Biomacromolecules最新文献

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Double-Network Hydrogel Based on Methacrylated Chitosan/Hyaluronic Acid Coacervate for Enhanced Wet-Tissue Adhesion.
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2025-03-18 DOI: 10.1021/acs.biomac.4c01645
Dafeng Deng, Deyi Peng, Jianhua Lv, Wenchang Zhang, Huaqin Tian, Tieqiang Wang, Mi Wu, Yan Zhao
{"title":"Double-Network Hydrogel Based on Methacrylated Chitosan/Hyaluronic Acid Coacervate for Enhanced Wet-Tissue Adhesion.","authors":"Dafeng Deng, Deyi Peng, Jianhua Lv, Wenchang Zhang, Huaqin Tian, Tieqiang Wang, Mi Wu, Yan Zhao","doi":"10.1021/acs.biomac.4c01645","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01645","url":null,"abstract":"<p><p>Developing robust wet tissue adhesives remains challenging due to interfacial water and irregular surfaces. While polyelectrolyte coacervates demonstrate promising hydrophobic/fluidic properties for wet adhesion, their low cohesion limits practical applications. Herein, a wet tissue bioadhesive based on coacervates formed from low- molecular-weight methacrylated chitosan (CSMA) and hyaluronic acid (HA) is reported. These homogeneous and transparent coacervates displayed high solid content (∼18.0%), fluidity (∼10<sup>5</sup> mPa·s), and tunable mechanical properties. Upon application to wet tissue surfaces, the coacervate can be photo-cross-linked to form a double-network hydrogel in situ, resulting in improved cohesion and durable adhesion. The resulting CSMA-HA hydrogel demonstrated robust adhesion to tissues, with a bursting pressure of 374 mmHg. Remarkably, the bursting pressure can be further enhanced (∼623 mmHg) after 24 h of PBS immersion due to dynamic bond reorganization and low swelling. The demonstrated stability under physiological conditions and robust wet adhesion position CSMA-HA coacervates as a transformative platform for tissue adhesive applications.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143655465","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Analysis of HSA-PAA Complexation Using SEC-SAXS Combination: Unraveling Stoichiometry, Reversibility, and Interaction Specificity.
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2025-03-17 DOI: 10.1021/acs.biomac.4c01749
Charaf Eddine Merzougui, Patrice Bacchin, Pierre Aimar, Christel Causserand, Pierre Roblin
{"title":"Analysis of HSA-PAA Complexation Using SEC-SAXS Combination: Unraveling Stoichiometry, Reversibility, and Interaction Specificity.","authors":"Charaf Eddine Merzougui, Patrice Bacchin, Pierre Aimar, Christel Causserand, Pierre Roblin","doi":"10.1021/acs.biomac.4c01749","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01749","url":null,"abstract":"<p><p>This work leverages the integration of size exclusion chromatography (SEC) with small-angle X-ray scattering (SAXS) to investigate the complex interactions between human serum albumin (HSA) and poly(acrylic acid) (PAA). The SEC-SAXS approach is proven in this study to effectively eliminate aggregates, enhancing data quality and revealing intricate details of protein-polymer associations. Initial findings demonstrate that HSA maintains its native structure across pH 5-8 and that HSA shows no significant interaction with the neutral polyethylene glycol (PEG). This highlights the critical role of charge regulation and electrostatic forces in HSA-PAA complex formation previously reported and the specificity of this interaction. The study further reveals that the HSA-PAA complex stoichiometry is highly dependent on PAA size, with larger PAA chains forming more elongated structures. The binding stoichiometry is then shown to increase nonlinearly, suggesting a delicate balance between attractive HSA-PAA and repulsive HSA-HSA interactions. Notably, HSA-PAA complexes exhibit reversible behavior, dissociating at pH > 5 and in media devoid of PAA.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143646492","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Side-Functionalization of Poly(l-methionine) for Ice Control.
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2025-03-14 DOI: 10.1021/acs.biomac.5c00086
Qingjing Niu, Ke Shang, Huimin Han, Binlin Chen, Kongying Zhu, Lixia Ren, Xiaoyan Yuan
{"title":"Side-Functionalization of Poly(l-methionine) for Ice Control.","authors":"Qingjing Niu, Ke Shang, Huimin Han, Binlin Chen, Kongying Zhu, Lixia Ren, Xiaoyan Yuan","doi":"10.1021/acs.biomac.5c00086","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00086","url":null,"abstract":"<p><p>Controlling ice growth is crucial during the cryopreservation of cells, but the current application of small molecules as cryoprotectants still remains a challenge. Inspired by structures of natural antifreeze (glyco)proteins, in this work, functionalized poly(l-methionine)s (PMets) are synthesized with different side groups including hydroxyl, threonine-mimetic with both methyl and hydroxyl groups (PMet-MOH), zwitterion with carboxyl and sulfonium (PMet-COOH), glycerol, and trehalose pendants. Results suggest that these functionalized PMets tend to self-assemble into 100-300 nm nanoparticles with positive charges in water. The functional structures have a remarkable influence on their ice control properties. It is supposed that PMet-MOH inhibits ice growth possibly through the adsorption mechanism by adjacent methyl and hydroxyl groups, whereas trehalose-tethered PMet can restrict diffusion of water molecules with the strongest ice recrystallization inhibition activity and zwitterionic PMet-COOH promotes ice nucleation obviously. This work offers valuable insight into the development of functional polypeptides as promising biocompatible cryoprotectants.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143622858","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Multiple Pendants-Bearing Triglucosides for Membrane Protein Studies: Effects of Pendant Length and Number on Micelle Interior Hydration and Protein Stability.
