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1.
Stroke ; 53(5): 1580-1588, 2022 05.
Artículo en Inglés | MEDLINE | ID: mdl-35105182

RESUMEN

BACKGROUND: In patients undergoing mechanical thrombectomy (MT), adjunctive antithrombotic might improve angiographic reperfusion, reduce the risk of distal emboli and reocclusion but possibly expose patients to a higher intracranial hemorrhage risk. This study evaluated the safety and efficacy of combined MT plus eptifibatide for acute ischemic stroke. METHODS: This was a propensity-matched analysis of data from 2 prospective trials in Chinese populations: the ANGEL-ACT trial (Endovascular Treatment Key Technique and Emergency Workflow Improvement of Acute Ischemic Stroke) in 111 hospitals between November 2017 and March 2019, and the EPOCH trial (Eptifibatide in Endovascular Treatment of Acute Ischemic Stroke) in 15 hospitals between April 2019 and March 2020. The primary efficacy outcome was good outcome (modified Rankin Scale score 0-2) at 3 months. Secondary efficacy outcomes included the distribution of 3-month modified Rankin Scale scores and poor outcome (modified Rankin Scale score 5-6) and successful recanalization. The safety outcomes included any intracranial hemorrhage, symptomatic intracranial hemorrhage, and 3-month mortality. Mixed-effects logistic regression models were used to account for within-hospital clustering in adjusted analyses. RESULTS: Eighty-one combination arm EPOCH subjects were matched with 81 ANGEL-ACT noneptifibatide patients. Compared with the no eptifibatide group, the eptifibatide group had significantly higher rates of successful recanalization (91.3% versus 81.5%; P=0.043) and 3-month good outcomes (53.1% versus 33.3%; P=0.016). No significant difference was found in the remaining outcome measures between the 2 groups. All outcome measures of propensity score matching were consistent with mixed-effects logistic regression models in the total population. CONCLUSIONS: This matched-control study demonstrated that MT combined with eptifibatide did not raise major safety concerns and showed a trend of better efficacy outcomes compared with MT alone. Overall, eptifibatide shows potential as a periprocedural adjunctive antithrombotic therapy when combined with MT. Further randomized controlled trials of MT plus eptifibatide should be prioritized. REGISTRATION: URL: https://www. CLINICALTRIALS: gov; Unique identifier: NCT03844594 (EPOCH), NCT03370939 (ANGEL-ACT).


Asunto(s)
Isquemia Encefálica , Accidente Cerebrovascular Isquémico , Accidente Cerebrovascular , Isquemia Encefálica/tratamiento farmacológico , Isquemia Encefálica/cirugía , Eptifibatida , Humanos , Hemorragias Intracraneales/etiología , Estudios Prospectivos , Accidente Cerebrovascular/tratamiento farmacológico , Accidente Cerebrovascular/cirugía , Trombectomía/métodos , Resultado del Tratamiento
2.
Sensors (Basel) ; 22(5)2022 Mar 04.
Artículo en Inglés | MEDLINE | ID: mdl-35271146

RESUMEN

In this paper, a multipopulation dynamic adaptive coevolutionary strategy is proposed for large-scale optimization problems, which can dynamically and adaptively adjust the connection between population particles according to the optimization problem characteristics. Based on analysis of the network evolution characteristics of collaborative search between particles, a dynamic adaptive evolutionary network (DAEN) model with multiple interconnection couplings is established in this algorithm. In the model, the swarm type is divided according to the judgment threshold of particle types, and the dynamic evolution of collaborative topology in the evolutionary process is adaptively completed according to the coupling connection strength between different particle types, which enhances the algorithm's global and local searching capability and optimization accuracy. Based on that, the evolution rules of the particle swarm dynamic cooperative search network were established, the search algorithm was designed, and the adaptive coevolution between particles in different optimization environments was achieved. Simulation results revealed that the proposed algorithm exhibited a high optimization accuracy and converging rate for high-dimensional and large-scale complex optimization problems.

