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1.
The implementation of graphene layers in gallium nitride (GaN) heterostructure growth can solve self‐heating problems in nitride‐based high‐power electronic and light‐emitting optoelectronic devices. In the present study, high‐quality GaN layers are grown on patterned graphene layers and 6H–SiC by metalorganic chemical vapor deposition. A periodic pattern of graphene layers is fabricated on 6H–SiC by using polymethyl methacrylate deposition and electron beam lithography, followed by etching using an Ar/O2 gas atmosphere. Prior to GaN growth, an AlN buffer layer and an Al0.2Ga0.8N transition layer are deposited. The atomic structures of the interfaces between the 6H–SiC and graphene, as well as between the graphene and AlN, are studied using scanning transmission electron microscopy. Phase separation of the Al0.2Ga0.8N transition layer into an AlN and GaN superlattice is observed. Above the continuous graphene layers, polycrystalline defective GaN is rapidly overgrown by better quality single‐crystalline GaN from the etched regions. The lateral overgrowth of GaN results in the presence of a low density of dislocations (≈109 cm−2) and inversion domains and the formation of a smooth GaN surface.  相似文献   

2.
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   

3.
An experimental study on the interaction between the top and bottom layer of a chemically functionalized graphene bilayer by mild oxygen plasma is reported. Structural, chemical, and electrical properties are monitored using Raman spectroscopy, transport measurements, conductive atomic force microscopy and X‐ray photoelectron spectroscopy. Single‐ and double‐sided chemical functionalization are found to give very different results: single‐sided modified bilayers show relatively high mobility (200–600 cm2 V?1 s?1 at room temperature) and a stable structure with a limited amount of defects, even after long plasma treatment (>60 s). This is attributed to preferential modification and limited coverage of the top layer during plasma exposure, while the bottom layer remains almost unperturbed. This could eventually lead to decoupling between top and bottom layers. Double‐sided chemical functionalization leads to a structure containing a high concentration of defects, very similar to graphene oxide. This opens the possibility to use plasma treatment not only for etching and patterning of graphene, but also to make heterostructures (through single‐sided modification of bilayers) for sensors and transistors and new graphene‐derivatives materials (through double‐sided modification).  相似文献   

4.
A porous, yet compact, RuO2/graphene hybrid is successfully prepared by using a disassembly–reassembly strategy, achieving effective and uniform loading of RuO2 nanoparticles inside compact graphene monolith. The disassembly process ensures the uniform loading of RuO2 nanoparticles into graphene monolith, while the reassembly process guarantees a high density yet simultaneously unimpeded ion transport channel in the composite. The resulting RuO2/graphene hybrid possesses a density of 2.63 g cm−3, leading to a record high volumetric capacitance of 1485 F cm−3 at the current density of 0.1 A g−1. When the current density is increased to 20 A g−1, it remains a high volumetric capacitance of 1188 F cm−3. More importantly, when the single electrode mass loading is increased to 12 mg cm−2, it still delivers a high volumetric capacitance of 1415 F cm−3 at the current density of 0.1 A g−1, demonstrating the promise of this disassembly–reassembly approach to create high volumetric performance materials for energy storage applications.  相似文献   

5.
Graphene‐oxide (GO) based porous structures are highly desirable for supercapacitors, as the charge storage and transfer can be enhanced by advancement in the synthesis. An effective route is presented of, first, synthesis of three‐dimensional (3D) assembly of GO sheets in a spherical architecture (GOS) by flash‐freezing of GO dispersion, and then development of hierarchical porous graphene (HPG) networks by facile thermal‐shock reduction of GOS. This leads to a superior gravimetric specific capacitance of ≈306 F g−1 at 1.0 A g−1, with a capacitance retention of 93% after 10 000 cycles. The values represent a significant capacitance enhancement by 30–50% compared with the GO powder equivalent, and are among the highest reported for GO‐based structures from different chemical reduction routes. Furthermore, a solid‐state flexible supercapacitor is fabricated by constructing the HPG with polymer gel electrolyte, exhibiting an excellent areal specific capacitance of ≈220 mF cm−2 at 1.0 mA cm−2 with exceptional cyclic stability. The work reveals a facile but efficient synthesis approach of GO‐based materials to enhance the capacitive energy storage.  相似文献   

