain basis and guidance for the preparation,researches and development of thermally conductive polymers and their composites.

Flexible Polydimethylsiloxane Composite with Multi-Scale Conductive Network for Ultra-Strong Electromagnetic Interference Protection

Highly conductive polymer composites(CPCs) with excellent mechanical flexibility are ideal materials for designing excellent electromagnetic interference(EMI) shielding materials,which can be used for the electromagnetic interference protection of flexible electronic devices.It is extremely urgent to fabricate ultra-strong EMI shielding CPCs with efficient conductive networks.In this paper,a novel silver-plated polylactide short fiber(Ag@PL ASF,AAF) was fabricated and was integrated with carbon nanotubes(CNT) to construct a multi-scale conductive network in polydimethylsiloxane(PDMS) matrix.The multi-scale conductive network endowed the flexible PDMS/AAF/CNT composite with excellent electrical conductivity of 440 S m-1and ultra-strong EMI shielding effectiveness(EMI SE) of up to 113 dB,containing only 5.0 vol% of AAF and 3.0 vol% of CNT(11.1wt% conductive filler content).Due to its excellent flexibility,the composite still showed 94% and 90% retention rates of EMI SE even after subjected to a simulated aging strategy(60℃ for 7 days) and 10,000 bending-releasing cycles.This strategy provides an important guidance for designing excellent EMI shielding materials to protect the workspace,environment and sensitive circuits against radiation for flexible electronic devices.

Piezoresistive behavior of elastomer composites with segregated network of carbon nanostructures and alumina

Electrically conductive elastomer composites(CECs)with segregated networks of conductive nanofillers show high potential in stretchable strain sensors due to balanced mechanical and electrical properties,yet the sensitivity at low strain is generally insufficient for practical application.Herein,we report an easy and effective way to improve the resistive response to low strain for CECs with segregated network structure via adding stiff alumina into carbon nanostructures(CNS).The CEC containing 0.7 wt%CNS and 5 wt%Al_(2)O_(3) almost sustains the same elasticity(elongation at break of~900%)and conductivity(0.8 S/m)as the control,while the piezoresistive sensitivity is significantly improved.Thermoplastic polyurethane(TPU)composites with a segregated network of hybrid nanofillers(CNS and Al_(2)O_(3))show much higher strain sensitivity(Gauge factor,GF-566)at low strain(45%strain)due to a local stress concentration effect,this sensitivity is superior to that of TPU/CNS composites(GF-11).Such a local stress concentration effect depends on alumina content and its distribution at the TPU particle interface.In addition,CECs with hybrid fillers show better reproducibility in cyclic piezoresistive behavior testing than the control.This work offers an easy method for fabricating CECs with a segregated filler network offering stretchable strain sensors with a high strain sensitivity.

Highly Elastic,Bioresorbable Polymeric Materials for Stretchable,Transient Electronic Systems

Substrates or encapsulants in soft and stretchable formats are key components for transient,bioresorbable electronic systems;however,elastomeric polymers with desired mechanical and biochemical properties are very limited compared to nontransient counterparts.Here,we introduce a bioresorbable elastomer,poly(glycolide-co-ε-caprolactone)(PGCL),that contains excellent material properties including high elongation-at-break(<1300%),resilience and toughness,and tunable dissolution behaviors.Exploitation of PGCLs as polymer matrices,in combination with conducing polymers,yields stretchable,conductive composites for degradable interconnects,sensors,and actuators,which can reliably function under external strains.Integration of device components with wireless modules demonstrates elastic,transient electronic suture system with on-demand drug delivery for rapid recovery of postsurgical wounds in soft,time-dynamic tissues.

Highly Flexible Fabrics/Epoxy Composites with Hybrid Carbon Nanofillers for Absorption-Dominated Electromagnetic Interference Shielding

