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1.
The construction of a novel 3D self‐supported integrated NixCo2?xP@NC (0 < x < 2) nanowall array (NA) on Ni foam (NF) electrode constituting highly dispersed NixCo2?xP nanoparticles, nanorods, nanocapsules, and nanodendrites embedded in N‐doped carbon (NC) NA grown on NF is reported. Benefiting from the collective effects of special morphological and structural design and electronic structure engineering, the NixCo2?xP@NC NA/NF electrodes exhibit superior electrocatalytic performance for water splitting with an excellent stability in a wide pH range. The optimal NiCoP@NC NA/NF electrode exhibits the best hydrogen evolution reaction (HER) activity in acidic solution so far, attaining a current density of 10 mA cm?2 at an overpotential of 34 mV. Moreover, the electrode manifests remarkable performances toward both HER and oxygen evolution reaction in alkaline medium with only small overpotentials of 37 mV at 10 mA cm?2 and 305 mV at 50 mA cm?2, respectively. Most importantly, when coupling with the NiCoP@NC NA/NF electrode for overall water splitting, an alkali electrolyzer delivers a current density of 20 mA cm?2 at a very low cell voltage of ≈1.56 V. In addition, the NiCoP@NC NA/NF electrode has outstanding long‐term durability at j = 10 mA cm?2 with a negligible degradation in current density over 22 h in both acidic and alkaline media.  相似文献   

2.
The development of highly efficient bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is crucial for improving the efficiency of overall water splitting, but still remains challenging issue. Herein, 3D self‐supported Fe‐doped Ni2P nanosheet arrays are synthesized on Ni foam by hydrothermal method followed by in situ phosphorization, which serve as bifunctional electrocatalysts for overall water splitting. The as‐synthesized (Ni0.33Fe0.67)2P with moderate Fe doping shows an outstanding OER performance, which only requires an overpotential of ≈230 mV to reach 50 mA cm?2 and is more efficient than the other Fe incorporated Ni2P electrodes. In addition, the (Ni0.33Fe0.67)2P exhibits excellent activity toward HER with a small overpotential of ≈214 mV to reach 50 mA cm?2. Furthermore, an alkaline electrolyzer is measured using (Ni0.33Fe0.67)2P electrodes as cathode and anode, respectively, which requires cell voltage of 1.49 V to reach 10 mA cm?2 as well as shows excellent stability with good nanoarray construction. Such good performance is attributed to the high intrinsic activity and superaerophobic surface property.  相似文献   

3.
Organic crystals that combine high charge‐carrier mobility and excellent light‐emission characteristics are expected to be of interest for light‐emitting transistors and diodes, and may offer renewed hope for electrically pumped laser action. High‐luminescence‐efficiency cyano‐substituted oligo(p‐ phenylene vinylene) (CN‐DPDSB) crystals (η ≈ 95%) grown by the physical vapor transport method is reported here, with high mobilities (at ≈10?2 cm2 V?1 s?1 order of magnitude) as measured by time‐of‐flight. The CN‐DPDSB crystals have well‐balanced bipolar carrier‐transport characteristics (μhole≈ 2.5–5.5 × 10?2 cm2 V?1 s?1; μelectron ≈ 0.9–1.3 × 10?2 cm2 V?1 s?1) and excellent optically pumped laser properties. The threshold for amplified spontaneous emission (ASE) is about 4.6 μJ per pulse (23 KW cm?2), while the gain coefficient at the peak wavelength of ASE and the loss coefficient caused by scattering are ≈35 and ≈1.7 cm?1, respectively. This indicates that CN‐DPDSB crystals are promising candidates for organic laser diodes.  相似文献   

4.
Herein, a novel polymer‐templated strategy is described to obtain 2D nickel‐based MOF nanosheets using Ni(OH)2, squaric acid, and polyvinylpyrrolidone (PVP), where PVP has a dual role as a structure‐directing agent, as well as preventing agglomeration of the MOF nanosheets. Furthermore, a scalable method is developed to transform the 2D MOF sheets to Ni7S6/graphene nanosheet (GNS) heterobilayers by in situ sulfidation using thiourea as a sulfur source. The Ni7S6/GNS composite shows an excellent reversible capacity of 1010 mAh g?1 at 0.12 A g?1 with a Coulombic efficiency of 98% capacity retention. The electrochemical performance of the Ni7S6/GNS composite is superior not only to nickel sulfide/graphene‐based composites but also to other metal disulfide–based composite electrodes. Moreover, the Ni7S6/GNS anode exhibits excellent cycle stability (≈95% capacity retention after 2000 cycles). This outstanding electrochemical performance can be attributed to the synergistic effects of Ni7S6 and GNS, where GNS serves as a conducting matrix to support Ni7S6 nanosheets while Ni7S6 prevents restacking of GNS. This work opens up new opportunities in the design of novel functional heterostructures by hybridizing 2D MOF nanosheets with other 2D nanomaterials for electrochemical energy storage/conversion applications.  相似文献   

