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Hygroelectricity is proposed as a means to produce electric power from air by absorbing gaseous or vaporous water molecules, which are ubiquitous in the atmosphere. Here, using a synergy between a hygroscopic bulk graphene oxide with a heterogeneous structure and interface mediation between electrodes/materials with Schottky junctions, we develop a high-performance hygroelectric generator unit with an output voltage approaching 1.5 V. High voltage (e.g., 18 V with 15 units) can be easily reached by simply scaling up the number of hygroelectric generator units in series, enough to drive commercial electronic devices. This work provides insight for the design and development of hygroelectric generators that may promote the efficient conversion of potential energy in the environmental atmosphere to electricity for practical applications.

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It is challenging to construct exquisite microstructures for integrating extraordinary sensitivity, wide strain range detectability, low hysteresis, good linearity, and excellent reliability and stability in a single type of strain sensor. In this paper, we report a high-performance fibrous strain sensor with ultrahigh sensitivity (gauge factor up to 350), wide sensing range (0.1% to 150% strain), low hysteresis, good linearity over a large strain range (up to 50%), and excellent reliability and stability (>2000 cycles). Our fibrous strain sensor exhibits superior comprehensive properties to previous strain sensors, attributed to its hierarchical microstructure composed of twisted polyurethane fibers and microcracked poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) sensing layer on each fiber, bridged by carbon nanotube agglomerates. This sensor is attractive and promising for the full-range detection of human motion from subtle deformations to large movements. In addition, the spatial extensional strain distribution of human skin can also be detected by the sensing fabric woven by this fibrous sensor due to its knittability.

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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.

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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.

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Wearable sensors that can precisely detect vital signs are highly desirable for monitoring personal health conditions and medical diagnosis. In this paper, we report an ultrasensitive strain sensor consisting of a 150 nm thick highly conductive dimethylsulfoxide-doped poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) sensing layer and an elastic fluorosilicone rubber substrate. This sensor exhibits a high sensitivity at small strains (e.g., gauge factor at 0.6% strain = 280), low limit of detection (<0.2% strain), and excellent repeatability and cycling stability. Therefore, it is promising for practically detecting vital signs, tiny human motions, and sounds. Furthermore, the semitransparent shallow blue color and the soft rubbery substrate make the strain sensor beautiful and comfortable to the human body.

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Harvesting solar energy for desalination and sewage treatment has been considered as a promising solution to produce clean water. However, state-of-the-art technologies often require optical concentrators and complicated systems with multiple components, leading to poor efficiency and high cost. Here, we demonstrate an extremely simple and standalone solar energy converter consisting of only an as-prepared 3D cross-linked honeycomb graphene foam material without any other supporting components. This simple all-in-one material can act as an ideal solar thermal converter capable of capturing and converting sunlight into heat, which in turn can distill water from various water sources into steam and produce purified water under ambient conditions and low solar flux with very high efficiency. High specific water production rate of 2.6 kg h-1 m-2 g-1 was achieved with near ∼87% under 1 sun intensity and >80% efficiency even under ambient sunlight (<1 sun). This scalable sheet-like material was used to obtain pure drinkable water from both seawater and sewage water under ambient conditions. Our results demonstrate a competent monolithic material platform providing a paradigm change in water purification by using a simple, point of use, reusable, and low-cost solar thermal water purification system for a variety of environmental conditions.

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A high-performance actuator should be able to deliver large-shape deformations, fast actuations and sensitive responses to multiple stimuli. Here, we report such an actuator constructed from one layer of polyvinylidene fluoride (PVDF) with a high coefficient of thermal expansion (CTE), and another layer of small sheets of graphene oxide (SGO) with a negative CTE. The opposite deformations of both actuation layers make the SGO/PVDF bilayer actuator highly sensitive to the temperature stimulus with a large bending sensitivity of 1.5 cm-1 °C-1. Upon irradiation with 60 mW cm-2 infrared light, this SGO/PVDF bilayer actuator displayed an extremely rapid tip displacement rate of 140 mm s-1. Furthermore, this actuator can also sensitively respond to moisture because of its SGO layer, showing a curvature change from -22 to 13 cm-1 upon changing the relative humidity (RH) from 11% to 86%. This actuator can generate a contractile or relaxed stress 18 times that of mammalian skeletal muscle, under light irradiation or moisture with a response time as short as 1 s, being capable of lifting an object with a weight 80 times that of itself. Furthermore, it also showed excellent stability and repeatability.

