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1.
Robust hollow spheres consisting of molecular‐scale alternating titania (Ti0.91O2) nanosheets and graphene (G) nanosheets are successfully fabricated by a layer‐by‐layer assembly technique with polymer beads as sacrificial templates using a microwave irradiation technique to simultaneously remove the template and reduce graphene oxide into graphene. The molecular scale, 2D contact of Ti0.91O2 nanosheets and G nanosheets in the hollow spheres is distinctly different from the prevenient G‐based TiO2 nanocomposites prepared by simple integration of TiO2 and G nanosheets. The nine times increase of the photocatalytic activity of G‐Ti0.91O2 hollow spheres relative to commercial P25 TiO2 is confirmed with photoreduction of CO2 into renewable fuels (CO and CH4). The large enhancement in the photocatalytic activity benefits from: 1) the ultrathin nature of Ti0.91O2 nanosheets allowing charge carriers to move rapidly onto the surface to participate in the photoreduction reaction; 2) the sufficiently compact stacking of ultrathin Ti0.91O2 nanosheets with G nanosheets allowing the photogenerated electron to transfer fast from the Ti0.91O2 nanosheets to G to enhance lifetime of the charge carriers; and 3) the hollow structure potentially acting as a photon trap‐well to allow the multiscattering of incident light for the enhancement of light absorption.  相似文献   

2.
In the present work, we report enhanced photocatalytic degradation of methylene blue dye in aqueous solution by using ultra-thin anatase TiO2 nanosheets (NSs) combined with graphene oxide (GO) as a photocatalyst. The two-dimensional ultra-thin anatase TiO2 NSs are fabricated via chemical exfoliation. By completely delaminating a lepidocrocite-type layered protonic titanate HxTi2−x/4x/4O4·H2O (x=0.7, □: vacancy) into individual layers through ion exchange with tetrabutylammonium (TBA+) cations, well-dispersed ultra-thin colloidal Ti0.91O2 NSs with a lateral size up to a few micrometers are obtained. Subsequent acid treatment induces colloidal Ti0.91O2 to reassemble and precipitate into a gelation form, followed by thermal annealing to convert the Ti0.91O2 gelation into anatase TiO2 nanosheets as photocatalyst for methylene blue degradation. TiO2 NSs show a high photocatalytic degradation efficiency of 53.2% due to the ultra-thin thickness for facile electron transfering and large surface area for methylene blue absorption. Moreover, photocatalytic effect can be further improved by simply adding GO suspension to achieve colloidal self-assembly of GO and TiO2 NSs. An optimal GO content of 3 wt% further increases the photocatalytic degradation efficiency to 91.2% due to faster electron–hole seperation and improved surface area provided by GO. This work provides a simple but effective approach by combing graphene oxide with TiO2 nanosheets synthesized via the exfoliation method for methylene blue degradation.  相似文献   

3.
Highly stable graphene oxide (GO)‐based multilayered ultrathin films can be covalently immobilized on solid supports through a covalent‐based method. It is demonstrated that when (3‐aminopropyl) trimethoxysilane (APTMS), which works as a covalent cross‐linking agent, and GO nanosheets are assembled in an layer‐by‐layer (LBL) manner, GO nanosheets can be covalently grafted on the solid substrate successfully to produce uniform multilayered (APTMS/GO)N films over large‐area surfaces. Compared with conventional noncovalent LBL films constructed by electrostatic interactions, those assembled using this covalent‐based method display much higher stability and reproducibility. Upon thermal annealing‐induced reduction of the covalent (APTMS/GO)N films, the obtained reduced GO (RGO) films, (APTMS/RGO)N, preserve their basic structural characteristics. It is also shown that the as‐prepared covalent (APTMS/RGO)N multilayer films can be used as highly stable source/drain electrodes in organic field‐effect transistors (OFETs). When the number of bilayers of the (APTMS/RGO)N film exceeds 2 (ca. 2.7 nm), the OFETs based on (APTMS/RGO)N electrodes display much better electrical performance than devices based on 40 nm Au electrodes. The covalent protocol proposed may open up new opportunities for the construction of graphene‐based ultrathin films with excellent stability and reproducibility, which are desired for practical applications that require withstanding of multistep post‐production processes.  相似文献   