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2025-03-14 DOI: 10.1021/acs.biomac.5c00036
Aiman Sadaf, Hong Sik Yun, Hajin Lee, Samantha Stanfield, Baoliang Lan, Kristine Salomon, Menebere Woubshete, Seonghoon Kim, Muhammad Ehsan, Hyemi Bae, Bernadette Byrne, Claus J Loland, Xiangyu Liu, Lan Guan, Wonpil Im, Pil Seok Chae
{"title":"Multiple Pendants-Bearing Triglucosides for Membrane Protein Studies: Effects of Pendant Length and Number on Micelle Interior Hydration and Protein Stability.","authors":"Aiman Sadaf, Hong Sik Yun, Hajin Lee, Samantha Stanfield, Baoliang Lan, Kristine Salomon, Menebere Woubshete, Seonghoon Kim, Muhammad Ehsan, Hyemi Bae, Bernadette Byrne, Claus J Loland, Xiangyu Liu, Lan Guan, Wonpil Im, Pil Seok Chae","doi":"10.1021/acs.biomac.5c00036","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00036","url":null,"abstract":"<p><p>Membrane proteins play central roles in cell physiology and are the targets of over 50% of FDA-approved drugs. In the present study, we prepared single alkyl-chained triglucosides decorated with multiple pendants, designated multiple pendant-bearing glucosides (MPGs), to enhance membrane protein stability. The new detergents feature two and four pendants of varying size at the hydrophilic-lipophilic interfaces, designated MPG-Ds and MPG-Ts, respectively. When tested with model membrane proteins, including the human adrenergic receptor (β<sub>2</sub>AR), the tetra-pendant-bearing MPGs (MPG-Ts) demonstrated superior performance compared to the dipendant analogs (MPG-Ds) and the gold standard DDM. All-atom molecular dynamics (MD) simulations results reveal that the four-pendant configuration of this detergent is remarkably effective in excluding water from the hydrophobic micelle interiors compared to the dipendant MPGs and DDM, an unprecedented feature of this new detergent. Our findings provide a novel strategy for designing water-resistant detergents, advancing the field of membrane protein research.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143629978","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Regulating the Characteristic Networks of Biodegradable Poly(l-malic acid-ε-caprolactone) Shape-Memory Materials: From Plastics to Elastomers.
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2025-03-13 DOI: 10.1021/acs.biomac.5c00163
Jing Song, Jiali Jiao, Chenguang Jiang, Yaxin Qiu, Defeng Wu
{"title":"Regulating the Characteristic Networks of Biodegradable Poly(l-malic acid-ε-caprolactone) Shape-Memory Materials: From Plastics to Elastomers.","authors":"Jing Song, Jiali Jiao, Chenguang Jiang, Yaxin Qiu, Defeng Wu","doi":"10.1021/acs.biomac.5c00163","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00163","url":null,"abstract":"<p><p>Developing new biodegradable polyesters with well-defined structures is of interest. We reported an attractive two-component aliphatic polyester-based thermoset, which was prepared via the esterification of biomass-derived l-malic acid oligomers and three-arm poly(ε-caprolactone) (3a-PCL) triols. The chemical network formed via the ester bonding and physical network caused by the crystallization of a 3a-PCL arm chain coexist in the thermoset, and the competition of the two characteristic networks leads to a negative correlation between the degree of covalent cross-linking and the degree of crystallization; thereby, the mechanical state of the thermosets can be easily tuned: from the plastic to elastomer state. Moreover, the crystallization temperature and melting point of the thermosets range in 30 °C ∼ 50 °C and -7 °C ∼ 18 °C, respectively, which are favorable for shape morphing as the thermosets are used as shape-memory materials. This work also provides valuable information about tailoring the mechanical and thermal properties of star-shaped polyester-based thermosets.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143622854","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
In Vitro Evaluation of Gelatin-Based Hydrogels as Potential Fillers for Corneal Wounds. 明胶水凝胶作为角膜伤口潜在填充物的体外评估
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2025-03-13 DOI: 10.1021/acs.biomac.4c01759
Cristina Romo-Valera, Eric A Appel, Jaime Etxebarria, Jon Arluzea, Noelia Andollo
{"title":"In Vitro Evaluation of Gelatin-Based Hydrogels as Potential Fillers for Corneal Wounds.","authors":"Cristina Romo-Valera, Eric A Appel, Jaime Etxebarria, Jon Arluzea, Noelia Andollo","doi":"10.1021/acs.biomac.4c01759","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01759","url":null,"abstract":"<p><p>Corneal persistent epithelial defects are common ophthalmic injuries that can cause significant visual and structural damage. While diagnosis is straightforward, treatment remains challenging. Noninvasive therapies like eye drops are preferred, but severe neurotrophic keratopathy may require surgical interventions. This study explores gelatin-based hydrogels as noninvasive alternatives for corneal repair. Four photo-cross-linkable hydrogels with gelatin and riboflavin phosphate (RFP) were evaluated: a control and variants incorporating 2.5% dextran (D), 0.4% hyaluronic acid (HA), or 1% methylcellulose (MC). In vitro assessments included physicochemical properties, biocompatibility, and release kinetics alongside ex vivo wound healing assays. The gelatin-RFP hydrogel maintained corneal transparency, while additives reduced it. Dextran slowed compound release, and HA and MC reduced the release rate of larger molecules. All hydrogels showed excellent biocompatibility, and ex vivo models confirmed re-epithelialization, though slower than controls. The unmodified gelatin-RFP hydrogel demonstrated the best potential for corneal tissue engineering, supporting its future clinical translation.