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A high-performance moisture triggered nanogenerator is fabricated by using graphene quantum dots (GQDs) as the active material. GQDs are prepared by direct oxidation and etching of natural graphite powder, which have small sizes of 2-5 nm and abundant oxygen-containing functional groups. After the treatment by electrochemical polarization, the GQDs-based moisture triggered nanogenerator can deliver a high voltage up to 0.27 V under 70% relative humidity variation, and a power density of 1.86 mW cm-2 with an optimized load resistor. The latter value is much higher than the moisture-electric power generators reported previously. The GQD moisture triggered nanogenerator is promising for self-power electronics and miniature sensors.

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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.

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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.

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The properties and functions of graphene oxide (GO)-based materials strongly depend on the lateral size and size distribution of GO nanosheets; therefore, GO and its derivatives with narrow size distributions are highly desired. Here we report the size fractionation of GO nanosheets by controlled directional freezing of GO aqueous dispersions. GO nanosheets with a narrow size distribution can be obtained by controlling the growth rate of the freezing front. This interesting phenomenon can be explained by the adsorption of GO nanosheets on the ice crystal surface in combination with the stratification of GO nanosheets at the ice growth front. Such a convenient size fractionation approach will be essential for practical applications of chemically modified graphene, including GO, reduced GO, and their assemblies or composites.

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Graphene, with large delocalized π electron cloud on a two-dimensional (2D) atom-thin plane, possesses excellent carrier mobility, large surface area, high light transparency, high mechanical strength, and superior flexibility. However, the lack of intrinsic band gap, poor dispersibility, and weak reactivity of graphene hinder its application scope. Heteroatom-doping regulation and surface modification of graphene can effectively reconstruct the sp2 bonded carbon atoms and tailor the surface chemistry and interfacial interaction, while microstructure mediation on graphene can induce the special chemical and physical properties because of the quantum confinement, edge effect, and unusual mass transport process. Based on these regulations on graphene, series of methods and techniques are developed to couple the promising characters of graphene into the macroscopic architectures for potential and practical applications. In this Account, we present our effort on graphene regulation from chemical modification to microstructure control, from the morphology-designed macroassemblies to their applications in functional systems excluding the energy-storage devices. We first introduce the chemically regulative graphene with incorporated heteroatoms into the honeycomb lattice, which could open the intrinsic band gap and provide many active sites. Then the surface modification of graphene with functional components will improve dispersibility, prevent aggregation, and introduce new functions. On the other hand, microstructure mediation on graphene sheets (e.g., 0D quantum dots, 1D nanoribbons, and 2D nanomeshes) is demonstrated to induce special chemical and physical properties. Benefiting from the effective regulation on graphene sheets, diverse methods including dimension-confined strategy, filtration assembly, and hydrothermal treatment have been developed to assemble individual graphene sheets to macroscopic graphene fibers, films, and frameworks. These rationally regulated graphene sheets and well-constructed assemblies present promising applications in energy-conversion materials and device systems focusing on actuators that can convert different energy forms (e.g., electric, chemical, photonic, thermal, etc.) to mechanical actuation and electrical generators that can directly transform environmental energy to electric power. These results reveal that graphene sheets with surface chemistry and microstructure regulations as well as their rationally designed assemblies provide a promising and abundant platform for development of diverse functional devices. We hope that this Account will promote further efforts toward fundamental research on graphene regulation and the wide applications of advanced designed assemblies in new types of energy-conversion materials/devices and beyond.

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Thin films of a thiocyanate ion (SCN-)-doped organometal halide perovskite, CH3NH3PbI3-x(SCN)x, were used as a sensing material for developing high-performance gas sensors. The CH3NH3PbI3-x(SCN)x-based chemiresistor-type sensor can sensitively and selectively detect acetone and nitrogen dioxide (NO2) at room temperature with high sensitivities of 5.6 × 10-3 and 5.3 × 10-1 ppm-1. The limits of detection for acetone and NO2 were measured to be 20 ppm and 200 ppb. This sensor also exhibited excellent repeatability, and its environmental stability was greatly improved by doping the perovskite with SCN- ions.

