Electrofluids with Tailored Rheoelectrical Properties: Liquid Composites with Tunable Network Structures as Stretchable Conductors.

Flexible and stretchable electronics require both sensing elements and stretching-insensitive electrical connections. Conductive polymer composites and liquid metals are highly deformable but change their conductivity upon elongation and/or contain rare metals. Solid conductive composites are limited in mechanoelectrical properties and are often combined with macroscopic Kirigami structures, but their use is limited by geometrical restraints. Here, we introduce "Electrofluids", concentrated conductive particle suspensions with transient particle contacts that flow under shear that bridge the gap between classic solid composites and liquid metals. We show how Carbon Black (CB) forms large agglomerates when using incompatible solvents that reduce the electrical percolation threshold by 1 order of magnitude compared to more compatible solvents, where CB is well-dispersed. We analyze the correlation between stiffness and electrical conductivity to create a figure of merit of first electrofluids. Sealed elastomeric tubes containing different types of electrofluids were characterized under uniaxial tensile strain, and their electrical resistance was monitored. We found a dependency of the piezoresistivity with the solvent compatibility. Electrofluids enable the rational design of sustainable soft electronics components by simple solvent choice and can be used both as sensor and electrode materials, as we demonstrate.

Construction of Hierarchical Conductive Networks for LiNi0.8Mn0.1Co0.1O2 Cathode toward Stable Cycling at High Areal Mass Loadings.

Realizing high-performance thick electrodes is considered as a practical strategy to promote the energy density of lithium-ion batteries. However, establishing effective transport pathways for both lithium-ions and electrons in a thick electrode is very challenging. This study develops a hierarchical conductive network structure for constructing high-performance NMC811 (LiNi0.8Mn0.1Co0.1O2) cathode toward stable cycling at high areal mass loadings. The hierarchical conductive networks are composed of a Li+/e- mixed conducting interface (lithium polyacrylate/hydroxyl-functionalized multiwalled carbon nanotubes) on NMC811 particles, and a segregated network of single-walled carbon nanotubes in the electrode, without any additional binders or carbon black. Such strategy endows the NMC811 cathode (up to 250 µm and 50 mg cm-2) with low porosity/tortuosity, ultrahigh Li+/e- conductivities and excellent mechanical property at low carbon nanotube content (1.8 wt%). It significantly improves the electrochemical reaction homogeneity along the electrode depth, meanwhile effectively inhibits the side reactions at the electrode/electrolyte interface and cracks in the NMC particles during cycling. This work emphasizes the crucial role of the electronic/ionic cooperative transportation in the performance deterioration of thick cathodes, and provide guidance for architecture optimization and performance improvement of thick electrodes toward practical applications, not just for the NMC811 cathode.

Stabilizing the Bulk-Phase and Solid Electrolyte Interphase of Silicon Microparticle Anode by Constructing Gradient-Hierarchically Ordered Conductive Networks.

The poor bulk-phase and interphase stability, attributable to adverse internal stress, impede the cycling performance of silicon microparticles (µSi) anodes and the commercial application for high-energy-density lithium-ion batteries. In this work, a groundbreaking gradient-hierarchically ordered conductive (GHOC) network structure, ingeniously engineered to enhance the stability of both bulk-phase and the solid electrolyte interphase (SEI) configurations of µSi, is proposed. Within the GHOC network architecture, two-dimensional (2D) transition metal carbides (Ti3C2Tx) act as a conductive "brick", establishing a highly conductive inner layer on µSi, while the porous outer layer, composed of one-dimensional (1D) Tempo-oxidized cellulose nanofibers (TCNF) and polyacrylic acid (PAA) macromolecule, functions akin to structural "rebar" and "concrete", effectively preserves the tightly interconnected conductive framework through multiple bonding mechanisms, including covalent and hydrogen bonds. Additionally, Ti3C2Tx enhances the development of a LiF-enriched SEI. Consequently, the µSi-MTCNF-PAA anode presents a high discharge capacity of 1413.7 mAh g-1 even after 500 cycles at 1.0 C. Moreover, a full cell, integrating LiNi0.8Mn0.1Co0.1O2 with µSi-MTCNF-PAA, exhibits a capacity retention rate of 92.0% following 50 cycles. This GHOC network structure can offer an efficacious pathway for stabilizing both the bulk-phase and interphase structure of anode materials with high volumetric strain.