Epoxy-based nano-composites can be ideal electromagnetic interference(EMI)-shielding materials owing to their lightness,chemical inertness,and mechanical durability.However,poor conductivity and brittleness of the epoxy resin are challenges for fast-growing portable and flexible EMI-shielding applications,such as smart wristband,medical cloth,aerospace,and military equipment.In this study,we explored hybrid nanofillers of single-walled carbon nanotubes(SWCNT)/reduced graphene oxide(rGO)as conductive inks and polyester fabrics(PFs)as a substrate for flexible EMI-shielding composites.The highest electrical conductivity and fracture toughness of the SWCNT/rGO/PF/epoxy composites were 30.2 S m^(−1)and 38.5 MPa m^(1/2),which are~270 and 65%enhancement over those of the composites without SWCNTs,respectively.Excellent mechanical durability was demonstrated by stable electrical conductivity retention during 1000 cycles of bending test.An EMI-shielding effectiveness of~41 dB in the X-band frequency of 8.2-12.4 GHz with a thickness of 0.6 mm was obtained with an EM absorption-dominant behavior over a 0.7 absorption coefficient.These results are attributed to the hierarchical architecture of the macroscale PF skeleton and nanoscale SWCNT/rGO networks,leading to superior EMI-shielding performance.We believe that this approach provides highly flexible and robust EMI-shielding composites for next-generation wearable electronic devices.

Enabling high-performance all-solid-state lithium batteries with high ionic conductive sulfide-based composite solid electrolyte and ex-situ artificial SEI film

All-solid-state lithium batteries(ASSLBs) employing sulfide electrolyte and lithium(Li) anode have received increasing attention due to the intrinsic safety and high energy density.However,the thick electrolyte layer and lithium dendrites formed at the electrolyte/Li anode interface hinder the realization of high-performance ASSLBs.Herein,a novel membrane consisting of Li_(6)PS_(5) Cl(LPSCl),poly(ethylene oxide)(PEO) and Li-salt(LiTFSI) was prepared as sulfide-based composite solid electrolyte(LPSCl-PEO3-LiTFSI)(LPSCl:PEO=97:3 wt/wt;EO:Li=8:1 mol/mol),which delivers high ionic conductivity(1.1 × 10^(-3) S cm^(-1)) and wide electrochemical window(4.9 V vs.Li^(+)/Li) at 25 ℃.In addition,an ex-situ artificial solid electrolyte interphase(SEI) film enriched with LiF and Li3 N was designed as a protective layer on Li anode(Li(SEI)) to suppress the growth of lithium dendrites.Benefiting from the synergy of sulfide-based composite solid electrolyte and ex-situ artificial SEI,cells of S-CNTs/LPSCI-PEO3-LiTFSI/Li(SEI) and Al_(2)O_(3)@LiNi_(0.5)Co_(0.3)Mn_(0.2)O_(2)/LPSCl-PEO3-LiTFSI/Li(SEI) are assembled and both exhibit high initial discharge capacity of 1221.1 mAh g^(-1)(135.8 mAh g^(-1)) and enhanced cycling stability with 81.6% capacity retention over 200 cycles at 0.05 C(89.2% over 100 cycles at 0.1 C).This work provides a new insight into the synergy of composite solid electrolyte and artificial SEI for achieving high-performance ASSLBs.

Tetris-Style Stacking Process to Tailor the Orientation of Carbon Fiber Scaffolds for Efficient Heat Dissipation

As the miniaturization of electronic devices and complication of electronic packaging,there are growing demands for thermal interfacial materials with enhanced thermal conductivity and the capability to direct the heat toward heat sink for highly efficient heat dissipation.Pitch-based carbon fiber(CF)with ultrahigh axial thermal conductivity and aspect ratios exhibits great potential for developing thermally conductive composites as TIMs.However,it is still hard to fabricate composites with aligned carbon fiber in a general approach to fully utilize its excellent axial thermal conductivity in specific direction.Here,three types of CF scaffolds with different oriented structure were developed via magnetic field-assisted Tetris-style stacking and carbonization process.By regulating the magnetic field direction and initial stacking density,the self-supporting CF scaffolds with horizontally aligned(HCS),diagonally aligned and vertically aligned(VCS)fibers were constructed.After embedding the polydimethylsiloxane(PDMS),the three composites exhibited unique heat transfer properties,and the HCS/PDMS and VCS/PDMS composites presented a high thermal conductivity of 42.18 and 45.01 W m^(−1)K^(−1)in fiber alignment direction,respectively,which were about 209 and 224 times higher than that of PDMS.The excellent thermal conductivity is mainly ascribed that the oriented CF scaffolds construct effective phonon transport pathway in the matrix.In addition,fishbone-shaped CF scaffold was also produced by multiple stacking and carbonization process,and the prepared composites exhibited a controlled heat transfer path,which can allow more versatility in the design of thermal management system.

