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  1. Free, publicly-accessible full text available January 11, 2025
  2. Abstract

    Stimuli-responsive elastic metamaterials augment unique subwavelength features and wave manipulation capabilities with a degree of tunability, which enables them to cut across different time scales and frequency regimes. Here, we present an experimental framework for robust local resonance bandgap control enabled by enhanced magneto-mechanical coupling properties of a magnetorheological elastomer, serving as the resonating stiffness of a metamaterial cell. During the curing process, ferromagnetic particles in the elastomeric matrix are aligned under the effect of an external magnetic field. As a result, particle chains with preferred orientation form along the field direction. The resulting anisotropic behavior significantly boosts the sensitivity of the metamaterial’s elastic modulus to the imposed field during operation, which is then exploited to control the dispersive dynamics and experimentally shift the location and width of the resonance-based bandgap along the frequency axis. Finally, numerical simulations are used to project the performance of the magnetically-tunable metamaterial at stronger magnetic fields and increased levels of material anisotropy, as a blueprint for broader implementations of in situ tunable active metamaterials.

     
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  3. Achieving a mesoporous structure in superinsulation materials is pivotal for guaranteeing a harmonious relationship between low thermal conductivity, high porosity, and low density. Herein, we report silica-based cryogel and aerogel materials by implementing freeze-drying and ambient-pressure-drying processes respectively. The obtained freeze-dried cryogels yield thermal conductivity of 23 mW m −1 K −1 , with specific surface area of 369.4 m 2 g −1 , and porosity of 96.7%, whereas ambient-pressure-dried aerogels exhibit thermal conductivity of 23.6 mW m −1 K −1 , specific surface area of 473.8 m 2 g −1 , and porosity of 97.4%. In addition, the fiber-reinforced nanocomposites obtained via freeze-drying feature a low thermal conductivity (28.0 mW m −1 K −1 ) and high mechanical properties (∼620 kPa maximum compressive stress and Young's modulus of 715 kPa), coupled with advanced flame-retardant capabilities, while the composite materials from the ambient pressure drying process have thermal conductivity of 28.8 mW m −1 K −1 , ∼200 kPa maximum compressive stress and Young's modulus of 612 kPa respectively. The aforementioned results highlight the capabilities of both drying processes for the development of thermal insulation materials for energy-efficient applications. 
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  4. Abstract

    2D molecular entities build next-generation electronic devices, where abundant elements of organic molecules are attractive due to the modern synthetic and stimuli control through chemical, conformational, and electronic modifications in electronics. Despite its promising potential, the insufficient control over charge states and electronic stabilities must be overcome in molecular electronic devices. Here, we show the reversible switching of modulated charge states in an exfoliatable 2D-layered molecular conductor based on bis(ethylenedithio)tetrathiafulvalene molecular dimers. The multiple stimuli application of cooling rate, current, voltage, and laser irradiation in a concurrent manner facilitates the controllable manipulation of charge crystal, glass, liquid, and metal phases. The four orders of magnitude switching of electric resistance are triggered by stimuli-responsive charge distribution among molecular dimers. The tunable charge transport in 2D molecular conductors reveals the kinetic process of charge configurations under stimuli, promising to add electric functions in molecular circuitry.

     
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  5. Abstract The macro-porous ceramics has promising durability and thermal insulation performance. As porous ceramics find more and more applications across many industries, a cost-effective and scalable additive manufacturing technique for fabricating macro-porous ceramics is highly desirable. Herein, we reported a facile additive manufacturing approach to fabricate porous ceramics and control the printed porosity. Several printable ceramic inks were prepared, and the foaming agent was added to generate gaseous bubbles in the ink, followed by the direct ink writing and the ambient-pressure and room-temperature drying to create the three-dimensional geometries. A set of experimental studies were performed to optimize the printing quality. The results revealed the optimal process parameters for printing the foamed ceramic ink with a high spatial resolution and fine surface quality. Varying the concentration of the foaming agent enables the controllability of the structural porosity. The maximum porosity can reach 85%, with a crack-free internal porous structure. The tensile tests showed that the printed macro-porous ceramics possessed enhanced durability with the addition of fiber. With a high-fidelity three-dimensional (3D) printing process and the precise controllability of the porosity, we showed that the printed samples exhibited a remarkably low thermal conductivity and durable mechanical strength. 
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  6. Abstract

    Tailoring thermal transport by structural parameters could result in mechanically fragile and brittle networks. An indispensable goal is to design hierarchical architecture materials that combine thermal and mechanical properties in a continuous and cohesive network. A promising strategy to create such a hierarchical network targets additive manufacturing of hybrid porous voxels at nanoscale. Here we describe the convergence of agile additive manufacturing of porous hybrid voxels to tailor hierarchically and mechanically tunable objects. In one strategy, the uniformly distributed porous silica voxels, which form the basis for the control of thermal transport, are non-covalently interfaced with polymeric networks, yielding hierarchic super-elastic architectures with thermal insulation properties. Another additive strategy for achieving mechanical strength involves the versatile orthogonal surface hybridization of porous silica voxels retains its low thermal conductivity of 19.1 mW m−1 K−1, flexible compressive recovery strain (85%), and tailored mechanical strength from 71.6 kPa to 1.5 MPa. The printed lightweight high-fidelity objects promise thermal aging mitigation for lithium-ion batteries, providing a thermal management pathway using 3D printed silica objects.

     
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  7. Abstract

    Chemical energy ferroelectrics are generally solid macromolecules showing spontaneous polarization and chemical bonding energy. These materials still suffer drawbacks, including the limited control of energy release rate, and thermal decomposition energy well below total chemical energy. To overcome these drawbacks, we report the integrated molecular ferroelectric and energetic material from machine learning-directed additive manufacturing coupled with the ice-templating assembly. The resultant aligned porous architecture shows a low density of 0.35 g cm−3, polarization-controlled energy release, and an anisotropic thermal conductivity ratio of 15. Thermal analysis suggests that the chlorine radicals react with macromolecules enabling a large exothermic enthalpy of reaction (6180 kJ kg−1). In addition, the estimated detonation velocity of molecular ferroelectrics can be tuned from 6.69 ± 0.21 to 7.79 ± 0.25 km s−1by switching the polarization state. These results provide a pathway toward spatially programmed energetic ferroelectrics for controlled energy release rates.

     
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  8. Abstract

    The macro-porous ceramics has promising durability and thermal insulation performances. A cost-effective and scalable additive manufacturing technique for the fabrication of macro-porous ceramics, with a facile approach to control the printed porosity is reported in the paper. Several ceramic inks were prepared, the foaming agent was used to generate gaseous bubbles in the ink, followed by the direct ink writing and the ambient-pressure and room-temperature drying to create the three-dimensional geometries. The experimental studies were performed to optimize the printing quality. A set of studies revealed the optimal printing process parameters for printing the foamed ceramic ink with a high spatial resolution and fine surface quality. Varying the concentration of the foaming agent enabled the controllability of the structural porosity. The maximum porosity can reach 85%, with a crack-free internal porous structure. The tensile tests showed that the printed macro-porous ceramics have enhanced durability with the addition of fiber. With a high-fidelity 3D printing process and precise control of the porosity, the printed samples exhibited a low thermal conductivity and high mechanical strength.

     
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