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1.
The excellent electronic and electrochemical properties make 2D MXenes suitable candidates for sensors, batteries, and supercapacitors. However, the metallic-like behavior of MXenes hinders their potential for optoelectronic devices such as photodetectors. In this study, the band gap of metalloid Ti3C2Tx MXene is successfully opened to 1.53 eV with phenylsulfonic acid groups and realized a transistor and high-performance near-infrared photodetector array for a flexible vision sensory-neuromorphic system. The phenylsulfonic acid groups modified Ti3C2Tx MXene (S-Ti3C2Tx)-based flexible photodetector has a maximum responsivity of 8.50×102 A W−1 and a detectivity of 3.69×1011 Jones under 1064 nm laser irradiation. Moreover, the fabricated flexible vision sensory-neuromorphic system for image recognition realizes a high recognition rate >0.99, leading to great potential in the field of biological visual simulation and biomimetic eye. Besides conventional devices with Au as the conductive electrodes, all Ti3C2Tx MXene-based devices are also fabricated with S-Ti3C2Tx as the photosensitive material and unmodified Ti3C2Tx as the conductive electrodes, exhibiting comparable optoelectronic performances.  相似文献   

2.
The freestanding MXene films are promising for compact energy storage ascribing to their high pseudocapacitance and density, yet the sluggish ion transport caused by the most densely packed structure severely hinders their rate capability. Here, a reassembly strategy for constructing freestanding and flexible MXene-based film electrodes with a tunable porous structure is proposed, where the Ti3C2Tx microgels disassembled from 3D structured hydrogel are reassembled together with individual Ti3C2Tx nanosheets in different mass ratios to form a densely packed 3D network in microscale and a film morphology in macroscale. The space utilization of produced film can be maximized by a good balance of the density and porosity, resulting in a high volumetric capacitance of 736 F cm−3 at an ultrahigh scan rate of 2000 mV s−1. The fabricated supercapacitor yields a superior energy density of 40 Wh L−1 at a power density of 0.83 kW L−1, and an energy density of 21 Wh L−1 can be still maintained even when the power density reaches 41.5 kW L−1, which are the highest values reported to date for symmetric supercapacitors in aqueous electrolytes. More promisingly, the reassembled films can be used as electrodes of flexible supercapacitors, showing excellent flexibility and integrability.  相似文献   

3.
The rational design of economic and high-performance electrocatalytic water-splitting systems is of great significance for energy and environmental sustainability. Developing a sustainable energy conversion-assisted electrocatalytic process provides a promising novel approach to effectively boost its performance. Herein, a self-sustained water-splitting system originated from the heterostructure of perovskite oxide with 2D Ti3C2Tx MXene on Ni foam (La1-xSrxCoO3/Ti3C2Tx MXene/Ni) that shows high activity for solar-powered water evaporation and simultaneous electrocatalytic water splitting is presented. The all-in-one interfacial electrocatalyst exhibits highly improved oxygen evolution reaction (OER) performance with a low overpotential of 279 mV at 10 mA cm−2 and a small Tafel slope of 74.3 mV dec−1, superior to previously reported perovskite oxide-based electrocatalysts. Density functional theory calculations reveal that the integration of La0.9Sr0.1CoO3 with Ti3C2Tx MXene can lower the energy barrier for the electron transfer and decrease the OER overpotential, while COMSOL simulations unveil that interfacial solar evaporation could induce OH enrichment near the catalyst surfaces and enhance the convection flow above the catalysts to remove the generated gas, remarkably accelerating the kinetics of electrocatalytic water splitting.  相似文献   