5.
2D soft nanomaterials are an emerging research field due to their versatile chemical structures, easily tunable properties, and broad application potential. In this study, a benzene‐bridged polypyrrole film with a large area, up to a few square centimeters, is synthesized through an interfacial polymerization approach. As‐prepared semiconductive films exhibit a bandgap of ≈2 eV and a carrier mobility of ≈1.5 cm2 V?1 s?1, inferred from time‐resolved terahertz spectroscopy. The samples are employed to fabricate in‐plane micro‐supercapacitors (MSCs) by laser scribing and exhibit an ultrahigh areal capacitance of 0.95 mF cm?2, using 1‐ethyl‐3‐methylimidazolium tetrafluoroborate ([EMIM][BF4]) as an electrolyte. Importantly, the maximum energy and power densities of the developed MSCs reach values up to 50.7 mWh cm?3 and 9.6 kW cm?3, respectively; the performance surpassing most of the 2D material‐based MSCs is reported to date.  相似文献   

6.
Highly stretchable, high‐mobility, and free‐standing coplanar‐type all‐organic transistors based on deformable solid‐state elastomer electrolytes are demonstrated using ionic thermoplastic polyurethane (i‐TPU), thereby showing high reliability under mechanical stimuli as well as low‐voltage operation. Unlike conventional ionic dielectrics, the i‐TPU electrolyte prepared herein has remarkable characteristics, i.e., a large specific capacitance of 5.5 µF cm?2, despite the low weight ratio (20 wt%) of the ionic liquid, high transparency, and even stretchability. These i‐TPU‐based organic transistors exhibit a mobility as high as 7.9 cm2 V?1 s?1, high bendability (Rc, radius of curvature: 7.2 mm), and good stretchability (60% tensile strain). Moreover, they are suitable for low‐voltage operation (VDS = ?1.0 V, VGS = ?2.5 V). In addition, the electrical characteristics such as mobility, on‐current, and threshold voltage are maintained even in the concave and convex bending state (bending tensile strain of ≈3.4%), respectively. Finally, free‐standing, fully stretchable, and semi‐transparent coplanar‐type all‐organic transistors can be fabricated by introducing a poly(3,4‐ethylenedioxythiophene):polystyrene sulfonic acid layer as source/drain and gate electrodes, thus achieving low‐voltage operation (VDS = ?1.5 V, VGS = ?2.5 V) and an even higher mobility of up to 17.8 cm2 V?1 s?1. Moreover, these devices withstand stretching up to 80% tensile strain.  相似文献   

7.
Metal–organic frameworks (MOFs) and MOF‐derived nanostructures are recently emerging as promising catalysts for electrocatalysis applications. Herein, 2D MOFs nanosheets decorated with Fe‐MOF nanoparticles are synthesized and evaluated as the catalysts for water oxidation catalysis in alkaline medium. A dramatic enhancement of the catalytic activity is demonstrated by introduction of electrochemically inert Fe‐MOF nanoparticles onto active 2D MOFs nanosheets. In the case of active Ni‐MOF nanosheets (Ni‐MOF@Fe‐MOF), the overpotential is 265 mV to reach a current density of 10 mA cm?2 in 1 m KOH, which is lowered by ≈100 mV after hybridization due to the 2D nanosheet morphology and the synergistic effect between Ni active centers and Fe species. Similar performance improvement is also successfully demonstrated in the active NiCo‐MOF nanosheets. More importantly, the real catalytic active species in the hybrid Ni‐MOF@Fe‐MOF catalyst are unraveled. It is found that, NiO nanograins (≈5 nm) are formed in situ during oxygen evolution reaction (OER) process and act as OER active centers as well as building blocks of the porous nanosheet catalysts. These findings provide new insights into understanding MOF‐based catalysts for water oxidation catalysis, and also shed light on designing highly efficient MOF‐derived nanostructures for electrocatalysis.  相似文献   

