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1.
《Ceramics International》2022,48(14):20324-20331
As one of the typical MXenes materials, 2D Ti3C2Tx has attracted extensive attention in the field of energy storage. However, due to the restacking problem of Ti3C2Tx nanosheets, the electrochemical performance of Ti3C2Tx is unsatisfactory. In this paper, a scheme is proposed to obtain 3D aerogel with 1D channels by directional freeze drying of Ti3C2Tx. With the help of the unidirectional channels, the 3D Ti3C2Tx/Sodium alginate (SA) aerogel can effectively solve the stacking problem of Ti3C2Tx nanosheets, and it also accelerates the diffusion of ions. The Ti3C2Tx/SA-5 electrode can still reach the mass capacitance of 284.5 F g?1 and the areal capacitance of 4030.4 mF cm?2 at 2 mV s?1 when the loading is 14.2 mg cm?2 in 1 M H2SO4 electrolyte. In addition, the electrode showed good cycling performance without capacitor degradation after 20,000 cycles at 50 mV s?1. These results suggest that by using the strategy of building special 3D structure of 2D MXene with 1D unidirectional channels, high performance supercapacitor electrodes with high mass loading can be realized.  相似文献   

2.
As one of the novel two-dimensional metal carbides, Ti3C2Tx has received intense attention for lithium-ion batteries. However, Ti3C2Tx has low intrinsic capacity due to the fact that the surface functionalization of F and OH blocks Li ion transport. Herein a novel “plane-line-plane” three-dimensional (3D) nanostructure is designed and created by introducing the carbon nanotubes (CNTs) and SnO2 nanoparticles to Ti3C2Tx via a simple hydrothermal method. Due to the capacitance contribution of SnO2 as well as the buffer role of CNTs, the as-fabricated sandwich-like CNTs@SnO2/Ti3C2Tx nanocomposite shows high lithium ion storage capabilities, excellent rate capability and superior cyclic stability. The galvanostatic electrochemical measurements indicate that the nanocomposite exhibits a superior capacity of 604.1 mAh g?1 at 0.05?A?g?1, which is higher than that of raw Ti3C2Tx (404.9 mAh g?1). Even at 3?A?g?1, it retains a stable capacity (91.7 mAh g?1). This capacity is almost 5.6 times higher than that of Ti3C2Tx (16.6 mAh g?1) and 58 times higher than that of SnO2/Ti3C2Tx (1.6 mAh g?1). Additionally, the capacity of CNTs@SnO2/Ti3C2Tx for the 50th cycle is 180.1 mAh g?1 at 0.5?A?g?1, also higher than that of Ti3C2Tx (117.2 mAh g?1) and SnO2/Ti3C2Tx (65.8 mAh g?1), respectively.  相似文献   

3.
《Ceramics International》2020,46(13):21482-21488
Two-dimensional transition metal carbide (MXene) is a promising electrode material for supercapacitors because of its excellent electrochemical properties. Here, we report a controllable and facile strategy to prepare a freestanding and flexible N-doped Ti3C2Tx (N–Ti3C2Tx) film electrode with a hydrothermal method using hydrazine hydrate (N2H4∙H2O) as a nitrogen source. At a scan rate of 2 mV s−1, the N–Ti3C2Tx film electrode exhibits a high specific capacitance of 340 F g−1 and no capacitance degradation after 10,000 cycles in 1 M H2SO4 electrolyte. These results show that the N–Ti3C2Tx film could be used as an outstanding electrode material for high-performance supercapacitors. The operation of hydrazine treatment provides a more practical and convenient experimental method for N-doping.  相似文献   

