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  1. Genetically engineered neurons express membrane-bound enzymes that can catalyze oxidative polymerization on the cell surface. 
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    Free, publicly-accessible full text available August 9, 2024
  2. Abstract

    Stretchable polymer semiconductors (PSCs) have seen great advancements alongside the development of soft electronics. But it remains a challenge to simultaneously achieve high charge carrier mobility and stretchability. Herein, we report the finding that stretchable PSC thin films (<100-nm-thick) with high stretchability tend to exhibit multi-modal energy dissipation mechanisms and have a large relative stretchability (rS) defined by the ratio of the entropic energy dissipation to the enthalpic energy dissipation under strain. They effectively recovered the original molecular ordering, as well as electrical performance, after strain was released. The highestrSvalue with a model polymer (P4) exhibited an average charge carrier mobility of 0.2 cm2V−1s−1under 100% biaxial strain, while PSCs with lowrSvalues showed irreversible morphology changes and rapid degradation of electrical performance under strain. These results suggestrScan be used as a parameter to compare the reliability and reversibility of stretchable PSC thin films.

     
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  3. Self-healing soft electronic and robotic devices can, like human skin, recover autonomously from damage. While current devices use a single type of dynamic polymer for all functional layers to ensure strong interlayer adhesion, this approach requires manual layer alignment. In this study, we used two dynamic polymers, which have immiscible backbones but identical dynamic bonds, to maintain interlayer adhesion while enabling autonomous realignment during healing. These dynamic polymers exhibit a weakly interpenetrating and adhesive interface, whose width is tunable. When multilayered polymer films are misaligned after damage, these structures autonomously realign during healing to minimize interfacial free energy. We fabricated devices with conductive, dielectric, and magnetic particles that functionally heal after damage, enabling thin-film pressure sensors, magnetically assembled soft robots, and underwater circuit assembly.

     
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    Free, publicly-accessible full text available June 2, 2024
  4. Abstract

    CLARITY is a tissue preservation and optical clearing technique whereby a hydrogel is formed directly within the architectural confines of ex vivo brain tissue. In this work, the extent of polymer gel formation and crosslinking within tissue was assessed using Raman spectroscopy and rheology on CLARITY samples prepared with a range of acrylamide monomer (AAm) concentrations (1%, 4%, 8%, 12% w/v). Raman spectroscopy of individual neurons within hybrids revealed the chemical presence and distribution of polyacrylamide within the mouse hippocampus. Consistent with rheological measurements, lower %AAm concentration decreased shear elastic modulus G’, providing a practical correlation with sample permeability and protein retention. Permeability of F(ab)’2 secondary fluorescent antibody changes from 9.3 to 1.4 µm2 s−1going from 1 to 12%. Notably, protein retention increased linearly relative to standard PFA-fixed tissue from 96.6% when AAm concentration exceeded 1%, with 12% AAm samples retaining up to ~ 99.3% native protein. This suggests that though 1% AAm offers high permeability, additional %AAm may be required to enhance protein. Our quantitative results on polymer distribution, stability, protein retention, and macromolecule permeability can be used to guide the design of future CLARITY-based tissue-clearing solutions, and establish protocols for characterization of novel tissue-polymer hybrid biomaterials using chemical spectroscopy and rheology.

     
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  5. null (Ed.)
    Owing to their excellent mechanical flexibility, mixed-conducting electrical property, and extraordinary chemical turnability, conjugated polymers have been demonstrated to be an ideal bioelectronic interface to deliver therapeutic effect in many different chronic diseases. This review article summarizes the latest advances in implantable electronics using conjugated polymers as electroactive materials and identifies remaining challenges and opportunities for developing electronic medicine. Examples of conjugated polymer-based bioelectronic devices are selectively reviewed in human clinical studies or animal studies with the potential for clinical adoption. The unique properties of conjugated polymers are highlighted and exemplified as potential solutions to address the specific challenges in electronic medicine. 
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  6. Abstract

    Electrochemical cells that utilize metals (e.g., lithium, sodium, zinc) as anodes are under intense investigation as they are projected to replace the current lithium‐ion batteries to serve as a more energy‐dense option for commercial applications. In addition, metal electrodes provide opportunities for fundamental research of different phenomena, such as ion transport and electrochemical kinetics, in the complex environment of reactive metal‐electrodeposition. In this work, computationally and experimentally the competing effects related to transport and kinetics during the metal electrodeposition process are examined. Using Brownian dynamics simulations, it is shown that slower deposition kinetics results in a more compact and uniform Li morphology. This finding is experimentally implemented by designing ion‐containing polymeric coatings on the electrodes that simultaneously provide pathways for lithium‐ion transport, while impeding the charge transfer (Li++ e→ Li) at heterogeneous surfaces. It is further shown that these ionic polymer interfaces can significantly extend the cell‐lifetime of a lithium metal battery in both ether‐based and carbonate‐based electrolytes. Through theoretical and experimental investigations, it is found that a low kinetic to transport rate ratio is a major factor in influencing the Li plating morphology. The plating morphology can be further fine‐tuned by increasing ionic conductivity.

     
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  7. null (Ed.)
  8. Abstract Next-generation wearable electronics require enhanced mechanical robustness and device complexity. Besides previously reported softness and stretchability, desired merits for practical use include elasticity, solvent resistance, facile patternability and high charge carrier mobility. Here, we show a molecular design concept that simultaneously achieves all these targeted properties in both polymeric semiconductors and dielectrics, without compromising electrical performance. This is enabled by covalently-embedded in-situ rubber matrix (iRUM) formation through good mixing of iRUM precursors with polymer electronic materials, and finely-controlled composite film morphology built on azide crosslinking chemistry which leverages different reactivities with C–H and C=C bonds. The high covalent crosslinking density results in both superior elasticity and solvent resistance. When applied in stretchable transistors, the iRUM-semiconductor film retained its mobility after stretching to 100% strain, and exhibited record-high mobility retention of 1 cm 2 V −1 s −1 after 1000 stretching-releasing cycles at 50% strain. The cycling life was stably extended to 5000 cycles, five times longer than all reported semiconductors. Furthermore, we fabricated elastic transistors via consecutively photo-patterning of the dielectric and semiconducting layers, demonstrating the potential of solution-processed multilayer device manufacturing. The iRUM represents a molecule-level design approach towards robust skin-inspired electronics. 
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