Evolution of Naturally Dried MXene-Based Composite Aerogels with Flash Joule Annealing for Large-Scale Production of Highly Sensitive Customized Sensors.

MXene aerogels, known for good electrical properties, offer immense potential for the development of high-sensitivity pressure sensors. However, the intrinsic challenges stemming from the poor self-assembly capability and high hydrophilicity of MXene impedes the natural drying process of MXene-based hydrogels, thereby constraining their application on a large-sacle in sensor technology. Herein, we propose a graphene-assisted approach aimed at modulating the hydrophobicity and enhancing framework strength of MXene through a well-designed prefreezing technique incorporating three-dimensional (3D) spherical macro-porous structures. This synergistic strategy enables the fabrication of naturally dried MXene aerogels across various size scales. Moreover, the integration of 3D spherical macro-porous structures improves elasticity and electrical responsiveness of aerogels. Consequently, the aerogel sensor exhibits great performances, including high sensitivity (1250 KPa-1), low detection limit (0.4 Pa), wide frequency response range (0.1-8 Hz), and excellent stability (1000 cycles). This sensor proves adept at monitoring pressure signals ranging from lightweight paper to human motion. Additionally, the application of customized laser engraving endows aerogels with unique functionalities, such as compressibility and immunity to strain, stretchability and resistance to compression, as well as wind detection. Thus, our proposed approach holds significant promise as a scalable method for the mass production of aerogels with versatile applications. This article is protected by copyright. All rights reserved.

Ultralow-resistance electrochemical capacitor for integrable line filtering.

Electrochemical capacitors are expected to replace conventional electrolytic capacitors in line filtering for integrated circuits and portable electronics1-8. However, practical implementation of electrochemical capacitors into line-filtering circuits has not yet been achieved owing to the difficulty in synergistic accomplishment of fast responses, high specific capacitance, miniaturization and circuit-compatible integration1,4,5,9-12. Here we propose an electric-field enhancement strategy to promote frequency characteristics and capacitance simultaneously. By downscaling the channel width with femtosecond-laser scribing, a miniaturized narrow-channel in-plane electrochemical capacitor shows drastically reduced ionic resistances within both the electrode material and the electrolyte, leading to an ultralow series resistance of 39 mΩ cm2 at 120 Hz. As a consequence, an ultrahigh areal capacitance of up to 5.2 mF cm-2 is achieved with a phase angle of -80° at 120 Hz, twice as large as one of the highest reported previously4,13,14, and little degradation is observed over 1,000,000 cycles. Scalable integration of this electrochemical capacitor into microcircuitry shows a high integration density of 80 cells cm-2 and on-demand customization of capacitance and voltage. In light of excellent filtering performances and circuit compatibility, this work presents an important step of line-filtering electrochemical capacitors towards practical applications in integrated circuits and flexible electronics.

Strain-Stiffening Ionogel with High-Temperature Tolerance via the Synergy of Ionic Clusters and Hydrogen Bonds.

Highly stretchable and conductive ionogels have great potential in flexible electronics and soft robotic skins. However, current ionogels are still far from being able to accurately duplicate the mechanically responsive behavior of real human skin. Furthermore, durable robotic skins that are applicable under harsh conditions are still lacking. Herein, a strong noncovalent interaction, ionic clusters, is combined with hydrogen bonds to obtain a physically cross-linked ionogel (PCI). Benefiting from the strong ionic bonding of the ionic cluster, the PCI shows strain-stiffening behavior similar to that of human skin, thus enabling it to have a perception-strengthening ability. Additionally, the strong ionic clusters can also ensure the PCI remains stable at high temperatures. Even when the temperature is raised to 200 °C, the PCI can maintain the gel state. Moreover, the PCI exhibits high transparency, recyclability, good adhesion, and high conductivity. Such excellent features distinguish the PCI from ordinary ionogels, providing a new way to realize skin-like sensing in harsh environments for future bionic machines.

Aqueous hybrid electrochemical capacitors with ultra-high energy density approaching for thousand-volts alternating current line filtering.

