Dynamic covalent polymer networks (DCPN) have historically attracted attention for their unique roles in chemical recycling and self-healing, which are both relevant for sustainable societal development. Efforts in these directions have intensified in the past decade with notable progress in newly discovered dynamic covalent chemistry, fundamental material concepts, and extension toward emerging applications including energy and electronic devices. Beyond that, the values of DCPN in discovering/designing functional properties not offered by classical thermoplastic and thermoset polymers have recently gained traction. In particular, the dynamic bond exchangeability of DCPN has shown unparalleled design versatility in various areas including shape-shifting materials/devices, artificial muscles, and microfabrication. Going beyond this basic bond exchangeability, various molecular mechanisms to manipulate network topologies (topological transformation) have led to opportunities to program polymers, with notable concepts such as living networks and topological isomerization. In this review, we provide an overview of the above progress with particular focuses on molecular design strategies for the exploitation of functional material properties. Based on this, we point out the remaining issues and offer perspectives on how this class of materials can shape the future in ways that are complementary with classical thermoplastic and thermoset polymers.

Dynamic Covalent Polymer Networks: A Molecular Platform for Designing Functions beyond Chemical Recycling and Self-Healing.

Dynamic covalent bonds in self-healing, shape memory, and controllable stiffness hydrogels

This Perspective focuses on thiol-mediated uptake, that is, the entry of substrates into cells enabled by oligochalcogenides or mimics, often disulfides, and inhibited by thiol-reactive agents. A short chronology from the initial observations in 1990 until today is followed by a summary of cell-penetrating poly(disulfide)s (CPDs) and cyclic oligochalcogenides (COCs) as privileged scaffolds in thiol-mediated uptake and inhibitors of thiol-mediated uptake as potential antivirals. In the spirit of a Perspective, the main part brings together topics that possibly could help to explain how thiol-mediated uptake really works. Extreme sulfur chemistry mostly related to COCs and their mimics, cyclic disulfides, thiosulfinates/-onates, diselenolanes, benzopolysulfanes, but also arsenics and Michael acceptors, is viewed in the context of acidity, ring tension, exchange cascades, adaptive networks, exchange affinity columns, molecular walkers, ring-opening polymerizations, and templated polymerizations. Micellar pores (or lipid ion channels) are considered, from cell-penetrating peptides and natural antibiotics to voltage sensors, and a concise gallery of membrane proteins, as possible targets of thiol-mediated uptake, is provided, including CLIC1, a thiol-reactive chloride channel; TMEM16F, a Ca-activated scramblase; EGFR, the epithelial growth factor receptor; and protein-disulfide isomerase, known from HIV entry or the transferrin receptor, a top hit in proteomics and recently identified in the cellular entry of SARS-CoV-2.

Thiol-Mediated Uptake

As with all stylish 2D functional materials, tellurene and tellurides possessing excellent physical and chemical properties such as high environmental stability, tunable narrow bandgap, and lower thermal conductivity, have aroused the great interest of the researchers. These properties of such materials also form the basis for relatively newfangled scholarly fields involving advanced topics, especially for broadband photodetectors. Integrating the excellent properties of many 2D materials, tellurene/telluride-based photodetectors show great flexibility, higher frequency response or faster time response, high signal-to-noise ratio, and so on, which make them leading the frontier of photodetector research. To fully understand the excellent properties of tellurene/tellurides and their optoelectronic applications, the recent advances in tellurene/telluride-based photodetectors are maximally summarized. Benefiting from the solid research in this field, the challenges and opportunities of tellurene/tellurides for future optoelectronic applications are also discussed in this review, which might provide possibilities for the realization of state-of-the-art high-performance tellurene/telluride-based devices.

/pdf/emerging-two-dimensional-tellurene-and-tellurides-for-t1b1h7cb.pdf

Emerging Two-Dimensional Tellurene and Tellurides for Broadband Photodetectors.

Bioadhesives have emerged as transformative and versatile tools in healthcare, offering the ability to attach tissues with ease and minimal damage. These materials present numerous opportunities for tissue repair and biomedical device integration, creating a broad landscape of applications that have captivated clinical and scientific interest alike. However, fully unlocking their potential requires multifaceted design strategies involving optimal adhesion, suitable biological interactions, and efficient signal communication. In this Review, we delve into these pivotal aspects of bioadhesive design, highlight the latest advances in their biomedical applications, and identify potential opportunities that lie ahead for bioadhesives as multifunctional technology platforms.

