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Abstract: Cellulose-based nanomaterials are fascinating renewable biosystems, yet low thermal conductivity and dielectric permittivity often limit their potential applications in flexible electronics. We report dielectric properties of composite films prepared by vacuum filtration or solvent casting method from the native (CNF) or carboxylated (TCNF) cellulose nanofibrils and high electrically and thermally conductive 2D titanium carbide (Ti3C2Tx) MXenes. Measurements over broad frequency and temperature ranges revealed the influence of preparation method and type of nanofibrils matrix on the overall dielectric response, as well as a notable impact of absorbed water, particularly on the cellulose’s secondary β and γ relaxations. A detailed investigation of material with the lowest amount of impurities, vacuum-filtered MXene/CNF composites, confirmed that the dielectric response follows the predictions of the percolation theory. The resulting strong enhancement of the dielectric permittivity on increasing MXene content demonstrates the potential of developed composites for applications in eco-friendly dielectric and piezoelectric devices.
Keywords: percolation theory, piezoelectric devices, dielectric properties, nanomaterials, carbides, biological systems, biological models, carbohydrates
Published in DKUM: 08.09.2025; Views: 0; Downloads: 3
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Abstract: In this work, we developed a numerical approach based on an experimental platform to determine the working conditions on a cryoplatform and to predict and evaluate the cryogenic printing of hydrogels. Although hydrogels have good biocompatibility, their material properties make it difficult to print them with high precision and shape fidelity. To overcome these problems, a cryogenic cooling platform was introduced to accelerate the physical stabilisation of each deposited layer during the printing process. By precisely controlling solidification (crystallisation), each printed material can withstand its own weight to maintain shape fidelity, and the porosity of the scaffolds can also be controlled more selectively. The thermophysical properties of gelatine hydrogels were investigated to gain a better understanding of the phase change upon freezing. The corresponding material properties and experimental observations of gelatine solidification served as the basis for developing a computational fluid model (CFD) to mimic the solidification of gelatine hydrogels using a cryoplatform at different process conditions and extruder speeds. The goal was to develop a tool simple enough to predict acceptable process conditions for printing gelatine hydrogels using a cryoplatform.
Keywords: gelatine, hydrogel, cryoprinting, CFD simulation, solidification modelling
Published in DKUM: 20.03.2025; Views: 0; Downloads: 12
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Abstract: The fabrication of biomaterials to be used in segmental bone defects, mimicking the bone's organic-inorganic architecture and mechanical properties to induce osteogenesis, persists as a key challenge. The purpose of this study was to elucidate the effect of a lightweight, morphologically graded, and multiphase self-standing scaffold structure prepared from a combination of gelatine (Gel), collagen type 1 (Col) and/or hydroxyapatite (HAP) nanoparticles by a unidirectional freeze-casting process at different temperatures (−20, −40, −60 °C), followed by carbodiimide induced cross-linking, on their in-vitro mechanical stability and bioactive properties. In addition, the rheological study of differently formulated Gel solutions has been performed to determine the effect of Col and HAP content on their microstructural arrangement, which, together with the freezing kinetic, affects Gel/Col orientation and cross-linking, and, thus, the scaffold's mechanical strength and stability. A bone-like anisotropic, interconnected, and graded porosity (from 120 to a few μm) scaffold structure with up to 30% total porosity and ~61 μm average pores' diameter is obtained by using a higher Col content (Col: Gel = 2:5) and freezing temperature (−20 °C) while forming a few μm thick close-to-parallel lamellae, separated with a 10–100 μm space when prepared at −60 °C. Such a structure influenced in-vitro stability strongly (lower swelling without weight loss), being accompanied with a ~76% increase of compression strength (to 37 kPa) and ~67% decrease of elastic modulus (to 17 kPa) when prepared with HAP and incubated in HBSS for 7 days. On the other hand, a significant reduction of both strength (~78%, to 15 kPa) and elasticity (~95%, to 5 kPa) was noted for a scaffold prepared with HAP at −60 °C, being related to faster degradation and the formation of a highly opened structure on the bottom, required to stimulate the bone ingrowth, while a more closed network structure on the top to adhere with the surrounding soft tissue. None of the scaffolds induced cytotoxicity to human bone-derived osteoblasts, even after 19 days of incubation, but rather improved their viability while promoting cells' adhesions, proliferation, and differentiation, being supported with an increased alkaline phosphatase activity and rod-like CaP formation.