6.
The use of conductive frameworks as the host scaffold to obtain nanostructured sulfur cathodes is an efficient way to increase the sulfur utilization for redox reaction in Li‐S batteries with large discharge capacity and high energy density. However, due to dynamical interfaces driven by phase evolution between the conductive hosts and S‐containing guests during cycling, the cathode still faces poor stability. Herein, the use of O‐/N‐containing nanocarbon as the conductive host sheds a light on the role of the dynamic interface between the carbon host and S‐containing guest for a stable Li‐S cell. The outstanding reversibility and stability of N‐doped C/S cathodes are attributed to the favorable guest‐host interaction at the electron‐modified interface, manifesting as (i) a chemical gradient to adsorb polar polysulfides and (ii) ameliorative deposition and recharging of Li2S on the region of electron‐rich pyridinic N and a graphene domain surrounding quaternary N. Highly reversible, efficient and stable Li storage properties such as mitigated polarization and charge barrier, high capacity of 1370 and 964 mAh g−1 at 0.1 and 1.0 C, respectively, and 70% of capacity retention after 200 cycles are achieved. Mechanistic insight into the capacity fading inspires the rational design on electrodes for high‐performance electrochemical systems.  相似文献   

7.
2D transition metal dichalcogenides (TMDCs) have emerged as promising candidates for post‐silicon nanoelectronics owing to their unique and outstanding semiconducting properties. However, contact engineering for these materials to create high‐performance devices while adapting for large‐area fabrication is still in its nascent stages. In this study, graphene/Ag contacts are introduced into MoS2 devices, for which a graphene film synthesized by chemical vapor deposition (CVD) is inserted between a CVD‐grown MoS2 film and a Ag electrode as an interfacial layer. The MoS2 field‐effect transistors with graphene/Ag contacts show improved electrical and photoelectrical properties, achieving a field‐effect mobility of 35 cm2 V?1 s?1, an on/off current ratio of 4 × 108, and a photoresponsivity of 2160 A W?1, compared to those of devices with conventional Ti/Au contacts. These improvements are attributed to the low work function of Ag and the tunability of graphene Fermi level; the n‐doping of Ag in graphene decreases its Fermi level, thereby reducing the Schottky barrier height and contact resistance between the MoS2 and electrodes. This demonstration of contact interface engineering with CVD‐grown MoS2 and graphene is a key step toward the practical application of atomically thin TMDC‐based devices with low‐resistance contacts for high‐performance large‐area electronics and optoelectronics.  相似文献   

8.
Molybdenum phosphide (MoP) is a promising non‐noble‐metal electrocatalyst in the hydrogen evolution reaction (HER), but practical implementation is impeded by the sluggish HER kinetics and poor chemical stability. Herein, a novel high‐efficiency HER electrocatalyst comprising MoP nanoflakes intercalated nitrogen‐doped graphene nanobelts (MoP/NG), which are synthesized by one‐step thermal phosphiding organic–inorganic hybrid dodecylamine (DDA) inserted MoO3 nanobelts, is reported. The intercalated DDA molecules are in situ carbonized into the NG layer and the sandwiched MoO3 layer is converted into MoP nanoflakes which are intercalated between the NG layers forming the alternatingly stacked MoP/NG hybrid nanobelts. The MoP nanoflakes provide abundant edge sites and the sandwiched MoP/NG hybrid enables rapid ion/electron transport thus yielding excellent electrochemical activity and stability for HER. The MoP/NG shows a low overpotential of 94 mV at 10 mA cm−2, small Tafel slope of 50.1 mV dec−1, and excellent electrochemical stability with 99.5% retention for over 22 h.  相似文献   

9.
The influence of polymer modifier chain length on the thermal conductivity of polyamide 6/graphene (GA) nanocomposites, including through-plane (λz) and in-plane (λx) directions were investigated. Here, three chain lengths of double amino-terminated polyethylene glycol (NH2–PEG–NH2) were used to covalently functionalize graphene with graphene content of 5.0 wt%. Results showed that λz was enhanced with the chain length of NH2–PEG–NH2 increased, but λx reached a maximum value at a certain chain length of NH2–PEG–NH2. The maximum λz and λx of GA are 0.406 W m−1 K−1 and 9.710 W m−1 K−1, respectively. This study serves as a foundation for further research on the thermal conductive property of graphene nanocomposites using different chain lengths of polymer modifier to improve the λz and λx of the thermal conductive materials.  相似文献   