Thermally Conductive,Healable Glass Fiber Cloth Reinforced Polymer Composite based onβ-Hydroxyester Bonds Crosslinked Epoxy with Improved Heat Resistance

To simultaneously endow thermal conductivity,high glass transition temperature(Tg)and healing capability to glass fiber/epoxy(GFREP)composite,dynamic crosslinked epoxy resin bearing reversibleβ-hydroxyl ester bonds was reinforced with boron nitride nanosheets modified glass fiber cloth(GFC@BNNSs).The in-plane heat conduction paths were constructed by electrostatic self-assembly of polyacrylic acid treated GFC and polyethyleneimine decorated BNNSs.Then,the GFC@BNNSs were impregnated with the mixture of lower concentration(3-glycidyloxypropyl)trimethoxysilane grafted BN micron sheets,3,4-epoxycyclohexylmethyl 3,4-epoxycyclohexanecarboxylate and hexahydro-4-methylphthalic anhydride,which accounted for establishing the through-plane heat transport pathways and avoiding serious deterioration of mechanical performances.The resultant GFREP composite containing less boron nitride particles(17.6 wt%)exhibited superior in-plane(3.29 W·m^(-1)·K^(-1))and through-plane(1.16 W·m^(-1)·K^(-1))thermal conductivities,as well as high Tg of 204℃(Tg of the unfilled epoxy=177℃).The reversible transesterification reaction enabled closure of interlaminar cracks within the composite,achieving decent healing efficiencies estimated by means of tensile strength(71.2%),electrical breakdown strength(83.6%)and thermal conductivity(69.1%).The present work overcame the disadvantages of conventional thermally conductive composites,and provided an efficient approach to prolong the life span of thermally conductive GFREP laminate for high-temperature resistant integrated circuit application.

Thermally Conductive and Insulating Epoxy Composites by Synchronously Incorporating Si-sol Functionalized Glass Fibers and Boron Nitride Fillers

Glass fibers(GFs)/epoxy laminated composites always present weak interlaminar shear strength(ILSS)and low cross-plane thermal conductivity coefficient(λ⊥).In this work,silica-sol,synthesized from tetraethyl orthosilicate(TEOS)and KH-560 via sol-gel method,was employed to functionalize the surface of GFs(Si-GFs).Together with a spherical boron nitride(BNN-30),the thermally conductive BNN-30/Si-GFs/epoxy laminated composites were then fabricated.Results demonstrate that Si-sol is beneficial to the improvement of mechanical properties for epoxy laminated composites(especially for ILSS).The BNN-30/Si-GFs/epoxy laminated composites with 15 wt%BNN-30 fillers display the optimal comprehensive properties.In-planeλ(λ//)andλ⊥reach the maximum of 2.37 and 1.07 W.m-1.K-1,146.9%and 132.6%higher than those of SiGFs/epoxy laminated composites(λ//=0.96 W.m-1.K-1 andλ⊥=0.46 W.m-1K-1),respectively,and also about 10.8 and 4.9 times those of pure epoxy resin(λ//=λ⊥,0.22 W.m-1.K-1).And the heat-resistance index(THRI),dielectric constant(ε),dielectric loss(tanδ),breakdown strength(E0),surface resistivity(ρs)as well as volume resistivity(ρv)are 197.3℃,4.95,0.0046,22.3 kV.mm-1,1.8×1014Ω,and 2.1×1014Ω.cm,respectively.

Polymer-based EMI shielding composites with 3D conductive networks:A mini-review

High-frequency electromagnetic waves and electronic products can bring great convenience to people’s life,but lead to a series of electromagnetic interference(EMI)problems,such as great potential dangers to the normal operation of elec-tronic components and human safety.Therefore,the research of EMI shield-ing materials has attracted extensive attention by the scholars.Among them,polymer-based EMI shielding materials with light weight,high specific strength,and stable properties have become the current mainstream.The construction of 3D conductive networks has proved to be an effective method for the prepara-tion of polymer-based EMI shielding materials with excellent shielding effective-ness(SE).In this paper,the shielding mechanism of polymer-based EMI shield-ing materials with 3D conductive networks is briefly introduced,with emphasis on the preparation methods and latest research progress of polymer-based EMI shielding materials with different 3D conductive networks.The key scientific and technical problems to be solved in the field of polymer-based EMI shielding materials are also put forward.Finally,the development trend and application prospects of polymer-based EMI shielding materials are prospected.

