Abstract:First detailed quantum chemical calculation on the reaction mechanism of electron-beam initiated cross-linking reaction of methacrylated dextran are presented.
“…The use of electron-beam irradiation to initiate radical formation is another method avoiding the use of radicalforming chemicals. The preparation of cryogels based on synthetic polymers [59], but also on polysaccharide- [60] and GAG-methacrylates [24][25][26], by this fast and efficient method has been reported. Photoinitiated free radical polymerization using UV (200-400 nm) or visible (400-800 nm) light is another option to crosslink (meth)acrylated polymers and is often used in the preparations of tissue engineering scaffolds [61,62].…”
Cryogels are a class of macroporous, interconnective hydrogels polymerized at sub-zero temperatures forming mechanically robust, elastic networks. In this review, latest advances of cryogels containing mainly glycosaminoglycans (GAGs) or composites of GAGs and other natural or synthetic polymers are presented. Cryogels produced in this way correspond to the native extracellular matrix (ECM) in terms of both composition and molecular structure. Due to their specific structural feature and in addition to an excellent biocompatibility, GAG-based cryogels have several advantages over traditional GAG-hydrogels. This includes macroporous, interconnective pore structure, robust, elastic, and shape-memory-like mechanical behavior, as well as injectability for many GAG-based cryogels. After addressing the cryogelation process, the fabrication of GAG-based cryogels and known principles of GAG monomer crosslinking are discussed. Finally, an overview of specific GAG-based cryogels in biomedicine, mainly as polymeric scaffold material in tissue regeneration and tissue engineering-related controlled release of bioactive molecules and cells, is provided.
“…The use of electron-beam irradiation to initiate radical formation is another method avoiding the use of radicalforming chemicals. The preparation of cryogels based on synthetic polymers [59], but also on polysaccharide- [60] and GAG-methacrylates [24][25][26], by this fast and efficient method has been reported. Photoinitiated free radical polymerization using UV (200-400 nm) or visible (400-800 nm) light is another option to crosslink (meth)acrylated polymers and is often used in the preparations of tissue engineering scaffolds [61,62].…”
Cryogels are a class of macroporous, interconnective hydrogels polymerized at sub-zero temperatures forming mechanically robust, elastic networks. In this review, latest advances of cryogels containing mainly glycosaminoglycans (GAGs) or composites of GAGs and other natural or synthetic polymers are presented. Cryogels produced in this way correspond to the native extracellular matrix (ECM) in terms of both composition and molecular structure. Due to their specific structural feature and in addition to an excellent biocompatibility, GAG-based cryogels have several advantages over traditional GAG-hydrogels. This includes macroporous, interconnective pore structure, robust, elastic, and shape-memory-like mechanical behavior, as well as injectability for many GAG-based cryogels. After addressing the cryogelation process, the fabrication of GAG-based cryogels and known principles of GAG monomer crosslinking are discussed. Finally, an overview of specific GAG-based cryogels in biomedicine, mainly as polymeric scaffold material in tissue regeneration and tissue engineering-related controlled release of bioactive molecules and cells, is provided.
“…The existence of the α(1 → 6) glycosidic bond leads to the solubility of dextran in water and some polar organic solvents (e.g., DMSO, and DMF), which qualified it for various biomedical applications. , However, the highly hydrophilic feature of this natural polymer restricts its application range. Some chemical modification strategies, including esterification using both organic and inorganic reagents, − etherification, , sulfonation, , silylation, , and polymer grafting, − have been employed toward induction of hydrophobicity, which allows the encapsulation of drugs through emulsion chemistry. Another approach toward modified dextran is its cross-linking using both physical interactions and chemical reactions. − The chemical modification leads to a decrease in the rate of enzymatic biodegradation processes …”
“…219,230 However, the highly hydrophilic feature of this natural polymer restricts its application range. Some chemical modification strategies, including esterification using both organic and inorganic reagents, 232−234 etherification, 216,235 sulfonation, 236,237 silylation, 238,239 and polymer grafting, 240−242 have been employed toward induction of hydrophobicity, which allows the encapsulation of drugs through emulsion chemistry. Another approach toward modified dextran is its cross-linking using both physical interactions 243 and chemical reactions.…”
It is an unquestionable fact that cancer, also called
malignancy, has or will soon become the major global health care problem
with an increasing incidence worldwide. Conventional treatment approaches
(e.g., radiation or chemotherapy) treat both cancerous and surrounding
normal tissues simultaneously, which leads to a poor therapeutic effect
on tumors and severe toxic side effects on healthy tissues. Considering
these thematic issues, the design and development of more efficient
treatment approaches is one of the most important demands of health
care in the near future. In this context, the emergence of nanotechnology
opens new opportunities for addressing the issues of conventional
drug delivery systems (DDSs) for cancer therapy. Theranostic nanomedicines
are indebted to the advent of nanotechnology and were introduced by
Funkhouser in 2002. These nanomedicines are the newest DDSs that combine
diagnostic and therapeutic properties into a single platform. Theranostic
nanomedicines are generally composed of targeting agents, diagnostic
tracers, effective drug(s), and biomaterial(s) as the matrix to the
formulation. Among these, biomaterials have a pivotal role in theranostic
nanomedicines due to their direct influence on the system effectiveness.
In this context, natural polymers can be considered as potential candidates,
mainly due to their inherent physicochemical as well as biological
advantages. However, natural polymers have some drawbacks, which can
be addressed through the chemical modification approach. In this review,
we will highlight the recent progress in the development of theranostic
nanomedicines based on chemically modified natural polymers as well
as research prospects for the future.
“…In our recent study, we focused on dextran methacrylate (Dex-MA), which, due to the presence of a polymerizable methacrylic group (-MA), is capable of forming biocompatible, insoluble macroscopic hydrogels at low doses of ionizing radiation [ 29 ]. Another successful application of radiation for cross-linking of dextran methacrylate and hyaluronan methacrylate cryogels has been demonstrated by Reichelt and coworkers [ 30 , 31 , 32 , 33 ]. Therefore, radiation technology seems to be a versatile, additive-free and clean tool to produce chemically cross-linked, biocompatible hydrogels based on methacrylated polysaccharides.…”
Dextran methacrylate (Dex-MA) is a biodegradable polysaccharide derivative that can be cross-linked by ionizing radiation. It is therefore considered a potential replacement for synthetic hydrophilic polymers in current radiation technologies used for synthesizing hydrophilic cross-linked polymer structures such as hydrogels, mainly for medical applications. This work is focused on the initial steps of radiation-induced cross-linking polymerization of Dex-MA in water. Rate constants of two major transient water radiolysis products—hydroxyl radicals (•OH) and hydrated electrons (eaq−)—with various samples of Dex-MA (based on 6–500 kDa dextrans of molar degree of substitution or DS with methacrylate groups up to 0.66) as well as non-substituted dextran were determined by pulse radiolysis with spectrophotometric detection. It has been demonstrated that these rate constants depend on both the molecular weight and DS; reasons for these effects are discussed and reaction mechanisms are proposed. Selected spectral data of the transient species formed by •OH- and eaq−-induced reactions are used to support the discussion. The kinetic data obtained in this work and their interpretation are expected to be useful for controlled synthesis of polysaccharide-based hydrogels and nanogels of predefined structure and properties.
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