PolymerPub Date : 2024-12-21DOI: 10.1016/j.polymer.2024.127968
Gloria Signorato, Lea R. Klauke, Philipp Haida, Tobias Vossmeyer, Volker Abetz
{"title":"Superparamagnetic Iron Oxide Nanoparticle – Vitrimer Nanocomposites: Reprocessable and Multi-Responsive Materials","authors":"Gloria Signorato, Lea R. Klauke, Philipp Haida, Tobias Vossmeyer, Volker Abetz","doi":"10.1016/j.polymer.2024.127968","DOIUrl":"https://doi.org/10.1016/j.polymer.2024.127968","url":null,"abstract":"The field of stimuli-responsive soft materials is rapidly evolving, particularly with recent advances in the design and fabrication of magnetic soft materials. Magnetically responsive elastomers, which incorporate magnetic particles into an elastomeric matrix, exhibit rapid and reversible actuation in the presence of a magnetic field, making them highly suitable for the development of flexible, remote-controlled soft robots. However, conventional crosslinked elastomer materials often lack recyclability and the versatile properties associated with vitrimer materials. Vitrimers, which are dynamically crosslinked polymers, can be reprocessed upon heating and offer valuable features such as recyclability and self-healing. In this study, we developed vitrimer nanocomposites by incorporating 5 to 15 wt.% superparamagnetic iron oxide nanoparticles (SPIONs) into a vinylogous urethane vitrimer matrix, yielding materials that exhibit both thermal and magnetic responsiveness. Furthermore, a novel acetoacetylated ligand with a phosphonic acid anchoring group was utilized to modify the surface of SPIONs, enhancing their stability and enabling their covalent linking to the vitrimer matrix. The crosslinking of the nanoparticles to the matrix improves the mechanical properties, including increased tensile stress and strain. Since the nanoparticles are covalently bound to the matrix, the resulting material can be reprocessed and recycled without compromising the uniform distribution of SPIONs, thereby promoting a closed-loop cycle of reuse and recycling while preserving the mechanical and magnetic properties of the nanocomposites. The integration of SPIONs into vinylogous urethane vitrimers results in the development of sustainable advanced materials with enhanced stability and functionality, highlighting their potential across various applications.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"78 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2024-12-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867606","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}
PolymerPub Date : 2024-12-20DOI: 10.1016/j.polymer.2024.127971
Bar Shlomo-Avitan, Majd Machour, Samah Saied Ahmad, Yoav Friedler, Shulamit Levenberg, Michael S. Silverstein
{"title":"Emulsion-templated macroporous polycaprolactone: Synthesis, degradation, additive manufacturing, and cell-growth","authors":"Bar Shlomo-Avitan, Majd Machour, Samah Saied Ahmad, Yoav Friedler, Shulamit Levenberg, Michael S. Silverstein","doi":"10.1016/j.polymer.2024.127971","DOIUrl":"https://doi.org/10.1016/j.polymer.2024.127971","url":null,"abstract":"PolyHIPEs are macroporous polymers templated within high internal phase emulsions (HIPEs). The ability to tailor the macromolecular and porous structures makes polyHIPEs of interest for three dimensional tissue engineering scaffolds. In this work, polyHIPEs with densities ranging from 0.18 to 0.28 g/cc were synthesized from novel biodegradable poly(ɛ-caprolactone) (PCL) macromers based on methacrylated oligomeric PCL diols of various molecular weights. Different types of internal phases generated porous structures that varied from networks of channels to highly interconnected voids. The crosslinked macromolecular structure limited PCL crystallization, resulting in elastomeric behavior with moduli of around 20 kPa. The HIPEs proved suitable for 3D printing both in air and in an innovative gel-bath. The suitability of the polyHIPEs for tissue engineering applications was indicated by their moduli, by their complete degradation within 4 h in 3 M NaOH, and by the mesenchymal stem cells adhering and proliferating. The high level of viability can be attributed to the porosity that enables sufficient nutrient and waste diffusion. These results provide a foundation for designing 3D HIPE inks for printing macroporous tissue engineering scaffolds.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"55 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867344","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}