Advances in Monte Carlo Method for Simulating the Electrical Percolation Behavior of Conductive Polymer Composites with a Carbon-Based Filling.

Conductive polymer composites (CPCs) filled with carbon-based materials are widely used in the fields of antistatic, electromagnetic interference shielding, and wearable electronic devices. The conductivity of CPCs with a carbon-based filling is reflected by their electrical percolation behavior and is the focus of research in this field. Compared to experimental methods, Monte Carlo simulations can predict the conductivity and analyze the factors affecting the conductivity from a microscopic perspective, which greatly reduces the number of experiments and provides a basis for structural design of conductive polymers. This review focuses on Monte Carlo models of CPCs with a carbon-based filling. First, the theoretical basis of the model's construction is introduced, and a Monte Carlo simulation of the electrical percolation behaviors of spherical-, rod-, disk-, and hybridfilled polymers and the analysis of the factors influencing the electrical percolation behavior from a microscopic point of view are summarized. In addition, the paper summarizes the progress of polymer piezoresistive models and polymer foaming structure models that are more relevant to practical applications; finally, we discuss the shortcomings and future research trends of existing Monte Carlo models of CPCs with carbon-based fillings.

Pathways toward wearable and high-performance sensors based on hydrogels: toughening networks and conductive networks.

Wearable hydrogel sensors provide a user-friendly option for wearable electronics and align well with the existing manufacturing strategy for connecting and communicating with large numbers of Internet of Things devices. This is attributed to their components and structures, which exhibit exceptional adaptability, scalability, bio-compatibility, and self-healing properties, reminiscent of human skin. This review focuses on the recent research on principal structural elements of wearable hydrogels: toughening networks and conductive networks, highlighting the strategies for enhancing mechanical and electrical properties. Wearable hydrogel sensors are categorized for an extensive exploration of their composition, mechanism, and design approach. This review provides a comprehensive understanding of wearable hydrogels and offers guidance for the design of components and structures in order to develop high-performance wearable hydrogel sensors.

Laser-Formed Sensors with Electrically Conductive MWCNT Networks for Gesture Recognition Applications.

Currently, an urgent need in the field of wearable electronics is the development of flexible sensors that can be attached to the human body to monitor various physiological indicators and movements. In this work, we propose a method for forming an electrically conductive network of multi-walled carbon nanotubes (MWCNT) in a matrix of silicone elastomer to make stretchable sensors sensitive to mechanical strain. The electrical conductivity and sensitivity characteristics of the sensor were improved by using laser exposure, through the effect of forming strong carbon nanotube (CNT) networks. The initial electrical resistance of the sensors obtained using laser technology was ~3 kOhm (in the absence of deformation) at a low concentration of nanotubes of 3 wt% in composition. For comparison, in a similar manufacturing process, but without laser exposure, the active material had significantly higher values of electrical resistance, which was ~19 kOhm in this case. The laser-fabricated sensors have a high tensile sensitivity (gauge factor ~10), linearity of >0.97, a low hysteresis of 2.4%, tensile strength of 963 kPa, and a fast strain response of 1 ms. The low Young's modulus values of ~47 kPa and the high electrical and sensitivity characteristics of the sensors made it possible to fabricate a smart gesture recognition sensor system based on them, with a recognition accuracy of ~94%. Data reading and visualization were performed using the developed electronic unit based on the ATXMEGA8E5-AU microcontroller and software. The obtained results open great prospects for the application of flexible CNT sensors in intelligent wearable devices (IWDs) for medical and industrial applications.

Reconfigurable Electrical Networks within a Conductive Hydrogel Composite.