3.
Small ; 17(41): e2102639, 2021 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-34510732

RESUMEN

With the accelerating update of advanced electronic gadgets, a great deal of attention is being paid today to the function integration and intelligent design of electronic devices. Herein, a novel kind of multitasking 3D oxygen-deficient WO3- x ∙ 2H2 O/Ag/ceramic microscaffolds, possessing simultaneous giant energy density, ultrahigh mechanical strength, and reversible electrochromic performance is proposed, and fabricated by a 3D printing technique. The ceramic microscaffolds ensure outstanding mechanical strength and stability, the topology optimized porous lattice structure provides developed surface area for coloration as well as abundant easily accessible channels for rapid ion transportation, and the bifunctional oxygen-defective pseudomaterials enable the large areal capacity and impressive electrochromic performance. As a result, this 3D-printed multitasking microscaffolds simultaneously perform structure-designable, electrochromic, compression resistant, and energy storage functions, behaving with true 3D structure with tailorable curvatures, excellent compressive strength (61.9 MPa), large color variations (>145% in b* value), good aesthetic visual quality as well as exciting electrochemical performances for energy storage including ultrahigh areal capacitance (10.05 F cm-2 at 5 mA cm-2 ), record-high energy density (0.60 mWh cm-2 ), and superior long-term cycling stability (88.6% capacity retention after 10 000 cycles). This work opens up the possibility for high-performance multi-functional coupling structural materials and integrated systems.

4.
Nanotechnology ; 29(18): 184003, 2018 May 04.
Artículo en Inglés | MEDLINE | ID: mdl-29442068

RESUMEN

In this study, mesoporous carbon hollow microspheres (PCHMs) with tunable textural properties have been prepared through a facile hard template etching method. The PCHMs were characterized by scanning electron microscopy, transmission electron microscopy, x-ray diffraction, Raman spectra, and nitrogen adsorption and desorption systems. Uniform PCHMs with shell thickness ranging from 23 nm to 55 nm are realized. PCHMs with different textural properties can regulate dielectric and electromagnetic (EM) wave absorption effectively. The composite of paraffin wax mixed with 10 wt% PCHMs (the shell thickness of PCHMs is 35 nm) exhibits a minimum coefficient value of -53.8 dB at 8.8 GHz, with a thickness of 3.4 mm. Besides, it is remarkable that the effective absorption bandwidth covers all the X band with as low as a 10 wt% filler ratio, compared with other spherical EM wave absorbers. The excellent EM wave absorption capability of PCHMs can be ascribed to the better impendence matching and strong EM wave attenuation constant based on tunable textural properties. Our results provide a facile strategy to tune dielectric properties of spherical carbon absorbers based on textural properties, and can be extended to other spherical absorbers.

5.
Phys Chem Chem Phys ; 17(17): 11763-9, 2015 May 07.
Artículo en Inglés | MEDLINE | ID: mdl-25869225

RESUMEN

We have performed first-principles evolutionary searches for stable Ti-N compounds and have found, in addition to the well-known rock-salt TiN, new ground states Ti3N2, Ti4N3, Ti6N5 at atmospheric pressure, and Ti2N and TiN2 at higher pressures. The latter nitrogen-rich structure contains encapsulated N2 dumbbells with a N-N distance of 1.348 Å at 60 GPa. TiN2 is predicted to be mechanically stable and quenchable. Our calculations on the mechanical properties (bulk modulus, shear modulus, Young's modulus, Poisson's ratio, and hardness) are in excellent agreement with the available experimental data. Further analyses of the electronic density of states, crystal orbital Hamilton population and the electron localization function reveal that the hardness is enhanced by strengthening directional covalent bonds and disappearance of Ti-Ti metallic bonding.

6.
Zhonghua Wai Ke Za Zhi ; 53(7): 553-7, 2015 Jul 01.
Artículo en Zh | MEDLINE | ID: mdl-26359082

RESUMEN

The formation mechanisms of rare intracranial aneurysms are various, which lead to various kinds of treatment methods. The present article summarized the pathogenesis, pathologic changes in vascular walls and imaging features of rare intracranial aneurysms including segmental ectasia, aneurysms with dissection, aneurysms with intramural hemorrhage, mycotic aneurysms, aneurysms related to HIV, neoplastic aneurysms and traumatic aneurysms through literature review.