{"title":"Self-healing, high mechanical strength and adhesive supramolecular hydrogel based on triblock copolymer for flexible electronics","authors":"Yingying Huang, Yuxuan Yang, Yuhao Yang, Shiying Chen, Simin Liu, Xiongzhi Zhang","doi":"10.1016/j.polymer.2024.127966","DOIUrl":"https://doi.org/10.1016/j.polymer.2024.127966","url":null,"abstract":"The development of conductive hydrogels with high mechanical strength, self-healing and adhesive for applications in flexible electronics remains challenging. In this work, triblock copolymer poly(2-hydroxyethyl acrylate-<em>co</em>-1-benzyl-3-vinylimidazolium bromide)-<em>b</em>-polyazobenzene-<em>b-</em>poly(2-hydroxyethyl acrylate-<em>co</em>-1-benzyl-3-vinylimidazolium bromide) were synthesized through reversible addition-fragmentation chain transfer polymerization. The assembly of triblock copolymer, and cucurbit[8]uril based dynamic host-guest interactions were employed to fabricate 3D network of supramolecular hydrogel. Investigations on the properties of the supramolecular hydrogel show that the dynamic and reversible supramolecular interactions endow the hydrogel with high stretchability (1120%) and high self-healing efficient (98%, 48 h). Interestingly, the soft poly(2-hydroxyethyl acrylate) segments and intermediate functional groups contribute to the adhesive performance hydrogel. Thanks to its excellent conductivity, the as-obtained hydrogel exhibits remarkable capacity for detecting various levels of motion. The supramolecular hydrogel is great significance for the efficient development of wearable electronics and flexible devices with high mechanical strength, self-healing, adhesive, photo-responsivity, conductivity and biocompatibility.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"1 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857976","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}
PolymerPub Date : 2024-12-20DOI: 10.1016/j.polymer.2024.127970
Davide Tranchida, Dietmar Salaberger, Lada Vukusic, Gerhard Hubner, Mithun Goswami, Andreas Albrecht, Susana Filipe
{"title":"Advanced characterization of recycled polyolefins: a holistic approach to study their microstructure and contaminations","authors":"Davide Tranchida, Dietmar Salaberger, Lada Vukusic, Gerhard Hubner, Mithun Goswami, Andreas Albrecht, Susana Filipe","doi":"10.1016/j.polymer.2024.127970","DOIUrl":"https://doi.org/10.1016/j.polymer.2024.127970","url":null,"abstract":"Achieving the detailed knowledge of recycled materials composition is a formidable task due to the presence of organic and inorganic contaminations. Additionally, the complexity of the microstructure is far superior to the one of virgin materials where the production process is well controlled. Nonetheless, this task is of paramount importance because properties are affected in crucial ways. In this work we studied recycled polyolefin grades with several techniques, in particular through their adaptation to the analysis of this class of materials, to combine the information and obtain a detailed knowledge of their characteristics. Thermogravimetric Analysis (TGA), X-Ray Fluorescence (XRF), X-Ray Computed Tomography (CT) and Scanning Electron Microscopy (SEM) were used to characterize inorganic contaminations. CT and Fourier Transform Infrared Spectroscopy (FTIR) were used to characterize organic contaminations. Microstructure details were evaluated by Nuclear Magnetic Resonance (NMR) and fractionation and thermal analysis methods. Also the limitations of the various techniques are addressed.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"27 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867345","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}
{"title":"Synergistic Toughening of Polylactide by Layer Structure and Network Structure","authors":"Mingtao Sun, Ziqing Zhang, Yipeng He, Weixia Yan, Muhuo Yu, Keqing Han","doi":"10.1016/j.polymer.2024.127969","DOIUrl":"https://doi.org/10.1016/j.polymer.2024.127969","url":null,"abstract":"This work demonstrates that environmental-friendly bio-based and biodegradable polylactide (PLA) can be significantly toughened by processing modification alone. The notched Izod impact strength of the prepared PLA increased from 3.4 kJ/m<sup>2</sup> to 89.9 kJ/m<sup>2</sup> without other components incorporated. We emphasized the changes in crystalline structure and traced the layer and network structures through etching experiment and dissolution experiment. The results manifested that the synergistic effect of layer structure formed by in-situ oriented crystallites and the network structure generated by stereocomplex crystallites (SCs) with stronger intermolecular force and high density tie chains was the dominant reason for the toughness enhancement. Moreover, the tensile strength and Vicat softening temperature of PLA was improved simultaneously, which reached 92.4 MPa and 167.6 °C, respectively. Notably, by comparing with the petroleum-based engineering plastics, the prepared PLA exhibits excellent comprehensive performance and can be used as a green engineering plastic to expand its potential applications.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"55 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857973","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}
PolymerPub Date : 2024-12-18DOI: 10.1016/j.polymer.2024.127965
Masoud Zamani, Dayron M. Leyva Rodriguez, Ziwen Zhang, Camila Sabatini, Mark T. Swihart, Michelle B. Visser, Chong Cheng