Filtering capacitors with wide operating voltage range are essential for smoothing ripples in line-powered system, which are still unsatisfactory due to low energy density and limited working voltage scopes. Herein, we report an aqueous hybrid electrochemical capacitor with areal specific energy density of 1.29 mF V2 cm-2 at 120 Hz, greater than common aqueous ones. Interestingly, it can be easily integrated at scale to show excellent flexibility, controllable and stable filtering performance, in which an integrated device (e.g., seven units in series) exhibits fluctuation of 96 mV, 10 times smaller than an aluminum electrolytic capacitor with similar capacitance. A record-high 1,000 V can also be achieved after integrating 670 units, exceeding those reported so far, and about 1.5 times of commercial bulk aluminum electrolytic capacitors (~700 V). This work opens up a new insight for promising applications in multiple electricity transmission systems that requiring high smoothness under harsh voltage.

Superelastic graphene aerogel-based metamaterials.

Ultralight, ultrastrong, and supertough graphene aerogel metamaterials combining with multi-functionalities are promising for future military and domestic applications. However, the unsatisfactory mechanical performances and lack of the multiscale structural regulation still impede the development of graphene aerogels. Herein, we demonstrate a laser-engraving strategy toward graphene meta-aerogels (GmAs) with unusual characters. As the prerequisite, the nanofiber-reinforced networks convert the graphene walls' deformation from the microscopic buckling to the bulk deformation during the compression process, ensuring the highly elastic, robust, and stiff nature. Accordingly, laser-engraving enables arbitrary regulation on the macro-configurations of GmAs with rich geometries and appealing characteristics such as large stretchability of 5400% reversible elongation, ultralight specific weight as small as 0.1 mg cm-3, and ultrawide Poisson's ratio range from -0.95 to 1.64. Additionally, incorporating specific components into the pre-designed meta-structures could further achieve diversified functionalities.

A reconfigurable and magnetically responsive assembly for dynamic solar steam generation.

Interfacial solar vapor generation is a promising technique to efficiently get fresh water from seawater or effluent. However, for the traditional static evaporation models, further performance improvement has encountered bottlenecks due to the lack of dynamic management and self-regulation on the evolving water movement and phase change in the evaporation process. Here, a reconfigurable and magnetically responsive evaporator with conic arrays is developed through the controllable and reversible assembly of graphene wrapped Fe3O4 nanoparticles. Different from the traditional structure-rigid evaporation architecture, the deformable and dynamic assemblies could reconfigure themselves both at macroscopic and microscopic scales in response to the variable magnetic field. Thus, the internal water transportation and external vapor diffusion are greatly promoted simultaneously, leading to a 23% higher evaporation rate than that of static counterparts. Further, well-designed hierarchical assembly and dynamic evaporation system can boost the evaporation rate to a record high level of 5.9 kg m-2 h-1. This proof-of-concept work demonstrates a new direction for development of high performance water evaporation system with the ability of dynamic reconfiguration and reassembly.

Ultrafast Electrochemical Capacitors with Carbon Related Materials as Electrodes for AC Line Filtering.

High-frequency responsive electrochemical capacitors (ECs), which can directly convert alternating current (AC) to direct current (DC), are getting more essential for the rapid development of electronic devices. In order to satisfy the requirements of ECs with fast rate capability and appreciable capacitance density, numerous efforts have been made towards the preparation and design of the electrode material, which is a decisive factor in the performance of ECs. Carbon-related electrode materials have been widely shown to significantly increase the performance of ECs because of their light weight, high strength, and high processability. In this concept, the latest advances in the rational design and controllable fabrication of carbon-related electrode materials, including planar 2D materials, random 3D, and vertical carbon materials are summarized. Moreover, the state of the art of carbon-based ECs is discussed from the viewpoint of the structure of the electrode and performance of ECs. Finally, this concept presents integrated perspectives on the further design and preparation of carbon related ECs.

Bridged Carbon Fabric Membrane with Boosted Performance in AC Line-Filtering Capacitors.

