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1.
Flexible power sources have shown great promise in next‐generation bendable, implantable, and wearable electronic systems. Here, flexible and binder‐free electrodes of Na3V2(PO4)3/reduced graphene oxide (NVP/rGO) and Sb/rGO nanocomposites for sodium‐ion batteries are reported. The Sb/rGO and NVP/rGO paper electrodes with high flexibility and tailorability can be easily fabricated. Sb and NVP nanoparticles are embedded homogenously in the interconnected framework of rGO nanosheets, which provides structurally stable hosts for Na‐ion intercalation and deintercalation. The NVP/rGO paper‐like cathode delivers a reversible capacity of 113 mAh g?1 at 100 mA g?1 and high capacity retention of ≈96.6% after 120 cycles. The Sb/rGO paper‐like anode gives a highly reversible capacity of 612 mAh g?1 at 100 mA g?1, an excellent rate capacity up to 30 C, and a good cycle performance. Moreover, the sodium‐ion full cell of NVP/rGO//Sb/rGO has been fabricated, delivering a highly reversible capacity of ≈400 mAh g?1 at a current density of 100 mA g?1 after 100 charge/discharge cycles. This work may provide promising electrode candidates for developing next‐generation energy‐storage devices with high capacity and long cycle life.  相似文献   

2.
Thin‐film electronics are urged to be directly laminated onto human skin for reliable, sensitive biosensing together with feedback transdermal therapy, their self‐power supply using the thermoelectric and moisture‐induced‐electric effects also has gained great attention (skin and on‐skin electronics (On‐skinE) themselves are energy storehouses). However, “thin‐film” On‐skinE 1) cannot install “bulky” heatsinks or sweat transport channels, but the output power of thermoelectric generator and moisture‐induced‐electric generator relies on the temperature difference (?T ) across generator and the ambient humidity (AH), respectively; 2) lack a routing and accumulation of sweat for biosensing, lack targeted delivery of drugs for precise transdermal therapy; and 3) need insulation between the heat‐generating unit and heat‐sensitive unit. Here, two breathable nanowood biofilms are demonstrated, which can help insulate between units and guide the heat and sweat to another in‐plane direction. The transparent biofilms achieve record‐high transport///transport (//: along cellulose nanofiber alignment direction, ⊥: perpendicular direction) of heat (925%) and sweat (338%), winning applications emphasizing on ?T/AH‐dependent output power and “reliable” biosensing. The porous biofilms are competent in applications where “sensitive” biosensing (transporting// sweat up to 11.25 mm s?1 at the 1st second), “insulating” between units, and “targeted” delivery of saline‐soluble drugs are of uppermost priority.  相似文献   

3.
A novel polymer encapsulation strategy to synthesize metal isolated‐single‐atomic‐site (ISAS) catalysts supported by porous nitrogen‐doped carbon nanospheres is reported. First, metal precursors are encapsulated in situ by polymers through polymerization; then, metal ISASs are created within the polymer‐derived p‐CN nanospheres by controlled pyrolysis at high temperature (200–900 °C). Transmission electron microscopy and N2 sorption results reveal this material to exhibit a nanospheric morphology, a high surface area (≈380 m2 g?1), and a porous structure (with micropores and mesopores). Characterization by aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy and X‐ray absorption fine structure confirms the metal to be present as metal ISASs. This methodology is applicable to both noble and nonprecious metals (M‐ISAS/p‐CN, M = Co, Ni, Cu, Mn, Pd, etc.). In particular, the Co‐ISAS/p‐CN nanospheres obtained using this method show comparable (E1/2 = 0.838 V) electrochemical oxygen reduction activity to commercial Pt/C with 20 wt% Pt loading (E1/2 = 0.834 V) in alkaline media, superior methanol tolerance, and outstanding stability, even after 5000 cycles.  相似文献   