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143622853","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synthetic Strategy to Build High-Molecular-Weight Poly(L-tyrosine) and Its Unexplored β-Sheet Block Copolymer Nanoarchitectures.
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2025-03-12 DOI: 10.1021/acs.biomac.5c00046
Parshuram Kambale, Rahul Nisal, Manickam Jayakannan
{"title":"Synthetic Strategy to Build High-Molecular-Weight Poly(L-tyrosine) and Its Unexplored β-Sheet Block Copolymer Nanoarchitectures.","authors":"Parshuram Kambale, Rahul Nisal, Manickam Jayakannan","doi":"10.1021/acs.biomac.5c00046","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00046","url":null,"abstract":"<p><p>Synthesis of high-molecular-weight polypeptides and their block copolymer macromolecular architectures from β-sheet-promoting L-amino acids is still an unresolved problem. Here, an elegant steric hindrance-assisted ring-opening polymerization (SHAROP) strategy is introduced to access β-sheet poly(L-tyrosine) having more than 250 units. The scope of the synthetic methodology is expanded to access unexplored poly(L-tyrosine)-based higher-order β-sheet block copolymer nanoassemblies. In this strategy, a <i>tert-</i>butyl benzyl unit is employed as a steric handle that imbibes the solubility by promoting the α-helical conformation in the propagating polypeptide chains. The living ROP process enables the synthesis of well-defined block copolymers initiated by poly(L-tyrosine) living-chain ends or growing the poly(L-tyrosine) chains from the pre-existing macroinitiators of poly(L-glutamate) or poly(L-lysine). Acid-catalyzed postpolymerization deprotection restores the poly(L-tyrosine) blocks in their nascent β-sheet conformations. Thioflavin-T fluorescence assay establishes the β-sheet core-shell structures of these nanoassemblies, which are found to be nontoxic to mammalian cell lines.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143612819","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Accelerated Missense Mutation Identification in Intrinsically Disordered Proteins Using Deep Learning.
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2025-03-12 DOI: 10.1021/acs.biomac.4c01124
Swarnadeep Seth, Aniket Bhattacharya
{"title":"Accelerated Missense Mutation Identification in Intrinsically Disordered Proteins Using Deep Learning.","authors":"Swarnadeep Seth, Aniket Bhattacharya","doi":"10.1021/acs.biomac.4c01124","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01124","url":null,"abstract":"<p><p>We use a combination of Brownian dynamics (BD) simulation results and deep learning (DL) strategies for the rapid identification of large structural changes caused by missense mutations in intrinsically disordered proteins (IDPs). We used ∼6500 IDP sequences from MobiDB database of length 20-300 to obtain gyration radii from BD simulation on a coarse-grained single-bead amino acid model (HPS2 model) used by us and others [Dignon, G. L. <i>PLoS Comput. Biol.</i> 2018, 14, e1005941,Tesei, G. <i>Proc. Natl. Acad. Sci. U.S.A.</i> 2021, 118, e2111696118,Seth, S. <i>J. Chem. Phys.</i> 2024, 160, 014902] to generate the training sets for the DL algorithm. Using the gyration radii ⟨<i>R</i><sub>g</sub>⟩ of the simulated IDPs as the training set, we develop a multilayer perceptron neural net (NN) architecture that predicts the gyration radii of 33 IDPs previously studied by using BD simulation with 97% accuracy from the sequence and the corresponding parameters from the HPS model. We now utilize this NN to predict gyration radii of every permutation of missense mutations in IDPs. Our approach successfully identifies mutation-prone regions that induce significant alterations in the radius of gyration when compared to the wild-type IDP sequence. We further validate the prediction by running BD simulations on the subset of identified mutants. The neural network yields a (10<sup>4</sup>-10<sup>6</sup>)-fold faster computation in the search space for potentially harmful mutations. Our findings have substantial implications for rapid identification and understanding of diseases related to missense mutations in IDPs and for the development of potential therapeutic interventions. The method can be extended to accurate predictions of other mutation effects in disordered proteins.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143612818","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Fabrication of pH- and Ultrasound-Responsive Polymeric Micelles: The Effect of Amphiphilic Block Copolymers with Different Hydrophilic/Hydrophobic Block Ratios for Self-Assembly and Controlled Drug Release.