Flexible conductive polymer composites for smart wearable strain sensors

Wearable strain sensors based on flexible conductive polymer composites(FCPCs)have attracted great attention due to their applications in the fields of human–machine interaction,disease diagnostics,human motion detection,and soft robotic skin.In recent decades,FCPC‐based strain sensors with high stretchability and sensitivity,short response time,and excellent stability have been developed,which are expected to be more versatile and intelligent.Smart strain sensors are required to provide wearable comfort,such as breathability,selfcooling ability,and so forth.To adapt to the harsh environment,wearable strain sensors should also be highly adaptive to protect the skin and the sensor itself.In addition,portable power supply system,multisite sensing capability,and multifunctionality are crucial for the next generation of FCPC‐based strain sensor.

Recent Progress in All-Solution-Processed Organic Solar Cells

All-solution-processed organic solar cells(OSCs)(from the bottom electrode to the top electrode)are highly attractive thanks to their low cost,lightweight and high-throughput production.However,achieving highly efficient all-solution-processed OSCs remains a significant challenge.One of the key issues is the lack of high-quality solution-processed electrode systems that can replace indium tin oxide(ITO)and vacuum-deposited metal electrodes.In this paper,we comprehensively review recent advances in all-solution-processed osCs,and classified the devices as the top electrode materials,including silver nanowires(AgNWs),conducting polymers and composite conducting materials.The correlation between electrode materials,properties of electrodes,and device performance in all-solution-processed OSCs is elucidated.In addition,the critical roles of the active layer and interface layer are also discussed.Finally,the prospects and challenges of all-solution-processed OSCs are presented.

Avoiding heating interference and guided thermal conduction in stretchable devices using thermal conductive composite islands

The miniaturization and high integration of devices demand significant thermal management materials.Current technologies for the thermal management of electronics show some limitations in the case of multiple chip arrays.A device in multiple chip array is affected by heat from adjacent devices,along with thermal conductive composite.To address this problem,we present a nano composite of aligned boron nitride(BN)nanosheet islands with porous polydimethylsiloxane(PDMS)foam to have mechanical stability and non-thermal interference.The islands of tetrahedrally-structured BN in the composite have a high thermal conductivity of 1.219 W·m^(-1)·K^(-1) in the through-plane direction(11.234W·m^(-1)·K^(-1)in the in-plane direction)with 16 wt.%loading of BN.On the other hand,porous PDMS foam has a low thermal conductivity of 0.0328W·m^(-1)·K^(-1) in the through-plane direction at 70%porosity.Heat pathways are then formed only in the structured BN islands of the composite.The porous PDMS foam can be applied as a thermal barrier between structured BN islands to inhibit thermal interference in multiple device arrays.Furthermore,this composite can maintain selective thermal dissipation performance with 70%tensile strain.Another beauty of the work is that it could have guided heat dissipation by assembling of multiple layers which have high vertical thermal conductive islands,while inhibiting thermal interference.The selective heat dissipating composite can be applied as a heatsink for multiple chip arrays electronics.

Influence of conductive network composite structure on the electromechanical performance of ionic electroactive polymer actuators

The influence of the nanostructure of the conductive network composite(CNC)on the performance of ionic electroactive polymer(IEAP)actuators has been examined in detail.We have studied IEAP actuators consisting of CNCs with different volume densities of gold nanoparticles(AuNPs)and the polymer network.Varying the concentration of AuNPs in CNC thin films was used as a means to control the CNC-ion interfacial area and the electrical resistance of the CNC,with minimum effect on the mechanical properties of the actuator.Increasing the interfacial area and reducing the resistance,while maintaining porosity of the composite,provide means for generating motion of more ions into the CNC at a significantly shorter time,which results in generation of strain at a faster rate.We have demonstrated that cationic strain in actuators with denser CNCs is improved by more than 460%.Denser CNC structures have larger interfacial areas,which results in attraction/repulsion of more ions in a shorter time,thus generation of a larger mechanical strain at a faster rate.Also,time-dependent response to a square-wave voltage was improved by increasing the AuNP concentration in the CNC.Under 0.1 Hz frequency,the cationic strain was increased by 64%when the AuNP concentration was increased from 4 to 20 ppm.