4.
《Ceramics International》2022,48(3):3884-3894
Different kinds of two-dimensional hybrid electrodes have high theoretical capacitance and energy density. However, the origin of the electrochemical storage mechanism still remains elusive in alkaline, acid and neutral electrolytes. Herein, the interstratification-assembled Ti3C2Tx MXene/NiCo-LDHs electrodes were successfully prepared and studied in different electrolytes by in-situ Raman spectroscopy. The results show that H2O molecules in neutral electrolyte combine with –OH at the end of Ti3C2Tx MXene during charging, and debonding occurs during discharge. Similarly, this reaction also occurs in the discharge process with NiCo-LDHs and provides smaller pseudocapacitance characteristics. Although this pseudocapacitance reaction also occurs in acidic and alkaline electrolytes, however, the difference is that the hydrogen ions will promote the electrochemical performance of Ti3C2Tx MXene and has a certain corrosion consumption effect on NiCo-LDHs, but generally improve the electrochemical performance of Ti3C2Tx MXene/NiCo-LDHs. Interestingly, the OH? in alkaline electrolyte can promote the electrochemical performance of NiCo-LDHs, and produce a new electrochemical reaction with –F between the layers of Ti3C2Tx MXene, which greatly improves the overall electrochemical performance of this hybrid electrodes. As a result, Ti3C2Tx MXene/NiCo-LDHs electrodes have the best electrochemical performance in alkaline electrolyte with capacitance of 283 F g?1, energy density of 14.2 Wh kg?1 and power density of 3007.1 W kg?1. This work lays a foundation for the preparation of high-performance two-dimensional hybrid electrochemical energy storage devices.  相似文献   

5.
《Ceramics International》2022,48(11):15721-15728
Developing a new strategy to effectively prevent the restacking of MXene nanosheets will have significant impacts on designing flexible supercapacitor electrodes. Herein, a novel Ti3C2Tx/polyvinyl alcohol (PVA) porous sponge with 3D interconnected structures is prepared by sol-gel and freeze-dried methods. This Ti3C2Tx/PVA porous sponge is used as the template of in-situ polyaniline (PANI) polymerization, and the fabricated PANI@Ti3C2Tx/PVA hydrogel composite is applied as flexible supercapacitors electrodes. 1D conductive polymer chains PVA could increase the interlayer spacing of Ti3C2Tx nanosheets, which is beneficial to expose more electrochemical active sites. The supercapacitor based on PANI@Ti3C2Tx/PVA hydrogel composite exhibits the coexistence of double-layer capacitance and pseudocapacitance behavior. This supercapacitor shows a maximum areal specific capacitance of 103.8 mF cm?2 at 2 A m?2, and it also exhibits a maximum energy density of 9.2 μWh·cm?2 and an optimum power density of 800 μW cm?2. The capacitance of this supercapacitor is almost not change under different bending angles. Moreover, 99% capacitance retention is achieved after 10 000 charge/discharge cycles of the supercapacitor. The synergistic effect between PANI and Ti3C2Tx/PVA composite may improve the number of reactive sites and provide efficient channels for ion diffusion/electron transport.  相似文献   

6.
MXenes with a large surface area have been widely studied to improve the pseudocapacitance of electrode materials by combining conductive polymer materials. In this article, a superficial strategy to enhance the electrochemical properties by in situ polymerization of a pyrrole monomer between the Ti3C2Tx layers modified with 1,5-naphthalene disulfonic acid (NA) and cetyltrimethylammonium bromide (CTAB) was investigated. It is found that polypyrrole (PPy) and Ti3C2Tx can be combined through strong interactions between each other, and the specific capacitance of the modified Ti3C2Tx/PPy composite was increased to a maximum value of 437 F g−1, which was more than thrice higher than that of pure PPy. The composite also exhibited good cycling performance (76% capacitance retention after 1000 cycles). Moreover, owing to the synergistic effect between the PPy and Ti3C2Tx layers, the composite provided better electron or ion transfer and surface redox processes than that of pure PPy, which indicated that this composite can be used as a promising electrode material for supercapacitors. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 47003.  相似文献   

7.
《Ceramics International》2021,47(18):25531-25540
Ti3C2Tx exhibits excellent electromagnetic (EM) shielding and electrochemical properties. However, the inherent re-stacking tendency and easy oxidation of Ti3C2Tx limit its further application. In this study, a multi-walled carbon nanotube/polyaniline composite (CNT/PANI, denoted as C–P) was introduced into Ti3C2Tx nanosheets to obtain a Ti3C2Tx–CNT/PANI composite (T@CP). Owing to the integrated effects of Ti3C2Tx and C–P, the contribution of absorption was significantly improved, which finally enhanced the EM shielding performance of T@CP. The highest total EM shielding effectiveness (SET) was close to 50 dB (49.8 dB), which was substantially higher than that of pure Ti3C2Tx (45.3 dB). Moreover, T@CP demonstrated outstanding supercapacitive performance. The specific capacitance of T@CP (2134.5 mF/cm2 at 2 mV/s) was considerably higher than that of pure Ti3C2Tx (414.3 mF/cm2 at 2 mV/s). These findings provide a new route for the development of high-efficiency Ti3C2Tx-based bifunctional EM shielding and electrochemical materials.  相似文献   

