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  1. Abstract

    Many commodity plastics, such as thermoplastic polyurethanes (PUs), require reinforcement for use as commercial products. Cellulose nanocrystals (CNCs) offer a “green” and scalable approach to polymer reinforcement as they are exceptionally stiff, recyclable, and abundant. Unfortunately, achieving efficient CNC reinforcement of PUs with industrial melt processing techniques is difficult, mostly due to the incompatibility of the hydrophobic PU with hydrophilic CNCs, limiting their dispersion. Here, a hydrophilic PU is synthesized to achieve strong reinforcement in melt‐processed nanocomposite fibers using filter paper‐sourced CNCs. The melt‐spun fibers, exhibiting smooth surfaces even at high CNC loading (up to 25 wt%) indicating good CNC dispersion, are bench‐marked against solvent‐cast films—solvent processing is not scalable but disperses CNCs well and produces strong CNC reinforcement. Mechanical analysis shows the CNC addition stiffens both nanocomposite films and fibers. The stress and strain at break, however, are not significantly affected in films, whereas adding CNCs to fibers increases the stress‐at‐break while reducing the strain‐at‐break. Compared to earlier studies employing a hydrophobic (and stiffer) PU, CNC addition to a hydrophilic PU substantially increases the fiber stiffness and strength. This work therefore suggests that rendering thermoplastics more hydrophilic might pave the way for “greener” polymer composite products using CNCs.

     
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  2. Abstract

    Polyelectrolytes are ubiquitous in biology, from the polynucleotide chain in our DNA, the hyaluronic acid in the vitreous body of the eye (Gaoet al.,Int J Ophthalmol, 8, 437–440, 2015) to the myosin and actin fibrils that make up our muscles. While synthetic polyelectrolytes are well studied, their correlation to biological polyelectrolytes is just beginning. This review will examine the polyelectrolytes that make up fundamental cell biology from a macromolecular perspective and the implications polyelectrolyte theory has on biological function. © 2020 Society of Industrial Chemistry

     
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  3. Abstract

    As wearable technologies redefine the way people exchange information, receive entertainment, and monitor health, the development of sustainable power sources that capture energy from the user's everyday activities garners increasing interest. Electric fishes, such as the electric eel and the torpedo ray, provide inspiration for such a power source with their ability to generate massive discharges of electricity solely from the metabolic processes within their bodies. Inspired by their example, the device presented in this work harnesses electric power from ion gradients established by capturing the carbon dioxide (CO2) from human breath. Upon localized exposure to CO2, this novel adaptation of reverse electrodialysis chemically generates ion gradients from a single initial solution uniformly distributed throughout the device instead of requiring the active circulation of two different external solutions. A thorough analysis of the relationship between electrical output and the concentration of carbon capture agent (monoethanolamine, MEA), the amount of CO2captured, and the device geometry informs device design. The prototype device presented here harvests enough energy from a breath‐generated ion gradient to power small electronic devices, such as a light‐emitting diode (LED).

     
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  4. Inspired by spider silk's hierarchical diversity, we leveraged peptide motifs with the capability to tune structural arrangement for controlling the mechanical properties of a conventional polymer framework. The addition of nanofiller with hydrogen bonding sites was used as another pathway towards hierarchical tuning via matrix–filler interactions. Specifically, peptide–polyurea hybrids (PPUs) were combined with cellulose nanocrystals (CNCs) to develop mechanically-tunable nanocomposites via tailored matrix–filler interactions (or peptide–cellulose interactions). In this material platform, we explored the effect of these matrix–filler interactions on the secondary structure, hierarchical ordering, and mechanical properties of the peptide hybrid nanocomposites. Interactions between the peptide matrix and CNCs occur in all of the PPU/CNC nanocomposites, preventing α-helical ordering, but promoting inter-molecular hydrogen bonded β-sheet formation. Depending on peptide and CNC content, the Young's modulus varies from 10 to 150 MPa. Unlike conventional cellulose-reinforced polymer nanocomposites, the mechanical properties of these composite materials are dictated by a balance of CNC reinforcement, peptidic ordering, and microphase-separated morphology. This research highlights that leveraging peptide–cellulose interactions is a strategy to create materials with targeted mechanical properties for a specific application using a limited selection of building blocks. 
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  5. Electrical excitability of cells, tissues and organs is a fundamental phenomenon in biology and physiology. Signatures of excitability include transient currents resulting from a constant or varying voltage gradient across compartments. Interestingly, such signatures can be observed with non-biologically-derived, macromolecular systems. Initial key literature, dating to roughly the late 1960’s into the early 1990’s, is reviewed here. We suggest that excitability in response to electrical stimulation is a material phenomenon that is exploited by living organisms, but that is not exclusive to living systems. Furthermore, given the ubiquity of biological hydrogels, we also speculate that excitability in protocells of primordial organisms might have shared some of the same molecular mechanisms seen in non-biological macromolecular systems, and that vestigial traces of such mechanisms may still play important roles in modern organisms’ biological hydrogels. Finally, we also speculate that bio-mimicking excitability of synthetic macromolecular systems might have practical biomedical applications. 
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