{"title":"Synthesis of Polymer-Clindamycin Conjugates through Lipase-Catalyzed Esterification and RAFT Polymerization","authors":"Masoud Zamani, Dayron M. Leyva Rodriguez, Ziwen Zhang, Camila Sabatini, Mark T. Swihart, Michelle B. Visser, Chong Cheng","doi":"10.1016/j.polymer.2024.127965","DOIUrl":"https://doi.org/10.1016/j.polymer.2024.127965","url":null,"abstract":"Relative to free antibiotics, polymer-antibiotic conjugates (PACs) can possess modified solubility, sustained release behavior, and prolonged bioactivity in biological systems. As one of the most potent and ubiquitous antibiotics, clindamycin (Clin) has broad-spectrum antibiotic activity with versatile medical applications. However, polymer-Clin conjugates have not been reported yet. This can be partly ascribed to the difficulties in selective modification of Clin which possesses multiple reactive hydroxyl groups. In this study, we employed immobilized lipase as a bio-based catalyst for the facile and highly regioselective synthesis of a methacrylic-functionalized monomer-Clin conjugate via a one-step reaction. Reversible addition fragmentation chain transfer (RAFT) polymerization was then employed to synthesize copolymers of the monomer-Clin conjugate with 2-hydroxymethyl methacrylate or 3-[(3-acrylamidopropyl) dimethylammonio]propanoate to achieve water-insoluble and water-soluble Clin-containing PACs, respectively. These PACs possessed well-defined structures with high Clin content (33-46 wt%), as confirmed by <sup>1</sup>H NMR and gel permeation chromatography characterizations. Living nature of the RAFT process for the synthesis of PACs was verified by a chain-extension experiment. With sustained Clin release behavior, these PACs further demonstrated notable antibacterial activities against Streptococcus mutans, as verified by zone of inhibition tests. Collectively, this work presents an efficient method to synthesize different types of Clin-containing PACs, with potential for use in diverse antibacterial applications.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"258 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142840899","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}
PolymerPub Date : 2024-12-18DOI: 10.1016/j.polymer.2024.127964
Die Luo, Ben Niu, Xin Wang, Xianru He
{"title":"Self-Healing Thermoplastic Elastomers Enabled by Dynamic Ordered Microphase Crosslinking of Random Copolymers","authors":"Die Luo, Ben Niu, Xin Wang, Xianru He","doi":"10.1016/j.polymer.2024.127964","DOIUrl":"https://doi.org/10.1016/j.polymer.2024.127964","url":null,"abstract":"Self-healing thermoplastic elastomers based on reversible supramolecular or covalent bonding often suffer from low mechanical strength to compensate their molecular mobility in ensuring effective end-to-end contact during repair. Herein, we propose a new strategy for self-healing elastomers using dynamic ordered microphase as the self-healing motif. A series of polyacrylonitrile-<em>co</em>-poly(<em>n</em>-butyl acrylate) copolymer elastomers are prepared by simple free radical polymerization. These elastomers, within a certain range of comonomer ratios, exhibit remarkable self-healing capabilities in bulk form. The ever-maintained strength of the repaired elastomer is attributed to the retention of intrinsic material strength by the dynamic ordered phase, rather than relying on reversible bonding typical of traditional self-healing materials. As a result, these elastomers deliver exceptional stretchability, mechanical strength of 7.45 MPa (vs. original 7.25 MPa), and toughness of up to 14.9 MJ m<sup>-3</sup>, in addition to complete healing within 3 h. The designed elastomers integrate rapid healing, high repaired strength and toughness, feasible preparation, and recyclability. The rather facile synthesis of these self-healing elastomers can be generalized to other deformable strength-required and fast healing-needed materials at low cost, showing great application potentials in new energy and wearable electronics.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"23 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142840897","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}
PolymerPub Date : 2024-12-17DOI: 10.1016/j.polymer.2024.127960
Bo Zhang, Qingzhe Mao, Wenchong He, Rongqing Zhou, Chongde Wu, Nicolas Hengl, Frederic Pignon, Yao Jin
{"title":"A self-cleaning biocatalytic membrane with adjusted polyphenol deposition for edible oil-water separation","authors":"Bo Zhang, Qingzhe Mao, Wenchong He, Rongqing Zhou, Chongde Wu, Nicolas Hengl, Frederic Pignon, Yao Jin","doi":"10.1016/j.polymer.2024.127960","DOIUrl":"https://doi.org/10.1016/j.polymer.2024.127960","url":null,"abstract":"Catechol-amine co-deposition membranes have garnered significant interest in enzyme immobilization, yet the deposited coating leads to excessive mass transfer resistance, negatively impacting membrane filtration performance. This work adjusts polyphenol deposition by utilizing the co-deposition structure with tannic acid (TA) and 3-aminopropyltriethoxysilane (APTES) with glycerol to enhance the filtration capability while maintaining enzyme activity. The glycerol addition has brought in a structural transition from dense nanosphere stacking to the loose flaky structure of greater bulkiness. Consequently, the resulting membrane showed a 69% of permeability improvement along with improved enzyme activity post-adjustment. In oil-water separation cycle tests, the biocatalytic membrane enabled the clarification of oil emulsions and facilitates offline self-cleaning, maintaining high permeability and recovery even after five cycles of heavy oil (4 g/L) filtration, showing great application potential in edible oil-water separation. The biocatalytic membrane of this work, derived from biomass and characterized by its facile preparation and minimal mass transfer resistance, presents a promising avenue for the integration of biocatalysis with filtration technologies within industrial production processes.