Sustainable polymers that stick inside and out.

A naturally occurring fatty acid yields a set of adhesives with different properties.

Efficient and Robust Dynamic Crosslinking for Compatibilizing Immiscible Mixed Plastics through In Situ Generated Singlet Nitrenes.

Creating a sustainable economy for plastics demands the exploration of new strategies for efficient management of mixed plastic waste. The inherent incompatibility of different plastics poses a major challenge in plastic mechanical recycling, resulting in phase-separated materials with inferior mechanical properties. Here, this study presents a robust and efficient dynamic crosslinking chemistry that effectively compatibilizes mixed plastics.

Observing the Dynamics of an Electrochemically Driven Active Material with Liquid Electron Microscopy.

Electrochemical liquid electron microscopy has revolutionized our understanding of nanomaterial dynamics by allowing for direct observation of their electrochemical production. This technique, primarily applied to inorganic materials, is now being used to explore the self-assembly dynamics of active molecular materials. Our study examines these dynamics across various scales, from the nanoscale behavior of individual fibers to the micrometer-scale hierarchical evolution of fiber clusters.

Nanoantennas report dissipative assembly in oscillatory electric fields.

Understanding driving forces for dissipative, i.e., out of equilibrium, assembly of nanoparticles from colloidal solution at liquid-solid interfaces provides the ability to design external cues for reconfigurable device response.

A Vitrimer Acts as a Compatibilizer for Polyethylene and Polypropylene Blends.

Polymer compatibilization plays a critical role in achieving polymer blends with favorable mechanical properties and enabling efficient recycling of mixed plastic wastes. Nonetheless, traditional compatibilization methods often require tailored designs based on the specific chemical compositions of the blends. In this study, we propose a new approach for compatibilizing polymer blends using a dynamically crosslinked polymer network, known as vitrimers.

Multiscale Molecular Dynamics Simulations of an Active Self-Assembling Material.

Inspired by the adaptability observed in biological materials, self-assembly processes have attracted significant interest for their potential to yield novel materials with unique properties. However, experimental methods have often fallen short in capturing the molecular details of the assembly process. In this study, we employ a multiscale molecular dynamics simulation approach, complemented by NMR quantification, to investigate the mechanism of self-assembly in a redox-fueled bioinspired system.

CryoEM reveals the complex self-assembly of a chemically driven disulfide hydrogel.

Inspired by the adaptability of biological materials, a variety of synthetic, chemically driven self-assembly processes have been developed that result in the transient formation of supramolecular structures. These structures form through two simultaneous reactions, forward and backward, which generate and consume a molecule that undergoes self-assembly. The dynamics of these assembly processes have been shown to differ from conventional thermodynamically stable molecular assemblies.

Fluoride-Catalyzed Siloxane Exchange as a Robust Dynamic Chemistry for High-Performance Vitrimers.

Sustainable development of new technologies requires materials having advanced physical and chemical properties while maintaining reprocessability and recyclability. Vitrimers are designed for this purpose; however, their dynamic covalent chemistries often have drawbacks or are limited to specialized polymers. Here, fluoride-catalyzed siloxane exchange is reported as an exceptionally robust chemistry for scalable production of high-performance vitrimers through industrial processing of commodity polymers such as poly(methyl methacrylate), polyethylene, and polypropylene.

Passive Automatic Switch Relying on Laplace Pressure for Efficient Underwater Low-Gas-Flux Bubble Energy Harvesting.

The buoyancy potential energy contained in bubbles released by subsea geological and biological activities represents a possible in situ energy source for underwater sensing and detection equipment. However, the low gas flux of the bubble seepages that exist widely on the seabed introduces severe challenges. Herein, a passive automatic switch relying on Laplace pressure is proposed for efficient energy harvesting from low-gas-flux bubbles.

Waste-Free Fully Electrically Fueled Dissipative Self-Assembly System.

The importance and prevalence of energy-fueled active materials in living systems have inspired the design of synthetic active materials using various fuels. However, several major limitations of current designs remain to be addressed, such as the accumulation of chemical wastes during the process, unsustainable active behavior, and the lack of precise spatiotemporal control. Here, we demonstrate a fully electrically fueled (e-fueled) active self-assembly material that can overcome the aforementioned limitations.

Precise Control of Dissipative Self-assembly by Light and Electricity.

Nature-inspired synthetic dissipative self-assemblies have attracted much attention recently. However, it remains a major challenge to achieve precise control over dissipative supramolecular assembly structures and functions of self-contained systems. Here we combine light and electricity as two clean, and spatiotemporally addressable fuels to provide precise control over the morphology for dissipative self-assembly of a perylene bisimide glycine (PBIg) building block in a self-contained solution.

Super-Aerophilic Biomimetic Cactus for Underwater Dispersed Microbubble Capture, Self-Transport, Coalescence, and Energy Harvesting.