8.
2D materials are promising to overcome the scaling limit of Si field‐effect transistors (FETs). However, the insulator/2D channel interface severely degrades the performance of 2D FETs, and the origin of the degradation remains largely unexplored. Here, the full energy spectra of the interface state densities (Dit) are presented for both n‐ and p‐ MoS2 FETs, based on the comprehensive and systematic studies, i.e., full rage of channel thickness and various gate stack structures with h‐BN as well as high‐k oxides. For n‐MoS2, Dit around the mid‐gap is drastically reduced to 5 × 1011 cm?2 eV?1 for the heterostructure FET with h‐BN from 5 × 1012 cm?2 eV?1 for the high‐k top‐gate. On the other hand, Dit remains high, ≈ 1013 cm?2 eV?1, even for the heterostructure FET for p‐MoS2. The systematic study elucidates that the strain induced externally through the substrate surface roughness and high‐k deposition process is the origin for the interface degradation on conduction band side, while sulfur‐vacancy‐induced defect states dominate the interface degradation on valance band side. The present understanding of the interface properties provides the key to further improving the performance of 2D FETs.  相似文献   

9.
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   

10.
Planar integrated systems of micro‐supercapacitors (MSCs) and sensors are of profound importance for 3C electronics, but usually appear poor in compatibility due to the complex connections of device units with multiple mono‐functional materials. Herein, 2D hierarchical ordered dual‐mesoporous polypyrrole/graphene (DM‐PG) nanosheets are developed as bi‐functional active materials for a novel prototype planar integrated system of MSC and NH3 sensor. Owing to effective coupling of conductive graphene and high‐sensitive pseudocapacitive polypyrrole, well‐defined dual‐mesopores of ≈7 and ≈18 nm, hierarchical mesoporous network, and large surface area of 112 m2 g?1, the resultant DM‐PG nanosheets exhibit extraordinary sensing response to NH3 as low as 200 ppb, exceptional selectivity toward NH3 that is much higher than other volatile organic compounds, and outstanding capacitance of 376 F g?1 at 1 mV s?1 for supercapacitors, simultaneously surpassing single‐mesoporous and non‐mesoporous counterparts. Importantly, the bi‐functional DM‐PG‐based MSC‐sensor integrated system represents rapid and stable response exposed to 10–40 ppm of NH3 after only charging for 100 s, remarkable sensitivity of NH3 detection that is close to DM‐PG‐based MSC‐free sensor, impressive flexibility with ≈82% of initial response value even at 180°, and enhanced overall compatibility, thereby holding great promise for ultrathin, miniaturized, body‐attachable, and portable detection of NH3.  相似文献   

11.
This paper describes a simple, vapor‐phase route for the synthesis of metastable α‐phase copper‐phthalocyanine (CuPc) single‐crystal nanowires through control of the growth temperature. The influence of the growth temperature on the crystal structures, morphology, and size of the CuPc nanostructures is explored using X‐ray diffraction (XRD), optical absorption, and transmission electron microscopy (TEM). α‐CuPc nanowires are successfully incorporated as active semiconductors in field‐effect transistors (FETs). Single nanowire devices exhibit carrier mobilities and current on/off ratios as high as 0.4 cm2 V?1 s?1 and >104, respectively.  相似文献   

12.
Since transition metal dichalcogenide (TMD) semiconductors are found as 2D van der Waals materials with a discrete energy bandgap, many 2D‐like thin field effect transistors (FETs) and PN diodes are reported as prototype electrical and optoelectronic devices. As a potential application of display electronics, transparent 2D FET devices are also reported recently. Such transparent 2D FETs are very few in report, yet no p‐type channel 2D‐like FETs are seen. Here, 2D‐like thin transparent p‐channel MoTe2 FETs with oxygen (O2) plasma‐induced MoOx/Pt/indium‐tin‐oxide (ITO) contact are reported for the first time. For source/drain contact, 60 s short O2 plasma and ultrathin Pt‐deposition processes on MoTe2 surface are sequentially introduced before ITO thin film deposition and patterning. As a result, almost transparent 2D FETs are obtained with a decent mobility of ≈5 cm2 V?1 s?1, a high ON/OFF current ratio of ≈105, and 70% transmittance. In particular, for normal MoTe2 FETs without ITO, O2 plasma process greatly improves the hole injection efficiency and device mobility (≈60 cm2 V?1 s?1), introducing ultrathin MoOx between Pt source/drain and MoTe2. As a final device application, a photovoltaic current modulator, where the transparent FET stably operates as gated by photovoltaic effects, is integrated.  相似文献   