10.
The emergence of memristive behavior in amorphous–crystalline 2D oxide heterostructures, which are synthesized by atomic layer deposition (ALD) of a few-nanometer amorphous Al2O3 layers onto atomically thin single-crystalline ZnO nanosheets, is demonstrated. The conduction mechanism is identified based on classic oxygen vacancy conductive channels. ZnO nanosheets provide a 2D host for oxygen vacancies, while the amorphous Al2O3 facilitates the generation and stabilization of the oxygen vacancies. The conduction mechanism in the high-resistance state follows Poole–Frenkel emission, and in the the low-resistance state is fitted by the Mott–Gurney law. From the slope of the fitting curve, the mobility in the low-resistance state is estimated to be ≈2400 cm2 V−1 s−1, which is the highest value reported in semiconductor oxides. When annealed at high temperature to eliminate oxygen vacancies, Al is doped into the ZnO nanosheet, and the memristive behavior disappears, further confirming the oxygen vacancies as being responsible for the memristive behavior. The 2D heterointerface offers opportunities for new design of high-performance memristor devices.  相似文献   

11.
Fiber‐shaped supercapacitors with improved specific capacitance and high rate capability are a promising candidate as power supply for smart textiles. However, the synergistic interaction between conductive filaments and active nanomaterials remains a crucial challenge, especially when hydrothermal or electrochemical deposition is used to produce a core (fiber)–shell (active materials) fibrous structure. On the other hand, although 2D pseudocapacitive materials, e.g., Ti3C2T x (MXene), have demonstrated high volumetric capacitance, high electrical conductivity, and hydrophilic characteristics, MXene‐based electrodes normally suffer from poor rate capability owing to the sheet restacking especially when the loading level is high and solid‐state gel is used as electrolyte. Herein, by hosting MXene nanosheets (Ti3C2T x ) in the corridor of a scrolled carbon nanotube (CNT) scaffold, a MXene/CNT fiber with helical structure is successfully fabricated. These features offer open spaces for rapid ion diffusion and guarantee fast electron transport. The solid‐state supercapacitor based on such hybrid fibers with gel electrolyte coating exhibits a volumetric capacitance of 22.7 F cm−3 at 0.1 A cm−3 with capacitance retention of 84% at current density of 1.0 A cm−3 (19.1 F cm−3), improved volumetric energy density of 2.55 mWh cm−3 at the power density of 45.9 mW cm−3, and excellent mechanical robustness.  相似文献   

12.
Al2O3 and AlPxOy dielectric layers have been deposited on n-type InP substrates and the electrical properties of the interfaces have been evaluated by current-voltage and capacitance-voltage (C-V) measurements on metal- insulator-semiconductor diodes. Layers were deposited by combining trimethyl- aluminum, oxygen and phosphine in a low pressure chemical vapor deposition reactor in which the oxygen was excited in an r.f. plasma prior to mixing with the reactive gases in the deposition zone. The Al2O3 layers were invariably too conductive for meaningful C-V measurements; however, the AlPxOy layers not only were of high resistivity (? > 1016 Ω cm) but also exhibited interfacial properties superior to those of SiO2 layers on InP. The surface potential could be modulated over the full band gap of InP since the surface density was less than 1011 cm-2 eV-1 over much of the band gap.  相似文献   

13.
Recent studies have found that the existence of oxygen around the active sites may be essential for efficient electrochemical CO2-to-CO conversion. Hence, this work proposes the modulation of oxygen coordination and investigates the as-induced catalytic behavior in CO2RR. It designs and synthesizes conjugated phthalocyanine frameworks catalysts (CPF-Co) with abundant CoN4 centers as an active source, and subsequently modifies the electronic structure of CPF-Co by introducing graphene oxide (GO) with oxygen-rich functional groups. A systematic study reveals that the axial coordination between oxygen and the catalytic sites could form an optimized O-CoN4 structure to break the electron distribution symmetry of Co, thus reducing the energy barrier to the activation of CO2 to COOH*. Meanwhile, by adjusting the content of oxygen, the proper supports can also facilitate the charge transfer efficiency between the matrix layer and the catalytic sites. The optimized CPF-Co@LGO exhibits a high TOF value (2.81 s−1), CO selectivity (97.6%) as well as stability (24 h) at 21 mA cm−2 current density. This work reveals the modulation of oxygen during CO2RR and provides a novel strategy for the design of efficient electrocatalysts, which may inspire new exploration and principles for CO2RR.  相似文献   