4.
Golden bristlegrass‐like unique nanostructures comprising reduced graphene oxide (rGO) matrixed nanofibers entangled with bamboo‐like N‐doped carbon nanotubes (CNTs) containing CoSe2 nanocrystals at each node (denoted as N‐CNT/rGO/CoSe2 NF) are designed as anodes for high‐rate sodium‐ion batteries (SIBs). Bamboo‐like N‐doped CNTs (N‐CNTs) are successfully generated on the rGO matrixed nanofiber surface, between rGO sheets and mesopores, and interconnected chemically with homogeneously distributed rGO sheets. The defects in the N‐CNTs formed by a simple etching process allow the complete phase conversion of Co into CoSe2 through the efficient penetration of H2Se gas inside the CNT walls. The N‐CNTs bridge the vertical defects for electron transfer in the rGO sheet layers and increase the distance between the rGO sheets during cycles. The discharge capacity of N‐CNT/rGO/CoSe2 NF after the 10 000th cycle at an extremely high current density of 10 A g?1 is 264 mA h g?1, and the capacity retention measured at the 100th cycle is 89%. N‐CNT/rGO/CoSe2 NF has final discharge capacities of 395, 363, 328, 304, 283, 263, 246, 223, 197, 171, and 151 mA h g?1 at current densities of 1, 2, 4, 6, 8, 10, 12, 14, 16, 18, and 20 A g?1, respectively.  相似文献   

5.
By combining two kinds of solution‐processable two‐dimensional materials, a flexible transistor array is fabricated in which MoS2 thin film is used as the active channel and reduced graphene oxide (rGO) film is used as the drain and source electrodes. The simple device configuration and the 1.5 mm‐long MoS2 channel ensure highly reproducible device fabrication and operation. This flexible transistor array can be used as a highly sensitive gas sensor with excellent reproducibility. Compared to using rGO thin film as the active channel, this new gas sensor exhibits much higher sensitivity. Moreover, functionalization of the MoS2 thin film with Pt nanoparticles further increases the sensitivity by up to ~3 times. The successful incorporation of a MoS2 thin‐film into the electronic sensor promises its potential application in various electronic devices.  相似文献   

6.
This study develops a novel strategy, based on block copolymer self‐assembly in solution, for preparing two‐dimensional (2D) graphene‐based mesoporous nanohybrids with well‐defined large pores of tunable sizes, by employing polystyrene‐block‐poly(ethylene oxide) (PS‐b‐PEO) spherical micelles as the pore‐creating template. The resultant 2D nanohybrids possess a sandwich‐like structure with Fe2O3 nanoparticle‐embedded mesoporous polypyrrole (PPy) monolayers grown on both sides of reduced graphene oxide (rGO) nanosheets (denoted as mPPy‐Fe2O3@rGO). Serving as supercapacitor electrode materials, the 2D ternary nanohybrids exhibit controllable capacitive performance depending on the pore size, with high capacitance (up to 1006 F/g at 1 A/g), good rate performance (750 F/g at 20 A/g) and excellent cycling stability. Furthermore, the pyrolysis of mPPy‐Fe2O3@rGO at 800 °C yields 2D sandwich‐like mesoporous nitrogen‐doped carbon/Fe3O4/rGO (mNC‐Fe3O4@rGO). The mNC‐Fe3O4@rGO nanohybrids with a mean pore size of 12 nm show excellent electrocatalytic activity as an oxygen reduction reaction (ORR) catalyst with a four‐electron transfer nature, a high half‐wave‐potential of +0.84 V and a limiting current density of 5.7 mA/cm2, which are well comparable with those of the best commercial Pt/C catalyst. This study takes advantage of block copolymer self‐assembly for the synthesis of 2D multifunctional mesoporous nanohybrids, and helps to understand the control of their structures and electrochemical performance.  相似文献   

7.
As anodes of Li‐ion batteries, copper oxides (CuO) have a high theoretical specific capacity (674 mA h g?1) but own poor cyclic stability owing to the large volume expansion and low conductivity in charges/discharges. Incorporating reduced graphene oxide (rGO) into CuO anodes with conventional methods fails to build robust interaction between rGO and CuO to efficiently improve the overall anode performance. Here, Cu2O/CuO/reduced graphene oxides (Cu2O/CuO/rGO) with a 3D hierarchical nanostructure are synthesized with a facile, single‐step hydrothermal method. The Cu2O/CuO/rGO anode exhibits remarkable cyclic and high‐rate performances, and particularly the anode with 25 wt% rGO owns the best performance among all samples, delivering a record capacity of 550 mA h g?1 at 0.5 C after 100 cycles. The pronounced performances are attributed to the highly efficient charge transfer in CuO nanosheets encapsulated in rGO network and the mitigated volume expansion of the anode owing to its robust 3D hierarchical nanostructure.  相似文献   

