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Chemical Society Reviews Jun 2024Polymer prodrugs are based on the covalent linkage of therapeutic molecules to a polymer structure which avoids the problems and limitations commonly encountered with... (Review)
Review
Polymer prodrugs are based on the covalent linkage of therapeutic molecules to a polymer structure which avoids the problems and limitations commonly encountered with traditional drug-loaded nanocarriers in which drugs are just physically entrapped (, burst release, poor drug loadings). In the past few years, reversible-deactivation radical polymerization (RDRP) techniques have been extensively used to design tailor-made polymer prodrug nanocarriers. This synthesis strategy has received a lot of attention due to the possibility of fine tuning their structural parameters (, polymer nature and macromolecular characteristics, linker nature, physico-chemical properties, functionalization, ), to achieve optimized drug delivery and therapeutic efficacy. In particular, adjusting the nature of the drug-polymer linker has enabled the easy synthesis of stimuli-responsive polymer prodrugs for efficient spatiotemporal drug release. In this context, this review article will give an overview of the different stimuli-sensitive polymer prodrug structures designed by RDRP techniques, with a strong focus on the synthesis strategies, the macromolecular architectures and in particular the drug-polymer linker, which governs the drug release kinetics and eventually the therapeutic effect. Their biological evaluations will also be discussed.
Topics: Prodrugs; Polymerization; Drug Carriers; Humans; Polymers; Nanoparticles; Drug Liberation; Free Radicals
PubMed: 38775004
DOI: 10.1039/d2cs01060g -
Results and Problems in Cell... 2022Genomic DNA, which controls genetic information, is stored in the cell nucleus in eukaryotes. Chromatin moves dynamically in the nucleus, and this movement is closely...
Genomic DNA, which controls genetic information, is stored in the cell nucleus in eukaryotes. Chromatin moves dynamically in the nucleus, and this movement is closely related to the function of chromatin. However, the driving force of chromatin movement, its control mechanism, and the functional significance of movement are unclear. In addition to biochemical and genetic approaches such as identification and analysis of regulators, approaches based on the physical properties of chromatin and cell nuclei are indispensable for this understanding. In particular, the idea of polymer physics is expected to be effective. This paper introduces our efforts to combine biological experiments on chromatin kinetics with theoretical analysis based on polymer physics.
Topics: Chromatin; Polymers; Chromosomes; Cell Nucleus; DNA
PubMed: 36348110
DOI: 10.1007/978-3-031-06573-6_8 -
Molecules (Basel, Switzerland) Aug 2019Polymerization provides an efficient strategy for synthesizing macromolecules with versatile functionality [...].
Polymerization provides an efficient strategy for synthesizing macromolecules with versatile functionality [...].
Topics: Biological Products; Biosensing Techniques; Drug Delivery Systems; Food Technology; Humans; Information Storage and Retrieval; Polymerization; Polymers; Tissue Engineering; Water Purification
PubMed: 31426353
DOI: 10.3390/molecules24162976 -
International Journal of Molecular... Sep 2022Using hybrid multi-particle collision dynamics (MPCD) and a molecular dynamics (MD) method, we investigate the effect of arms and shear flow on dynamical and structural...
Using hybrid multi-particle collision dynamics (MPCD) and a molecular dynamics (MD) method, we investigate the effect of arms and shear flow on dynamical and structural properties of the comb long-chain branched (LCB) polymer with dense arms. Firstly, we analyze dynamical properties of the LCB polymer by tracking the temporal changes on the end-to-end distance of both backbones and arms as well as the orientations of the backbone in the flow-gradient plane. Simultaneously, the rotation and tumbling behaviors with stable frequencies are observed. In other words, the LCB polymer undergoes a process of periodic stretched-folded-stretched state transition and rotation, whose period is obtained by fitting temporal changes on the orientation to a periodic function. In addition, the impact induced by random and fast motions of arms and the backbone will descend as the shear rate increases. By analyzing the period of rotation behavior of LCB polymers, we find that arms have a function in keeping the LCB polymer's motion stable. Meanwhile, we find that the rotation period of the LCB polymer is mainly determined by the conformational distribution and the non-shrinkable state of the structure along the velocity-gradient direction. Secondly, structural properties are numerically characterized by the average gyration tensor of the LCB polymer. The changes in gyration are in accordance with the LCB polymer rolling when varying the shear rate. By analyzing the alignment of the LCB polymer and comparing with its linear and star counterparts, we find that the LCB polymer with very long arms, like the corresponding linear chain, has a high speed to reach its configuration expansion limit in the flow direction. However, the comb polymer with shorter arms has stronger resistance on configuration expansion against the imposed flow field. Moreover, with increasing arm length, the comb polymer in shear flow follows change from linear-polymer-like to capsule-like behavior.