High-frequency responsive capacitors with lightweight, flexibility, and miniaturization are among the most vital circuit components because they can be readily incorporated into various portable devices to smooth out the ripples for circuits. Electrode materials no doubt are at the heart of such devices. Despite tremendous efforts and recent advances, the development of flexible and scalable high-frequency responsive capacitor electrodes with superior performance remains a great challenge. Herein, a straightforward and technologically relevant method is reported to manufacture a carbon fabric membrane "glued" by nitrogen-doped nanoporous carbons produced through a polyelectrolyte complexation-induced phase separation strategy. The as-obtained flexible carbon fabric bearing a unique hierarchical porous structure, and high conductivity as well as robust mechanical properties, serves as the free-standing electrode materials of electrochemical capacitors. It delivers an ultrahigh specific areal capacitance of 2632 µF cm-2 at 120 Hz with an excellent alternating current line filtering performance, fairly higher than the state-of-the-art commercial ones. Together, this system offers the potential electrode material to be scaled up for AC line-filtering capacitors at industrial levels.

Vertical Graphene Arrays as Electrodes for Ultra-High Energy Density AC Line-Filtering Capacitors.

High-frequency responsive electrochemical capacitor (EC), as an ideal lightweight filtering capacitor, can directly convert alternating current (AC) to direct current (DC). However, current electrodes are stuck in limited electrode area and tortuous ion transport. Herein, strictly vertical graphene arrays (SVGAs) prepared by electric-field-assisted plasma enhanced chemical vapour deposition have been successfully designed as the main electrode to ensure ions rapidly adsorb/desorb in richly available graphene surface. SVGAs exhibit an outstanding specific areal capacitance of 1.72 mF cm-2 at Φ120 =80.6° even after 500 000 cycles, which is far better than that of most carbon-related materials. Impressively, the output voltage could also be improved to 2.5 V when using organic electrolyte. An ultra-high energy density of 0.33 µWh cm-2 can also be handily achieved. Moreover, ECs-SVGAs can well smooth arbitrary AC waveforms into DC signals, exhibiting excellent filtering performance.

Biomimetic Antigravity Water Transport and Remote Harvesting Powered by Sunlight.

Antigravity water transport plays important roles in various applications ranging from agriculture, industry, and environmental engineering. In natural trees, ubiquitous water-flow over 100 m high from roots through the hierarchical xylem to leaves is driven by sunlight-powered continuous evaporation and the negative pressure. Inspired by natural trees, herein an artificial trunk-leaf system is built up to structurally mimic natural trees for a continuous antigravity water delivery. The artificial tree consists of directional microchannels for antigravity water transport, and a top leaf-like hybrid hydrogel that are acts as continuous solar steam evaporator, plus a purposely engineered steam collector. It is found that continuous uniform microchannels of acetylated chitin optimize and enhance capillary rise (≈37 cm at 300 min) and reduce vertical water transport resistance. A remote water harvesting, and purification is performed with a high rate of 1.6 kg m-2 h-1 and 184 cm in height under 1 sun irradiation and the collection efficiency up to 100% by evaporative cooling technique. It is envisioned that the basic design principles underlying the artificial tree can be used to transform solar energy into potential energy.

Maximization of Spatial Charge Density: An Approach to Ultrahigh Energy Density of Capacitive Charge Storage.

Capacitive energy storage has advantages of high power density, long lifespan, and good safety, but is restricted by low energy density. Inspired by the charge storage mechanism of batteries, a spatial charge density (SCD) maximization strategy is developed to compensate this shortage by densely and neatly packing ionic charges in capacitive materials. A record high SCD (ca. 550 C cm-3 ) was achieved by balancing the valance and size of charge-carrier ions and matching the ion sizes with the pore structure of electrode materials, nearly five times higher than those of conventional ones (ca. 120 C cm-3 ). The maximization of SCD was confirmed by Monte Carlo calculations, molecular dynamics simulations, and in situ electrochemical Raman spectroscopy. A full-cell supercapacitor was further constructed; it delivers an ultrahigh energy density of 165 Wh L-1 at a power density of 150 WL-1 and retains 120 Wh L-1 even at 36 kW L-1 , opening a pathway towards high-energy-density capacitive energy storage.

Highly Ordered Graphene Solid: An Efficient Platform for Capacitive Sodium-Ion Storage with Ultrahigh Volumetric Capacity and Superior Rate Capability.

