Multimaterial Thermoset Synthesis: Switching Polymerization Mechanism with Light Dosage.

The synthesis of polymeric thermoset materials with spatially controlled physical properties using readily available resins is a grand challenge. To address this challenge, we developed a photoinitiated polymerization method that enables the spatial switching of radical and cationic polymerizations by controlling the dosage of monochromatic light. This method, which we call Switching Polymerizations by Light Titration (SPLiT), leverages the use of substoichiometric amounts of a photobuffer in combination with traditional photoacid generators.

Recyclable Organic Radical Electrodes for Metal-Free Batteries.

Organic batteries are one of the possible routes for transitioning to sustainable energy storage solutions. However, the recycling of organic batteries, which is a key step toward circularity, is not easily achieved. This work shows the direct recycling of poly(2,2,6,6-tetramethylpiperidinyloxy-4-yl) (PTMA) and poly(2,2,6,6-tetramethylpiperidinyloxy-4-yl acrylamide) (PTAm) based composite electrodes.

Nonconjugated Redox-Active Polymers: Electron Transfer Mechanisms, Energy Storage, and Chemical Versatility.

The storage of electric energy in a safe and environmentally friendly way is of ever-growing importance for a modern, technology-based society. With future pressures predicted for batteries that contain strategic metals, there is increasing interest in metal-free electrode materials. Among candidate materials, nonconjugated redox-active polymers (NC-RAPs) have advantages in terms of cost-effectiveness, good processability, unique electrochemical properties, and precise tuning for different battery chemistries.

Safer Polyurethane Foams with Cyclic Carbonates.

Polyurethanes (PUs) are a class of materials usually synthesized from isocyanates, diols, and water. Water is essential for producing carbon dioxide (CO ) which is used for the self-blowing of the foams. Due to safety concerns with the production of isocyanates, alternative chemistries have been evaluated and cyclic carbonate systems have shown great promise.

Quantifying internal charge transfer and mixed ion-electron transfer in conjugated radical polymers.

Macromolecular radicals are receiving growing interest as functional materials in energy storage devices and in electronics. With the need for enhanced conductivity, researchers have turned to macromolecular radicals bearing conjugated backbones, but results thus far have yielded conjugated radical polymers that are inferior in comparison to their non-conjugated partners. The emerging explanation is that the radical unit and the conjugated backbone (both being redox active) transfer electrons between each other, essentially "quenching" conductivity or capacity.

Polypeptide organic radical batteries.

In only a few decades, lithium-ion batteries have revolutionized technologies, enabling the proliferation of portable devices and electric vehicles, with substantial benefits for society. However, the rapid growth in technology has highlighted the ethical and environmental challenges of mining lithium, cobalt and other mineral ore resources, and the issues associated with the safe usage and non-hazardous disposal of batteries. Only a small fraction of lithium-ion batteries are recycled, further exacerbating global material supply of strategic elements.

100th Anniversary of Macromolecular Science Viewpoint: Fundamentals for the Future of Macromolecular Nitroxide Radicals.

Macromolecular radicals, radical polymers, and polyradicals bear unique functionalities derived from their pendant radical groups. The increasing need for organic functional materials is driving the growth in research interest in macromolecular radicals for batteries, electronics, memory, and imaging. This Viewpoint summarizes the current state-of-knowledge regarding the macromolecular nitroxide radicals' redox mechanism, conductivity, chain conformation, controlled polymerization, network structure, conjugated forms, and applications.

Solution-Processable Thermally Crosslinked Organic Radical Polymer Battery Cathodes.

Organic radical polymers are promising cathode materials for next-generation batteries because of their rapid charge transfer and high cycling stability. However, these organic polymer electrodes gradually dissolve in the electrolyte, resulting in capacity fade. Several crosslinking methods have been developed to improve the performance of these electrodes, but they are either not compatible with carbon additives or compromise the solution processability of the electrodes.

Layer-by-Layer Assembly of Polyaniline Nanofibers and MXene Thin-Film Electrodes for Electrochemical Energy Storage.

The growing demand for compact energy storage devices may be met through the use of thin-film microbatteries, which generally rely on charge storage in thin or conformal layers. A promising technique for creating thin-film electrodes is layer-by-layer (LbL) assembly, based on the alternating adsorption of oppositely charged species to a surface to form a nanostructured electrode. Thin-film energy storage devices must have a high energy density within a limited space, so new electrode structures, materials, and assembly methods are important.

Shape memory polyurethane-urea foams with improved toughness.

Current vascular aneurysm treatments often require either highly invasive strategy to surgically occlude an aneurysm or endovascular occlusion via metal coils. While endovascular coils are safer, they have limited efficacy. Endovascular coils that are integrated with shape memory polymer (SMP) foams have the potential to improve occlusion and reduce coil risks; however, the mechanical performance and limited homogeneity of SMP foams can hinder their effective use.

Highly Cross-Linked Shape Memory Polymers with Tunable Oxidative and Hydrolytic Degradation Rates and Selected Products Based on Succinic Acid.

Minimally invasive medical devices are of great interest, with shape memory polymers (SMPs) representing one such possibility for producing these devices. Previous work with low density, highly porous SMPs has demonstrated oxidative degradation, while attempts to incorporate hydrolytic degradation have resulted in rapidly decreasing glass transition temperature (T ), ultimately preventing strain fixity of the materials at clinically relevant temperatures. Through esterification of the amino alcohol triethanolamine, an alcohol containing network was synthesized and incorporated into SMPs.

Real-time insight into the doping mechanism of redox-active organic radical polymers.

Organic radical polymers for batteries represent some of the fastest-charging redox active materials available. Electron transport and charge storage must be accompanied by ion transport and doping for charge neutrality, but the nature of this process in organic radical polymers is not well understood. This is difficult to intuitively predict because the pendant radical group distinguishes organic radical polymers from conjugated, charged or polar polymers.

Multifunctional Shape-Memory Polymer Foams with Bio-inspired Antimicrobials.

Despite a number of clinically available hemostats, uncontrolled bleeding is the primary cause of trauma-related death. Shape-memory polymer (SMP) foams have a number of desirable properties for use as hemostats, including shape recovery to enable delivery into bleed sites, biocompatibility, and rapid blood clotting. To expand upon this material system, the current work aims to incorporate phenolic acids, which are honey-based antimicrobial agents, into SMP foams.

Development of siloxane-based amphiphiles as cell stabilizers for porous shape memory polymer systems.

Hypothesis: Polyurethane foaming surfactants are cell stabilized at the polymer-gas interface during foam blowing to prevent bubble coalescence. Siloxane-based surfactants are typically used to generate a surface tension gradient at the interface. The chemical structure of the hydrophobic and hydrophilic units affects surfactant properties, which can further influence foam morphology.