Asunto(s)
Diagnóstico por Imagen , Aneurisma Intracraneal/diagnóstico , Aneurisma Intracraneal/patología , Aneurisma Intracraneal/terapia , Dilatación Patológica , Humanos
7.
ChemSusChem ; 17(11): e202301818, 2024 Jun 10.
Artículo en Inglés | MEDLINE | ID: mdl-38566411

RESUMEN

With the growing demand for new energy storage devices, rechargeable aqueous zinc ion batteries (ZIBs) have attracted widespread attention due to their low cost and high safety. Among the cathode materials for ZIBs, polyanionic-based cathode materials with high voltage, high stability, and low cost have great potential. In this paper, tetragonal Na2VOP2O7 was prepared using a simple sol-gel method. The discharge platform voltage amounted to 1.8 V and had good rate and cycle performance due to the inductive effect of pyrophosphate. Then, a protective layer of Zn-hydroxyapatite (ZnHAP) modification was applied to the cathode surface, which can inhibit the hydrolysis of vanadium ions. The capacity was enhanced by 19 % after modification and the capacity retention after 100 cycles was also higher. Interestingly, the Na2VOP2O7 cathode also possesses a self-charging effect, recovering to 48 % of its initial capacity with an open-circuit voltage (OCV) of 1.1 V within a certain period, and light exposure can reduce the self-charging time by 83 %. These beneficial results indicate that the pyrophosphate bifunctional cathode with inductive effect has a great potential to construct high-voltage and multifunctional zinc ion battery.

8.
Mater Horiz ; 10(9): 3404-3415, 2023 Aug 29.
Artículo en Inglés | MEDLINE | ID: mdl-37350473

RESUMEN

Cloaking against electromagnetic detection is a well-researched topic; yet achieving multispectral camouflage over a wide temperature range remains challenging. Herein, an orientation-gradient co-optimized graded Gyroid-shellular (GGS) SiOC-based metastructure with a conformal MXene coating (M@SiOC) is proposed to achieve wide-temperature-range microwave/infrared/visible-light-compatible camouflage. Firstly, the combination of coordinate transformation and genetic algorithm endows the GGS architecture with optimal orientation and gradient, allowing superior microwave blackbody-like behavior. Secondly, a microwave-transparent, low-infrared-emissivity MXene metasurface is constructed in situ to permit wide-temperature-range infrared camouflage. Finally, the outstanding spectral selectivity of MXene enables camouflage against 1.06 µm-lidar and visible-light detection. As a result, the as-fabricated [110]-oriented GGS M@SiOC metamaterials exhibit outstanding wide-temperature-range multispectral camouflage: (i) ultrabroadband microwave absorption exceeding 80% in the X-Ku band from room temperature (RT) to 500 °C with absorption above 86.0% (91.4% on average) at 500 °C; (ii) excellent long-wavelength infrared camouflage for object temperatures from RT to 450 °C, reaching an infrared signal intensity of 78.5% for objects at 450 °C; and (iii) camouflage against both 1.06 µm-lidar and dark environment. Compared with traditional hierarchical metamaterials necessitating complex micro/nano-fabrication processes, this work provides a novel pathway toward the realization of structurally integrated multispectral stealth components by combining flexible metastructure design and high-fidelity additive manufacturing.