Bioadhesive Technology Platforms.

The rapid development of supramolecular polymer chemistry and constitutional dynamic chemistry over the last decades has made tremendous impact on the emergence of dynamic covalent polymers. These materials are formed through reversible covalent bonds, endowing them with adaptive and responsive features that have resulted in high interest throughout the community. Owing to their intriguing properties, such as self-healing, shape-memory effects, recyclability, degradability, stimuli-responsiveness, etc., the materials have found multiple uses in a wide range of areas. Of special interest is their increasing use for biomedical applications, and many examples have been demonstrated in recent years. These materials have thus been used for the recognition and sensing of biologically active compounds, for the modulation of enzyme activity, for gene delivery, and as materials for cell culture, delivery, and wound-dressing. In this review, some of these endeavors are discussed, highlighting the many advantages and unique properties of dynamic covalent polymers for use in biology and biomedicine.

/pdf/dynamic-covalent-polymers-for-biomedical-applications-xczt8zfreg.pdf

Dynamic covalent polymers for biomedical applications

Abstract Dynamic covalent polymers of different topology have been synthesized from an aromatic dialdehyde and α,ω‐dinitroalkanes via the nitroaldol reaction. All dinitroalkanes yielded dynamers with the dialdehyde, where the length of the dinitroalkane chain played a vital role in determining the structure of the final products. For longer dinitroalkanes, linear dynamers were produced, where the degree of polymerization reached a plateau at higher feed concentrations. In the reactions involving 1,4‐dinitrobutane and 1,5‐dinitropentane, specific macrocycles were formed through depolymerization of the linear chains, further driven by precipitation. At lower temperature, the same systemic self‐sorting effect was also observed for the 1,6‐dinitrohexane‐based dynamers. Moreover, the dynamers showed a clear adaptive behavior, displaying depolymerization and rearrangement of the dynamer chains in response to alternative building blocks as external stimuli.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/chem.202201863

Polymerization, Stimuli‐induced Depolymerization, and Precipitation‐driven Macrocyclization in a Nitroaldol Reaction System

Dynamic covalent gels have been synthesized from an aromatic trialdehyde and α,ω- dinitroalkanes via the nitroaldol reaction in organic solvents. The gelation process could be finetuned by changing the starting nitroalkanes, solvents, feed concentration, catalyst loading, or reaction temperature. The resulting organogels demonstrated good structural integrity and excellent self-healing ability. Intact xerogels were produced upon drying, without damaging the network, and the solvent-free network could recover its gel form in the presence of an organic solvent. Furthermore, the crosslinked dynameric gel depolymerized to small molecules in response to excess nitromethane. This article is protected by copyright. All rights reserved.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/marc.202300011

Self-healable, Regenerable, and Degradable Dynamic Covalent Nitroalcohol Organogels.

The Burkholderia genus encompasses multiple human pathogens, including potential bioterrorism agents, that are often extensively antibiotic resistant. The FixLJ pathway in Burkholderia is a two-component system that regulates virulence. Previous work showed that fixLJ mutations arising during chronic infection confer increased virulence while decreasing the activity of the FixLJ pathway. We hypothesized that small-molecule activators of the FixLJ pathway could serve as anti-virulence therapies. Here, we developed a high-throughput assay that screened over 28,000 compounds and identified 11 that could specifically active the FixLJ pathway. Eight of these compounds, denoted Burkholderia Fix Activator (BFA) 1-8, inhibited the intracellular survival of Burkholderia in THP-1-dervived macrophages in a fixLJ-dependent manner without significant toxicity. One of the compounds, BFA1, inhibited the intracellular survival in macrophages of multiple Burkholderia species. Predictive modeling of the interaction of BFA1 with Burkholderia FixL suggests that BFA1 binds to the putative ATP/ADP binding pocket in the kinase domain, indicating a potential mechanism for pathway activation. These results indicate that small-molecule FixLJ pathway activators are promising anti-virulence agents for Burkholderia and define a new paradigm for antibacterial therapeutic discovery.

Small-molecule activators of a bacterial signaling pathway inhibit virulence

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Dynamic covalent polymers for biomedical applications

Polymerization, Stimuli‐induced Depolymerization, and Precipitation‐driven Macrocyclization in a Nitroaldol Reaction System

Self-healable, Regenerable, and Degradable Dynamic Covalent Nitroalcohol Organogels.

Small-molecule activators of a bacterial signaling pathway inhibit virulence