As an emerging type of electrochemical energy storage devices, sodium-ion capacitors (SICs) are potentially capable of high energy density and high power density, as well as low cost and long lifespan. Unfortunately, the lack of high-performance capacitive cathodes that can fully couple with the well-developed battery-type anodes severely restricts the further development of SICs. Here, we develop a compact yet highly ordered graphene solid (HOGS), which combines the merits of high density and high porosity and, more attractively, possesses a highly ordered lamellar texture with low pore tortuosity. As the capacitive cathode of SICs,  HOGS delivers a record-high volumetric capacity (303 F cm-3 or 219 mA h cm-3 at 0.05 A g-1), a superior rate capability (185 F cm-3 or 139 mA h cm-3 even at 10 A g-1), and an outstanding cycling stability (over 80% after 10 000 cycles). The material design and construction strategies reported here can be easily extended to other metal-ion-based energy storage technologies, exhibiting universal potentials in compact electrochemical energy storage systems.

Arbitrary waveform AC line filtering applicable to hundreds of volts based on aqueous electrochemical capacitors.

Filtering capacitor is a necessary component in the modern electronic circuit. Traditional filtering capacitor is often limited by its bulky and rigid configuration and narrow workable scope of applications. Here, an aqueous hybrid electrochemical capacitor is developed for alternating current line filtering with an applicable wide frequency range from 1 to 10,000 Hz. This capacitor possesses an areal specific energy density of 438 µF V2 cm-2 at 120 Hz, which to the best of our knowledge is record high among aqueous electrochemical capacitors reported so far. It can convert arbitrary alternating current waveforms and even noises to straight signals. After integration of capacitor units, a workable voltage up to hundreds of volts (e.g., 200 V) could be achieved without sacrificing its filtering capability. The integrated features of wide frequency range and high workable voltage for this capacitor present promise for multi-scenario and applicable filtering capacitors of practical importance.

Plant leaves inspired sunlight-driven purifier for high-efficiency clean water production.

Natural vascular plants leaves rely on differences in osmotic pressure, transpiration and guttation to produce tons of clean water, powered by sunlight. Inspired by this, we report a sunlight-driven purifier for high-efficiency water purification and production. This sunlight-driven purifier is characterized by a negative temperature response poly(N-isopropylacrylamide) hydrogel (PN) anchored onto a superhydrophilic melamine foam skeleton, and a layer of PNIPAm modified graphene (PG) filter membrane coated outside. Molecular dynamics simulation and experimental results show that the superhydrophilicity of the relatively rigid melamine skeleton significantly accelerates the swelling/deswelling rate of the PNPG-F purifier. Under one sun, this rational engineered structure offers a collection of 4.2 kg m-2 h-1 and an ionic rejection of > 99% for a single PNPG-F from brine feed via the cooperation of transpiration and guttation. We envision that such a high-efficiency sunlight driven system could have great potential applications in diverse water treatments.

Confined Structures and Selective Mass Transport of Organic Liquids in Graphene Nanochannels.

Selective transport of liquids is an important process in the energy and environment industry. The increased energy consumption and the demands of clean water and fossil fuels have urged the development of high-performance membrane technologies. Nanoscale channels with the critical size for molecular sieving and atomistically smooth walls for significant boundary slippage are highly promising to balance the tradeoff between permeability and selectivity. In this work, we explore the molecular structures and dynamics of organic solvents and water, which are confined within nanoscale two-dimensional galleries between graphene or graphene oxide sheets. Molecular dynamics simulation results show that the layered order and significant interfacial slippage are universal for all molecular liquids, leading to notable flow enhancement for channels with a width of few nanometers, in the order of ethylene glycol > butanol > ethanol > hexane > toluene > water > acetone. The extracted dependence of permeability, selectivity on the channel width, and properties of molecular liquids clarify the underlying mechanisms of selective mass transport in nanofluidics, which help to understand and control the filtration and separation processes of molecular liquids. The performance of graphene oxide membranes for permeation and filtration is finally discussed based on the calculated flow resistance for pressure-driven flow or molecular diffusivity for diffusive flow, as well as the solubility and wettability of membranes.