14.
Sodium‐ion batteries (SIBs) have gained tremendous interest for grid scale energy storage system and power energy batteries. However, the current researches of anode for SIBs still face the critical issues of low areal capacity, limited cycle life, and low initial coulombic efficiency for practical application perspective. To solve this issue, a kind of hierarchical 3D carbon‐networks/Fe7S8/graphene (CFG) is designed and synthesized as freestanding anode, which is constructed with Fe7S8 microparticles well‐welded on 3D‐crosslinked carbon‐networks and embedded in highly conductive graphene film, via a facile and scalable synthetic method. The as‐prepared freestanding electrode CFG represents high areal capacity (2.12 mAh cm?2 at 0.25 mA cm?2) and excellent cycle stability of 5000 cycles (0.0095% capacity decay per cycle). The assembled all‐flexible sodium‐ion battery delivers remarkable performance (high areal capacity of 1.42 mAh cm?2 at 0.3 mA cm?2 and superior energy density of 144 Wh kg?1), which are very close to the requirement of practical application. This work not only enlightens the material design and electrode engineering, but also provides a new kind of freestanding high energy density anode with great potential application prospective for SIBs.  相似文献   

15.
A Cu‐supported, graphene nanoplatelet (GNP) electrodes are reported a as high performance anode in lithium ion battery. The electrode precursor is an easy‐to‐handle aqueous ink cast on cupper foil and following dried in air. The scanning electron microscopy evidences homogeneous, micrometric flakes‐like morphology. Electrochemical tests in conventional electrolyte reveal a capacity of about 450 mAh g−1 over 300 cycles, delivered at a current rate as high as 740 mA g−1. The graphene‐based electrode is characterized using a N‐butyl‐N‐methyl‐pyrrolidiniumbis (trifluoromethanesulfonyl) imide, lithium‐bis(trifluoromethanesulfonyl)imide (Py1,4TFSI–LiTFSI) ionic liquid‐based solution added by ethylene carbonate (EC): dimethyl carbonate (DMC). The Li‐electrolyte interface is investigated by galvanostatic and potentiostatic techniques as well as by electrochemical impedance spectroscopy, in order to allow the use of the graphene‐nanoplatelets as anode in advanced lithium‐ion battery. Indeed, the electrode is coupled with a LiFePO4 cathode in a battery having a relevant safety content, due to the ionic liquid‐based electrolyte that is characterized by an ionic conductivity of the order of 10−2 S cm−1, a transference number of 0.38 and a high electrochemical stability. The lithium ion battery delivers a capacity of the order of 150 mAh g−1 with an efficiency approaching 100%, thus suggesting the suitability of GNPs anode for application in advanced configuration energy storage systems.  相似文献   

16.
Iron corrosion causes a great damage to the economy due to the function attenuation of iron‐based devices. However, the corrosion products can be used as active materials for some electrocatalytic reactions, such as oxygen evolution reaction (OER). Herein, the oxygen corrosion on Fe foams (FF) to synthesize effective self‐supporting electrocatalysts for OER, leading to “turning waste into treasure,” is regulated. A dual chloride aqueous system of “NaCl‐NiCl2” is employed to tailor the structures and OER properties of corrosion layers. The corrosion behaviors identify that Cl? anions serve as accelerators for oxygen corrosion, while Ni2+ cations guarantee the uniform growth of corrosion layers owing to the appeared chemical plating. The synergistic effect of “NaCl‐NiCl2” generates one of the highest OER activities that only an overpotential of 212 mV is required to achieve 100 mA cm?2 in 1.0 m KOH solution. The as‐prepared catalyst also exhibits excellent durability over 168 h (one week) at 100 mA cm?2 and promising application for overall water splitting. Specially, a large self‐supporting electrode (9 × 10 cm2) is successfully synthesized via this cost‐effective and easily scale‐up approach. By combining with corrosion science, this work provides a significant stepping stone in exploring high‐performance OER electrocatalysts.  相似文献   

17.
Topological insulators have spurred worldwide interest, but their advantageous properties have scarcely been explored in terms of electrochemical energy storage, and their high-rate capability and long-term cycling stability still remain a significant challenge to harvest. p-Type topological insulator SnSb2Te4 nanodots anchoring on few-layered graphene (SnSb2Te4/G) are synthesized as a stable anode for high-rate lithium-ion batteries and potassium-ion batteries through a ball-milling method. These SnSb2Te4/G composite electrodes show ultralong cycle lifespan (478 mAh g−1 at 1 A g−1 after 1000 cycles) and excellent rate capability (remaining 373 mAh g−1 even at 10 A g−1) in Li-ion storage owing to the rapid ion transport accelerated by the PN heterojunction, virtual electron highways provided by the conductive topological surface state, and extraordinary pseudocapacitive contribution, whose excellent phase reversibility is confirmed by synchrotron in situ X-ray powder diffraction. Surprisingly, durable lifespan even at practical levels of mass loading (>10 mg cm−2) for Li-ion storage and excellent K-ion storage performance are also observed. This work provides new insights for designing high-rate electrode materials by boosting conductive topological surfaces, atomic doping, and the interface interaction.  相似文献   

