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Abstract In this work, a systematic investigation is conducted on stress‐assisted erosion of the photocurable and degradable elastomer poly(glycerol sebacate) acrylate (PGSA). Without external stress, it is confirmed that the elastomer undergoes surface erosion in an aqueous environment. Upon the application of mechanical stress, the results revealed that the surface erosion rate is dramatically accelerated. By studying the stress corrosion cracking (SCC) phenomena, it is demonstrated that the crack growth speed depends on the applied load and is significantly faster than the surface erosion rate of the elastomer. It is further shown that with decreasing the cross‐link density of the elastomer, the crack growth speed during SCC can be slowed down due to the increased viscoelasticity of the material.more » « less
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Abstract Radiative cooling has been recently intensively explored for thermal management and enhancing energy efficiency. Yet, traditional materials with singular emissivity fall short in dynamic thermal management, highlighting the need for materials that can adjust their thermal radiation in real time. Active modulation methods, requiring external stimuli such as mechanical stretch, electric potential, or humidity change, offer adaptability but can increase energy use and complexity. Passive approaches, using materials' inherent thermal‐responsive properties, face manufacturing and scalability challenges. Here, a scalable yet effective passive approach is introduced for adaptive thermal modulation based on gold (Au) and liquid crystal elastomer (LCE) with a reversible response to environmental temperature changes. This modulator enables a “low thermal resistance” state through actuation‐induced microcracks that expose a high‐emissivity polymer substrate, and a “high thermal resistance” state by closing these microcracks and forming a high thermal resistance air gap between the modulator and the target object. The flexible design and fixed external dimensions of the Au‐LCE thermal modulator make it adaptable to various surface geometries. Furthermore, by adjusting the LCE's chemical composition, the modulator's transition temperature can be tailored, broadening its applications from enhancing building energy efficiency to improving clothing thermal comfort.more » « less
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null (Ed.)We investigate the rate-dependent fracture of vitrimers by conducting a tear test. Based on the relationship between the fracture energy and the thickness of vitrimer films, we, for the first time, obtain the intrinsic fracture energy and bulk dissipation of vitrimers during crack extension. The intrinsic fracture energy strongly depends on tear speed, and such dependence can be well explained by Eyring theory. In contrast, the bulk dissipation only weakly depends on tear speed, which is drastically different from observations on traditional viscoelastic polymers. We ascribe such a weak rate-dependence to the strong force-sensitivity of the exchange reaction of the dynamic covalent bond in the vitrimer.more » « less
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We have discovered a peculiar form of fracture that occurs in polymer network formed by covalent adaptable bonds. Due to the dynamic feature of the bonds, fracture of this network is rate dependent, and the crack propagates in a highly nonsteady manner. These phenomena cannot be explained by the existing fracture theories, most of which are based on steady-state assumption. To explain these peculiar characteristics, we first revisit the fundamental difference between the transient network and the covalent network in which we highlighted the transient feature of the cracks. We extend the current fracture criterion for crack initiation to a time-evolution scheme that allows one to track the nonsteady propagation of a crack. Through a combined experimental modeling effort, we show that fracture in transient networks is governed by two parameters: the Weissenberg number that defines the history path of crack-driving force and an extension parameter Z that tells how far a crack can grow. We further use our understanding to explain the peculiar experimental observation. To further leverage on this understanding, we show that one can “program” a specimen’s crack extension dynamics by tuning the loading history.more » « less
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Abstract The realization of low thermal conductivity at high temperatures (0.11 W m−1K−1800 °C) in ambient air in a porous solid thermal insulation material, using stable packed nanoparticles of high‐entropy spinel oxide with 8 cations (HESO‐8 NPs) with a relatively high packing density of ≈50%, is reported. The high‐density HESO‐8 NP pellets possess around 1000‐fold lower thermal diffusivity than that of air, resulting in much slower heat propagation when subjected to a transient heat flux. The low thermal conductivity and diffusivity are realized by suppressing all three modes of heat transfer, namely solid conduction, gas conduction, and thermal radiation, via stable nanoconstriction and infrared‐absorbing nature of the HESO‐8 NPs, which are enabled by remarkable microstructural stability against coarsening at high temperatures due to the high entropy. This work can elucidate the design of the next‐generation high‐temperature thermal insulation materials using high‐entropy ceramic nanostructures.more » « less
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Abstract The fabrication of pressure sensitive adhesives (PSAs) using liquid crystal elastomers (LCEs), which are known for their excellent dissipation properties, is explored in this work. The adhesive properties of the PSAs are evaluated using the 180° peeling test at various conditions. The performance of the LCE adhesives is found to show significant rate and temperature dependence. When the adhesion energy is plotted against the rate, LCE shows an anomalously large power law exponent (n≈ 1.17) compared to existing PSAs (n≈ 0.1–0.6). The unusual rate sensitivity is hypothesized to originate from the synergy of soft elasticity and non‐linear viscoelasticity. The adhesive properties at various rates and temperatures are correlated to the results from dynamic mechanical analysis. Moreover, the large strain stiffening behavior of LCE under uniaxial tension reveals the distinctive advantages offered by LCE as adhesives. Time‐temperature superposition is used to obtain a master curve of adhesion energy that spans rates beyond typical experimental limits. The extreme rate dependence and the large strain stiffening of LCE yield a new category of adhesives that possess special properties, such as reversible adhesion and impact resistance, unlike traditional adhesives.more » « less