Ultrathin, lightweight, and flexible electromagnetic-interference (EMI) shielding materials are urgently required to manage increasingly serious radiation pollution. 2D transition-metal carbides (MXenes) are considered promising alternatives to graphene for providing excellent EMI-shielding performance due to their outstanding metallic electrical conductivity. However, the hydrophilicity of MXene films may affect their stability and reliability when applied in moist or wet environments. Herein, for the first time, an efficient and facile approach is reported to fabricate freestanding, flexible, and hydrophobic MXene foam with reasonable strength by assembling MXene sheets into films followed by a hydrazine-induced foaming process. In striking contrast to well-known hydrophilic MXene materials, the MXene foams surprisingly exhibit hydrophobic surfaces and outstanding water resistance and durability. More interestingly, a much enhanced EMI-shielding effectiveness of ≈70 dB is achieved for the lightweight MXene foam as compared to its unfoamed film counterpart (53 dB) due to the highly efficient wave attenuation in the favorable porous structure. Therefore, the hydrophobic, flexible, and lightweight MXene foam with an excellent EMI-shielding performance is highly promising for applications in aerospace and portable and wearable smart electronics.
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Thermally removable nanoparticle templates were used for the fabrication of self-supported N-doped mesoporous carbons with a trace amount of Fe (Fe-N/C). Experimentally Fe-N/C was prepared by pyrolysis of poly(2-fluoroaniline) (P2FANI) containing a number of FeO(OH) nanorods that were prepared by a one-pot hydrothermal synthesis and homogeneously distributed within the polymer matrix. The FeO(OH) nanocrystals acted as rigid templates to prevent the collapse of P2FANI during the carbonization process, where a mesoporous skeleton was formed with a medium surface area of about 400 m(2)/g. Subsequent thermal treatments at elevated temperatures led to the decomposition and evaporation of the FeO(OH) nanocrystals and the formation of mesoporous carbons with the surface area markedly enhanced to 934.8 m(2)/g. Electrochemical measurements revealed that the resulting mesoporous carbons exhibited apparent electrocatalytic activity for oxygen reduction reactions (ORR), and the one prepared at 800 °C (Fe-N/C-800) was the best among the series, with a more positive onset potential (+0.98 V vs RHE), higher diffusion-limited current, higher selectivity (number of electron transfer n > 3.95 at +0.75 V vs RHE), much higher stability, and stronger tolerance against methanol crossover than commercial Pt/C catalysts in a 0.1 M KOH solution. The remarkable ORR performance was attributed to the high surface area and sufficient exposure of electrocatalytically active sites that arose primarily from N-doped carbons with minor contributions from Fe-containing species.
Highly conductive polymer nanocomposites are greatly desired for electro magnetic interference (EMI) shielding applications. Although transition metal carbide/carbonitride (MXene) has shown its huge potential for producing highly conductive films and bulk materials, it still remains a great challenge to fabricate extremely conductive polymer nanocomposites with outstanding EMI shielding performance at minimal amounts of MXenes. Herein, an electrostatic assembly approach for fabricating highly conductive MXene@ polystyrene nanocomposites by electrostatic assembling of negative MXene nanosheets on positive polystyrene microspheres is demonstrated, fol lowed by compression molding. Thanks to the high conductivity of MXenes and their highly efficient conducting network within polystyrene matrix, the resultant nanocomposites exhibit not only a low percolation threshold of 0.26 vol% but also a superb conductivity of 1081 S m −1 and an outstanding EMI shielding performance of >54 dB over the whole Xband with a max imum of 62 dB at the low MXene loading of 1.90 vol%, which are among the best performances for electrically conductive polymer nanocomposites by far. Moreover, the same nanocomposite has a highly enhanced storage modulus, 54% and 56% higher than those of neat polystyrene and conven tional MXene@polystyrene nanocomposite, respectively. This work provides a novel methodology to produce highly conductive polymer nanocomposites for highly efficient EMI shielding applications.