4.
A zeolitic‐imidazolate‐framework (ZIF) nanocrystal layer‐protected carbonization route is developed to prepare N‐doped nanoporous carbon/graphene nano‐sandwiches. The ZIF/graphene oxide/ZIF sandwich‐like structure with ultrasmall ZIF nanocrystals (i.e., ≈20 nm) fully covering the graphene oxide (GO) is prepared via a homogenous nucleation followed by a uniform deposition and confined growth process. The uniform coating of ZIF nanocrystals on the GO layer can effectively inhibit the agglomeration of GO during high‐temperature treatment (800 °C). After carbonization and acid etching, N‐doped nanoporous carbon/graphene nanosheets are formed, with a high specific surface area (1170 m2 g?1). These N‐doped nanoporous carbon/graphene nanosheets are used as the nonprecious metal electrocatalysts for oxygen reduction and exhibit a high onset potential (0.92 V vs reversible hydrogen electrode; RHE) and a large limiting current density (5.2 mA cm?2 at 0.60 V). To further increase the oxygen reduction performance, nanoporous Co‐Nx/carbon nanosheets are also prepared by using cobalt nitrate and zinc nitrate as cometal sources, which reveal higher onset potential (0.96 V) than both commercial Pt/C (0.94 V) and N‐doped nanoporous carbon/graphene nanosheets. Such nanoporous Co‐Nx/carbon nanosheets also exhibit good performance such as high activity, stability, and methanol tolerance in acidic media.  相似文献   

5.
A novel, in situ simultaneous reduction‐hydrolysis technique (SRH) is developed for fabrication of TiO2‐‐graphene hybrid nanosheets in a binary ethylenediamine (En)/H2O solvent. The SRH technique is based on the mechanism of the simultaneous reduction of graphene oxide (GO) into graphene by En and the formation of TiO2 nanoparticles through hydrolysis of titanium (IV) (ammonium lactato) dihydroxybis, subsequently in situ loading onto graphene through chemical bonds (Ti–O–C bond) to form 2D sandwich‐like nanostructure. The dispersion of TiO2 hinders the collapse and restacking of exfoliated sheets of graphene during reduction process. In contrast with prevenient G‐TiO2 nanocomposites, abundant Ti3+ is detected on the surface of TiO2 of the present hybrid, caused by reducing agent En. The Ti3+ sites on the surface can serve as sites for trapping photogenerated electrons to prevent recombination of electron–hole pairs. The high photocatalytic activity of G‐TiO2 hybrid is confirmed by photocatalytic conversion of CO2 to valuable hydrocarbons (CH4 and C2H6) in the presence of water vapor. The synergistic effect of the surface‐Ti3+ sites and graphene favors the generation of C2H6, and the yield of the C2H6 increases with the content of incorporated graphene. The work may open a new doorway for new significant application of graphene for selectively catalytic C–C coupling reaction  相似文献   

6.
TiO2 nanorods are self‐assembled on the graphene oxide (GO) sheets at the water/toluene interface. The self‐assembled GO–TiO2 nanorod composites (GO–TiO2 NRCs) can be dispersed in water. The effective anchoring of TiO2 nanorods on the whole GO sheets is confirmed by transmission electron microscopy (TEM), X‐ray diffraction (XRD), Fourier transform IR spectroscopy (FTIR), and thermogravimetric analysis (TGA). The significant increase of photocatalytic activity is confirmed by the degradation of methylene blue (MB) under UV light irridiation. The large enhancement of photocatalytic activity is caused by the effective charge anti‐recombination and the effective absorption of MB on GO. The effective charge transfer from TiO2 to GO sheets is confirmed by the significant photoluminescence quenching of TiO2 nanorods, which can effectively prevent the charge recombination during photocatalytic process. The effective absorption of MB on GO is confirmed by the UV‐vis spectra. The degradation rate of MB in the second cycle is faster than that in the first cycle because of the reduction of GO under UV light irradiation.  相似文献   