13.
Hybrid metal–organic frameworks (MOFs) demonstrate great promise as ideal electrode materials for energy‐related applications. Herein, a well‐organized interleaved composite of graphene‐like nanosheets embedded with MnO2 nanoparticles (MnO2@C‐NS) using a manganese‐based MOF and employed as a promising anode material for Li‐ion hybrid capacitor (LIHC) is engineered. This unique hybrid architecture shows intriguing electrochemical properties including high reversible specific capacity 1054 mAh g?1 (close to the theoretical capacity of MnO2, 1232 mAh g?1) at 0.1 A g?1 with remarkable rate capability and cyclic stability (90% over 1000 cycles). Such a remarkable performance may be assigned to the hierarchical porous ultrathin carbon nanosheets and tightly attached MnO2 nanoparticles, which provide structural stability and low contact resistance during repetitive lithiation/delithiation processes. Moreover, a novel LIHC is assembled using a MnO2@C‐NS anode and MOF derived ultrathin nanoporous carbon nanosheets (derived from other potassium‐based MOFs) cathode materials. The LIHC full‐cell delivers an ultrahigh specific energy of 166 Wh kg?1 at 550 W kg?1 and maintained to 49.2 Wh kg?1 even at high specific power of 3.5 kW kg?1 as well as long cycling stability (91% over 5000 cycles). This work opens new opportunities for designing advanced MOF derived electrodes for next‐generation energy storage devices.  相似文献   

14.
Metal–organic frameworks (MOFs) and relative structures with uniform micro/mesoporous structures have shown important applications in various fields. This paper reports the synthesis of unprecedented mesoporous NixCo3?xO4 nanorods with tuned composition from the Co/Ni bimetallic MOF precursor. The Co/Ni‐MOFs are prepared by a one‐step facile microwave‐assisted solvothermal method rather than surface metallic cation exchange on the preformed one‐metal MOF template, therefore displaying very uniform distribution of two species and high structural integrity. The obtained mesoporous Ni0.3Co2.7O4 nanorod delivers a larger‐than‐theoretical reversible capacity of 1410 mAh g?1 after 200 repetitive cycles at a small current of 100 mA g?1 with an excellent high‐rate capability for lithium‐ion batteries. Large reversible capacities of 812 and 656 mAh g?1 can also be retained after 500 cycles at large currents of 2 and 5 A g?1, respectively. These outstanding electrochemical performances of the ternary metal oxide have been mainly attributed to its interconnected nanoparticle‐integrated mesoporous nanorod structure and the synergistic effect of two active metal oxide components.  相似文献   

15.
Metal‐organic gels (MOGs) appear as a blooming alternative to well‐known metal‐organic frameworks (MOFs). Porosity of MOGs has a microstructural origin and not strictly crystalline like in MOFs; therefore, gelation may provide porosity to any metal‐organic system, including those with interesting properties but without a porous crystalline structure. The easy and straightforward shaping of MOGs contrasts with the need of binders for MOFs. In this contribution, a series of MOGs based on the assembly of 1D‐coordination polymer nanofibers of formula [M(DTA)]n (MII: Ni, Cu, Pd; DTA: dithiooxamidato) are reported, in which properties such as porosity, chemical inertness, mechanical robustness, and stimuli‐responsive electrical conductivity are brought together. The strength of the M? S bond confers an unusual chemical resistance, withstanding exposure to acids, alkalis, and mild oxidizing/reducing chemicals. Supercritical drying of MOGs provides ultralight metal‐organic aerogels (MOAs) with densities as low as 0.03 g cm?3 and plastic/brittle behavior depending on the nanofiber aspect ratio. Conductivity measurements reveal a semiconducting behavior (10?12 to 10?7 S cm?1 at 298 K) that can be improved by doping (10?5 S cm?1). Moreover, it must be stressed that conductivity of MOAs reversibly increases (up to 10?5 S cm?1) under the presence of acetic acid.  相似文献   

16.
Solution‐processed, low cost thin films of layered semiconductors such as transition metal dichalcogenides (TMDs) are potential candidates for future printed electronics. Here, n‐type electrolyte‐gated transistors (EGTs) based on porous WS2 nanosheet networks as the semiconductor are demonstrated. The WS2 nanosheets are liquid phase exfoliated to form aqueous/surfactant stabilized inks, and deposited at low temperatures (T < 120 °C) in ambient atmosphere by airbrushing. No solvent exchange, further additives, or complicated processing steps are required. While the EGTs are primarily n‐type (electron accumulation), some hole transport is also observable. The EGTs show current modulations > 104 with low hysteresis, channel width‐normalized on‐conductances of up to 0.27 µS µm?1 and estimated electron mobilities around 0.01 cm2 V?1 s?1. In addition, the WS2 nanosheet networks exhibit relatively high volumetric capacitance values of 30 F cm?3. Charge transport within the network depends significantly on the applied lateral electric field and is thermally activated, which supports the notion that hopping between nanosheets is a major limiting factor for these networks and their future application.  相似文献   