Soft materials that exhibit compliance, programmability, and reconfigurability can have a transformative impact as electronic skin for applications in wearable electronics/soft robotics. There has been significant progress in soft conductive materials; however, achieving electrically controlled and reversible changes in conductivity and circuit connectivity remains challenging. To overcome this limitation, a soft material architecture with reconfigurable conductive networks of silver flakes embedded within a hydrogel matrix is presented. The conductive networks can be reversibly created/disconnected through various stimuli, including current, humidity, or temperature. Such stimuli affect electrical connectivity of the hydrogel by controlling its water content, which can be modulated by evaporation under ambient conditions (passive dehydration), evaporation through electrical Joule heating (active dehydration), or absorption of additional water (rehydration). The resulting change in electrical conductivity is reversible and repeatable, endowing the composite with on-demand reconfigurable conductivity. To highlight this material's unique properties, it is shown that conductive traces can be reconfigured after severe damage and revert to lower conductivity after rehydration. Additionally, a quadruped robot is demonstrated that can respond to stimuli by changing direction following exposure to excess water, thereby achieving reprogrammable locomotion behaviors.

Significantly Enhanced Electromagnetic Interference Shielding Performances of Epoxy Nanocomposites with Long-Range Aligned Lamellar Structures.

High­efficiency electromagnetic interference (EMI) shielding materials are of great importance for electronic equipment reliability, information security and human health. In this work, bidirectional aligned Ti3C2Tx@Fe3O4/CNF aerogels (BTFCA) were firstly assembled by bidirectional freezing and freeze-drying technique, and the BTFCA/epoxy nanocomposites with long-range aligned lamellar structures were then prepared by vacuum-assisted impregnation of epoxy resins. Benefitting from the successful construction of bidirectional aligned three-dimensional conductive networks and electromagnetic synergistic effect, when the mass fraction of Ti3C2Tx and Fe3O4 are 2.96 and 1.48 wt%, BTFCA/epoxy nanocomposites show outstanding EMI shielding effectiveness of 79 dB, about 10 times of that of blended Ti3C2Tx@Fe3O4/epoxy (8 dB) nanocomposites with the same loadings of Ti3C2Tx and Fe3O4. Meantime, the corresponding BTFCA/epoxy nanocomposites also present excellent thermal stability (Theat-resistance index of 198.7 °C) and mechanical properties (storage modulus of 9902.1 MPa, Young's modulus of 4.51 GPa and hardness of 0.34 GPa). Our fabricated BTFCA/epoxy nanocomposites would greatly expand the applications of MXene and epoxy resins in the fields of information security, aerospace and weapon manufacturing, etc.

The Effect of the Co-Blending Process on the Sensing Characteristics of Conductive Chloroprene Rubber/Natural Rubber Composites.

Three different blending procedures were used to create multiwalled carbon nanotube (MWCNT)-modified chloroprene rubber (CR)/natural rubber (NR) blended composites (MWCNT/CR-NR). The effects of the blending process on the morphology of the conductive network and interfacial contacts were researched, as well as the resistance-strain response behavior of the composites and the mechanism of composite sensitivity change under different processes. The results show that MWCNT/CR-NR composites have a wide strain range (ε = 300%) and high dynamic resistance-strain response repeatability. Different blending procedures have different effects on the morphology of the conductive network and the interfacial interactions of the composites. If the blending procedures have wider conductive phase spacing and stronger interfacial contacts, the change in the conductive path and tunneling distance occurs more rapidly, and the material has a higher resistance-strain response sensitivity.

Serpentine-Inspired Strain Sensor with Predictable Cracks for Remote Bio-Mechanical Signal Monitoring.

Flexible strain sensors have attracted intense interest due to their application as intelligent wearable electronic devices. However, it is still a huge challenge to achieve a flexible sensor with simultaneous high sensitivity, excellent durability, and a wide sensing region. In this work, a crack-based strain sensor with a paired-serpentine conductive network is fabricated onto flexible film by screen printing. The innovative conductive network exhibits a controlled crack morphology during stretching, which endows the prepared sensor with outstanding sensing characteristics, including high sensitivity (gauge factor up to 2391.5), wide detection (rang up to 132%), low strain detection limit, a fast response time (about 40 ms), as well as excellent durability (more than 2000 stretching/releasing cycles). Benefiting from these excellent performances, full-range human body motions including subtle physiological signals and large motions are accurately detected by the prepared sensor. Furthermore, wearable electronic equipment integrated with a wireless transmitter and the prepared strain sensor shows great potential for remote motion monitoring and intelligent mobile diagnosis for humans. This work provides an effective strategy for the fabrication of novel strain sensors with highly comprehensive performance.

Highly Stable Potassium-Ion Battery Enabled by Nanoengineering of an Sb Anode.