8.
The ingenious design of a freestanding flexible electrode brings the possibility for power sources in emerging wearable electronic devices. Here, reduced graphene oxide (rGO) wraps carbon nanotubes (CNTs) and rGO tightly surrounded by MnO2 nanosheets, forming a 3D multilevel porous conductive structure via vacuum freeze‐drying. The sandwich‐like architecture possesses multiple functions as a flexible anode for lithium‐ion batteries. Micrometer‐sized pores among the continuously waved rGO layers could extraordinarily improve ion diffusion. Nano‐sized pores among the MnO2 nanosheets and CNT/rGO@MnO2 particles could provide vast accessible active sites and alleviate volume change. The tight connection between MnO2 and carbon skeleton could facilitate electron transportation and enhance structural stability. Due to the special structure, the rGO‐wrapped CNT/rGO@MnO2 porous film as an anode shows a high capacity, excellent rate performance, and superior cycling stability (1344.2 mAh g−1 over 630 cycles at 2 A g−1, 608.5 mAh g−1 over 1000 cycles at 7.5 A g−1). Furthermore, the evolutions of microstructure and chemical valence occurring inside the electrode after cycling are investigated to illuminate the structural superiority for energy storage. The excellent electrochemical performance of this freestanding flexible electrode makes it an attractive candidate for practical application in flexible energy storage.  相似文献   

9.
Development of efficient and durable non‐Pt catalysts for hydrogen evolution reaction (HER) in acid media is highly desirable. Iron nitride has emerged as a promising catalyst for its cost‐effective nature, but the corresponding acidic stability must be promoted. Herein, phosphorus‐decorated Fe2N and reduced graphene oxide (P‐Fe2N/rGO) composite are designed and synthesized. X‐ray photoelectron spectroscopy and X‐ray absorption fine structure (XAFS) show that a thin layer amorphous iron phosphide is coated on the surface of Fe2N nanoparticles, which could be responsible for the well resistance of chemical corrosion in acidic media. Meanwhile, the P‐decoration could tune the electronic state and coordination environment of iron atom as evidenced by XAFS, resulting in dramatically enhanced electrocatalytic activity of P‐Fe2N/rGO. Density functional theory calculations reveal that both the P‐connected N atoms and the Fe atoms in P‐Fe2N/rGO catalyst are the main active sites for H* adsorption. The hydrogen‐binding free energy |ΔGH*| value is close to zero for P‐Fe2N/rGO, suggesting a good balance between the Volmer and Heyrovsky/Tafel steps in HER kinetics. As expected, P‐Fe2N/rGO catalyst could achieve a low ηonset of 22.4 mV, a small Tafel plot of 48.7 mV dec?1, and remarkable stability for HER in acid electrolyte.  相似文献   

10.
Recently, binary ZnCo2O4 has drawn enormous attention for lithium‐ion batteries (LIBs) as attractive anode owing to its large theoretical capacity and good environmental benignity. However, the modest electrical conductivity and serious volumetric effect/particle agglomeration over cycling hinder its extensive applications. To address the concerns, herein, a rapid laser‐irradiation methodology is firstly devised toward efficient synthesis of oxygen‐vacancy abundant nano‐ZnCo2O4/porous reduced graphene oxide (rGO) hybrids as anodes for LIBs. The synergistic contributions from nano‐dimensional ZnCo2O4 with rich oxygen vacancies and flexible rGO guarantee abundant active sites, fast electron/ion transport, and robust structural stability, and inhibit the agglomeration of nanoscale ZnCo2O4, favoring for superb electrochemical lithium‐storage performance. More encouragingly, the optimal L‐ZCO@rGO‐30 anode exhibits a large reversible capacity of ≈1053 mAh g?1 at 0.05 A g?1, excellent cycling stability (≈746 mAh g?1 at 1.0 A g?1 after 250 cycles), and preeminent rate capability (≈686 mAh g?1 at 3.2 A g?1). Further kinetic analysis corroborates that the capacitive‐controlled process dominates the involved electrochemical reactions of hybrid anodes. More significantly, this rational design holds the promise of being extended for smart fabrication of other oxygen‐vacancy abundant metal oxide/porous rGO hybrids toward advanced LIBs and beyond.  相似文献   