9.
J Phys Chem A ; 116(26): 6955-66, 2012 Jul 05.
Artículo en Inglés | MEDLINE | ID: mdl-22662961

RESUMEN

The decomposition reaction rate in the BCl(3)-C(3)H(6)-H(2) gas phase reaction system in preparing boron carbides was investigated based on the most favorable reaction pathways proposed by Jiang et al. [Theor. Chem. Accs. 2010, 127, 519] and Yang et al. [J. Theor. Comput. Chem. 2012, 11, 53]. The rate constants of all the elementary reactions were evaluated with the variational transition state theory. The vibrational frequencies for the stationary points as well as the selected points along the minimum energy paths (MEPs) were calculated with density functional theory at the B3PW91/6-311G(d,p) level and the energies were refined with the accurate model chemistry method G3(MP2). For the elementary reaction associated with a transition state, the MEP was obtained with the intrinsic reaction coordinates, while for the elementary reaction without transition state, the relaxed potential energy surface scan was employed to obtain the MEP. The rate constants were calculated for temperatures within 200-2000 K and fitted into three-parameter Arrhenius expressions. The reaction rates were investigated by using the COMSOL software to solve numerically the coupled differential rate equations. The results show that the reactions are, consistent with the experiments, appropriate at 1100-1500 K with the reaction time of 30 s for 1100 K, 1.5 s for 1200 K, 0.12 s for 1300 K, 0.011 s for 1400 K, or 0.001 s for 1500 K, for propene being almost completely consumed. The completely dissociated species, boron carbides C(3)B, C(2)B, and CB, have very low concentrations, and C(3)B is the main product at higher temperatures, while C(2)B is the main product at lower temperatures. For the reaction time 1 s, all these concentrations approach into a nearly constant. The maximum value (in mol/m(3)) is for the highest temperature 1500 K with the orders of -13, -17, and -23 for C(3)B, C(2)B, and CB, respectively. It was also found that the logarithm of the overall reaction rate and reciprocal temperature have an excellent linear relationship within 700-2000 K with a correlation coefficient of 0.99996. This corresponds to an apparent activation energy 337.0 kJ/mol, which is comparable with the energy barrier 362.6 kJ/mol of the rate control reaction at 0 K but is higher than either of the experiments 208.7 kJ/mol or the Gibbs free energy barrier 226.2 kJ/mol at 1200 K.

10.
Adv Sci (Weinh) ; 9(30): e2204086, 2022 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-36026560

RESUMEN

Solar-thermal conversion is considered as a green and simple means to improve the performance of energy storage materials, but often limited by the intrinsic photothermal properties of materials and crude structure design. Herein, inspired by the unique light trapping effect of wide leaf spiral grass during photosynthesis, a biomimetic structural photothermal energy storage system is developed, to further promote the solar thermal-driven pseudo capacitance improvement. In this system, three-dimensional printed tortional Kelvin cell arrays structure with interesting light trapping property functions as "spiral leaf blades" to improve the efficiency of light absorption, while graphene quantum dots/MXene nanohybrids with wide photothermal response range and strong electrochemical activity serve as "chloroplast" for photothermal conversion and energy storage. As expected, the biomimetic structure-enhanced photothermal supercapacitor achieves an ideal solar thermal-driven pseudo capacitance enhancement (up to 304%), an ultrahigh areal capacitance of 10.47 F cm-2 , remarkable photothermal response (surface temperature change of 50.1 °C), excellent energy density (1.18 mWh cm-2 ) and cycling stability (10000 cycles). This work not only offers a novel enhancement strategy for photothermal applications, but also inspires new structure designs for multifunctional energy storage and conversion devices.


Asunto(s)
Grafito , Puntos Cuánticos , Puntos Cuánticos/química , Poaceae
11.
J Colloid Interface Sci ; 607(Pt 1): 242-252, 2022 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-34500423

RESUMEN

Bismuth titanate (Bi12TiO20) with unique sillenite structure has been shown to be an excellent photocatalyst for environmental remediation. However, the narrow light-responsive range and rapid recombination of photoinduced electrons-holes limit the photocatalytic performance of Bi12TiO20. To overcome the limitations, a practical and feasibleway is to fabricate heterojunctions by combining Bi12TiO20 with suitable photocatalysts. Here, using a facile chemical precipitation method, a novel and hierarchical core-shell structure of n-Bi12TiO20@p-BiOI (BTO@BiOI) heterojunction was rationally designed and synthesized by loading BiOI nanosheets on BTO nanofibers. The constructed BTO@BiOI composites exhibited significant charge transfer ability due to the synergistic effects of the built-in electric field between BTO and BiOI as well as close interfacial contacts. In addition, the narrow bandgapcharacteristics of the BiOI led to wide light absorption ranges. Therefore, the BTO@BiOI heterojunction exhibited an improved photocatalytic performance under visible light irradiation. The NO removal efficiency of optimal BTO@BiOI was 45.7%, which was significantly higher compared tothat of pure BTO (3.6%) or BiOI (23.1%). Moreover, the cycling experiment revealed that BTO@BiOI composite has a good stability and reusability. The possible mechanism of photocatalytic NO oxidation over BTO@BiOI was investigated in detail.