A lead-free two-dimensional perovskite for a high-performance flexible photoconductor and a light-stimulated synaptic device.

Organo-lead halide perovskites have emerged as promising materials for high-performance photodetectors. However, the toxicity of lead cations in these materials limits their further applications. Here, a flexible photoconductor is developed based on lead-free two-dimensional (2D) perovskite (PEA)2SnI4via a one-step solution processing method. The flexible transparent electrodes are patterned from rGO/(PEDOT:PSS) hybrid films. The stability and reproducibility of the devices are significantly improved on adding 30 mol% SnF2 to the perovskite. The flexible photoconductors show a photoresponsivity of 16 A W-1 and a detectivity of 1.92 × 1011 Jones under 470 nm illumination, which are higher than those of most of the similar devices. Besides, the devices possess much better mechanical flexibility and durability than the flexible devices with an Au electrode. Finally, this flexible photoconductor is applied as a light-stimulated synaptic device and can mimic the short-term plasticity of biological synapses. This is the first study to report that lead-free 2D perovskite can be used in flexible photoconductors and synaptic devices.

Chemical Approach to Ultrastiff, Strong, and Environmentally Stable Graphene Films.

Reduced graphene oxide (rGO) sheets prepared by a modified Hofmann method (Ho-rGO) have large graphitic domains with few structural defects, facilitating the dense packing between rGO sheets to enhance the mechanical performances of the resultant graphene films. Graphene films are fabricated by the filtration of the aqueous dispersions of Ho-rGO sheets and further treated by thermal annealing. They display high moduli (stiffness) of 54.6 ± 1.4 GPa and high tensile strengths of 521 ± 19 MPa. They also exhibit high toughness and good electrical properties. The intact structure of Ho-rGO sheets narrows the nanochannels in the film matrices, greatly reducing the water infiltration into films and providing the graphene films with excellent environmental stability. These graphene films are attractive for practical applications because of their light weights and ultrastiff and ultrastrong mechanical properties.

Topological Design of Ultrastrong and Highly Conductive Graphene Films.

Nacre-like graphene films are prepared by evaporation-induced assembly of graphene oxide dispersions containing small amounts of cellulose nanocrystal (CNC), followed by chemical reduction with hydroiodic acid. CNC induces the formation of wrinkles on graphene sheets, greatly enhancing the mechanical properties of the resultant graphene films. The graphene films deliver an ultrahigh tensile strength of 765 ± 43 MPa (up to 800 MPa in some cases), a large failure strain of 6.22 ± 0.19%, and a superior toughness of 15.64 ± 2.20 MJ m-3 , as well as a high electrical conductivity of 1105 ± 17 S cm-1 . They have a great potential for applications in flexible electronics because of their combined excellent mechanical and electrical properties.

Organic dispersions of graphene oxide with arbitrary concentrations and improved chemical stability.

We report a simple method that can dissolve graphene oxide (GO) in pure organic solvents (e.g., propylene carbonate) as readily as in pure water to form stable dispersions of single layer GO sheets. The GO sheets dispersed in propylene carbonate exhibited much better structural stability than those in water.

Ultrahigh-Conductivity Polymer Hydrogels with Arbitrary Structures.

A poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) hydrogel is prepared by thermal treatment of a commercial PEDOT:PSS (PH1000) suspension in 0.1 mol L-1 sulfuric acid followed by partially removing its PSS component with concentrated sulfuric acid. This hydrogel has a low solid content of 4% (by weight) and an extremely high conductivity of 880 S m-1 . It can be fabricated into different shapes such as films, fibers, and columns with arbitrary sizes for practical applications. A highly conductive and mechanically strong porous fiber is prepared by drying PEDOT:PSS hydrogel fiber to fabricate a current-collector-free solid-state flexible supercapacitor. This fiber supercapacitor delivers a volumetric capacitance as high as 202 F cm-3 at 0.54 A cm-3 with an extraordinary high-rate performance. It also shows excellent electrochemical stability and high flexibility, promising for the application as wearable energy-storage devices.