7.
An ex situ strategy for fabrication of graphene oxide (GO)/metal oxide hybrids without assistance of surfactant is introduced. Guided by this strategy, GO/Al2O3 hybrids are fabricated by two kinds of titration methods in which GO and Al2O3 colloids are utilized as titrant for hybrids of low and high GO content respectively. After sintered by spark plasma sintering, few‐layer graphene (FG)/Al2O3 nanocomposites are obtained and GO is well reduced to FG simultaneously. A percolation threshold as low as 0.38 vol.% is achieved and the electrical conductivity surpasses 103 Sm?1 when FG content is only 2.35 vol.% in FG/Al2O3 composite, revealing the homogeneous dispersion and high quality of as‐prepared FG. Furthermore, it is found that the charge carrier type changes from p‐ to n‐type as graphene content becomes higher. It is deduced that this conversion is related to the doping effect induced by Al2O3 matrix and is thickness‐dependent with respect to FG.  相似文献   

8.
There has been significant progress in the field of semiconductor photocatalysis, but it is still a challenge to fabricate low‐cost and high‐activity photocatalysts because of safety issues and non‐secondary pollution to the environment. Here, 2D hexagonal nanoplates of α‐Fe2O3/graphene composites with relatively good distribution are synthesized for the first time using a simple, one‐step, template‐free, hydrothermal method that achieves the effective reduction of the graphene oxide (GO) to graphene and intimate and large contact interfaces of the α‐Fe2O3 nanoplates with graphene. The α‐Fe2O3/graphene composites showed significantly enhancement in the photocatalytic activity compared with the pure α‐Fe2O3 nanoplates. At an optimal ratio of 5 wt% graphene, 98% of Rhodamine (RhB) is decomposed with 20 min of irradiation, and the rate constant of the composites is almost four times higher than that of pure α‐Fe2O3 nanoplates. The decisive factors in improving the photocatalytic performance are the intimate and large contact interfaces between 2D hexagonal α‐Fe2O3 nanoplates and graphene, in addition to the high electron withdrawing/storing ability and the highconductivity of reduced graphene oxide (RGO) formed during the hydrothermal reaction. The effective charge transfer from α‐Fe2O3 nanoplates to graphene sheets is demonstrated by the significant weakening of photoluminescence in α‐Fe2O3/graphene composites.  相似文献   

9.
Construction of multifunctional stimuli‐responsive nanosystems intelligently responsive to inner physiological and/or external irradiations based on nanobiotechnology can enable the on‐demand drug release and improved diagnostic imaging to mitigate the side‐effects of anticancer drugs and enhance the diagnostic/therapeutic outcome simultaneously. Here, a triple‐functional stimuli‐responsive nanosystem based on the co‐integration of superparamagnetic Fe3O4 and paramagnetic MnOx nanoparticles (NPs) onto exfoliated graphene oxide (GO) nanosheets by a novel and efficient double redox strategy (DRS) is reported. Aromatic anticancer drug molecules can interact with GO nanosheets through supramolecular π stacking to achieve high drug loading capacity and pH‐responsive drug releasing performance. The integrated MnOx NPs can disintegrate in mild acidic and reduction environment to realize the highly efficient pH‐responsive and reduction‐triggered T1‐weighted magnetic resonance imaging (MRI). Superparamagnetic Fe3O4 NPs can not only function as the T2‐weighted contrast agents for MRI, but also response to the external magnetic field for magnetic hyperthermia against cancer. Importantly, the constructed biocompatible GO‐based nanoplatform can inhibit the metastasis of cancer cells by downregulating the expression of metastasis‐related proteins, and anticancer drug‐loaded carrier can significantly reverse the multidrug resistance (MDR) of cancer cells.  相似文献   