8.
The incorporation of nanosized pseudocapacitive materials and structure design are general strategies to enhance the electrochemical performance of MXene-based materials. Herein, the decoration of manganese dioxide (MnO2) nanosheets on MXene (Ti3C2Tx) surfaces was prepared by a facile liquid phase coprecipitation method. Ti3C2Tx is initially modified by polydopamine (PDA) coating to ensure the homogeneous distribution of MnO2 nanosheets and tight and close connections between MnO2 and the Ti3C2Tx backbone. Due to the obtained three-dimensional (3D) nanostructure, facilitating electron transport within the electrode and promoting electrolyte ion accessibility, the δ-MnO2@Ti3C2Tx-0.06 electrode yields superior electrochemical performances, such as a rather large areal capacity of 1233.1 mF cm?2 and high specific capacitance of 337.6 F g?1 at 2 mV s?1, as well as high cyclic stability for 10000 cycles. Furthermore, δ-MnO2@Ti3C2Tx-0.06 composites are employed as positive electrodes, and activated carbon (AC) materials act as negative electrodes with an aqueous electrolyte of 1 M Na2SO4 to assemble asymmetric supercapacitors. The prototype device is reversible at cell voltages from 0 to 1.8 V, and manifests a maximum energy density of 31.4 Wh kg?1 and a maximum power density of 2700 W kg?1. These encouraging results show enormous possibilities for energy storage applications.  相似文献   

9.
Three-dimensional flower-like Ni(NiO) decorated on two-dimensional Ti3C2Tx/TiO2 composites were successfully synthesized by an in situ solvothermal reaction, and the electromagnetic (EM) wave absorption performance of the hybrids were explored at 2.00–18.00 GHz. The as-prepared Ni(NiO)/Ti3C2Tx/TiO2 composites include flower-like Ni(NiO) with uniform distribution on the surface of Ti3C2Tx MXenes and part of them get into the space between interlayers. The Ni(NiO)/Ti3C2Tx/TiO2 composites exhibit a maximum reflection loss (RL) value of ?41.74 dB at 14.96 GHz with the absorber thickness of merely 1.3 mm and the effective absorption bandwidth (EAB) reaches 3.20 GHz. The outstanding electromagnetic wave absorbing performance can be attributed to the dielectric loss of Ti3C2Tx MXenes and multi-phase heterostructures, the magnetic loss of Ni(NiO) and their synergistic loss mechanism. Moreover, the zigzag path formed by flower-like Ni(NiO) also has a great consumption effect on electromagnetic waves by incurring the eddy current under the affect of alternating EM waves. The laminated structure of Ti3C2Tx MXenes also dissipates microwaves by offering the space for multiple reflections and scattering. This paper furnished a novel modus for synthesizing original EM wave absorption materials and making the balance among thickness, broad bandwidth, oxidation resistance and light weight, which makes Ni(NiO)/Ti3C2Tx/TiO2 composites a hopeful material for microwave absorption (MA).  相似文献   

10.
To prevent restacking of the Ti3C2Tx layers, the Ti3C2Tx-foam has been successfully synthesized through thermal treatment of Ti3C2Tx-film with the hydrazine monohydrate. The interconnected porous structure of Ti3C2Tx-foam could effectively reduce the restacking of the Ti3C2Tx sheets and shorten the diffusion path of ions and accelerate the intercalation/de-intercalation of ions. The Ti3C2Tx-foam-80 used as free-standing electrode achieves a high areal capacitance of 271.2 mF/cm2 (122.7?F/g) at a scan rate of 5?mV/s in 1?M KOH electrolyte. It also exhibited a high capability rate of 65.5% from 5?mV/s to 100?mV/s and good cycle life with 88.7% retention of its initial after 10,000 cycles at a scan rate of 50?mV/s.  相似文献   