2D transition metal carbides and nitrides (MXenes) have gained extensive attention recently due to their versatile surface chemistry, layered structure, and intriguing properties. The assembly of MXene sheets into macroscopic architectures is an important approach to harness their extraordinary properties. However, it is difficult to construct a freestanding, mechanically flexible, and 3D framework of MXene sheets owing to their weak intersheet interactions. Herein, an interfacial enhancement strategy to construct multifunctional, superelastic, and lightweight 3D MXene architectures by bridging individual MXene sheets with polyimide macromolecules is developed. The resulting lightweight aerogel exhibits superelasticity with large reversible compressibility, excellent fatigue resistance (1000 cycles at 50% strain), 20% reversible stretchability, and high electrical conductivity of ≈4.0 S m−1. The outstanding mechanical flexibility and electrical conductivity make the aerogel promising for damping, microwave absorption coating, and flexible strain sensor. More interestingly, an exceptional microwave absorption performance with a maximum reflection loss of −45.4 dB at 9.59 GHz and a wide effective absorption bandwidth of 5.1 GHz are achieved.
The adhesion of soft connective tissues (tendons, ligaments, and cartilages) on bones in many animals can maintain high toughness (∽800 J m−2) over millions of cycles of mechanical loads. Such fatigue-resistant adhesion has not been achieved between synthetic hydrogels and engineering materials, but is highly desirable for diverse applications such as artificial cartilages and tendons, robust antifouling coatings, and hydrogel robots. Inspired by the nanostructured interfaces between tendons/ligaments/cartilages and bones, we report that bonding ordered nanocrystalline domains of synthetic hydrogels on engineering materials can give a fatigue-resistant adhesion with an interfacial fatigue threshold of 800 J m−2, because the fatigue-crack propagation at the interface requires a higher energy to fracture the ordered nanostructures than amorphous polymer chains. Our method enables fatigue-resistant hydrogel coatings on diverse engineering materials with complex geometries. We further demonstrate that the fatigue-resistant hydrogel coatings exhibit low friction and low wear against natural cartilages.
During the critical period, neuronal connections are shaped by sensory experience. While the basis for this temporarily heightened plasticity remains unclear, shared connections introducing activity correlations likely play a key role. Thus, we investigated the changing intracortical connectivity in primary auditory cortex (A1) over development. In adult, layer 2/3 (L2/3) neurons receive ascending inputs from layer 4 (L4) and also receive few inputs from subgranular layer 5/6 (L5/6). We measured the spatial pattern of intracortical excitatory and inhibitory connections to L2/3 neurons in slices of mouse A1 across development using laser-scanning photostimulation. Before P11, L2/3 cells receive most excitatory input from within L2/3. Excitatory inputs from L2/3 and L4 increase after P5 and peak during P9–16. L5/6 inputs increase after P5 and provide most input during P12–16, the peak of the critical period. Inhibitory inputs followed a similar pattern. Functional circuit diversity in L2/3 emerges after P16. In vivo two-photon imaging shows low pairwise signal correlations in neighboring neurons before P11, which peak at P15–16 and decline after. Our results suggest that the critical period is characterized by high pairwise activity correlations and that transient hyperconnectivity of specific circuits, in particular those originating in L5/6, might play a key role.
Biocatalytic anti-Markovnikov alkene hydroamination and hydration were achieved based on two concepts involving enzyme cascades: epoxidation–isomerization–amination for hydroamination and epoxidation–isomerization–reduction for hydration. An Escherichia coli strain coexpressing styrene monooxygenase (SMO), styrene oxide isomerase (SOI), ω-transaminase (CvTA), and alanine dehydrogenase (AlaDH) catalyzed the hydroamination of 12 aryl alkenes to give the corresponding valuable terminal amines in high conversion (many ≥86%) and exclusive anti-Markovnikov selectivity (>99:1). Another E. coli strain coexpressing SMO, SOI, and phenylacetaldehyde reductase (PAR) catalyzed the hydration of 12 aryl alkenes to the corresponding useful terminal alcohols in high conversion (many ≥80%) and very high anti-Markovnikov selectivity (>99:1). Importantly, SOI was discovered for stereoselective isomerization of a chiral epoxide to a chiral aldehyde, providing some insights on enzymatic epoxide rearrangement. Harnessing this stereoselective rearrangement, highly enantioselective anti-Markovnikov hydroamination and hydration were demonstrated to convert α-methylstyrene to the corresponding (S)-amine and (S)-alcohol in 84–81% conversion with 97–92% ee, respectively. The biocatalytic anti-Markovnikov hydroamination and hydration of alkenes, utilizing cheap and nontoxic chemicals (O2, NH3, and glucose) and cells, provide an environmentally friendly, highly selective, and high-yielding synthesis of terminal amines and alcohols.
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