18.
The reversible formation of chemical bonds has potential for tuning multi‐electron redox reactions in emerging energy‐storage applications, such as lithium?sulfur batteries. The dissolution of polysulfide intermediates, however, results in severe shuttle effect and sluggish electrochemical kinetics. In this study, quinonoid imine is proposed to anchor polysulfides and to facilitate the formation of Li2S2/Li2S through the reversible chemical transition between protonated state (? NH+ ?) and deprotonated state (? N?). When serving as the sulfur host, the quinonoid imine‐doped graphene affords a very tiny shuttle current of 2.60 × 10?4 mA cm?2, a rapid redox reaction of polysulfide, and therefore improved sulfur utilization and enhanced rate performance. A high areal specific capacity of 3.72 mAh cm?2 is achieved at 5.50 mA cm?2 on the quinonoid imine‐doped graphene based electrode with a high sulfur loading of 3.3 mg cm?2. This strategy sheds a new light on the organic redox mediators for reversible modulation of electrochemical reactions.  相似文献   

19.
Synergistic improvements in the electrical conductivity and catalytic activity for the oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) are of paramount importance for rechargeable metal–air batteries. In this study, one‐nanometer‐scale ultrathin cobalt oxide (CoOx) layers are fabricated on a conducting substrate (i.e., a metallic Co/N‐doped graphene substrate) to achieve superior bifunctional activity in both the ORR and OER and ultrahigh output power for flexible Zn–air batteries. Specifically, at the atomic scale, the ultrathin CoOx layers effectively accelerate electron conduction and provide abundant active sites. X‐ray absorption spectroscopy reveals that the metallic Co/N‐doped graphene substrate contributes to electron transfer toward the ultrathin CoOx layer, which is beneficial for the electrocatalytic process. The as‐obtained electrocatalyst exhibits ultrahigh electrochemical activity with a positive half‐wave potential of 0.896 V for ORR and a low overpotential of 370 mV at 10 mA cm?2 for OER. The flexible Zn–air battery built with this catalyst exhibits an ultrahigh specific power of 300 W gcat ?1, which is essential for portable devices. This work provides a new design pathway for electrocatalysts for high‐performance rechargeable metal–air battery systems.  相似文献   

20.
《Advanced Powder Technology》2020,31(11):4541-4551
In this study we synthesized LiFePO4/carbon/reduced graphene oxide (LFP/C/rGO) composite cathode materials using a method involving sol–gel processing, spray-drying, and calcination. To improve the electrochemical performance of LFP/C, we tested graphene oxides (GOs) of various morphologies as conductive additives, including pristine GO, three-dimensional GO, and hydrothermal porous GO (HTGO). Among our samples, the cathode material prepared through spray-drying with the addition of 1 wt% of HTGO (denoted SP-LFP/C/1%rHTGO) displayed the best electrochemical performance; its discharge capacities at 0.1C, 1C, 5C, and 10C were 160.5, 151.8, 138.8, and 130.3 mA h g−1, respectively. From measurements of its long-term cycling performance, the discharge capacity in the first cycle and the capacity retention after 30 cycles at 0.1C were 160.2 mA h g−1 and 99.6%, respectively; at 10C, these values were 132.2 mA h g−1 and 91.8%, respectively. The electronic conductivity of SP-LFP/C/1%rHTGO (6.58 × 10−5 S cm−1) was higher than that of the pristine LFP/C (9.24 × 10−6 S cm−1). The Li+ ion diffusivities (DLi+) of the SP-LFP/C/1%HTGO cathode, measured using AC impedance (3.91 × 10−13 cm2 s−1) and cyclic voltammetry (6.66 × 10−10 cm2 s−1 for discharge), were superior to those of the LFP/C cathode (9.31 × 10−15 cm2 s−1 and 1.79 × 10−10 cm2 s−1 for discharge, respectively). Galvanostatic intermittent titration revealed that the value of DLi+ was located in a reasonable range from 1 × 10−10 to 1 × 10−17 cm2 s−1; its value dropped to its lowest point when the state of charge was close to 50%. Thus, the use of spray-drying and the addition of conductive HTGO (having a 3D wrinkled morphology and interconnected pore structure) can enhance the electronic conductivity and Li+ ion diffusivity of LFP/C cathode materials, thereby improving the electrochemical performance significantly.  相似文献   

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