We present the nanoengineering of Sb particles assisted by a conductive and stress-relieving network of carbon quantum dots (CQDs) and poly(3,4-ethylene dioxythiophene) poly(styrenesulfonate) (PEDOT:PSS), in the proper design of anode materials with high specific capacity and excellent stability for potassium-ion batteries (KIBs). The nanosized Sb particles are prepared by the CQDs as functional tuners in the morphology and surface, which tune the size to nanolevel and provide fast ionic channels and a soft matrix to relieve the volume changes. As the additional conductive and stress-relieving network layer, PEDOT:PSS offers enhanced electron/ion pathways and maintains the integrity of the Sb@CQD composite electrode. In the KIB, the prepared Sb anode exhibits battery performance with a high specific capacity of 480 mA h g-1 at 0.5 A g-1 and a high-capacity retention of 95.4% over 350 cycles.

Flame-Retardant PEDOT:PSS/LDHs/Leather Flexible Strain Sensor for Human Motion Detection.

Flexible piezoresistive sensors have demonstrated great potential in human-motion-detection applications. However, it still remains a challenge to fabricate strain sensors with high sensitivity, broad sensing range, and good linear response to strain. In this report, a simple and scalable fabrication strategy is developed to construct high performance strain sensors by using leather as the substrates to filtrate poly(3,4-ethylenedioxythiophene): poly(4-styrenesulfonate) (PEDOT:PSS) modified layered double hydroxides (LDHs) suspensions. The naturally aligned collagen fibers in leather enable size selection for the 2D conductive materials and as such dual-conductive pathways are effectively formed on the surface and in the matrix of leather. Due to the unique design of conductive networks, the prepared sensor possesses high gauge factor (maximum value of 2326.84), tunable strain range (0-70%), fast tensile response time (160 ms), and good stability in 1000 stretching-relaxing/compression-relaxing cycles, making it suitable for various human motion detections including coughing and large-scale motions of joint bending. In addition, the incorporated LDHs is a non-toxic flame retardant, which is helpful to reduce electronic fire risk and can bring added value to the sensor.

Nitrogen-Doped Carbon Networks with Consecutive Conductive Pathways from a Facile Competitive Carbonization-Etching Strategy for High-Performance Energy Storage.

Recently, new carbonization strategies for synthesizing structure-controlled and high-performance carbon electrode materials have attracted great attentions in the field of energy storage and conversion. Here a competitive carbonization-etching strategy to prepare nitrogen-doped carbon polyhedron@carbon nanosheet (NCP@CNS) hybrids derived from zeolitic imidazolate framework-8 is presented. Consecutive conductive networks are constructed in the NCP@CNS hybrids during a unique carbonization-etching pyrolysis, where a competition between the formation of NCPs and CNSs exists. When the NCP@CNS hybrids are employed as supercapacitor electrodes, their hierarchically porous NCPs serve as ion-buffering reservoirs for offering fast ion transport channels, and the CNSs within hybrids not only link the NCPs together to build electron transfer pathways but also restrict the volume fluctuation of electrodes during charging and discharging process. As a result, the as-fabricated NCP@CNS electrode displays excellent electrochemical performances including a superior specific capacitance of 320 F g-1 , a high energy density of 22.2 W h kg-1 (5.6 W h kg-1 for symmetric device), and a long cycle life with capacitance retention of ≈101.8% after 5000 cycles. This study opens an encouraging avenue toward the tailored synthesis of metal-organic frameworks (MOFs)-derived carbon electrodes for renewable energy storage applications and devices.

A Conductive Network and Dipole Field for Harnessing Photogenerated Charge Kinetics.

Photogenerated charge separation and directional transfer to active sites are pivotal steps in photocatalysis, which limit the efficiency of redox reactions. Here, a conductive network and dipole field are employed to harness photogenerated charge kinetics by using a Ti3 C2 /TiO2 network (TTN). The TTN exhibits a prolonged charge-carrier lifetime (1.026 ns) and an 11.76-fold increase in hexavalent chromium photoreduction reaction kinetics compared to TiO2 nanoparticles (TiO2 NPs). This super photocatalytic performance is derived from the efficient photogenerated charge kinetics, which is steered by the conductive network and dipole field. The conductivity enhancement of the TiO2 network is achieved by continuous chemical bonds, which promotes electron-hole (e-h) separation. In addition, at the interface of Ti3 C2 and TiO2 , band bending induced by the dipole field promotes photogenerated electron spatially directed transfer to the catalytic sites on Ti3 C2 . This study demonstrates that a conductive network and dipole field offer a new concept to harness charge kinetics for photocatalysis.