11.
Although hypodermic needles are a “gold standard” for transdermal drug delivery (TDD), microneedle (MN)-mediated TDD denotes an unconventional approach in which drug compounds are delivered via micron-size needles. Herein, an isotropic XeF2 dry etching process is explored to fabricate silicon-based solid MNs. A photolithographic process, including mask writing, UV exposure, and dry etching with XeF2 is employed, and the MN fabrication is successfully customized by modifying the CAD designs, photolithographic process, and etching conditions. This study enables fabrication of a very dense MNs (up to 1452 MNs cm−2) with height varying between 80 and 300 µm. Geometrical features are also assessed using scanning electron microscopy (SEM) and 3D laser scanning microscope. Roughness of the MNs are improved from 0.71 to 0.35 µm after titanium and chromium coating. Mechanical failure test is conducted using dynamic mechanical analyzer to determine displacement and stress/strain values. The coated MNs are subjected to less displacement (≈15 µm) upon the applied force. COMSOL Multiphysics analysis indicates that MNs are safe to use in real-life applications with no fracture. This technique also enables the production of MNs with distinct shape and dimensions. The optimized process provides a wide range of solid MN types to be utilized for epidermis targeting.  相似文献   

12.
The accuracy of traditional bischromophore‐based ratiometric probes is always compromised by undesirable energy/charge transferring interactions between the internal reference moiety and the sensing chromophore. In this regard, ratiometric sensing with a monochromophore system is highly desirable. Herein, an unprecedented monochromophore‐based ratiometric probe, which consists of a hydrophilic backbone poly(N‐vinylpyrrolidone) (PVP) and single chromophore of platinum(II) tetraphenylporphyrin (Pt‐TPP) is reported. Combination of the specific assembled clustering‐triggered fluorescent emission (oxygen‐insensitive) with the original Pt‐TPP phosphorescence (oxygen‐sensitive) enables successful construction of a monochromophore‐based ratiometric nanosensor for directly tracing hypoxia in vivo, along with the preferable facilitation of enhanced permeation and retention effect and long excitation wavelength. The unique ratiometric signals enable the direct observation from normoxic to hypoxic environment in both living A549 cells and a tumor‐bearing mice model, providing a significant paradigm of a monochromophore‐based dual‐emissive system with the specific assembled cluster emission. The work satisfactorily demonstrates a valuable strategy for designing monochromophore‐based dual‐emissive materials, and validates its utility for in vivo ratiometric biological sensing without the common energy/charge interference in bischromophore‐based system.  相似文献   

13.
The extraction of interstitial fluid (ISF) from skin using microneedles (MNs) has attracted growing interest in recent years due to its potential for minimally invasive diagnostics and biosensors. ISF collection by absorption into a hydrogel MN patch is a promising way that requires the materials to have outstanding swelling ability. Here, a gelatin methacryloyl (GelMA) patch is developed with an 11 × 11 array of MNs for minimally invasive sampling of ISF. The properties of the patch can be tuned by altering the concentration of the GelMA prepolymer and the crosslinking time; patches are created with swelling ratios between 293% and 423% and compressive moduli between 3.34 MPa and 7.23 MPa. The optimized GelMA MN patch demonstrates efficient extraction of ISF. Furthermore, it efficiently and quantitatively detects glucose and vancomycin in ISF in an in vivo study. This minimally invasive approach of extracting ISF with a GelMA MN patch has the potential to complement blood sampling for the monitoring of target molecules from patients.  相似文献   