12.
J Colloid Interface Sci ; 611: 137-148, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-34942487

RESUMEN

Converting CO2 into chemical energy by using solar energy is an environmental strategy to achieve carbon neutrality. In this paper, two dimensionality (2D) SrTiO3-x nanosheets with oxygen vacancies were synthesized successfully. Oxygen vacancies will generate defect levels in the band structure of SrTiO3-x. So, SrTiO3-x nanosheets have good photocatalytic CO2 reduction performance under visible light. In order to further improve its photocatalytic efficiency, Bi was used to dope Sr site and Ti site in SrTiO3-x nanosheets respectively. It is found that Sr site is the adsorption site of CO2 molecules. When Bi replaced Sr, CO2 adsorption on the surface of SrTiO3-x nanosheets was weakened. When Bi replaced Ti, there has no effect on CO2 adsorption. Due to the synergistic effect of Bi doping, oxygen vacancies, and Sr active site, the 1.0% Bi-doped Ti site in SrTiO3-x (1.0% Bi-Ti-STO) had the best photocatalytic performance under visible light (λ ≥ 420 nm). CO and CH4 yields were 5.58 umol/g/h and 0.36 umol/g/h. Photocatalytic CO2 reduction path has always been the focus of exploration. The in-situ FTIR spectrum proved the step of photocatalytic CO2 reduction and COO- and COOH are important intermediates in the photocatalytic CO2 reaction.

13.
J Colloid Interface Sci ; 628(Pt A): 673-683, 2022 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-35940151

RESUMEN

In this article, a 3D photocatalytic support with different Poisson's ratio was used for the first time to control the photocatalytic production rate of hydrogen. It was created by a stereo-lithography method, and the support with the most negative Poisson's ratio got the best result. The Poisson's ratio of the 3D structure influences the rate of hydrogen production, and it is important for the photocatalyst supports to be porous for light to penetrate into them. A series of Ce doped CdS photocatalysts were produced and immobilized on 3D multicellular Al2O3 supports. By changing the proportion of Ce3+ doped into the CdS photocatalysts 1 % of Ce3+ exhibited optimal hydrogen production, which was 222.9 % compared to that of the pure CdS. Using the 3D photocatalytic support with different Poisson's ratio, the photocatalytic production rate of hydrogen increased by 128 %.


Asunto(s)
Hidrógeno , Porosidad
14.
Adv Sci (Weinh) ; 9(16): e2201118, 2022 May.
Artículo en Inglés | MEDLINE | ID: mdl-35481671

RESUMEN

Heterogeneous interface design to boost interfacial polarization has become a feasible way to realize high electromagnetic wave absorbing (EMA) performance of dielectric materials. However, interfacial polarization in simple structures such as particles, rods, and flakes is weak and usually plays a secondary role. In order to enhance the interfacial polarization and simultaneously reduce the electronic conductivity to avoid reflection of electromagnetic wave, a more rational geometric structure for dielectric materials is desired. Herein, a Ti3 C2 Tx /MoS2 self-rolling rod-based foam is proposed to realize excellent interfacial polarization and achieve high EMA performance at ultralow density. Different surface tensions of Ti3 C2 Tx and ammonium tetrathiomolybdate are utilized to induce the self-rolling of Ti3 C2 Tx sheets. The rods with a high aspect ratio not only remarkably improve the polarization loss but also are beneficial to the construction of Ti3 C2 Tx /MoS2 foam, leading to enhanced EMA capability. As a result, the effective absorption bandwidth of Ti3 C2 Tx /MoS2 foam covers the whole X band (8.2-12.4 GHz) with a density of only 0.009 g cm-3 , at a thickness of 3.3 mm. The advantages of rod structures are verified through simulations in the CST microwave studio. This work inspires the rational geometric design of micro/nanostructures for new-generation EMA materials.

