Macromolecular Rapid Communications最新文献

{"title":"Biopolymer Derived Gel Polymer Electrolytes: Current Status and Future Perspectives.","authors":"Amul Jain, Koushik Mahata, Onkarnath, Sanjib Banerjee","doi":"10.1002/marc.202500472","DOIUrl":"https://doi.org/10.1002/marc.202500472","url":null,"abstract":"<p><p>The growing shift towards renewable energy and the expansion of portable electronics have intensified the demand for safer, more efficient, and eco-friendly energy storage technologies. The urgent need for safe, high-performance, and environmentally sustainable energy storage systems has driven significant interest in gel polymer electrolytes (GPEs), particularly derived from natural biopolymers. Biopolymer-based GPEs (BGPEs) offer a promising alternative to synthetic counterparts, due to biodegradability, low toxicity, and rich functionality. Presents the recent advancements in the design, synthesis, and application of BGPEs in electrochemical devices. The synthesis methodologies including physical blending, chemical crosslinking, UV-curing, electrospinning, and in situ polymerization are evaluated for their effects on ionic conductivity, mechanical integrity, and thermal stability. Emphasis is placed on the ion transport mechanisms, highlighting the roles of functional groups, polymer crystallinity, and structural morphology in optimizing performance. Additionally, challenges such as moisture sensitivity, limited electrochemical windows, and mechanical fragility which impacts device performance are discussed alongside potential mitigation strategies. BGPEs are poised to play a transformative development in next-generation energy storage. Conclude with future directions in materials design, scalable processing, and multifunctional device integration to accelerate the commercialization of bio-based electrolytes.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00472"},"PeriodicalIF":4.3,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144726254","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Role of High Fidelity Vs. Low Fidelity Experimental Data in Machine Learning Model Performance for Predicting Polymer Solubility.","authors":"Mona Amrihesari, Manali Banerjee, Raul Olmedo, Blair Brettmann","doi":"10.1002/marc.202500454","DOIUrl":"https://doi.org/10.1002/marc.202500454","url":null,"abstract":"<p><p>Reliable classification of polymer-solvent compatibility is essential for solution formulation and materials discovery. Applying machine learning (ML) and artificial intelligence to this task is of growing interest in polymer science, but the effectiveness of such models depends on the quality/nature of the training data. This study evaluates how experimental data fidelity, as set by the experimental method, influences ML model performance by comparing classifiers trained on two experimental datasets: one generated from turbidity-based measurements using a Crystal16 parallel crystallizer as a high-fidelity source and another derived from visual solubility inspection as a low-fidelity dataset. Both datasets were encoded using one-hot encoding for polymers and Morgan fingerprints for solvents and modeled using XGBoost classifiers to predict solubility labels as soluble, insoluble, and partially soluble. Confusion matrices showed that models trained on high-fidelity data better captured partially soluble behavior and more clearly distinguished between classes, highlighting the advantage of quantitative measurements over subjective classification. We also found that adding temperature as a feature improved prediction accuracy for the low-fidelity dataset-a key consideration for literature-derived data, which often lacks this information. These findings underscore the importance of experimental rigor and completeness when developing generalizable ML-based tools for polymer solubility prediction.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00454"},"PeriodicalIF":4.3,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144726270","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Transfer Learning for Polymer Mechanics: A Fusion Approach to Bridge Molecular Dynamics Simulations and Experiments in SSBR.","authors":"Siqi Zhan, Zhenyuan Li, Hengheng Zhao, Zhanjie Liu, Qian Li, Shilong Ji, Weifeng Zhang, Qingsong Zhao, Liqun Zhang, Jun Liu","doi":"10.1002/marc.202500386","DOIUrl":"https://doi.org/10.1002/marc.202500386","url":null,"abstract":"<p><p>The stress-strain curve is a key indicator of the mechanical behavior of polymeric materials and plays a vital role in optimizing the performance of solution-polymerized styrene-butadiene rubber (SSBR). Molecular dynamics (MD) simulations enable the investigation of microscale deformation mechanisms, yet their use of unrealistically high strain rates leads to stress values that diverge significantly from experimental results. To address this discrepancy, we proposed a weighted fusion framework that integrates transfer learning with a hybrid long short-term memory-multilayer perceptron (LSTM-MLP) model and the eXtreme Gradient Boosting (XGBoost) algorithm. A dataset of 100 simulated stress-strain curves was generated from 20 distinct SSBR molecular systems across five strain rates, supplemented with five experimental curves for SSBR (grade 2557TH) under varying tensile rates. The model was pretrained on the simulated data and fine-tuned using the limited experimental data, enabling stress-strain predictions consistent with experiments. Comparative analyses against alternative machine learning baselines confirmed the model's superior accuracy. Additionally, correlation analysis revealed how the four structural units of SSBR-styrene, 1,2-butadiene, cis-1,4-butadiene, and trans-1,4-butadiene-influence mechanical behavior, offering theoretical insights for targeted performance enhancement.