14.
Under development for next‐generation wearable electronics are flexible, knittable, and wearable energy‐storage devices with high energy density that can be integrated into textiles. Herein, knittable fiber‐shaped zinc–air batteries with high volumetric energy density (36.1 mWh cm?3) are fabricated via a facile and continuous method with low‐cost materials. Furthermore, a high‐yield method is developed to prepare the key component of the fiber‐shaped zinc–air battery, i.e., a bifunctional catalyst composed of atomically thin layer‐by‐layer mesoporous Co3O4/nitrogen‐doped reduced graphene oxide (N‐rGO) nanosheets. Benefiting from the high surface area, mesoporous structure, and strong synergetic effect between the Co3O4 and N‐rGO nanosheets, the bifunctional catalyst exhibits high activity and superior durability for oxygen reduction and evolution reactions. Compared to a fiber‐shaped zinc–air battery using state‐of‐the‐art Pt/C + RuO2 catalysts, the battery based on these Co3O4/N‐rGO nanosheets demonstrates enhanced and stable electrochemical performance, even under severe deformation. Such batteries, for the first time, can be successfully knitted into clothes without short circuits under external forces and can power various electronic devices and even charge a cellphone.  相似文献   

15.
A one‐step in situ tailoring of NiCo2S4 nanostructures is demonstrated on fluorine‐doped tin oxide (FTO) as Pt‐free counter electrodes (CEs) for dye‐sensitized solar cells (DSSCs) with performance surpassing that of a conventional Pt‐sputtered CE. An interconnected NiCo2S4 nanosheet network is successfully constructed on the FTO glass via a hydrothermal method, attributed to the synergistic effect of structure‐directing hexamethylenetetramine and L‐cysteine. A growth mechanism is proposed, and the effects of nanostructures and sulfur atomic percentages on the electrocatalytic performance are discussed in depth. A DSSC with the optimized interconnected NiCo2S4 nanosheet CE exhibits higher power conversion efficiency (7.22%) compared to that with a conventional Pt‐sputtered CE (6.87%) due to excellent charge transport properties and enhanced electrocatalytic activity of the NiCo2S4 nanostructures. This work showcases the strong potential of nanostructured ternary chalcogenides, which are composed of earth‐abundant elements and prepared through a single‐step hydrothermal process without tedious posttreatments, to reduce the dependence of platinum in DSSCs and other electrochemical devices.  相似文献   

16.
Metal nanocrystals (NCs) are grown directly on the surface of reduced graphene oxide (rGO), which can maximize the rGO‐NCs contact/interaction to achieve the enhanced catalytic activity. However, it is difficult to control the size and morphology of metal NCs by in situ method due to the effects of functional groups on the surface of GO, and as a result, the metal NCs/rGO hybrids are conventionally synthesized by two‐step method. Herein, one‐pot synthesis of Pt–Co alloy NCs is demonstrated with concave‐polyhedrons and concave‐nanocubes bounded by {hkl} and {hk0} high‐index facets (HIFs) distributed on rGO. GO can affect the geometry and electronic structure of Pt–Co NCs. Thanks to the synergy of the HIFs and the electronic effect of the intimate contact/interaction between Pt–Co alloy and rGO, these as‐prepared Pt–Co NCs/rGO hybrids presents enhanced catalytic properties for the electrooxidation of formic acid, as well as for the oxygen reduction reaction.  相似文献   

17.
Controllable and efficient synthesis of noble metal/transition‐metal oxide (TMO) composites with tailored nanostructures and precise components is essential for their application. Herein, a general mercaptosilane‐assisted one‐pot coassembly approach is developed to synthesize ordered mesoporous TMOs with agglomerated‐free noble metal nanoparticles, including Au/WO3, Au/TiO2, Au/NbOx, and Pt/WO3. 3‐mercaptopropyl trimethoxysilane is applied as a bridge agent to cohydrolyze with metal oxide precursors by alkoxysilane moieties and interact with the noble metal source (e.g., HAuCl4 and H2PtCl4) by mercapto (? SH) groups, resulting in coassembly with poly(ethylene oxide)‐b‐polystyrene. The noble metal decorated TMO materials exhibit highly ordered mesoporous structure, large pore size (≈14–20 nm), high specific surface area (61–138 m2 g?1), and highly dispersed noble metal (e.g., Au and Pt) nanoparticles. In the system of Au/WO3, in situ generated SiO2 incorporation not only enhances their thermal stability but also induces the formation of ε‐phase WO3 promoting gas sensing performance. Owning to its specific compositions and structure, the gas sensor based on Au/WO3 materials possess enhanced ethanol sensing performance with a good response (Rair/Rgas = 36–50 ppm of ethanol), high selectivity, and excellent low‐concentration detection capability (down to 50 ppb) at low working temperature (200 °C).  相似文献   