15.
J Comput Chem ; 32(13): 2745-55, 2011 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-21717476

RESUMEN

The reaction rate of propene pyrolysis was investigated based on the elementary reactions proposed in Qu et al., J Comput Chem 2009, 31, 1421. The overall reaction rate was developed with the steady-state approximation and the rate constants of the elementary reactions were determined with the variational transition state theory. For the elementary reaction having transition state, the vibrational frequencies of the selected points along the minimum energy path were calculated with density functional theory at B3PW91/6-311G(d,p) level and the energies were improved with the accurate model chemistry method G3(MP2). For the elementary reaction without transition state, the frequencies were calculated with CASSCF/6-311G(d,p) and the energies were refined with the multireference configuration interaction method MRCISD/6-311G(d,p). The rate constants were evaluated within 200-2000 K and the fitted three-parameter expressions were obtained. The results are consistent with those in the literatures in most cases. For the overall rate, it was found that the logarithm of the rate and the reciprocal temperature have excellent linear relationship above 400 K, predicting that the rate follows a typical first-order law at high temperatures of 800-2000 K, which is also consistent with the experiments. The apparent activation energy in 800-2000 K is 317.3 kJ/mol from the potential energy surface of zero Kelvin. This value is comparable with the energy barriers, 365.4 and 403.7 kJ/mol, of the rate control steps. However, the apparent activation energy, 215.7 kJ/mol, developed with the Gibbs free energy surface at 1200 K is consistent with the most recent experimental result 201.9 ± 0.6 kJ/mol.

16.
ACS Appl Mater Interfaces ; 13(29): 34984-34995, 2021 Jul 28.
Artículo en Inglés | MEDLINE | ID: mdl-34278775

RESUMEN

Superlubricity is a fascinating phenomenon which attracts people to continuously expand ultralow friction and wear from microscale to macroscale. Despite the impressive advances in this field, it is still limited to specific materials and extreme operating conditions. Introducing a heterostructure with intrinsic lattice mismatch into delicate topologies mimicked from nature provides a promising alternative toward macroscopic superlubricity. Herein, 3D-printed MoS2/MoSe2 heterostructures with bioinspired circular-cored square/hexagonal honeycomb topologies were developed. Compared to 3D-printed Al2O3, all topological structures with both high hardness and excellent flexural strength achieve more than 30% decrease in the friction coefficient. The circular-cored hexagonal honeycomb composite with 30% area density exhibits a stable ultralow friction coefficient of 0.09 and a low wear rate of 2.5 × 10-5 mm3·N-1 m-1 under 5 N. Even under 10 N, a highly desirable coefficient value of 0.08 can be maintained within 370 s. The extraordinary ultralow friction could be attributed to the small contact area, high lubricant mass loading, efficient collection and storage of both abrasive debris and lubricant, and the self-orientation in the lubricating film. This work provides new insights into developing high-efficiency lubrication devices and aids in the industrial application of macroscopic superlubricity in future life.

17.
J Comput Chem ; 31(7): 1421-42, 2010 May.
Artículo en Inglés | MEDLINE | ID: mdl-20082392

RESUMEN

The gas-phase reaction pathways in preparing pyrolytic carbon with propene pyrolysis have been investigated in detail with a total number of 110 transition states and 50 intermediates. The structure of the species was determined with density functional theory at B3PW91/6-311G(d,p) level. The transition states and their linked intermediates were confirmed with frequency and the intrinsic reaction coordinates analyses. The elementary reactions were explored in the pathways of both direct and the radical attacking decompositions. The energy barriers and the reaction energies were determined with accurate model chemistry method at G3(MP2) level after an examination of the nondynamic electronic correlations. The heat capacities and entropies were obtained with statistical thermodynamics. The Gibbs free energies at 298.15 K for all the reaction steps were reported. Those at any temperature can be developed with classical thermodynamics by using the fitted (as a function of temperature) heat capacities. It was found that the most favorable paths are mainly in the radical attacking chain reactions. The chain was proposed with 26 reaction steps including two steps of the initialization of the chain to produce H and CH(3) radicals. For a typical temperature (1200 K) adopted in the experiments, the highest energy barriers were found in the production of C(3) to be 203.4 and 193.7 kJ/mol. The highest energy barriers for the production of C(2) and C were found 174.1 and 181.4 kJ/mol, respectively. These results are comparable with the most recent experimental observation of the apparent activation energy 201.9 +/- 0.6 or 137 +/- 25 kJ/mol.