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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.

RESUMEN

Phototransistors with a structure of a nitrogen-doped graphene quantum dots (NGQDs)-perovskite composite layer and a mildly reduced graphene oxide (mrGO) layer are fabricated through a solution-processing method. This hybrid phototransistor exhibits broad detection range (from 365 to 940 nm), high photoresponsivity (1.92 × 104 A W-1 ), and rapid response to light on-off (≈10 ms). NGQDs offer an effective and fast path for electron transfer from the perovskite to the mrGO, resulting in the improvement of photocurrent and photoswitching characteristics. The high photoresponsivity can also be ascribed to a photogating effect in the device. In addition, the phototransistor shows good stability with poly(methyl methacrylate) encapsulation, and can maintain 85% of its initial performance for 20 d in ambient air.

RESUMEN

Halide perovskites have high light absorption coefficients, long charge carrier diffusion lengths, intense photoluminescence, and slow rates of non-radiative charge recombination. Thus, they are attractive photoactive materials for developing high-performance optoelectronic devices. These devices are also cheap and easy to be fabricated. To realize the optimal performances of halide perovskite-based optoelectronic devices (HPODs), perovskite photoactive layers should work effectively with other functional materials such as electrodes, interfacial layers and encapsulating films. Conventional two-dimensional (2D) materials are promising candidates for this purpose because of their unique structures and/or interesting optoelectronic properties. Here, we comprehensively summarize the recent advancements in the applications of conventional 2D materials for halide perovskite-based photodetectors, solar cells and light-emitting diodes. The examples of these 2D materials are graphene and its derivatives, mono- and few-layer transition metal dichalcogenides (TMDs), graphdiyne and metal nanosheets, etc. The research related to 2D nanostructured perovskites and 2D Ruddlesden-Popper perovskites as efficient and stable photoactive layers is also outlined. The syntheses, functions and working mechanisms of relevant 2D materials are introduced, and the challenges to achieving practical applications of HPODs using 2D materials are also discussed.

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The development of ecofriendly electrocatalysts with earth-abundant metal elements for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is important for overall water splitting to generate clean and sustainable chemical energy. Here, we report a self-standing cobalt disulfide/graphite foam (CoS2/GF) electrocatalytic electrode for this purpose. It showed high catalytic activities for both the HER and OER, requiring only a cell voltage of 1.74 V to achieve a current density of 20 mA cm-2 for overall water splitting in an alkaline electrolyte. This three-dimensional microporous electrocatalytic electrode is cheap and available in a large area; thus, it is attractive for practical applications.

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Versatile graphene oxide putty-like material (GOP) with excellent processability is developed by mediating a graphene oxide suspension with aniline. Arbitrarily predesigned architectures on both microscopic and macroscopic scales can be molded easily. GOP cannot only be used as starting material for direct 3D printing of particular configurations, but also can be tailored into the patterned structures on various substrates for large-scale production of device arrays.

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Graphene, because of its superior electrical/thermal conductivity, high surface area, excellent mechanical flexibility, and stability, is currently receiving significant attention and benefit to fabricate actuator devices. Here, a sole graphene oxide (GO) film responsive actuator with an integrated self-detecting sensor has been developed. The film exhibits an asymmetric surface structure on its two sides, creating a promising actuation ability triggered by multistimuli, such as moisture, thermals, and infrared light. Meanwhile, the built-in laser-writing reduced graphene oxide (rGO) sensor in the film can detect its own deformation in real time. Smart perceptual fingers in addition to rectangular-shaped and even four-legged walking robots have been developed based on the responsive GO film.

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Solvated reduced graphene oxide (S-rGO) membranes are stable in organic solvents, and strong acidic, alkaline, or oxidative media. They show high rejections to small molecules with charges the same as that of S-rGO coatings or neutral molecules larger than 3.4 nm, while retaining their high permeances to organic solvents.