18.
Single‐atom catalysts are becoming a hot research topic owing to their unique characteristics of maximum specific activity and atomic utilization. Herein, a new single‐atom nanozyme (SAN) based on single Fe atoms anchored on N‐doped carbons supported on carbon nanotube (CNT/FeNC) is proposed. The CNT/FeNC with robust atomic Fe–Nx moieties is synthesised, showing superior peroxidase‐like activity. Furthermore, the CNT/FeNC is used as the signal element in a series of paper‐based bioassays for ultrasensitive detection of H2O2, glucose, and ascorbic acid. The SAN provides a new type of signal element for developing various biosensing techniques.  相似文献   

19.
Objective: The present study was aimed to investigate the effect of salient microneedle (MN) geometry parameters like length, density, shape and type on transdermal permeation enhancement of Zolmitriptan (ZMT).

Methods: Two types of MN devices viz. AdminPatch® arrays (ADM) (0.6, 0.9, 1.2 and 1.5?mm lengths) and laboratory fabricated polymeric MNs (PM) of 0.6?mm length were employed. In the case of PMs, arrays were applied thrice at different places within a 1.77?cm2 skin area (PM-3) to maintain the MN density closer to 0.6?mm ADM. Scaling analyses was done using dimensionless parameters like concentration of ZMT (Ct/Cs), thickness (h/L) and surface area of the skin (Sa/L2).

Results: Micro-injection molding technique was employed to fabricate PM. Histological studies revealed that the PM, owing to their geometry/design, formed wider and deeper microconduits when compared to ADM of similar length. Approximately 3.17- and 3.65-fold increase in ZMT flux values were observed with 1.5?mm ADM and PM-3 applications when compared to the passive studies. Good correlations were observed between different dimensionless parameters with scaling analyses. Numerical simulations, using MATLAB and COMSOL software, based on experimental data and histological images provided information regarding the ZMT skin distribution after MN application.

Discussion: Both from experimental studies and simulations, it was inferred that PM were more effective in enhancing the transdermal delivery of ZMT when compared to ADM.

Conclusions: The study suggests that MN application enhances the ZMT transdermal permeation and the geometrical parameters of MNs play an important role in the degree of such enhancement.  相似文献   

20.
Micromotor‐mediated synthesis of thread‐like hydrogel microstructures in an aqueous environment is presented. The study utilizes a catalytic micromotor assembly (owing to the presence of a Pt layer), with an on‐board chemical reservoir (i.e., polymerization mixture), toward thread‐like radical‐polymerization via autonomously propelled bots (i.e., TRAP bots). Synergistic coupling of catalytically active Pt layer, together with radical initiators (H2O2 and FeCl3 (III)), and PEGDA monomers preloaded into the TRAP bot, results in the polymerization of monomeric units into elongated thread‐like hydrogel polymers coupled with self‐propulsion. Interestingly, polymer generation via TRAP bots can also be triggered in the absence of hydrogen peroxide for cellular/biomedical application. The resulting polymeric hydrogel microstructures are able to entrap living cells (NIH 3T3 fibroblast cells), and are easily separable via a centrifugation or magnetic separation (owing to the presence of a Ni layer). The cellular biocompatibility of TRAP bots is established via a LIVE/DEAD assay and MTS cell proliferation assay (7 days observation). This is the first study demonstrating real‐time in situ hydrogel polymerization via an artificial microswimmer, capable of enmeshing biotic/abiotic microobjects in its reaction environment, and lays a strong foundation for advanced applications in cell/tissue engineering, drug delivery, and cleaner technologies.  相似文献   

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