Access to 2,4-Disubstituted Pyrrole-Based Polymer with Long-Wavelength and Stimuli-Responsive Properties via Copper-Catalyzed [3+2] Polycycloaddition.

Pyrrole-based polymers (PBPs), a type of fascinating functional polymers, play a crucial role in materials science. However, efficient synthetic strategies of PBPs with diverse structures are mainly focused on conjugated polypyrroles and still remain challenging. Herein, an atom and step economy protocol is described to access various 2,4-disubstituted PBPs by in situ formation of pyrrole core structure via copper-catalyzed [3+2] polycycloaddition of dialkynones and diisocyanoacetates. A series of PBPs is prepared with high molecular weight (Mw up to 18 200 Da) and moderate to good yield (up to 87%), which possesses a fluorescent emission located in the green to yellow light region. Blending the PBPs with polyvinyl alcohol, the stretchable composite films exhibit a significant strengthening of the mechanical properties (tensile stress up to 59 MPa, elongation at break >400%) and an unprecedented stress-responsive luminescence enhancement that over fourfold fluorescent emission intensity is maintained upon stretching up to 100%. On the basis of computational studies, the unique photophysical and mechanical properties are attributed to the substitution of carbonyl chromophores on the pyrrole unit.

Revealing Surface/Interface Chemistry of the Ordered Aramid Nanofiber/MXene Structure for Infrared Thermal Camouflage and Electromagnetic Interference Shielding.

The past decade has witnessed the advances of infrared (IR) thermal camouflage materials, but challenges remain in breaking the trade-off nature between emissivity and mechanical properties. In response, we identify the key role of a moderate reprotonation rate in the aramid nanofiber (ANF)/MXene film toward a surface-to-bulk alignment. Theoretical simulation demonstrates that the ordered ANF/MXene surface eliminates the local high electric field by field confinement and localization, responsible for the low IR emissivity. By scrutinizing the surface/interface chemistry, the processing optimization is achieved to develop an ordered and densely stacked ANF/MXene film, which features a low emissivity of 16%, accounting for sound IR thermal camouflage performances including a wide camouflage temperature range of 50-200 °C, a large reduction in radiation temperature from 200.5 to 63.6 °C, and long-term stability. This design also enables good mechanical performance such as a tensile strength of 190.8 MPa, a toughness of 12.1 MJ m-3, and a modulus of 7.9 GPa, responsible for better thermal camouflage applications. The tailor-made ANF/MXene film further attains an electromagnetic interference (EMI) shielding effectiveness (40.4 dB) in the X-band, manifesting its promise for IR stealth compatible EMI shielding applications. This work will shed light on the dynamic topology reconstruction of camouflage materials for boosting thermal management technology.

A flexible, robust and multifunctional montmorillonite/aramid nanofibers@MXene electromagnetic shielding nanocomposite with an alternating structure for enhanced Joule heating and fire-resistant protective performance.

With the rapidly increasing development of portable devices and flexible electronic devices, multifunctional composites with excellent mechanical strength, great electromagnetic interference shielding, great Joule heating performance and strong fire-resistant protective performance are noticeably required. Herein, inspired by the sandwich structure, we have designed a montmorillonite/aramid nanofibers@MXene (MMT/ANFs@MXene) nanocomposite with an alternating multilayered structure via a simple AVF process. In this nanocomposite, the ANFs/MMT (AT) layer acts as a mechanically reinforced and insulation protection layer, while the MXene layer maintains a complete conductive network. The superior alternating multilayered structure endows the nanocomposite with outstanding mechanical properties (154.66 MPa, 14.22%) and excellent EMI shielding effectiveness values (58.4 dB). In addition, the fire-resistant protective performance of the nanocomposite improves its safety and reliability, especially, the EMI shielding effectiveness is maintained at ∼34 dB after burning for 30 s. Besides, the MMT/ANFs@MXene nanocomposite shows excellent Joule heating performance with a fast thermal response, low driving voltage and long-time temperature stability, which could reach 110.2 °C at only 3 V applied voltage within 10 s. As a result, this work presents a novel strategy for constructing multifunctional composites with outstanding overall performance, which will broaden application areas and prospects in thermal management and EMI shielding in wearable products.

Toward high-performance nanofibrillated cellulose/aramid fibrid paper-based composites via polyethyleneimine-assisted decoration of silica nanoparticle onto aramid fibrid.

Flexible paper-based nanocomposites dielectrics are of crucial importance in electrical insulation and advanced electrical power systems. In this work, a novel nanofibrillated cellulose/aramid fibrid (NFC/AF) composite was fabricated by vacuum-assisted filtration process. In order to improve the dielectric property of the composites, carboxylated nano-SiO2 was chemically coated onto aramid fibrid via molecular self-assembly with the aid of phosphoric acid (PA) pretreatment and subsequent polyethyleneimine (PEI) functionalization. It was found that composites prepared by NFC and (PEI/SiO2)-modified AF (after crosslinking) ((PEI/SiO2)-AF) showed dense structure, which was mainly due to enhanced interfacial interaction between AF and NFC. Consequently, NFC/(PEI/SiO2)-AF paper-based composites showed better tensile toughness (∼6 % elongation at break) and mechanical strength (∼36.28 MPa), in comparison with NFC/AF. More importantly, the electrical insulation performance and thermal stability of the composites were significantly improved. Accordingly, this work provides a facile approach to fabricate high-performance dielectric composites especially for high-temperature electrical insulation applications.