Human ocean activities are inseparable from the supply of energy. The energy contained in the gas-phase components dispersed in seawater is a potential universal energy source for eupelagic or deep-sea equipment. However, the low energy density of bubbles dispersed in water introduces severe challenges to the potential energy harvesting of gas-phase components.

Sugar-Fueled Dissipative Living Materials.

Dissipative behaviors in biology are fuel-driven processes controlled by living cells, and they shape the structural and functional complexities in biological materials. This concept has inspired the development of various forms of synthetic dissipative materials controlled by time-dependent consumption of chemical or physical fuels, such as reactive chemical species, light, and electricity. To date, synthetic living materials featuring dissipative behaviors directly controlled by the fuel consumption of their constituent cells is unprecedented.

Facile Synthesis of Multifunctional Bioreducible Polymers for mRNA Delivery.

Bioreducible polymeric mRNA carriers are an emerging family of vectors for gene delivery and vaccine development. A few bioreducible systems have been generated through aqueous-phase ring-opening polymerization of lipoic acid derivatives, however this methodology limits hydrophobic group incorporation and functionality into resulting polymers. Herein, a poly(active ester)disulfide polymer is synthesized that can undergo facile aminolysis with amine-containing substrates under stoichiometric control and mild reaction conditions to yield a library of multifunctional polydisulfide polymers.

Electrically Fueled Active Supramolecular Materials.

Fuel-driven dissipative self-assemblies play essential roles in living systems, contributing both to their complex, dynamic structures and emergent functions. Several dissipative supramolecular materials have been created using chemicals or light as fuel. However, electrical energy, one of the most common energy sources, has remained unexplored for such purposes.

Multifunctional Dendronized Polypeptides for Controlled Adjuvanticity.

Vaccination has been playing an important role in treating both infectious and cancerous diseases. Nevertheless, many diseases still lack proper vaccines due to the difficulty to generate sufficient amounts of antigen-specific antibodies or T cells. Adjuvants provide an important route to improve and direct immune responses.

Apatinib suppresses the migration, invasion and angiogenesis of hepatocellular carcinoma cells by blocking VEGF and PI3K/AKT signaling pathways.

Hepatocellular carcinoma (HCC) is a commonly diagnosed malignancy worldwide with poor prognosis and high metastasis and recurrence rates. Although apatinib has been demonstrated to have potential antitumor activity in multiple solid tumors, the underlying mechanism of apatinib in HCC treatment remains to be elucidated. In the present study, apatinib were used to treat HCC cells transfected with or without VEGFR2 overexpression vectors.

Multivalent Peptide-Functionalized Bioreducible Polymers for Cellular Delivery of Various RNAs.

RNA-based therapeutics have garnered tremendous attention due to their potential to revolutionize protein replacement therapies, immunotherapy, and treatment of genetic disorders. The lack of safe and efficient RNA delivery methods has significantly hindered the clinical translation and widespread application of RNA-based therapeutics. With differing sizes and structures of therapeutic RNA molecules, a critical challenge of the field is to develop RNA delivery systems that accommodate these variations while retaining high biocompatibility and efficacy.

Direct Silyl Ether Metathesis for Vitrimers with Exceptional Thermal Stability.

Vitrimers are a new class of polymeric materials that simultaneously offer the desired physical properties of thermosets and malleability/reprocessability of thermoplastics. Despite significant progress being made in the field of vitrimers, there exists a critical need for the development of robust dynamic covalent chemistries for the production of strong and thermally stable vitrimers. In this work, we discovered a new silyl ether metathesis reaction and used it for the preparation of vitrimers with exceptional thermal stability.

A Three-Armed Polymer with Tunable Self-Assembly and Self-Healing Properties Based on Benzene-1,3,5-tricarboxamide and Metal-Ligand Interactions.

The dynamic nature of supramolecules makes them useful in the fields of smart devices. The combination of multiple dynamic interactions in one material may bring some enhanced properties in mechanical property, self-healing property, or recyclability. Thus, it is significantly meaningful to design new materials with multi-dynamic bonds and clarify their bonding mechanisms.

Correction to "Immunomodulation of the NLRP3 Inflammasome through Structure-Based Activator Design and Functional Regulation via Lysosomal Rupture".

[This corrects the article DOI: 10.1021/acscentsci.8b00218.

Immunomodulation of the NLRP3 Inflammasome through Structure-Based Activator Design and Functional Regulation via Lysosomal Rupture.

The NLRP3 inflammasome plays a role in the inflammatory response to vaccines, in antimicrobial host defense, and in autoimmune diseases. However, its mechanism of action remains incompletely understood. NLRP3 has been shown to be activated by diverse stimuli including microbial toxins, ATP, particulate matter, etc.

Recyclable, Strong, and Highly Malleable Thermosets Based on Boroxine Networks.

Traditional thermoset materials have favorable material properties but are unable to reprocess and are difficult to recycle. Small molecule boroxines have been shown to undergo a reversible exchange reaction. Herein we employ boroxine as dynamic cross-links to construct a novel type of thermoset material that is strong, highly malleable, and recyclable.