Topics: Molecular Conformation; Molecular Dynamics Simulation; Polymers; Rotation
PubMed: 36232591
DOI: 10.3390/ijms231911290 -
Chemical Communications (Cambridge,... Sep 2022Multiple reviews have been written concerning conjugated macromonomers and polymers both as general descriptions and for specific applications. In most examples,... (Review)
Review
Multiple reviews have been written concerning conjugated macromonomers and polymers both as general descriptions and for specific applications. In most examples, conjugation occurs electronic communication continuous overlap of π orbitals, most often on carbon. These systems can be considered to offer traditional forms of conjugation. In this review, we attempt to survey macromonomers and polymers that offer conjugation involving novel forms of carbon and/or other elements but with conjugation achieved other bonding formats, including many where the mechanism(s) whereby such behavior is observed remain unresolved. In particular, this review emphasizes silsesquioxane containing polymeric materials that offer properties found typically in conjugated polymers. However, conjugation in these polymers appears to occur saturated siloxane bonds within monomeric units that make up a variety of polymer systems. Multiple photophysical analytical methods are used as a means to demonstrate conjugation in systems where traditional conjugation is not apparent.
Topics: Carbon; Chemical Phenomena; Polymers; Siloxanes
PubMed: 36069250
DOI: 10.1039/d2cc03968k -
Advanced Healthcare Materials Sep 2019Hydrogels based on natural polymers have bright application prospects in biomedical fields due to their outstanding biocompatibility and biodegradability. However, the... (Review)
Review
Hydrogels based on natural polymers have bright application prospects in biomedical fields due to their outstanding biocompatibility and biodegradability. However, the poor mechanical performances of pure natural polymer-based hydrogels greatly limit their application prospects. Recently, a variety of strategies has been applied to prepare natural polymer-based hydrogels with enhanced mechanical properties, which generally exhibit stiffening, strengthening, and stretchable behaviors. This article summarizes the recent progress of natural polymer-based hydrogels with enhanced mechanical properties. From a structure point of view, four kinds of hydrogel are reviewed; double network hydrogels, nanocomposite hydrogels, click chemistry-based hydrogels, and supramolecular hydrogels. For each typical hydrogel, its preparation, structure, and mechanical performance are introduced in detail. At the end of this article, the current challenges and future prospects of hydrogels based on natural polymers are discussed and it is pointed out that 3D printing may offer a new platform for the development of natural polymer-based hydrogels.
Topics: Click Chemistry; Hydrogels; Mechanical Phenomena; Nanocomposites; Polymers
PubMed: 31364824
DOI: 10.1002/adhm.201900670 -
Advanced Science (Weinheim,... Jul 2021Through advances in molecular design, understanding of processing parameters, and development of non-traditional device fabrication techniques, the field of wearable and... (Review)
Review
Through advances in molecular design, understanding of processing parameters, and development of non-traditional device fabrication techniques, the field of wearable and implantable skin-inspired devices is rapidly growing interest in the consumer market. Like previous technological advances, economic growth and efficiency is anticipated, as these devices will enable an augmented level of interaction between humans and the environment. However, the parallel growing electronic waste that is yet to be addressed has already left an adverse impact on the environment and human health. Looking forward, it is imperative to develop both human- and environmentally-friendly electronics, which are contingent on emerging recyclable, biodegradable, and biocompatible polymer technologies. This review provides definitions for recyclable, biodegradable, and biocompatible polymers based on reported literature, an overview of the analytical techniques used to characterize mechanical and chemical property changes, and standard policies for real-life applications. Then, various strategies in designing the next-generation of polymers to be recyclable, biodegradable, or biocompatible with enhanced functionalities relative to traditional or commercial polymers are discussed. Finally, electronics that exhibit an element of recyclability, biodegradability, or biocompatibility with new molecular design are highlighted with the anticipation of integrating emerging polymer chemistries into future electronic devices.
Topics: Biocompatible Materials; Electronics; Humans; Polymers; Prostheses and Implants
PubMed: 34014619
DOI: 10.1002/advs.202101233 -
International Journal of Pharmaceutics Jun 2022Weakly acidic polymers, historically used as enteric coatings, are increasingly being employed in solubility-enhancing amorphous solid dispersion (ASD) formulations....
Weakly acidic polymers, historically used as enteric coatings, are increasingly being employed in solubility-enhancing amorphous solid dispersion (ASD) formulations. However, there is a lack of fundamental understanding around how these carboxylic acid-containing polymers dissolve, in particular when molecularly mixed with a lipophilic drug, as in an ASD. Identification of critical factors dominating their dissolution is vital for rational design of new polymers with enhanced release properties to address contemporary ASD delivery challenges, notably achieving good release at higher drug loadings. Herein, after identification of polymer solubilization via ionization as the rate limiting step for dissolution, hydroxypropylmethyl cellulose phthalate (HP-50) was converted to a salt by neutralization of the phthalic acid groups with different bases. Surface normalized dissolution was performed to assess the dissolution rate improvement achieved by polymer pre-ionization via salt formation. Polymer salts showed ∼ 3-fold faster release than HP-50 at pH 6.8 (50 mM sodium phosphate buffer). Importantly, a polymer salt was able to maintain a rapid dissolution rate, irrespective of the buffer capacity of the medium, whereas the protonated polymer showed greatly diminished dissolution as medium buffer capacity decreased toward physiological gastrointestinal tract values. HP-50 and two polymer salts were formulated into ASDs with miconazole, a lipophilic and weakly basic antifungal drug, at a 20% drug loading. Rapid drug release rates were achieved with polymer salt ASDs, whereby drug release was 14 times faster than from the protonated HP-50 ASD. This study highlights the critical role of polymer ionization and buffer capacity in the dissolution of HP-50-based systems and how pre-ionization via polymer salt formation is a successful strategy for the design of new polymers for improved ASD performance.