10.
This work describes a new one‐step large‐scale electrochemical synthesis of graphene/polyaniline (PANI) composite films using graphite oxide (GO) and aniline as the starting materials. The size of the film could be controlled by the area of indium tin oxide (ITO). Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X‐ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), and ultraviolet–visible absorption spectrum (UV–vis) results demonstrated that the graphene/PANI composite film was successfully synthesized. The obtained graphene/PANI composite film showed large specific area, high conductivity, good biocompatibility, and fast redox properties and had perfect layered and encapsulated structures. Electrochemical experiments indicated that the composite film had high performances and could be widely used in applied electrochemical fields. As a model, horseradish peroxidase (HRP) was entrapped onto the film‐modi?ed glassy carbon electrode (GCE) and used to construct a biosensor. The immobilized HRP showed a pair of well‐de?ned redox peaks and high catalytic activity for the reduction of H2O2. Furthermore, the graphene/PANI composite film could be directly used as the supercapacitor electrode. The supercapacitor showed a high specific capacitance of 640 F g?1 with a retention life of 90% after 1000 charge/discharge cycles.  相似文献   

11.
This work proposes a new perovskite solar cell structure by including lithium‐neutralized graphene oxide (GO‐Li) as the electron transporting layer (ETL) on top of the mesoporous TiO2 (m‐TiO2) substrate. The modified work‐function of GO after the intercalation of Li atoms (4.3 eV) exhibits a good energy matching with the TiO2 conduction band, leading to a significant enhancement of the electron injection from the perovskite to the m‐TiO2. The resulting devices exhibit an improved short circuit current and fill factor and a reduced hysteresis. Furthermore, the GO‐Li ETL partially passivates the oxygen vacancies/defects of m‐TiO2 by resulting in an enhanced stability under prolonged 1 SUN irradiation.  相似文献   

12.
Here, a facile approach for the in situ fabrication of metal sulfide (MS)‐graphene (G) nanocomposite, CdS‐G and PbS‐G, on indium?tin oxide (ITO) glass is demonstrated using a simple and scalable direct‐laser‐writing method in ambient air. Through the CO2 laser irradiation of a metal‐complex‐containing polyethersulfone layer on ITO glass, both the crystallization of laser‐induced MS (LIMS) and the formation of laser‐induced graphene (LIG) are synchronously achieved in one step, giving rise to a laser‐induced MS‐G nanocomposite photoelectrode, denoted as LI‐MS‐G@ITO. In such a laser‐scribing process, polyethersulfone not only acts as the carbon source to grow LIG but also provides an in situ source of S2? to produce LIMS with the aids of carbothermic reduction of sulfur element in polyethersulfone. The obtained LI‐MS‐G@ITO inherits the porous network architecture of polyethersulfone‐derived LIG, in which the LIMS nanocrystals uniformly decorate the multilayered graphene sheets with good dispersion, presenting a fast and stable photocurrent response with high reproducibility, which, as a proof‐of‐concept, further facilitates the use of a LI‐CdS‐G@ITO photoanode as an efficient transducer for photoelectrochemical detection of Cu2+ with high sensitivity and selectivity. This work can offer a universal and versatile protocol for the in situ and synchronous fabrication of novel MS‐G nanocomposites for sensitive photoelectrochemical analysis.  相似文献   