Keywords: biomimetic scaffolds, rheology, unidirectional freeze-casting, morphology, compression properties, bioactivity
Published in DKUM: 10.03.2025; Views: 0; Downloads: 12
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Abstract: The fabrication of nanocellulose-based substrates with high dielectric permittivity and anisotropic thermal conductivity to replace synthetic thermoplastics in flexible organic electronics remains a big challenge. Herein, films were prepared from native (CNF) and carboxylated (TCNF) cellulose nanofibrils, with and without the addition of thermally conductive multi-layered Ti3C2Tx MXene, to examine the impact of polar (− OH, − COOH) surface groups on the film morphological, moisturizing, dielectric, and thermal dissipation properties. The electrostatic repulsion and hydrogen bonding interaction between the hydrophilic surface/terminal groups on CNF/TCNF and MXene was shown to render their self-assembly distribution and organization into morphologically differently structured films, and, consequently, different properties. The pristine CNF film achieved high intrinsic dielectric permittivity (ε' ~ 9), which was further increased to almost ε' ~ 14 by increasing (50 wt%) the MXene content. The well-packed and aligned structure of thinner TCNF films enables the tuning of both the composite’s dielectric permittivity (ε' ~ 6) and through-plane thermal conductivity (K ~ 2.9 W/mK), which increased strongly (ε' ~ 17) at higher MXene loading giving in-plane thermal conductivity of ~ 6.3 W/mK. The air-absorbed moisture ability of the films contributes to heat dissipation by releasing it. The dielectric losses remained below 0.1 in all the composite films, showing their potential for application in electronics.
Keywords: nanofibrillated cellulose, Ti3C2T, Mxene, film preparation, moisture content, thermal conductivity
Published in DKUM: 03.09.2024; Views: 36; Downloads: 18
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Abstract: Cellulose nanocrystals (CNCs) and chitosan (Cht) have been studied extensively for oxygen and water vapour barrier coatings in biodegradable, compostable or recyclable paper packaging. However, rare studies have been performed by using scalable, inexpensive, and fast continuous slot-die coating processes, and none yet in combination with fast' and high-throughput near-infrared (NIR) light energy drying. In this frame, we studied the feasibility of a moderately concentrated (11 wt%) anionic CNC and (2 wt%) cationic Cht coating (both containing 20 wt% sorbitol related to the weight of CNC/Cht), by using plain and pigment pre-treated papers. The effect of coating parameters (injection speed, dry thickness settings) were investigated on coating quantity (dry weight, thickness) and homogeneity (coverage), papers' structure (thickness, grammage, density), whiteness, surface wettability, barrier (air, oxygen and water vapour) properties and adhesion (surface strength). The coating homogeneity was dependent primarily on the suspensions' viscosity, and secondarily on the applied coating parameters, whereby CNCs could be applied at 1–2 times higher injection speeds (up to 80 mL/min) and versatile coating weights, but required a relatively longer time to dry. The CNCs thus exhibited outstanding air (4.2–1.5 nm/Pa s) and oxygen (2.7–1.1 cm3 mm/m2 d kPa) barrier performance at 50% RH and 22–33 g/m2 deposition, whereas on top deposited Cht (3–4 g/m2) reduced its wetting time and improved the water vapour barrier (0.23–0.28 g mm/m2 d Pa). The balanced barrier properties were achieved due to the polar characteristic of CNCs, the hydrophobic nature of Cht and the quantity of the applied bilayer coating that can provide sustainable paper-based packaging.
Keywords: paper, nanocellulose, chitosan, slot‑die coating, near-infrared (NIR) drying, barrier properties
Published in DKUM: 06.05.2024; Views: 227; Downloads: 25
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