4.
Rechargeable magnesium batteries (RMBs) are promising next-generation low-cost and high-energy devices. Among all RMBs, anode-free magnesium metal batteries that use in situ magnesium-plated current collectors as negative electrodes can afford optimal energy densities. However, anode-free magnesium metal batteries have remained elusive so far, as their practical application is plagued by low Mg plating/stripping efficiency due to nonuniform Mg deposition on conventional anode current collectors. Herein, for the first time, an anode-free Mg-metal battery is developed by employing a 3D MXene (Ti3C2Tx) film with horizontal Mg electrodeposition. The magnesiophilic oxygen and reactive fluorine terminations in MXene enable an enriched local magnesium-ion concentration and a durable magnesium fluoride-rich solid electrolyte interphase on the Ti3C2Tx film surface. Meanwhile, Ti3C2Tx MXene exhibits a high lattice geometrical fit with Mg (≈96%) to guide the horizontal electrodeposition of Mg. Consequently, the developed Ti3C2Tx film achieves reversible Mg plating/stripping with high Coulombic efficiencies (>99.4%) at high-current-density (5.0 mA cm−2) and high-Mg-utilization (50%) conditions. When this Ti3C2Tx film is coupled with a pre-magnesized Mo6S8 cathode, the anode-free Mg-metal full-cell prototype exhibits a volumetric energy density five times higher than its standard Mg-metal counterpart. This work provides insights into the rational design of anode current collectors to guide horizontal Mg electrodeposition for anode-free Mg metal batteries.  相似文献   

5.
2D transition metal carbides and nitrides, namely MXenes, are normally synthesized in acidic solutions and are delaminated in basic solutions. This results in versatile materials with unique physical/chemical properties suitable for various practical applications. However, solution-based chemical treatments can affect the chemical structures of MXenes, which accelerates the oxidation reactions and degrades their intrinsic properties. Here, long-term stable Ti3C2Tx dispersion in deep eutectic solvents (DESs) that resisted oxidation degradation for up to 28 weeks is demonstrated. As an anti-oxidative dispersion medium, DESs helped prevent oxidation of Ti3C2Tx layers due to hydrogen bond accepting and donating molecules passivated surface of the Ti3C2Tx. In addition, DES molecules in bulk solution can also be hydrated in the presence of water, which stabilizes reactive oxygen by forming stable DES-water cluster. Therefore, the use of DESs enhanced the delamination of the Ti3C2Tx nanosheets, while preventing oxidation of the nanosheets in solution and even in their dried state. As a result, thick and thin films of Ti3C2Tx fabricated using DESs exhibited stable sheet resistance in comparison with pristine-Ti3C2Tx. In addition, Ti3C2Tx dispersed in DESs can be applied as electrodes for electrochemical capacitors, in which they showed higher chemical stability and better performance than pristine Ti3C2Tx.  相似文献   

6.
Flexible wearable strain sensors have received extensive attention in human–computer interaction, soft robotics, and human health monitoring. Despite significant efforts in developing stretchable electronic materials and structures, developing flexible strain sensors with stable interfaces and low hysteresis remains a challenge. Herein, Ti3C2Tx MXene/AgNWs/liquid metal strain sensors (MAL strain sensor) with self-healing function are developed by exploiting the strong interactions between Ti3C2Tx MXene/AgNWs/LM and the disulfide and hydrogen bonds inside the self-healing poly(dimethylsiloxane) elastomers. AgNWs lap the Ti3C2Tx MXene sheets, and the LM acts as a bridge to increase the lap between Ti3C2Tx MXene and AgNWs, thereby improving the interface interaction between them and reducing hysteresis. The MAL strain sensor can simultaneously achieve high sensitivity (gauge factor for up to 3.22), high linearity (R2 = 0.98157), a wide range of detection (e.g., 1%–300%), a fast response time (145 ms), excellent repeatability, and stability.In addition, the MAL strain sensor before and after self-healing is combined with a small fish and an electrothermally driven soft robot, respectively, allowing real-time monitoring of the swinging tail of the small fish and the crawling of the soft robot by resistance changes.  相似文献   

7.
The fast growth of portable smart electronics and internet of things have greatly stimulated the demand for miniaturized energy storage devices. Micro‐supercapacitors (MSCs), which can provide high power density and a long lifetime, are ideal stand‐alone power sources for smart microelectronics. However, relatively few MSCs exhibit both high areal and volumetric capacitance. Here rapid production of flexible MSCs is demonstrated through a scalable, low‐cost stamping strategy. Combining 3D‐printed stamps with arbitrary shapes and 2D titanium carbide or carbonitride inks (Ti3C2Tx and Ti3CNTx, respectively, known as MXenes), flexible all‐MXene MSCs with controlled architectures are produced. The interdigitated Ti3C2Tx MSC exhibits high areal capacitance: 61 mF cm?2 at 25 µA cm?2 and 50 mF cm?2 as the current density increases by 32 fold. The Ti3C2Tx MSCs also showcase capacitive charge storage properties, good cycling lifetime, high energy and power densities, etc. The production of such high‐performance Ti3C2Tx MSCs can be easily scaled up by designing pad or cylindrical stamps, followed by a cold rolling process. Collectively, the rapid, efficient production of flexible all‐MXene MSCs with state‐of‐the‐art performance opens new exciting opportunities for future applications in wearable and portable electronics.  相似文献   