Ferromagnetic Ti3CNCl2-decorated RGO aerogel: From 3D interconnecting conductive network construction to ultra-broadband microwave absorber with thermal insulation property.

It remains urgent challenges to adopt suitable strategies to consume unwanted microwave pollution emitted by high-tech electronic devices satisfactorily. Confronted with narrow effective absorption bandwidth (EAB) and high filler loading bottlenecks of MXene-Based microwave absorber, herein, we employ Lewis molten salt etching approach to both exfoliate Ti3AlCN powders into Ti3CNCl2 suspension and intercalate ferromagnetic composition into interlamination simultaneously. By utilizing the crosslinking effect of dopamine, the Ti3CNCl2 are anchored on the surfaces of graphene oxide (GO) nanosheets, constructing interconnecting microstructure. Both the 3D conductive network and the modification of MXene manifest crucial impacts on enhancing microwave absorption performance of the resulting ultra-lightweight reduced GO (RGO)-based aerogel. The minimum intensity of reflection loss achieves -62.62 dB with the absorber mass loading of 0.7 wt%. Remarkably, more than 90% of the incident microwave is qualified to be absorbed over the whole Ku band. The EAB is broadened while tailoring the thickness to 3 mm, ranging from 10.2 to 18 GHz. Besides, the aerogel presents valuable thermal insulation properties. Our methodology of synthesizing MXene/RGO aerogel not only provides promising insights into microstructural construction but also endows the possibility for integrating thermal insulation property towards next-generation high-performance microwave absorption devices.

Dense All-Electrochem-Active Electrodes for All-Solid-State Lithium Batteries.

The energy density presents the core competitiveness of lithium (Li)-ion batteries. In conventional Li-ion batteries, the utilization of the gravimetric/volumetric energy density at the electrode level is unsatisfactory (<84 wt% and <62 vol%, respectively) due to the existence of non-electrochemical active parts among the 3D porous electrodes, including electrolytes, binders, and carbon additives. These are regarded as indispensable and irreducible components of the electronic and ionic transport network. Here, a dense "all-electrochem-active" (AEA) electrode for all-solid-state Li batteries is proposed, which is entirely constructed from a family of superior mixed electronic-ionic-conducting cathodes, to minimize the energy density gap between the accessible and theoretical energy density at the electrode level. Furthermore, with the ionic-electronic-conductive network self-supported from the AEA cathode, the dense hybrid sulfur (S)-based AEA electrode exhibits a high compacted filling rate of 91.8%, which indicates a high energy density of 777 W h kg-1 and 1945 W h L-1 at the electrode level based on the total cathodes and anodes when at 70 °C.

Tailoring conductive network nanostructures of ZIF-derived cobalt-decorated N-doped graphene/carbon nanotubes for microwave absorption applications.

Confronted with microwave pollution issues, there is an urgent need for microwave absorption materials that possess optimal combinations of dielectric loss and magnetic loss properties. While a variety of studies focus on the components, the construction of nanostructure is rarely studied, which is of equivalent significance to microwave absorber design. In this work, Co-ZIF-67 was adopted as self-template to grow N-doped graphene/carbon nanotube interlinked conductive networks in-situ under a one-step carbonization process with tailored microwave absorption properties. Diverse microwave absorption performance could be achieved by directly adjusting the proportions among ingredients and the calcination temperature, obtaining a maximum value of reflection loss of -65.45 dB at 17.5 GHz with a sample thickness of just 1.5 mm. The effective absorption bandwidth could be tailored from 3.75 to 18 GHz among different thickness as required. The nanostructures had an apparent impact on the corresponding microwave absorption performance, in which the N-doped carbon-based conductive networks, ferromagnetic cobalt atoms, and interfaces among heterostructure strengthened the dipolar polarization and conductivity loss, magnetic loss, and interfacial polarization, respectively. This synthesis strategy offers a promising pathway for integrating nanostructures and functions, catering to requirements for designing and optimizing prospective microwave absorbers.