11.
Ti3C2Tx is a promising intercalation-type electrode material for capacitive deionization (CDI). However, Ti3C2Tx, obtained from traditional synthesized Ti3AlC2, is with large particle size and undersized interlayer space, which can easily lead to the longer ion diffusion path, fewer adsorption sites, and higher ion diffusion barrier in CDI process. In this work, subsize and Na+ intercalated Ti3C2Tx (Na+-Ti3C2Tx-MS) was prepared by HF etching KCl-assisted molten-salt synthesized Ti3AlC2 and following NaOH treatment. The Na+-Ti3C2Tx-MS achieves a high electrosorption capacity of 14.8 mg/g and a high charge efficiency of 0.81 at the applied voltage of 1.2 V in 100 mg/L NaCl solution. Besides, the stable desalination performance of Na+-Ti3C2Tx-MS has been confirmed. The superior performance of Na+-Ti3C2Tx-MS can be attributed to the subsize particle and larger interlayer space. Both two factors can effectively increase ions adsorption sites, shorten diffusion path lengths, and reduce diffusion barriers in the CDI process.  相似文献   

12.
《Ceramics International》2021,47(21):30082-30090
As an emerging label-free detection technology, surface-enhanced Raman scattering (SERS) has been used for biological detection, food safety, and environmental pollution owing to its high sensitivity, specificity and rapid response. However, traditional SERS substrates are unstable, prone to agglomeration, and demonstrate low productivity and high production cost. In this work, hybrids of a two-dimensional electron gas (2DEG) Ti3C2Tx monolayer and Au nanorods (AuNRs) were fabricated via self-assembly. Ti3C2Tx:AuNRs ratios were prepared, and each hybrid's SERS activity was evaluated through 4-aminothiophenol (pATP) detection. The Ti3C2Tx/AuNRs-1 substrate exhibited the weakest SERS performance, whereas the Ti3C2Tx/AuNRs-3 substrate had the best SERS activity enhancement, with a pATP limit of detection (LOD) of 10−9 M. When 30 sites on substrates were selected for SERS detection, the relative standard deviation (RSD) was found to be only 7.18 %, revealing the good performance sensitivity and high reproducibility of the Raman signal. The sensitivity of Ti3C2Tx/AuNRs-3 was also assessed with respect to a hazardous chemical, 1,2-bis (4-pyridyl) ethylene (BPE), revealing an LOD of 10−12 M. For thiram, the LOD of Ti3C2Tx/AuNRs-3 was 10−8 M, which is considerably lower than the 1 ppm industry safety standard. A relative standard deviation RSD of 7.94 % indicates the high reproducibility and uniformity of the Raman signal of thiram for Ti3C2Tx/AuNRs-3. Compared with the LODs of 10−5 M and 10−6 M for commercial substrates T-SERS and Au nanorod arrays (AuNRAs), respectively, the 10−8 M LOD of our synthesized Ti3C2Tx/AuNRs indicates good sensitivity. Three kinds of pesticides were detected by Ti3C2Tx/AuNRs, and only Raman signal of thiram can be found, revealing the good selectivity for thiram. These results for Ti3C2Tx/AuNRs suggest its potential to serve as a novel SERS platform.  相似文献   

13.
《Ceramics International》2022,48(17):24656-24665
This study aims to provide insights into the absorption and shielding performances of Fe3O4 modified oligo-layered Ti3C2Tx towards microwave electromagnetic interference. Oligo-layered Ti3C2Tx was modified by Fe3O4 nanoparticles (60 nm) via a facile electrostatic assembly approach at different loading rates. This composite was shown to have high dielectric constant and high permeability compared with oligo-layered Ti3C2Tx. The microwave electromagnetic absorbing and shielding performances were monitored through a vector network instrument with focuses on the EMI performance. The sample Ti3C2Tx/Fe3O4 with a 5:1 mass ratio of Ti3C2Tx to Fe3O4 displayed the optimized EMI shielding performance. The average SE value was 62.19 dB, and the maximum value was 68.72 dB at 18 GHz with a 2.6 mm thickness. The EMI shielding mechanism was understood based on the conductive loss, magnetic loss, dipole polarization, and multiple scattering. Results suggests that Ti3C2Tx/Fe3O4 composites are expected to be superior EMI shielding material.  相似文献   

