The design of amorphous entangled systems, specifically from soft and active materials, has the potential to open exciting new classes of active, shape-shifting, and task-capable 'smart' materials. However, the global emergent mechanics that arise from the local interactions of individual particles are not well understood. In this study, we examine the emergent properties of amorphous entangled systems in an collection of u-shaped particles ("smarticles") and in living entangled aggregate of worm blobs (). In simulations, we examine how material properties change for a collective composed of smarticles as they undergo different forcing protocols. We compare three methods of controlling entanglement in the collective: external oscillations of the ensemble, sudden shape-changes of all individuals, and sustained internal oscillations of all individuals. We find that large-amplitude changes of the particle's shape using the shape-change procedure produce the largest average number of entanglements, with respect to the aspect ratio (/), thus improving the tensile strength of the collective. We demonstrate applications of these simulations by showing how the individual worm activity in a blob can be controlled through the ambient dissolved oxygen in water, leading to complex emergent properties of the living entangled collective, such as solid-like entanglement and tumbling. Our work reveals principles by which future shape-modulating, potentially soft robotic systems may dynamically alter their material properties, advancing our understanding of living entangled materials, while inspiring new classes of synthetic emergent super-materials.
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http://dx.doi.org/10.1039/d2sm01573k | DOI Listing |
Food Chem
December 2024
Institute of Agro-Product Processing, Jiangsu Academy of Agricultural Sciences, Nanjing 210014, PR China; School of Food and Biological Engineering, Jiangsu University, Zhenjiang, 212013, PR China. Electronic address:
Mung bean hull polyphenols (MBPs) have the potential to retard starch digestion by altering its multi-scale structures. However, the regulatory mechanism and the key structural characteristics that contribute to digestion resistance remain unclear. In this study, MBPs were non-covalently interacted with wheat starch (WS) under hydrothermal treatments.
View Article and Find Full Text PDFPolymers (Basel)
November 2024
College of Petrochemical Engineering, Liaoning Petrochemical University, Fushun 113001, China.
Ethylene/1-octene copolymers exhibit enhanced flexibility and impact resistance compared to polyethylene, which makes them well suited for applications in advanced plastics and elastomers. United-atom molecular dynamics (MD) simulations were conducted to explore the mechanical behavior and deformation mechanisms of ethylene/1-octene copolymers under uniaxial tensile loading. This study systematically examined the influence of temperature, polymer chain length, chain quantity, and strain rate, with a specific focus on how hexyl branch content impacts the mechanical properties of amorphous ethylene/1-octene copolymers.
View Article and Find Full Text PDFCarbohydr Polym
January 2025
State Key Laboratory of Materials-Oriented Chemical Engineering, School of Pharmaceutical Sciences, Nanjing Tech university, Nanjing 210009, Jiangsu Province, PR China.
Stimuli-responsive Pickering emulsions are promising in biocatalysis for their ease of product separation and emulsifier recovery. However, pH responsiveness, though simple and cost-effective, faces challenges in precise control and narrow transition ranges, limiting its use in enzymatic catalysis. Herein we introduced amorphous octenyl succinic anhydride-modified debranched starch chains (Am-OSA-St) to control emulsion properties within a pH range suitable for enzymatic catalysis.
View Article and Find Full Text PDFJ Chem Theory Comput
November 2024
School for Engineering of Matter, Transport and Energy, Arizona State University, P.O. Box 876106, Tempe, Arizona 85287,United States.
We investigate the relaxation dynamics of crystalline stems in relation to the molecular topology of the crystalline/amorphous interface, employing coarse-grained molecular dynamics. To efficiently generate model semicrystalline systems of linear polyethylene with a realistic interphase morphology, we simplified the Monte Carlo method by introducing molecular dynamics for faster relaxation. The structural properties of the generated systems are validated against experimental measurements, theoretical predictions, and existing simulation data.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
Department of Chemistry and Chemical Biology, Cornell University, Ithaca, NY, 14853-1301, USA.
Polymer electrolytes exhibit higher energy density and improved safety in lithium-ion batteries relative to traditionally used liquid electrolytes but are currently limited by their lower electrochemical performance. Aiming to access polymer electrolytes with competitive electrochemical properties, we developed the anionic ring-opening polymerization (AROP) of cyclic silaketals to synthesize amorphous silicon-containing polyether-based electrolytes with varying substituent bulk of the general formula [OSi(R)(CHCHO)] (R=alkyl, phenyl). As opposed to previously reported uncontrolled polycondensation routes toward low molecular weight polysilaketals, AROP allows access to targeted molecular weights above the entanglement threshold of the polymers.
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