17.
An integrated, free‐standing, and binder‐free type of flexible anode electrode is fabricated from numerous holey‐structured, 2D nickel‐based phosphide nanosheets connected with carbon nanotubes. This electrode architecture can not only uniformly disperse the nanosheets throughout the whole electrode to avoid aggregation or detachment, but also provide an ideal sodium ion and electrolyte diffusion and penetration network with high electronic conductivity. Meanwhile, bimetallic phosphide formation by introducing secondary metal species will lead to a synergistic effect to modify the electrochemical properties. Due to the excellent compositional and structural characteristics of this electrode, it delivers superior performance. This designed flexible anode with Ni1.5Co0.5Px nanosheets demonstrates a reversible capacity of 496.4 mAh g?1 at 0.5 C and a good rate capacity of 276.1 mAh g?1 at 8 C. Meanwhile, this connected integrated network woven from carbon nanotubes can effectively restrain volumetric expansion and shrinkage, and affect the conversion reaction products formation as well, from large‐sized microspheres to film structure, which is primarily credited with the improvement in electrochemical performance. This work may open up a new path for the synthesis of morphology‐controlled phosphides and promote the further development of flexible devices.  相似文献   

18.
As one of the emerging new transition‐metal dichalcogenides materials, molybdenum ditelluride (α‐MoTe2) is attracting much attention due to its optical and electrical properties. This study fabricates all‐2D MoTe2‐based field effect transistors (FETs) on glass, using thin hexagonal boron nitride and thin graphene in consideration of good dielectric/channel interface and source/drain contacts, respectively. Distinguished from previous works, in this study, all 2D FETs with α‐MoTe2 nanoflakes are dual‐gated for driving higher current. Moreover, for the present 2D dual gate FET fabrications on glass, all thermal annealing and lithography processes are intentionally exempted for fully non‐lithographic method using only van der Waal's forces. The dual‐gate MoTe2 FET displays quite a high hole and electron mobility over ≈20 cm2 V?1 s?1 along with ON/OFF ratio of ≈105 in maximum as an ambipolar FET and also demonstrates high drain current of a few tens‐to‐hundred μA at a low operation voltage. It appears promising enough to drive organic light emitting diode pixels and NOR logic functions on glass.  相似文献   

19.
In this paper a simple, casting solution technique for the preparation of two‐dimensional (2D) arrays of very‐high molecular weight (MW) 1D‐Pc supramolecular inorganic polymers is described. The soluble fluoroaluminium tetra‐tert‐butylphthalocyanine (ttbPcAlF) is synthesized and characterized, which can be self‐assembled to form 2D arrays of very‐high‐MW 1D‐Pc supramolecular inorganic polymers. High‐resolution transmission electron microscopy (HRTEM) demonstrates that the 1D‐ttbPcAlF, having a cofacial ring spacing of ~0.36 nm and an interchain distance of ~1.7 nm, self‐assembles into 2D‐nanosheets (~140 nm in length, ~20 nm in width, and equivalent to MW of 3.2 × 105 g mol?1). The film cast from a 1,2‐dichloroethane (DCE) solution shows a minimum hole‐mobility of ~0.3 cm2 V?1 s?1 at room temperature by flash‐photolysis time‐resolved microwave conductivity (TRMC) measurements and a fairly high dark dc‐conductivity of ~1 × 10?3 S cm?1.  相似文献   

20.
Developing nanostructured Ni and Co oxides with a small overpotential and fast kinetics of the oxygen evolution reaction (OER) have drawn considerable attention recently because their theoretically high efficiency, high abundance, low cost, and environmental benignity in comparison with precious metal oxides, such as RuO2 and IrO2. However, how to increase the specific activity area and improve their poor intrinsic conductivity is still challenging, which significantly limits the overall OER rate and largely prevent their utilization. Thus, developing effective OER electrocatalysts with abundant active sites and high electrical conductivity still remains urgent. In this work, a scrupulous design of OER electrode with a unique sandwich‐like coaxial structure of the three‐dimensional Ni@[Ni(2+/3+)Co2(OH)6–7]x nanotube arrays (3D NNCNTAs) is reported. A Ni nanotube array with open end is homogeneous coated with Ni and Co co‐hydroxide nanosheets ([Ni(2+/3+)Co2(OH)6–7]x) and is employed as multifunctional interlayer to provide a large surface area and fast electron transport and support the outermost [Ni(2+/3+)Co2(OH)6–7]x layer. The remarkable features of high surface area, enhanced electron transport, and synergistic effects have greatly assured excellent OER activity with a small overpotential of 0.46 V at the current density of 10 mA cm?2 and high stability.  相似文献   

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