14.
Currently, among the various emerging energy storage systems, the lithium–sulphur (Li-S) battery is expected to be one of the next-generation lithium secondary batteries with high efficiency. However, the practical application of Li-S batteries still faces many obstacles. To solve the shuttle effect of lithium polysulphides, ultrathin Ti3C2Tx nanosheets were prepared through the in-situ acid etching method and applied to separator modification to suppress the shuttle effect of lithium polysulphides. Ultrathin Ti3C2Tx nanosheets with enlarged interlayer spacing accelerated the migration of Li+. The abundant termination groups on the surface of Ti3C2Tx played the role of the lithium polysulphide capture centre. When the mass loading of separator modification materials was set as 0.025 mg cm−2, the as-prepared battery exhibited a reversible specific capacity as high as 780 mAh g−1 after 200 cycles at 0.2 C, and the single-cycle capacity decay rate was only 0.09%.  相似文献   

15.
《Ceramics International》2023,49(2):2081-2090
MXene, a novel two-dimensional material composed of alternating transition metal carbon/nitrogen, has the advantages of large specific surface area, many active sites, and short ion transport paths, and has shown great potential in the field of capacitors in the beginning. However, the unique two-dimensional structure is prone to collapse and accumulation, which inhibits the electron migration rate and ion penetration, resulting in poor energy storage capacity. In this paper, Ti3C2Tx/Ag/MWCNTs/Ag composites with good capacitive properties were successfully prepared by Ti3C2Tx which directly reduces silver nitrate solution and further introduces nanoscale MWCNTs. Ag NPs are introduced twice to grow and distribute uniformly on the surface and between the layers of Ti3C2Tx to play a supporting role. The introduction of MWCNTs in the intermediate process can enter the interlayer and act as spacers together with Ag NPs to prevent the collapse and stacking of Ti3C2Tx and improve its surface utilization. However, the preparation process unavoidably leads to partial oxidation of Ti3C2Tx, which deteriorates its electrochemical properties. Owing to the synergy between Ti3C2Tx, Ag NPs and MWCNTs, the Ti3C2Tx/Ag/MWCNTs/Ag composites show good electrical conductivity, low internal resistance (0.67 Ω) and extreme high capacitance contribution (97%) in electrochemical tests.  相似文献   

16.
Two-dimensional layered Ti3C2Tx MXene was prepared through hydrothermal etching method with LiF and hydrochloric (HCl) acid. Ti3C2Tx was further treated with oxygen plasma activated by microwave energy to obtain the activated Ti3C2Tx at different temperatures ranging from 350 °C to 550 °C. The gas-sensing properties of raw Ti3C2Tx and Ti3C2Tx activated with oxygen microwave plasma were tested toward different volatile organic compounds gases. The results indicated that Ti3C2Tx activated at 500 °C exhibited excellent gas-sensing properties at room temperature (25 °C) to 100 ppm ethanol with a value of 22.47, which is attributed to the enhancement of the amount of oxygen functional groups and defects on the MXene Ti3C2Tx film, and in turn to lead to more oxygen molecules adsorption and desorption reaction in the active defect sites. The enhancement of ethanol-sensing performance demonstrated that the activated Ti3C2Tx possess great potential in gas sensing.  相似文献   

17.
《Ceramics International》2021,47(21):29995-30004
Novel and highly effective electromagnetic interference (EMI) shielding materials are desirable to attenuate unwanted electromagnetic radiation or interference produced by electrical communication devices. Here, functional Ti3C2Tx@Ni particles with a core@shell and sandwich like structure were fabricated using the facile electroless plating technique. The core@shell structured Ti3C2Tx@Ni consists of a Ti3C2Tx core and a Ni shell. In the core, thin Ni layers are sandwiched in between Ti3C2Tx flakes. EMI shielding effectiveness (SE) values of Ti3C2Tx@Ni/wax composites increased with increasing Ti3C2Tx@Ni content. The average EMI SE value of 60 wt% Ti3C2Tx@Ni/wax composite was 43.12 dB, increased by 73% as compared with 24.93 dB for the same content of pristine Ti3C2Tx in wax in the frequency range 2–18 GHz. An average EMI SE of 74.14 dB was achieved in the 80 wt% Ti3C2Tx@Ni/wax. The enhanced EMI shielding performance should be ascribed to the synergic effect of the absorption loss of the Ti3C2Tx core and the magnetic loss of the Ni shell and the inner Ni layers.  相似文献   