Topics: Drug Compounding; Drug Liberation; Pharmaceutical Preparations; Polymers; Salts; Solubility
PubMed: 35661745
DOI: 10.1016/j.ijpharm.2022.121886 -
Accounts of Chemical Research Oct 2022The mismanagement and leakage of plastic waste into the environment are failures of modern society. Once in the environment, plastic waste degrades into microplastics on...
The mismanagement and leakage of plastic waste into the environment are failures of modern society. Once in the environment, plastic waste degrades into microplastics on a time scale dependent on the resin chemistry and the associated biotic or abiotic process. The high surface area of microplastics results in the contamination of ecosystems through the leaching of toxic chemicals compounded with plastics during manufacturing. In addition, the small size of microplastics increases the likelihood that they will be inhaled or ingested, which has led to the bioaccumulation of microplastics with documented harm. Furthermore, microplastics are more readily aerosolized and distributed by weather systems to areas remote from locations where plastic waste has been mismanaged. Consequently, the carbon cycle must now account for plastic waste discharge, degradation, and dispersal in the environment after the end of useful life on a global scale.Circularity in plastics recycling endeavors to solve the waste problem while promoting greater sustainability. Circularity can be conducted at different stages in the plastics life cycle. Post-industrial recycling enabling scrap recovery in manufacturing is desirable for industrial material efficiency. However, the degradation of polymer chains currently limits the extent to which scrap recovery may be practiced repeatedly on the same material, particularly when the conversion of secondary resin to various plastic products is intolerant to deviations in polymer properties. Post-consumer recycling, on the other hand, is desirable for erasing the manufacturing history and use history of plastic-containing products. Post-consumer recycling involves cleaning and sorting plastic waste into bales, followed by mechanical recycling to produce dense feedstocks for downstream chemical processes required for deconstruction, monomer refinement, and secondary resin production. The efficiency and intensity of chemical processes used to recover reusable monomers or polymers remain low for most plastics. Consequently, there is an urgent need for novel polymers with useful or advantageous properties designed for recycling by addressing the challenges of resource recovery for reuse.In this Account, I discuss the design, discovery, and development of circular plastics based on the chemistry of polydiketoenamines. The diketoenamine bond provides a vantage point for the creation of thermoplastics, elastomers, and thermosets from polytopic triketone and amine monomers. The dynamic covalent character of the diketoenamine bond can be exploited during scrap recovery to provide resilience during mechanical recycling, maintaining baseline properties of the primary resin through multiple cycles of reuse. Furthermore, the hydrolyzability of the diketoenamine bond in strong acid can be exploited for efficient monomer recovery during chemical recycling. A systems-level analysis of polydiketoenamine circularity reveals substantive benefits in low-carbon manufacturing as well as a context to quantify the market potential, identifying use cases where circularity might be most effective. Leveraging these insights, it is possible to guide the process chemistry development necessary to scale monomer and resin production to meet imminent needs for more circular plastics in the market. These insights also provide a glimpse into the underlying molecular mechanisms critical to circularity in a new plastics economy while firmly establishing a role for creativity in polymer chemistry to provide innovative solutions.
Topics: Amines; Carbon; Ecosystem; Elastomers; Microplastics; Plastics; Polymers
PubMed: 36108255
DOI: 10.1021/acs.accounts.2c00308 -
Journal of Chemical Information and... Nov 2023Molecular modeling and simulations are essential tools in polymer science and engineering, enabling researchers to predict and understand the properties of...
Molecular modeling and simulations are essential tools in polymer science and engineering, enabling researchers to predict and understand the properties of macromolecules, including their structure, dynamics, thermodynamics, and overall material characteristics. However, one of the key challenges in polymer simulation and modeling lies in the initial topology design, as existing programs often lack the capability to generate all types of polymer forms. In this study, we present PolyFlin, a powerful Python module that addresses this limitation by allowing the generation of a wide range of polymer structures, from simple homopolymers to complex copolymers, including grafts, cyclic, star, dendrimers, and nets. PolyFlin offers a versatile and efficient tool for exploring and creating diverse polymer architectures, facilitating advancements in various fields that require precise polymer modeling and simulation.
Topics: Polymers; Models, Molecular; Computer Simulation; Macromolecular Substances
PubMed: 37851376
DOI: 10.1021/acs.jcim.3c01221