8.
2D titanium carbide (Ti3C2Tx) MXene films, with their well-defined microstructures and chemical functionality, provide a macroscale use of nano-sized Ti3C2Tx flakes. Ti3C2Tx films have attractive physicochemical properties favorable for device design, such as high electrical conductivity (up to 20 000 S cm–1), impressive volumetric capacitance (1500 F cm–3), strong in-plane mechanical strength (up to 570 MPa), and a high degree of flexibility. Here, the appealing features of Ti3C2Tx-based films enabled by the layer-to-layer arrangement of nanosheets are reviewed. We devote attention to the key strategies for actualizing desirable characteristics in Ti3C2Tx-based functional films, such as high and tunable electrical conductivity, outstanding mechanical properties, enhanced oxidation-resistance and shelf life, hydrophilicity/hydrophobicity, adjustable porosity, and convenient processability. This review further discusses fundamental aspects and advances in the applications of Ti3C2Tx-based films with a focus on illuminating the relationship between the structural features and the resulting performances for target applications. Finally, the challenges and opportunities in terms of future research, development, and applications of Ti3C2Tx-based films are suggested. A comprehensive understanding of these competitive features and challenges shall provide guidelines and inspiration for the further development of Ti3C2Tx-based functional films, and contribute to the advances in MXene technology.  相似文献   

9.
Graphite anodes show great potential for potassium storage, however, their capacity fades quickly owing to substantial interlayer expansion/shrinkage (i.e., up to 60%) induced structural degradation. Here, Ti3C2Tx MXene nanosheets are used as a fast electron/potassium-ion dual-function conductor to construct the framework of all-integrated graphite nanoflake (GNF)/MXene (GNFM) electrodes. The continuous MXene framework constructs a 3D channel for fast electron/potassium-ion transfer and endows GNFM electrodes with a high structural stability. Owing to this unique MXene framework, GNFM electrodes exhibit much enhanced potassium storage performances than that of the conventional polymer-bonded electrodes even at high mass loadings. Moreover, GNFM electrodes also show impressive cyclability in non-flammable electrolytes and are further used as anodes to assemble novel non-flammable potassium-ion capacitors that show an excellent cyclability and high energy/power densities (113.1 Wh kg–1 and 12.2 kW kg–1). New insights into phase transition mechanism in GNFM electrodes are verified by operando XRD. Density functional theory calculations demonstrate that MXene can promote electron transfer and potassium diffusion in the heterointerface between GNF and MXene. Therefore, the results demonstrate that all-integrated GNFM electrodes designed with MXene as multifunctional frameworks provide a new paradigm for producing efficient potassium storage anodes.  相似文献   

10.
Since the discovery of Ti3C2Tx in 2011, the family of two‐dimensional transition metal carbides, carbonitrides, and nitrides (collectively known as MXenes) has quickly attracted the attention of those developing energy storage applications such as electrodes for supercapacitors with acidic aqueous electrolytes. The excellent performance of these MXenes is attributed to a pseudocapacitive energy storage mechanism, based on the non‐rectangular shape of cyclic voltammetry curves and changes in the titanium oxidation state detected by in situ X‐ray absorption spectroscopy. However, the pseudocapacitive mechanism is not well understood and no dimensional changes due to proton insertion have been reported. In this work, in situ X‐ray diffraction and density functional theory are used to investigate the charge storage mechanism of Ti3C2Tx in 1 m H2SO4. Results reveal that a 0.5 Å expansion and shrinkage of the c‐lattice parameter of Ti3C2Tx occur during cycling in a 0.9 V voltage window, showing that the charge storage mechanism is intercalation pseudocapacitance with implication for MXene use in energy storage and electrochemical actuators.  相似文献   