18.
《Ceramics International》2023,49(18):29962-29970
The few-layered Ti3C2Tx/WO3 nanorods foam composite material was synthesized by electrostatic self-assembly and bidirectional freeze-drying technologies. The phase structure and microstructure of synthesized samples was characterized by XRD, FESEM, TEM and their gas sensing properties estimated via a self-designed equipment with four test channels. The results demonstrate WO3 nanorods were successfully anchored on the surface and between layers of few-layered Ti3C2Tx MXene by electrostatic self-assembly strategy and the composite material simultaneously has a low-density foam morphology by means of bidirectional freeze-drying processes. There exists a typical heterostructure at the interfaces owing to the inseparable contact between the few-layered Ti3C2Tx MXene and WO3 nanorods. Compared with the original WO3 nanorods, the few-layered Ti3C2Tx/WO3 nanorods foam composite material displays excellent gas sensing properties for NO2 detection at low temperature, in particular the optimal value of gas sensing response (Rg/Ra) reaches to 89.46 toward 20 ppm NO2 at 200 °C. The gas sensing mechanism was also discussed. The increase of gas sensitivity is attributed to a fact that during the reaction process of gas sensing, the excellent conductivity of the few-layered Ti3C2Tx MXene provided faster transport channels of free carriers, and the heterojunctions formed by few-layered Ti3C2Tx MXene and WO3 nanorods enhanced the carriers separation efficiency. Meanwhile, the low-density layered structure of few-layered Ti3C2Tx/WO3 nanorods foam composite material provides convenient diffusion paths for gas molecules to the surface of WO3 nanorods.  相似文献   

19.
《Ceramics International》2015,41(6):7556-7564
In this work, three-dimensional hierarchical ZnCo2O4 flower-like microspheres have been synthesized on a large scale via a facile and economical citrate-mediated hydrothermal method followed by an annealing process in air. The as-synthesized ZnCo2O4 flower-like microspheres are constructed by numerous interweaving porous nanosheets. According to the experimental results, a formation mechanism involving the assembly of the nanosheets from nanoparticles into flower-like microsphere is proposed. As a virtue of their beneficial structural features, the ZnCo2O4 flower-like microspheres exhibit a high lithium storage capacity and excellent cycling stability (1136 mA h g−1 at 100 mA g−1 after 50 cycles). This remarkable electrochemical performance can be ascribed to the hierarchical structure and porous structures in the nanosheets, which effectively increases the contact area between the active materials and the electrolyte, shortening the Li+ diffusion pathway and buffering the volume variation during cycling.  相似文献   

20.
Light-weight and flexible 2D MXene-based polymer materials with low dielectric loss and high dielectric constant have drawn great attention in the power systems and modern electronic field. A series of Ti3C2Tx/EMA composites were fabricated via simple solution casting followed by a compression molding method with various mass concentrations of Ti3C2Tx (0, 1, 3, 5, 8, 10, 12, and 15 wt%). Morphological and micro structural properties of the prepared composites were studied via X-ray diffraction (XRD) and field-emission scanning electron microscope (FESEM), where the distribution of Ti3C2Tx in the Ti3C2Tx/EMA composites was confirmed. Thermal behaviors were analyzed by differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) investigations. The DSC analysis reveals that the % of crystallinity decreases from 11.06 with 1 wt% to 5.68 with 15 wt%, where Ti3C2Tx acts as an efficient nucleating agent. TGA data confirm the enhancement of the thermal stability of the composites upon increasing in Ti3C2Tx loading. The room temperature electrical and dielectric behavior of the studied composites were examined in the frequency range of 100 Hz–5 MHz. In this work, the 10 wt% of Ti3C2Tx loaded poly (ethylene-co-methyl acrylate) composite (EMA) showed higher dielectric permittivity (ε′ = 124.22) with lower dissipation loss (tan δ = 0.051) at 100 Hz among all weight percentages. The behavior of charge carriers in the prepared composites was studied by utilizing the impedance spectroscopy technique. The electrical parameters were calculated from the fitted Nyquist plots with a corresponding circuit model. I–V curves confirmed the conduction mechanisms of the composites. This beneficial enhancement in electrical properties recommends the composite can be utilized in flexible electronic storage devices.  相似文献   

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