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00386"},"PeriodicalIF":4.3,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144726271","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Catalyst-Free and Green Crosslinking of Epoxy-Functionalized EPDM With Dicarboxylic Acids: Insights into Curing Mechanism, Recyclability and Thermal Stability.","authors":"Chenru Tian, Ganggang Zhang, Jun Liu, Liqun Zhang","doi":"10.1002/marc.202500502","DOIUrl":"https://doi.org/10.1002/marc.202500502","url":null,"abstract":"<p><p>The conventional curing methods pose a significant environmental threat due to the use of toxic vulcanizing agents, the release of irritating volatile organic compounds, and the difficulties in recycling end-of-life rubber products. This work demonstrates a catalyst-free, facile, and eco-friendly crosslinking strategy based on the reaction between epoxy-functionalized ethylene-propylene-diene monomer (EEPDM) and dicarboxylic acids. The EEPDM was synthesized via a reusable reaction-controlled phase-transfer catalyst. Then, EEPDM could be effectively crosslinked by dicarboxylic acids without additional additives. The increased acidity of dicarboxylic acids could be conducive to improving the crosslinking rate. Moreover, the curing mechanism and the nature of the crosslinks were investigated, which is crucial for the recyclability of rubbers. The dicarboxylic acid-cured EEPDM exhibited undesirable side reactions, the extent of which showed a positive correlation with the acidity of carboxylic groups. This phenomenon could be primarily attributed to acid-catalyzed self-polymerization via epoxide ring-opening mechanisms, which would be detrimental to the reprocessability. Due to the formation of thermally stable ether linkages, the crosslinked EEPDM exhibited enhanced thermal-oxidative aging behavior. Hence, we envision that this catalyst-free, high-efficiency crosslinking strategy may offer a promising bridge between sustainable modification and high-performance for epoxy-functionalized rubbers, holding potential application in eco-friendly, low-odor automotive sealing strips.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00502"},"PeriodicalIF":4.3,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144726255","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Engineering pH-Responsive Nanocarriers via an Optimized Synthesis of PMOXA-b-PDPA Amphiphilic Diblock Copolymers.","authors":"John Peter Coats, Anamarija Nikoletić, Lukas Heuberger, Voichita Mihali, Cora-Ann Schoenenberger, Ionel Adrian Dinu, Cornelia G Palivan","doi":"10.1002/marc.202500418","DOIUrl":"https://doi.org/10.1002/marc.202500418","url":null,"abstract":"<p><p>pH-responsive nanocarriers have gain significant attention due to their ability to provide controlled cargo delivery with high precision in response to specific stimuli. However, the polymers used in the self-assembly of these nanocarriers must be carefully designed to meet the requirements of bio-relevant delivery. Here, we present an optimized synthesis of poly(2-methyl-2-oxazoline)-block-poly(2-(diisopropylamino)ethyl methacrylate) (PMOXA-b-PDPA) block copolymers tailored for obtaining carriers with vesicle architecture and thin membranes for an improved release behavior. By systematically modifying the synthesis conditions, we obtain a small library of copolymers, focusing on low molecular weight (MW) variants to reduce the membrane thickness of the resulting vesicles. We investigate the impact of membrane thickness on the kinetics and efficiency of cargo release in response to a pH shift from neutral to slightly acidic conditions that are particularly relevant in pathological environments like tumors. Model cargos of varying MWs, including doxorubicin hydrochloride, exhibited differential release profiles under these pH conditions. Together with no cytotoxicity, the thin membrane represents key aspects that support further development of such carriers for therapeutic applications.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00418"},"PeriodicalIF":4.3,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144726268","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synchrotron X-Ray Analysis and Morphology Evidence for Stereo-Assemblies of Periodic Aggregates in Poly(3-Hydroxybutyrate) with Unusual Photonic Iridescence","authors":"","doi":"10.1002/marc.202500453","DOIUrl":"10.1002/marc.202500453","url":null,"abstract":"<p>Y.-H. Liao, S. Nagarajan, E. M. Woo, W.-T. Chuang, and Y.