A Reductive Supramolecular Hydrogel: A Platform for Facile Fabrication of Diverse Metal-Nanoparticle-Decorated Conductive Networks with Spatiotemporal Control.

Nanoparticle-hydrogel hybrid composites have a great potential for a broad range of applications, such as antibacterial materials, stimuli-responsive materials and catalysis. A novel supramolecular hydrogel system was developed using an amino acid based amphiphile containing a terminal pyrrole moiety as a gelator. The pyrrole moiety could serve as both reducing agent and monomer, and a variety of metal precursors penetrating into the hydrogel could be reduced in situ into metal nanoparticles while the pyrrole moieties preorganized in hydrogel were oxidized into polyprroles, affording metal-nanoparticle-decorated covalent conductive networks. This strategy allows the facile fabrication of diverse mono- or multimetallic nanoparticle-polymer networks from one hydrogel by a simple reaction-diffusion approach. More importantly, besides homogeneous composites, unique multisegment heterogeneous systems with spatiotemporal control were also easily accessible. Furthermore, based on the same multifunctional molecule, the fabrication of hierarchically pore-structured metal-nanoparticles-polymers as well as metal-nanoparticles-carbon structures was also realized.

Flexible MXene-Decorated Fabric with Interwoven Conductive Networks for Integrated Joule Heating, Electromagnetic Interference Shielding, and Strain Sensing Performances.

Although flexible and multifunctional textile-based electronics are promising for wearable devices, it is still a challenge to seamlessly integrate excellent conductivity into textiles without sacrificing their intrinsic flexibility and breathability. Herein, the vertically interconnected conductive networks are constructed based on a meshy template of weave cotton fabrics with interwoven warp and weft yarns. The two-dimensional early transition metal carbides/nitrides (MXenes), with unique metallic conductivity and hydrophilic surfaces, are uniformly and intimately attached to the preformed fabric via a spray-drying coating approach. Through adjusting the spray-drying cycles, the degree of conductive interconnectivity for the fabrics is precisely tuned, thereby affording highly conductive and breathable fabrics with integrated Joule heating, electromagnetic interference (EMI) shielding and strain sensing performances. Interestingly, triggered by the interwoven conductive architecture, the MXene-decorated fabrics with a low loading of 6 wt % (0.78 mg cm-2) offer an outstanding electrical conductivity of 5 Ω sq-1. The promising electrical conductivity further endows the fabrics with superior Joule heating performance with a heating temperature up to 150 °C at a supply voltage of 6 V, excellent EMI shielding performance, and highly sensitive strain responses to human motion. Consequently, this work offers a novel strategy for the versatile design of multifunctional textile-based wearable devices.

A Hydrophobic, Self-Powered, Electromagnetic Shielding PVDF-Based Wearable Device for Human Body Monitoring and Protection.

With the rapid development of the electronics, information technology, and wearable devices, problems of the power crisis and electromagnetic radiation pollution have emerged. A piezoelectric wearable textile combined with electromagnetic shielding performance has become a favorable solution. Herein, a multifunctional PVDF-based wearable sensor with both electromagnetic shielding function and human body monitoring performance is proposed by incorporating silver nanowires (Ag NWs) and multiwall carbon nanotubes (MWCNTs) hybrid-networks into PVDF-casted commercial nonwoven fabrics (NWF). The coordination of Ag NWs and MWCNTs networks ensures the ideal electrical conductivity and mechanical strength. The maximum shielding value of the developed sensor reaches up to 34 dB when the area densities of the Ag NWs and MWCNT are kept at 1.9 and 2.0 mg/cm2, respectively. Additionally, the hydrophobicity of the as-proposed sensor (water contact angle of ∼110.0°) ensures the self-cleaning function and makes it resistive against water and dirt. Moreover, the sensor possesses a force-sensing property by generating different piezoelectric voltages (0, 0.4, 1.0, and 1.5 V) when stimulated by various forces (0, 20, 44, and 60 N). Not only can it respond to different external stress in a timely manner (response sensitivity of ∼0.024 V/N, response time of ∼35 ms), but it can also monitor different body movements, such as joint bending, running, and jumping. This work opens up a new prospect of monitoring the human body as well as protecting human health from electromagnetic radiation surroundings.