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1. Sequential Self-Folding of Shape Memory Polymer Sheets by Laser Rastering Toward Origami-Based Manufacturing

   https://doi.org/10.1115/1.4050463  

   Abdulhafez, Moataz; Line, Joshua; Bedewy, Mostafa (September 2021, Journal of Manufacturing Science and Engineering)

   null (Ed.)

   Abstract Origami-based fabrication strategies open the door for developing new manufacturing processes capable of producing complex three-dimensional (3D) geometries from two-dimensional (2D) sheets. Nevertheless, for these methods to translate into scalable manufacturing processes, rapid techniques for creating controlled folds are needed. In this work, we propose a new approach for controlled self-folding of shape memory polymer sheets based on direct laser rastering. We demonstrate that rapidly moving a CO2 laser over pre-strained polystyrene sheets results in creating controlled folds along the laser path. Laser interaction with the polymer induces localized heating above the glass transition temperature with a temperature gradient across the thickness of the thin sheets. This gradient of temperature results in a gradient of shrinkage owing to the viscoelastic relaxation of the polymer, favoring folding toward the hotter side (toward the laser source). We study the influence of laser power, rastering speed, fluence, and the number of passes on the fold angle. Moreover, we investigate process parameters that produce the highest quality folds with minimal undesired deformations. Our results show that we can create clean folds up to and exceeding 90 deg, which highlights the potential of our approach for creating lightweight 3D geometries with smooth surface finishes that are challenging to create using 3D printing methods. Hence, laser-induced self-folding of polymers is an inherently mass-customizable approach to manufacturing, especially when combined with cutting for integration of origami and kirigami. 

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2. Do polymer ligands block the catalysis of metal nanoparticles? Unexpected importance of binding motifs in improving catalytic activity

   https://doi.org/10.1039/D0TA03906C  

   Zhang, Lei; Wei, Zichao; Meng, Michael; Ung, Gaël; He, Jie (August 2020, Journal of Materials Chemistry A)

   null (Ed.)

   Metal nanoparticles (NPs) tethered by synthetic polymers are of broad interest for self-assembly, nanomedicine and catalysis. The binding motifs in polymer ligands usually as the end functional groups of polymers are mostly limited to thiolates. Since the binding motif only represents a tiny fraction of many repeating units in polymers, its importance is often ignored. We herein report the uniqueness of polymeric N-heterocyclic carbene (NHC) ligands in providing oxidative stability and promoting the catalytic activity of noble metal NPs. Two “grafting to” methods were developed for polymer NHCs for pre-synthesized metal NPs in various solvents and with different sizes. Remarkably, imidazolium-terminated polystyrene can modify gold NPs (AuNPs) within 2 min while reaching a similar grafting density to polystyrene-thiol (SH) requiring 6 h modification. We demonstrate that polymer NHCs are extremely stable at high temperature in air. Interestingly, the binding motifs of polymer ligands dominate the catalytic activity of metal NPs. Polymer NHC modified metal NPs showed improved activity regardless of the surface crowdedness. In the case of AuNPs, AuNPs modified with polystyrene NHCs are approximately 5.2 times more active than citrate-capped ones and 22 times more active than those modified with polystyrene thiolates. In view of ligand-controlled catalytic properties of metal NPs, our results illustrate the importance of binding motifs that has been overlooked in the past. 

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3. Self-strengthening tape junctions inspired by recluse spider webs

   https://doi.org/10.1039/D2MH00403H  

   Skopic, Ben H.; Koebley, Sean R.; Schniepp, Hannes C. (October 2022, Materials Horizons)

   Adhesive tapes are versatile and widely used yet lack adhesion strength due to their tendency to fail via peeling, a weak failure mode. A tape with surprising adhesive properties is the recluse spider's 50 nm-thin silk ribbon with a 1 : 150 aspect ratio. Junctions of these microscopic sticky tapes can withstand the material's tensile failure stress of ≈1 GPa. We modeled these natural tape–tape junctions and revealed a bi-modal failure behavior, critically dependent on the two tapes’ intersection angle. One mode leads to regular, low-strength peeling failure, while the other causes the junction to self-strengthen, eliminating the inherent weakness in peeling. This self-strengthening mechanism locks the two tapes together, increasing the junction strength by 550% and allowing some junctions to remain intact after tensile failure. This impressive adhesive strength of tapes has never before been observed or predicted. We found that recluse spiders make tape junctions with pre-stress to force the locked, high-strength failure mode. We used this approach to make junctions with synthetic adhesive tapes that overcame the weak peeling failure. 

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4. Programming and Reprogramming the Viscoelasticity and Magnetic Response of Magnetoactive Thermoplastic Elastomers

   https://doi.org/10.3390/polym15234607  

   Kostrov, Sergei A; Marshall, Josiah H; Maw, Mitchell; Sheiko, Sergei S; Kramarenko, Elena Yu (December 2023, Polymers)

   We present a novel type of magnetorheological material that allows one to restructure the magnetic particles inside the finished composite, tuning in situ the viscoelasticity and magnetic response of the material in a wide range using temperature and an applied magnetic field. The polymer medium is an A-g-B bottlebrush graft copolymer with side chains of two types: polydimethylsiloxane and polystyrene. At room temperature, the brush-like architecture provides the tissue mimetic softness and strain stiffening of the elastomeric matrix, which is formed through the aggregation of polystyrene side chains into aggregates that play the role of physical cross-links. The aggregates partially dissociate and the matrix softens at elevated temperatures, allowing for the effective rearrangement of magnetic particles by applying a magnetic field in the desired direction. Magnetoactive thermoplastic elastomers (MATEs) based on A-g-B bottlebrush graft copolymers with different amounts of aggregating side chains filled with different amounts of carbonyl iron microparticles were prepared. The in situ restructuring of magnetic particles in MATEs was shown to significantly alter their viscoelasticity and magnetic response. In particular, the induced anisotropy led to an order-of-magnitude enhancement of the magnetorheological properties of the composites. 

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5. Binding, unbinding and aggregation of crescent-shaped nanoparticles on nanoscale tubular membranes

   https://doi.org/10.1039/D0SM01642J  

   Spangler, Eric J.; Olinger, Alexander D.; Kumar, P. B.; Laradji, Mohamed (January 2021, Soft Matter)

   null (Ed.)

   Using molecular dynamics simulations of a coarse-grained implicit solvent model, we investigate the binding of crescent-shaped nanoparticles (NPs) on tubular lipid membranes. The NPs adhere to the membrane through their concave side. We found that the binding/unbinding transition is first-order, with the threshold binding energy being higher than the unbinding threshold, and the energy barrier between the bound and unbound states at the transition that increases with increasing the NP's arclength L np or curvature mismatch μ = R c / R np , where R c and R np are the radii of curvature of the tubular membrane and the NP, respectively. Furthermore, we found that the threshold binding energy increases with increasing either L np or μ . NPs with curvature larger than that of the tubule ( μ > 1) lie perpendicularly to the tubule's axis. However, for μ smaller than a specific arclength-dependent mismatch μ *, the NPs are tilted with respect to the tubule's axis, with the tilt angle that increases with decreasing μ . We also investigated the self-assembly of the NPs on the tubule at relatively weak adhesion strength and found that for μ > 1 and high values of L np , the NPs self-assemble into linear chains, and lie side-by-side. For μ < μ * and high L np , the NPs also self-assemble into chains, while being tilted with respect to the tubule's axis. 

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