18.
ACS Appl Mater Interfaces ; 12(36): 40433-40442, 2020 Sep 09.
Artículo en Inglés | MEDLINE | ID: mdl-32812729

RESUMEN

Carbon nitride has drawn widespread attention as a low-cost alternative to metal-based materials in the field of photocatalysis. However, the traditionally synthesized carbon nitrides always suffer a bulky architecture, which limits their intrinsic activities. Here, a cycloaddition reaction is proposed to synthesize a triazine-based precursor with implanted sodium and cyano groups, which are mostly retained in the resulting carbon nitride after the following polymerization. Incorporated sodium and cyano defects can not only tune the band structure of the carbon nitride but also provide more additive active sites. The optimized properties enable it an adorable photocatalytic hydrogen evolution rate of 1070 µmol h-1 g-1, varying by almost an order of magnitude from the pristine carbon nitride (79 µmol h-1 g-1). Moreover, a sequential self-assembly strategy has been adopted to further improve its architecture. As a consequence, a three-dimensional (3D) porous carbon nitride microtube cluster is constructed, indicating abundant exposed active sites and the faster separation of charge carriers. The corresponding photocatalytic hydrogen evolution rate is 1681 µmol h-1 g-1, which is very competitive compared with the reported pure carbon nitride photocatalysts. Briefly, this new approach may offer opportunities to fabricate task-specific carbon- and nitrogen-based materials from the molecular level.

19.
ACS Appl Mater Interfaces ; 11(10): 10198-10207, 2019 Mar 13.
Artículo en Inglés | MEDLINE | ID: mdl-30689343

RESUMEN

Lightweight absorption-dominated electromagnetic interference (EMI) shielding materials are more attractive than conventional reflection-dominated counterparts because they minimize the twice pollution of the reflected electromagnetic (EM) wave. Here, porous Ti2CT x MXene/poly(vinyl alcohol) composite foams constructed by few-layered Ti2CT x (f-Ti2CT x) MXene and poly(vinyl alcohol) (PVA) are fabricated via a facile freeze-drying method. As superior EMI shielding materials, their calculated specific shielding effectiveness reaches up to 5136 dB cm2 g-1 with an ultralow filler content of only 0.15 vol % and reflection effectiveness (SER) of less than 2 dB, representing the excellent absorption-dominated shielding performance. Contrast experiment reveals that the good impedance matching derived from the multiple porous structures, internal reflection, and polarization effect (dipole and interfacial polarization) plays a synergistic role in the improved absorption efficiency and superior EMI shielding performance. Consequently, this work provides a promising MXene-based EMI shielding candidate with lightweight and high strength features.

20.
ACS Appl Mater Interfaces ; 11(5): 5364-5372, 2019 Feb 06.
Artículo en Inglés | MEDLINE | ID: mdl-30624042

RESUMEN

The fabrication of a sandwich-like composite that consists of reduced graphene oxide (RGO) and Si3N4 ceramic (RGO/Si3N4) was achieved through the combination of modified freeze-drying approach and chemical vapor infiltration process. Due to a hierarchical structure and a high ratio of ID/ IG (1.27), the RGO/Si3N4 exhibits an unprecedented high polarization relaxation loss (PRL), which accounts for 32% of the whole dielectric loss. The outstanding PRL endows the RGO/Si3N4 composites with unique temperature-independent dielectric properties and electromagnetic (EM) wave absorption performance. Even at a low absorbent content of only 0.16 wt %, the effective absorption bandwidth of RGO/Si3N4 composites can cover the whole X-band (8.2-12.4 GHz) at broad sample thicknesses ranging from 4.3 to 4.6 mm and temperatures ranging from 323 to 873 K. The mechanism for the enhancement of PRL and conductive loss was explicitly investigated. The outstanding absorption performance toward EM waves indicated that the resultant porous RGO/Si3N4 composite can be a promising candidate for the applications under elevated temperature.

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