11.
MXenes are a large and rapidly expanding family of 2D materials that, owing to their unique optoelectronic properties and tunable surface termination, find a wide range of applications including energy storage and energy conversion. In this work, Ti3C2Tx MXene nanosheets are applied as a novel type of electron transport layer (ETL) in low‐temperature processed planar‐structured perovskite solar cells (PSCs). Interestingly, simple UV‐ozone treatment of the metallic Ti3C2Tx that increases the surface Ti? O bonds without any change in its bulk properties such as high electron mobility improves its suitability as an ETL. Improved electron transfer and suppressed recombination at the ETL/perovskite interface results in augmentation of the power conversion efficiency (PCE) from 5.00% in the case of Ti3C2Tx without UV‐ozone treatment to the champion PCE of 17.17%, achieved using the Ti3C2Tx film after 30 min of UV‐ozone treatment. As the first report on the use of pure MXene layer as an ETL in PSCs, this work shows the great potential of MXenes to be used in PSCs and displays their promise for applications in photovoltaic technology in general.  相似文献   

12.
High‐rate capability has become an important feature for energy storage devices, but it is often accompanied with a significant reduction in energy density. Therefore, developing an energy storage technology that combines high‐rate capability with high energy density is a great challenge for next‐generation electronic devices. Here, parallel circuitry is constructed at the nanoscale to lower the resistance for ion and electron transport that largely determines the rate performance. The parallel circuitry is constructed through intertwining continuous carbon nanotubes with an interpenetrating conductive assembly based on hierarchically layered MXene (Ti3C2Tx ) functionalized by KMnO4 (MnOx @Ti3C2Tx ). The assembly shows ultrafast rate capability, e.g., maintaining 50% capacity when the current density increases from 0.1 to 10 A g?1. Investigations of the kinetics and charge storage mechanisms confirm the efficiency of the designed parallel circuitry in improving rate capability by providing rapid pathways for ions and electrons, as well as dividing the current flow evenly into individual MnOx @Ti3C2Tx flakes in the assembly. The flexible MnOx @Ti3C2Tx based electrode endows zinc ion batteries with outstanding mechanical robustness and good power delivering performance. The paradigm presented here paves a new way for designing electrodes with high‐rate capability toward next‐generation energy storage technologies.  相似文献   

13.
Two-dimensional transition metal carbides and nitrides (MXenes) show tremendous potential for optoelectronic devices due to their excellent electronic properties. Here, a high-performance ultraviolet photodetector based on TiO2 nanorod arrays/Ti3C2Tx MXene van der Waals (vdW) Schottky junction by all-solution process technique is reported. The Ti3C2Tx MXene modulated by the Au electrode increases its work function from 4.41 to 5.14 eV to form a hole transport layer. Complemented by the dangling bond-free surface of Ti3C2Tx, the Fermi-level pinning effect is suppressed and the electric-field strength of the Schottky junction is enhanced, which promotes charge separation and transport. After applying a bias of −1.5 V, the photovoltaic effect is favorably reinforced, while the hole-trapping mechanism (between TiO2 and oxygen) and reverse pyroelectric effect are largely eliminated. As a result, the responsivity and specific detectivity of the device with FTO/TiO2 nanorod arrays/Ti3C2Tx/Au structure reach 1.95 × 105 mA W−1 and 4.3 × 1013 cm Hz1/2 W−1 (370 nm, 65 mW cm−2), respectively. This work provides an effective approach to enhance the performance of photodetectors by forming the vdW Schottky junction and choosing metal electrodes to modulate MXene as a suitable charge transport layer.  相似文献   

14.
MXenes exhibit excellent capacitance at high scan rates in sulfuric acid aqueous electrolytes, but the narrow potential window of aqueous electrolytes limits the energy density. Organic electrolytes and room-temperature ionic liquids (RTILs) can provide higher potential windows, leading to higher energy density. The large cation size of RTIL hinders its intercalation in-between the layers of MXene limiting the specific capacitance in comparison to aqueous electrolytes. In this work, different chain lengths alkylammonium (AA) cations are intercalated into Ti3C2Tx, producing variation of MXene interlayer spacings (d-spacing). AA-cation-intercalated Ti3C2Tx (AA-Ti3C2), exhibits higher specific capacitances, and cycling stabilities than pristine Ti3C2Tx in 1 m 1-ethly-3-methylimidazolium bis-(trifluoromethylsulfonyl)-imide (EMIMTFSI) in acetonitrile and neat EMIMTFSI RTIL electrolytes. Pre-intercalated MXene with an interlayer spacing of ≈2.2 nm, can deliver a large specific capacitance of 257 F g−1 (1428 mF cm−2 and 492 F cm−3) in neat EMIMTFSI electrolyte leading to high energy density. Quasi elastic neutron scattering and electrochemical impedance spectroscopy are used to study the dynamics of confined RTIL in pre-intercalated MXene. Molecular dynamics simulations suggest significant differences in the structures of RTIL ions and AA cations inside the Ti3C2Tx interlayer, providing insights into the differences in the observed electrochemical behavior.  相似文献   