13.
2D nanoscale oxides have attracted a large amount of research interest due to their unique properties. Here, a facile synthetic approach to prepare graphene‐mimicking, porous 2D Co3O4 nanofoils using graphene oxide (GO) as a sacrificial template is reported. The thermal instability of graphene, as well as the catalytic ability of Co3O4 particles to degrade carbon backbones, allow the fabrication of porous 2D Co3O4 nanofoils without the loss of the 2D nature of GO. Based on these results, a graphene mimicking as a route for large‐area 2D transition metal oxides for applications in electrochemical energy storage devices is proposed. As a proof of concept, it is demonstrated that graphene‐like, porous 2D Co3O4 nanofoils exhibit a high reversible capacity (1279.2 mAh g?1), even after 50 cycles. This capacity is far beyond the theoretical capacity of Co3O4 based on the conversion mechanism from Co3O4 to Li2O and metallic Co.  相似文献   

14.
Ultrathin MnO2/graphene oxide/carbon nanotube (G/M@CNT) interlayers are developed as efficient polysulfide‐trapping shields for high‐performance Li–S batteries. A simple layer‐by‐layer procedure is used to construct a sandwiched vein–membrane interlayer of thickness 2 µm and areal density 0.104 mg cm?2 by loading MnO2 nanoparticles and graphene oxide (GO) sheets on superaligned carbon nanotube films. The G/M@CNT interlayer provides a physical shield against both polysulfide shuttling and chemical adsorption of polysulfides by MnO2 nanoparticles and GO sheets. The synergetic effect of the G/M@CNT interlayer enables the production of Li–S cells with high sulfur loadings (60–80 wt%), a low capacity decay rate (?0.029% per cycle over 2500 cycles at 1 C), high rate performance (747 mA h g?1 at a charge rate of 10 C), and a low self‐discharge rate with high capacity retention (93.0% after 20 d rest). Electrochemical impedance spectroscopy, cyclic voltammetry, and scanning electron microscopy observations of the Li anodes after cycling confirm the polysulfide‐trapping ability of the G/M@CNT interlayer and show its potential in developing high‐performance Li–S batteries.  相似文献   

15.
Introducing solar energy into membrane filtration to decrease energy and chemicals consumption represents a promising direction in membrane fields. In this study, a kind of 0D/2D heterojunction is fabricated by depositing biomineralized titanium dioxide (TiO2) nanoparticles with delaminated graphitic carbon nitride (g‐C3N4) nanosheets, and subsequently a kind of 2D heterostructure membrane is fabricated via intercalating g‐C3N4@TiO2 heterojunctions into adjacent graphene oxide (GO) nanosheets by a vacuum‐assisted self‐assembly process. Due to the enlarged interlayer spacing of GO nanosheets, the initial permeation flux of GO/g‐C3N4@TiO2 membrane reaches to 4536 Lm?2 h?1 bar?1, which is more than 40‐fold of GO membranes (101 Lm?2 h?1 bar?1) when utilized for oil/water separation. To solve the sharp permeation flux decline, arising from the adsorption of oil droplets, the a sunlight‐driven self‐cleaning process is followed, maintaining a flux recovery ratio of more than 95% after ten cycles of filtration experiment. The high permeation flux and excellent sunlight‐driven flux recovery of these heterostructure membranes manifest their attractive potential application in water purification.  相似文献   

16.
Lead sulfide (PbS) colloidal quantum dots (CQDs) solar cells possess the advantages of absorption into the infrared, solution processing, and multiple exciton generation, making them very competitive as a low‐cost photovoltaic alternative. Employing an n‐i‐p ZnO/tetrabutylammonium (TBAI)–PbS/ethanedithiol (EDT)–PbS device configuration, the present study reports a 9.0% photovoltaic device through ZnMgO electrode engineering and graphene doping. Sol–gel‐derived Zn0.9Mg0.1O buffer layer shows better transparency and higher conduction band maximum than ZnO, and incorporation of graphene and chlorinated graphene oxide into the TBAI–PbS and EDT–PbS layer respectively boosts carrier collection, leading to device with significantly enhanced open circuit voltage and short‐circuit current density. It is believed that incorporation of graphene into PbS CQD film as proposed here, and more generally nanosheets of other materials, would potentially open a simple and powerful avenue to overcome the carrier transport bottleneck of CQD optoelectronic device, thus pushing device performance to a new level.  相似文献   