Enhanced Reproducibility of Positive Temperature Coefficient Effect of CB/HDPE/PVDF Composites with the Addition of Ionic Liquid

Developing an effective method for improving the reproducibility of positive temperature coefficient(PTC)effect is of great significance for large-scale application of polymer based PTC composites,owing to its contribution to the security and reliability.Herein,we developed a carbon black(CB)/high density polyethylene(HDPE)/poly(vinylidene fluoride)(PVDF)composite with outstanding PTC reproducibility,by incorporating 1-octyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([OMIm][NTf2])into the composite.After multiple repeated temperature cycles,the PTC performance of as-prepared material keeps almost unchanged and the varition of resistance at room temperature is less than 7%.Our studies revealed that[OMIm][NTf2]contributes to the improvement of PTC reproducibility in two ways:(i)it acts as an efficient plasticizer for refining the co-continuous phase morphology of HDPE/PVDE blends;(ii)it inhibits the crystallization of PVDF through the dilution effect,leading to more overlaps of the volume shrinkage process of HDPE and PVDF melt which results in the decrease of interface gap between HDPE and PVDF.This study demonstrated that ionic liquids as the multifunctional agents have great potential for improving the reproducibility in the application of the binary polymer based PTC composites.

Silk Fibroin Based Conductive Film for Multifunctional Sensing and Energy Harvesting

Development of biomaterial based flexible electronics has got intensive attention owing to the potential applications in the wearable and epidermal devices.Silk fibroin,as a natural textile material with excellent performance,has been widely concerned by industry and academy.However,the property of electrical insulation limits his development in the field of flexible electronics.In this paper,a regenerated silk fibroin/carbon nanotube(RSF/CNT)conductive film has been successfully fabricated and applied in flexible capacitive-type pressure sensor and wearable triboelectric nanogenerator by a facile method.The electrical conductivity and mechanical property of RSF/CNT film was optimized by investigating with different composite ratio from 10 to 90%(W_(RSF)/W_(CNT)).The RSF/CNT film has a good photothermal response and electric heating performance.We furtherly demonstrated that the RSF/CNT based sensor can be used as epidermal self-powered sensor for multifunction human motion monitoring and Morse code compilation.The observed research results have shown that the RSF/CNT film has a wide range of potential application prospects in the wearable electronics field.

3D打印调控铜线/聚乳酸复合材料的导热通路长度和数量

导热通路对理解导热高分子复合材料的导热行为至关重要,但目前有关导热通路属性(长度、数量)对高分子复合材料导热系数的影响机制缺乏深入研究.本文采用3D打印技术制备了铜线(Cw)导热通路长度和数量可控的一维铜线/聚乳酸(1D-Cw/PLA)导热复合材料,建立了针对一维导热通路的高分子复合材料的导热模型,明晰了其导热通路属性与其导热性能的定量关系.相同Cw用量下,1D-Cw/PLA导热复合材料的面内导热系数与导热通路的数量和长度呈正相关.采用本文构建的导热模型和经验方程对1D-Cw/PLA复合材料的导热系数进行预测,95%的置信度表明预测值与实测值无显著差异.

L.S.gratefully acknowledges the financial support from the Engineering and Physical Sciences Research Council(Nos.EP/L022559/1,EP/L022559/2,EP/V050311/1,and EP/W004399/1);Royal Society(Nos.RG130230 and IE161214);H2020 Marie Skłodowska-Curie Actions(No.790666);J.S.Z.was supported by a PhD Studentship provided by Queen Mary University of London and China Scholarship Council(CSC).

Advanced energy and sensor devices with novel applications(e.g.,mobile equipment,electric vehicles,and medical-healthcare systems)are one of the important foundations of modern intelligent life.However,there are still some scientific issues that seriously hinder the further development of devices,including unsustainability,high material cost,complex fabrication process,safety issues,and unsatisfactory performance.Nanocellulose has aroused tremendous attention in recent decades,because of its abundant resources,renewability,degradability,low-cost,and unique physical/chemical properties.These merits make nanocellulose as matrix materials to fabricate advanced functional composites for use in energy-related fields extremely competitive.Here,we comprehensively discuss the recent progress of nanocellulose for emerging energy storage/harvesting and sensor applications.The preparation methodologies of nanocellulose combined with conductive materials are firstly highlighted,including carbon materials,conductive polymers,metal/metal oxide nanoparticles,metal-organic frameworks(MOFs),and covalent organic frameworks(COFs).We then focus on the nanocellulose-based advanced materials for the application in the areas of supercapacitors,lithium-ion batteries,solar cells,triboelectric nanogenerators,moisture-enabled electric generators,and sensors.Lastly,the future research directions of nanocellulose-based functional materials in energy-related devices are presented.