15.
2D titanium carbide (Ti3C2Tx MXene) has potential application in flexible/transparent conductors because of its metallic conductivity and solution processability. However, solution‐processed Ti3C2Tx films suffer from poor hydration stability and mechanical performance that stem from the presence of intercalants, which are unavoidably introduced during the preparation of Ti3C2Tx suspension. A proton acid colloidal processing approach is developed to remove the extrinsic intercalants in Ti3C2Tx film materials, producing pristine Ti3C2Tx films with significantly enhanced conductivity, mechanical strength, and environmental stability. Typically, pristine Ti3C2Tx films show more than twofold higher conductivity (10 400 S cm?1 vs 4620 S cm?1) and up to 11‐ and 32‐times higher strength and strain energy at failure (112 MPa, 1,480 kJ m?3, vs 10 MPa, 45 kJ m?3) than films prepared without proton acid processing. Simultaneously, the conductivity and mechanical integrity of pristine films are also largely retained during the long‐term storage in H2O/O2 environment. The improvement in mechanical performance and conductivity is originated from the intrinsic strong interaction between Ti3C2Tx layers, and the absence of extrinsic intercalants makes pristine Ti3C2Tx films stable in humidity by blocking the intercalation of H2O/O2. This method makes the material more competitive for real‐world applications such as electromagnetic interference shielding.  相似文献   

16.
2D 1T phase MoS2 (1T-MoS2) nanosheet with metallic conductivity and expanded interlayer spacing is considered as a highly potential lithium storage electrode material but remains thermodynamic instability in aqueous media, seriously hindering the electrochemical performance. Herein, a versatile strategy is proposed for the preparation of thermodynamically stable 1T-MoS2/MXene heterostructures with the aid of delaminated Ti3C2Tx MXene (d-Ti3C2Tx) dispersion containing tetrabutylammonium hydroxide. The 2D d-Ti3C2Tx provides more uniform nucleation sites for MoS2, and the TBA+ ions can intercalate into MoS2 to induce the phase conversion from semiconducting 2H to 1T. Moreover, the electrochemical advantages of 1T-MoS2 and d-Ti3C2Tx can be united by the construction of a well-organized heterostructure. Outstanding rate performance is realized because of extra-large interlayer space of 1T MoS2 with TBA+ intercalation and decreased energy barrier for fast Li+ diffusion. Subsequently, a lithium-ion capacitor (LIC) is assembled based on 1T-MoS2/d-Ti3C2Tx as anode and hierarchically porous graphene nanocomposite with micro/mesoporous structure as a cathode. The LIC exhibits a large energy density up to 188 Wh kg−1, an ultra-high power density of 13 kW kg−1, together with remarkable capacity retention of 83% after 5000 cycles. This study demonstrates the great promise of 1T-MoS2/d-Ti3C2Tx heterostructures as anode for high-performance LICs.  相似文献   

17.
Although Ti3C2 MXene has shown great potential in energy storage field, poor conductivity and restacking between MXene flakes seriously hinders the maximization of its capacitance. Herein, a new strategy to solve the problems is developed. Gallery Al atoms in Ti3AlC2 are partially removed by simple hydrothermal etching to get Ti3C2Tx reserving appropriate Al interlayers (Ti3C2Tx@Al). Ti3C2Tx@Al keeps stable layered structure rather than isolated Ti3C2Tx flakes, which avoids flake restacking. The removal of partial Al frees up space for easy electrolyte infiltration while the reserved Al as “electron bridges” ensures high interlayer conductivity. As a result, the areal capacitance reaches up to 1087 mF cm?2 at 1 mA cm?2 and over 95% capacitance is maintained after 6000 cycles. The all‐solid‐state supercapacitor (ASSS) based on Ti3C2Tx@Al delivers a high capacitance of 242.3 mF cm?2 at 1 mV s?1 and exhibits stable performance at different bending states. Two ASSSs in tandem can light up a light‐emitting diode under the planar or wrapping around an arm. The established strategy provides a new avenue to improve capacitance performances of MXenes.  相似文献   