17.
A novel lyotropic liquid‐crystal (LC) based assembly strategy is developed for the first time, to fabricate composite films of vanadium pentoxide (V2O5) nanobelts and graphene oxide (GO) sheets, with highly oriented layered structures. It is found that similar lamellar LC phases can be simply established by V2O5 nanobelts alone or by a mixture of V2O5 nanobelts and GO nanosheets in their aqueous dispersions. More importantly, the LC phases can be retained with any proportion of V2O5 nanobelts and GO, which allows facile optimization of the ratio of each component in the resulting films. Named VrGO, composite films manifest high electrical conductivity, good mechanical stability, and excellent flexibility, which allow them to be utilized as high performance electrodes in flexible energy storage devices. As demonstrated in this work, the VrGO films containing 67 wt% V2O5 exhibit excellent capacitance of 166 F g?1 at 10 A g?1; superior to those of the previously reported composites of V2O5 and nanocarbon. Moreover, the VrGO film in flexible lithium ion batteries delivers a high capacity of 215 mAh g?1 at 0.1 A g?1; comparable to the best V2O5 based cathode materials.  相似文献   

18.
The sensing performance of chemical sensors can be achieved not only by modification or hybridization of sensing materials but also through new design in device geometry. The performance of a chemical sensing device can be enhenced from a simple three‐dimensional (3D) chemiresistor‐based gas sensor platform with an increased surface area by forming networked, self‐assembled reduced graphene oxide (R‐GO) nanosheets on 3D SU8 micro‐pillar arrays. The 3D R‐GO sensor is highly responsive to low concentration of ammonia (NH3) and nitrogen dioxide (NO2) diluted in dry air at room temperature. Compared to the two‐dimensional planar R‐GO sensor structure, as the result of the increase in sensing area and interaction cross‐section of R‐GO on the same device area, the 3D R‐GO gas sensors show improved sensing performance with faster response (about 2%/s exposure), higher sensitivity, and even a possibly lower limit of detection towards NH3 at room temperature.  相似文献   

19.
Two‐dimensional (2D) atomic layers such as graphene, and metal chalcogenides have recently attracted tremendous attention due to their unique properties and potential applications. Unfortunately, in most cases, the free‐standing nanosheets easily re‐stack due to their van der Waals forces, and lose the advantages of their separated atomic layer state. Here, a bottom‐up approach is developed to build three‐dimensional (3D) architectures by 2D nanosheets such as MoS2 and graphene oxide nanosheets as building blocks, the thin nature of which can be well retained. After simply chemical reduction, the resulting 3D MoS2‐graphene architectures possess high surface area, porous structure, thin walls and high electrical conductivity. Such unique features are favorable for the rapid diffusions of both lithium ions and electrons during lithium storage. As a consequence, MoS2‐graphene electrodes exhibit high reversible capacity of ≈1200 mAh g?1, with very good cycling performance. Moreover, such a simple and low‐cost assembly protocol can provide a new pathway for the large‐scale production of various functional 3D architectures for energy storage and conversions.  相似文献   

20.
A green, simple, and cost effective electrochemical method to synthesize pure graphene oxide (GO) and graphene nanosheets (GNs) using pencil in ionic liquid medium is reported. The morphology and microstructure of prepared GNs and GO are examined using scanning electron microscopy (SEM), transmission electron microscopy (TEM), atomic force microscopy (AFM), X‐ray diffraction (XRD), and Raman spectroscopy; the experiments confirm the formation of high quality graphene. The synthesized GO is used for the real‐time and label‐free surface plasmon resonance (SPR) sensing of the biological warfare agent Salmonella typhi.  相似文献   

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