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Abstract We demonstrate shear‐printed layered photonic films with vivid structural coloration from bio‐derived cellulose nanocrystals and highly aligned Ti₃C₂T_xMXene nanoflakes. These ultrathin films (700–1500 nm) show high light transmittance above 40% in the visible range. In reflectance mode, however, the films appear vividly colored and iridescent due to the multiple distinct photonic bandgaps in the visible and near‐infrared ranges, which are rarely observed in CNC composites. The structural coloration is controlled by the stacking of MXene nanoscale‐thin layers separated by the thicker cellulose nanocrystals matrix, as confirmed by photonic simulations. The unique combination of distinctly different optical appearances in transmittance and reflectance modes occurs in films printed with just a few layers. This is because of the molecularly smooth interfaces and the high refractive contrast between bio‐based and inorganic phases, which result in a concurrence of constructive and destructive interference. These lamellar biophotonic films open the possibilities for advanced radiative cooling, camouflaging, multifunctional capacitors, and optical filtration applications, while the cellulose nanocrystals matrix strengthens their flexibility, robustness, and facilitates sustainability. 

The structural integrity of MXene and MXene-based materials is important across applications from sensors to energy storage. While MXene processing has received significant attention, its structural integrity for real-world applications remains challenging due to its flake-like structure. Here the mechanical response of layered MXene-polymer nanocomposites (MPC) with high MXene concentration (>70 %) and bioinspired nacre-like brick-and-mortar architecture is investigated to offer insights for MPC design and processing. An automated finite element analysis (FEA) framework is developed to analyze MPC models with randomized geometries and multiple combinations of the parameter space. Specifically, the influence of concentration, aspect ratio (AR), flake thickness, flake distribution, and interfacial strength is investigated. The results reveal property trends such as increasing elastic modulus, strength, and toughness with increasing cohesive strength and concentration for lower AR (=40, 60) but a decreasing trend at higher AR of 75. Local structural features like flake distribution, overlapping MXene lengths, and interconnected polymers in adjacent layers was found a critical determinant of performance. For example, stronger cohesive interaction showed 6X high toughness (291 226 ) compared to weaker case (50 24 ), but the large scatter highlighted the impact of microstructural features. The results are compared and validated with theoretical, computational, and experimental work. The findings provide valuable guidance for optimizing MPC design and their processing. Finally, the automation of the framework allows the design to be extended beyond the current system and chosen material combinations. 

Stacking atomically thin two-dimensional (2D) nanosheet materials leads to unique synergy in their inherent properties due to an intimate combination and matching that is not possible via separate individual components and phases. However, traditional synthesis and assembly methods result in poor architectural control and restricted surface chemistry, thereby limiting their prospective potentials. This brief overview provides consideration of different synthesis and assembly methods for fabrication of diverse novel heterostructures. The advantages and challenges of existing methods are discussed. Finally, future perspectives regarding crafting of heterostructures with highly controllable architectures and interfacial/surface chemistry, and advanced characterization methods are highlighted. 

Abstract An innovative process to multifunctional vitrimer nanocomposites with a percolative MXene minor phase is reported, marking a significant advancement in creating stimuli‐repairable, reinforced, sustainable, and conductive nanocomposites at diminished loadings. This achievement arises from a Voronoi‐inspired biphasic morphological design via a straight‐forward three‐step process involving ambient‐condition precipitation polymerization of micron‐sized prepolymer powders, aqueous powder‐coating with 2D MXene (Ti₃C₂T_z), and melt‐pressing of MXene‐coated powders into crosslinked films. Due to the formation of MXene‐rich boundaries between thiourethane vitrimer domains in a pervasive low‐volume fraction conductive network, a low percolation threshold (≈0.19 vol.%) and conductive polymeric nanocomposites (≈350 S m⁻¹) are achieved. The embedded MXene skeleton mechanically bolsters the vitrimer at intermediate loadings, enhancing the modulus and toughness by 300% and 50%, respectively, without mechanical detriment compared to the neat vitrimer. The vitrimer's dynamic‐covalent bonds and MXene's photo‐thermal conversion properties enable repair in minutes through short‐term thermal treatments for full macroscopic mechanical restoration or in seconds under 785 nm light for rapid localized surface repair. This versatile fabrication method to nanocoated pre‐vitrimer powders and morphologically complex nanocomposites is compatible with classic composite manufacturing, and when coupled with the material's exceptional properties, holds immense potential for revolutionizing advanced composites and inspiring next‐generation smart materials.