18.
Freestanding, robust electrodes with high capacity and long lifetime are of critical importance to the development of advanced lithium–sulfur (Li–S) batteries for next‐generation electronics, whose potential applications are greatly limited by the lithium polysulfide (LiPS) shuttle effect. Solutions to this issue have mostly focused on the design of cathode hosts with a polar, sulfurphilic, conductive network, or the introduction of an extra layer to suppress LiPS shuttling, which either results in complex fabrication procedures or compromises the mechanical flexibility of the device. A robust Ti3C2Tx/S conductive paper combining the excellent conductivity, mechanical strength, and unique chemisorption of LiPSs from MXene nanosheets is reported. Importantly, repeated cycling initiates the in situ formation of a thick sulfate complex layer on the MXene surface, which acts as a protective membrane, effectively suppressing the shuttling of LiPSs and improving the utilization of sulfur. Consequently, the Ti3C2Tx/S paper exhibits a high capacity and an ultralow capacity decay rate of 0.014% after 1500 cycles, the lowest value reported for Li–S batteries to date. A robust prototype pouch cell and full cell of Ti3C2Tx/S paper // lithium foil and prelithiated germanium are also demonstrated. The preliminary results show that Ti3C2Tx/S paper holds great promise for future flexible and wearable electronics.  相似文献   

19.
2D Ti3C2Tx MXene, possessing facile preparation, high electrical conductivity, flexibility, and solution processability, shows good application potential for enhancing device performance of perovskite solar cells (PVSCs). In this study, tetrabutylammonium bromide functionalized Ti3C2Tx (TBAB-Ti3C2Tx) is developed as cathode buffer layer (CBL) to regulate the PCBM/Ag cathode interfacial property for the first time. By virtue of the charge transfer from TBAB to Ti3C2Tx demonstrated by electron paramagnetic resonance and density functional theory, the TBAB-Ti3C2Tx CBL with high electrical conductivity exhibits significantly reduced work function of 3.9 eV, which enables optimization of energy level alignment and enhancement of charge extraction. Moreover, the TBAB-Ti3C2Tx CBL can effectively inhibit the migration of iodine ions from perovskite layer to Ag cathode, which synergistically suppresses defect states and reduce charge recombination. Consequently, utilizing MAPbI3 perovskite without post-treatment, the TBAB-Ti3C2Tx based device exhibits a dramatically improved power conversion efficiency of 21.65% with significantly improved operational stability, which is one of the best efficiencies reported for the devices based on MAPbI3/PCBM with different CBLs. These results indicate that TBAB-Ti3C2Tx shall be a promising CBL for high-performance inverted PVSCs and inspire the further applications of quaternary ammonium functionalized MXenes in PVSCs.  相似文献   

20.
Surface chemistry and interlayer engineering determines the electrical properties of 2D MXene. However, it remains challenging to regulate the surface and interfacial chemistry of MXene simultaneously. Herein, simultaneous modulation of Ti3C2Tx MXene surface termination and layer spacing by alkali treatment are achieved. The electrical and electromagnetic properties of Ti3C2Tx are investigated in detail with respect to KOH and ammonia concentration dependence. A high concentration of KOH caused the Ti3C2Tx layer spacing to expand to 13.7 Å and the surface O/F ratio to increase to 33.84. Because of its weaker ionization effect, ammonia provides finer tuning compared to the drastic intercalation of KOH with a thorough sweeping of the F-containing groups. Ti3C2Tx is enriched with conductive -OH termination after ammonia treatment, which achieves an effective balance with the increased interlayer resistance. Therefore, NH3H2O-Ti3C2Tx achieves broad-band impedance matching and exhibits an efficient microwave loss of −49.1 dB at a low thickness of 1.7 mm, with an effective frequency bandwidth of 3.9 GHz. The results herein optimize the electrical properties of Ti3C2Tx using surface and interfacial chemistry to achieve broad microwave absorption, providing a framework for enhancing the electromagnetic wave loss of intrinsic MXene.  相似文献   

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