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2025-03-11 DOI: 10.1021/acs.biomac.4c01202
Hong-Xiang Wei, Ming-Hsin Liu, Tzu-Ying Wang, Meng-Hsiu Shih, Jiashing Yu, Yi-Cheun Yeh
{"title":"Fabrication of pH- and Ultrasound-Responsive Polymeric Micelles: The Effect of Amphiphilic Block Copolymers with Different Hydrophilic/Hydrophobic Block Ratios for Self-Assembly and Controlled Drug Release.","authors":"Hong-Xiang Wei, Ming-Hsin Liu, Tzu-Ying Wang, Meng-Hsiu Shih, Jiashing Yu, Yi-Cheun Yeh","doi":"10.1021/acs.biomac.4c01202","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01202","url":null,"abstract":"<p><p>Stimuli-responsive polymeric vehicles can change their physical or chemical properties when exposed to internal or external triggers, enabling precise spatiotemporal control of drug release. Nevertheless, systematic research is lacking in preparing dual stimuli-responsive amphiphilic block copolymers with different hydrophilic/hydrophobic block ratios in forming self-assembled structures. Here, we synthesized two types of block copolymers consisting of the hydrophobic segments (i.e., pH-responsive 2-(diethylamino)ethyl methacrylate (DEA) and ultrasound-responsive 2-methoxyethyl methacrylate (MEMA)) and hydrophilic poly(ethylene glycol) methyl ether (mPEG) segments, forming mPEG<sub>X</sub>-<i>b</i>-P(DEA<sub>Y</sub>-<i>co</i>-MEMA<sub>Z</sub>). These amphiphilic block copolymers can self-assemble to form polymeric micelles, and their structures (e.g., size) and properties (e.g., critical vesicle concentration, stability, stimuli-responsiveness to pH and ultrasound, drug loading efficiency, and controlled drug release performance) were thoroughly investigated. <i>In vitro</i> cell studies further demonstrate that ultrasound can efficiently trigger drug release from polymeric micelles, emphasizing their potential for controlled drug delivery in therapeutic applications.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143603005","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Surface-Vinylated Cellulose Nanocrystals as Cross-Linkers for Hydrogel Composites.
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2025-03-11 DOI: 10.1021/acs.biomac.4c01619
Marcel Kröger, Timo Pääkkönen, Lukas Fliri, Anna F Lehrhofer, Irina Sulaeva, Antje Potthast, Eero Kontturi
{"title":"Surface-Vinylated Cellulose Nanocrystals as Cross-Linkers for Hydrogel Composites.","authors":"Marcel Kröger, Timo Pääkkönen, Lukas Fliri, Anna F Lehrhofer, Irina Sulaeva, Antje Potthast, Eero Kontturi","doi":"10.1021/acs.biomac.4c01619","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01619","url":null,"abstract":"<p><p>Cellulose nanocrystal (CNC) fillers have been shown to significantly improve the performance of polymer composites and hydrogels, elevating both strength and toughness. Polymer grafting from the surface of the nanocrystals has been employed to enhance matrix-filler interactions and keep the fillers dispersed within the matrix. However, such approaches often rely on multistep syntheses and diligent process control. Here, we propose modifying the nanocrystal surface to carry vinyl moieties, turning the particles into cross-linking comonomers. Using allyl glycidyl ether in an aqueous modification route, we were able to decorate the CNCs with varying amounts of vinyl moieties. Subsequent dispersion in 2-hydroxy methacrylate and thermally initiated free radical polymerization yielded composite materials that showed superior mechanical performance compared to those obtained from monomeric cross-linkers and unmodified CNCs. The large discrepancies in the observed glass transition temperatures of the obtained materials suggest, however, that the impact of the fillers on the polymerization kinetics is significant and less easily explained.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143603022","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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