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"10 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142840905","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}
PolymerPub Date : 2024-12-16DOI: 10.1016/j.polymer.2024.127961
Juliana Belen Rial, María Luján Ferreira
{"title":"Synthesis and characterization of a novel catalyst based on magnetic chitosan beads for oxidoreductase enzyme biomimetic immobilization","authors":"Juliana Belen Rial, María Luján Ferreira","doi":"10.1016/j.polymer.2024.127961","DOIUrl":"https://doi.org/10.1016/j.polymer.2024.127961","url":null,"abstract":"Enzymes are biological catalysts intensively researched in several fields, including wastewater treatment. However, the structural vulnerability of enzymes limits their application. The design of enzyme mimetics is an interesting challenge in terms of selecting appropriate support for a (bio)mimetic and maintaining activity and stability after immobilization. In this work, a novel spherical solid composed of chitosan and magnetite nanoparticles was formulated to support hematin (as an oxidoreductase biomimetic). Magnetic chitosan beads were prepared via coprecipitation and gelification of Fe<sub>3</sub>O<sub>4</sub> nanoparticles and chitosan, respectively. The solid combines chitosan advantages (non-toxicity, abundance, physicochemical stability, and flexibility to be shaped into beads) with nanoparticulated Fe<sub>3</sub>O<sub>4</sub> properties (superparamagnetism and oxidoreductase mimic activity). A black solid with a regularly spherical shape, approximately 2 mm in diameter, was obtained. The solid was able to support hematin. Under optimal conditions, the incorporation of 3-aminopropyltriethoxysilane increased hematin immobilization efficiency. The synthesized solid presents catalase activity, decomposing 56% of hydrogen peroxide under optimal conditions, while without hematin, it only decomposes 33%. The solid presented catalytic activity and low leaching of iron in reaction medium, which makes it a potential catalyst to be applied in wastewater remediation in future work.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"46 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832296","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}
PolymerPub Date : 2024-12-16DOI: 10.1016/j.polymer.2024.127963
Yanghang Liu, Heyu Zhang, Tao Zhang, Yuefei Ding, Siqi Zhang, Dan Yu, Wei Wang
{"title":"Highly sensitive photochromic aerogel sensor for acidic gas detection based on SP/WPU/CNF composite materials","authors":"Yanghang Liu, Heyu Zhang, Tao Zhang, Yuefei Ding, Siqi Zhang, Dan Yu, Wei Wang","doi":"10.1016/j.polymer.2024.127963","DOIUrl":"https://doi.org/10.1016/j.polymer.2024.127963","url":null,"abstract":"Gas sensors are crucial in various applications such as environmental monitoring, industrial safety, and air quality control. However, many of these sensors still encounter significant challenges, including complex fabrication processes, low sensitivity, and poor stability. This study presents the development of a novel photochromic sensor using spiropyran (SP), waterborne polyurethane (WPU), and cellulose nanofiber (CNF) aerogel, aiming to overcome these challenges and provide highly sensitive detection of acidic gases. Under ultraviolet (UV) irradiation, the SP component in the aerogel isomerizes to its open-ring merocyanine (MC) form, which is further protonated to protonated merocyanine (MCH) in the presence of acid vapors. Systematic testing reveals that the SP/WPU/CNF aerogel sensor exhibits a rapid response time of 20 seconds under UV light irradiation and retains 75% of its photoresponsivity after 20 cycles, demonstrating excellent durability. Additionally, the sensor exhibits a response time of 20 seconds to acidic gases, with a color change from purple to yellow when exposed to HCl gas at concentrations as low as 1 ppm. After undergoing five protonation and recovery cycles, the sensor maintains a certain level of acid responsiveness. These exceptional properties highlight the potential of the SP/WPU/CNF aerogel-based sensor to be a highly sensitive, efficient, and stable solution for acidic gas detection.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"12 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832299","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}