-W. Tsai, “Synchrotron X-Ray Analysis and Morphology Evidence for Stereo-Assemblies of Periodic Aggregates in Poly(3-Hydroxybutyrate) With Unusual Photonic Iridescence,” <i>Macromolecular Rapid Communications</i> 42, no. 14 (2021): 2100281, https://doi.org/10.1002/marc.202100281.</p><p>The authors would like to note that, in Figure 3b, the <i>y</i>-axis was mislabeled as “Band spacing” instead of the correct label, “Growth Rates (µm/min).”</p><p>We would like to clarify that Figure S3 (Supporting Information), which was published alongside the main paper as part of the Supporting Information, includes the same two panels: Figure S3a (Supporting Information) shows band spacing versus crystallization temperature (T_c), and Figure S3b (Supporting Information) presents growth rate versus T_c with the <i>y</i>-axis correctly labeled as “Growth rate (µm/s).” This figure covers data from PHB/PEO (75/25) blend spherulites crystallized at T_c = 30, 45, 50, 70, and 80 °C.</p><p>The updated Figure 3 is included as follows to ensure consistency with SI units and to replace the previously mislabeled version.</p><p></p><p>The authors would also like to introduce the following additional clarifications and corrections to the text:</p><p>Figures 1e and 4–Spiral spin direction: The direction of spiral band rotation (i.e., clockwise or counterclockwise) is not uniform across the sample but depends on the local nucleation site orientation and location of nucleation in the film layer. As a result, different spherulites—or even regions within the same spherulite—can exhibit varied spiral senses. This sample-dependent variability explains why Figures 1e and 4 show opposite spin directions; each image captures a different nucleus with its own local orientation.</p><p>Figure 3a–Band spacing maximum: The original text referred to 43 °C as the point of maximum band spacing. However, Figure 3a shows that the band spacing of the PHB/PTA (75/25) blend increases with increasing T_c, reaching a maximum of ≈45 µm at T_c ≈ 43–45 °C, but this point is hard to define precisely. Beyond this temperature—around T_c ≈ 45 °C—the bands broaden significantly and lose definition, appearing to ‘disappear’.</p><p>Figures 12b and 13–Labelling inconsistency: Figure 12b shows a scan across five points—Ridge (a), Valley (b), Ridge (c), Valley (d), Ridge (e). By contrast, Figure 13 presents a separate, shorter scan consisting of four points: Valley (a), Ridge (b), Valley (c), Ridge (d). The authors wish to note that this apparent inconsistency is due to the different scan ranges and point counts, not due to a conflict in the data.</p><p>We apologize for these errors.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":"46 17","pages":""},"PeriodicalIF":4.3,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/marc.202500453","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144715041","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Self-Immolative Polyion Complexes.","authors":"Xueli Mei, Elizabeth R Gillies","doi":"10.1002/marc.202500419","DOIUrl":"https://doi.org/10.1002/marc.202500419","url":null,"abstract":"<p><p>Polyion complex (PICs) micelles are formed through the self-assembly of polyelectrolytes bearing opposite charges. The ability to form PICs under fully aqueous conditions makes them attractive for the encapsulation of biopolymers such as proteins and nucleic acids for potential therapeutic applications. Stimuli-responsive PIC micelles have the potential to release their cargo under specific biological conditions. We describe here the development of PIC micelles formed from two self-immolative polymers (SIPs) with complementary charges. The polycationic SIP, having pendent ammonium groups, undergoes depolymerization in response to light. The polyanionic SIP, bearing pendent carboxylates and a stabilizing PEG block, undergoes depolymerization in response to a pH change from 7.4 to 6. SIP PICs composed of a 0.6 anion:cation ratio remain well dispersed at pH 7.4, but degrade at pH 6, primarily due to depolymerization of the anionic block. Irradiation with UV light leads primarily to depolymerization of the cationic block. In vitro cytotoxicity assays with C2C12 cells indicate that the PICs are quite well tolerated by the cells with low cytotoxicity up to about 0.5 mg mL^-1. Overall, these PICs are a new platform that can potentially be used for the encapsulation and stimulus-mediated release of ionic cargo.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00419"},"PeriodicalIF":4.2,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144715040","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"All-Fiber Electronic Skin Based on Asymmetric Wool/PTFE Structure for Energy Harvesting and Self-Powered Sensing.","authors":"Jin Tao, Weidi Yin, Xin Lu, Jian Zang, Jiru Jia, Leigen Liu, Xibo Hao, Ya Yang","doi":"10.1002/marc.202500464","DOIUrl":"https://doi.org/10.1002/marc.202500464","url":null,"abstract":"<p><p>This paper reports on a fully textile electronic skin (e-skin) based on an asymmetric wool/polytetrafluoroethylene (PTFE) structure, which is fabricated through an innovative filling core yarn and weft interweaving technique, enabling self-driven contact detection and motion sensing functions. The e-skin features a three-layer woven structure, with the outer layer made of PTFE (high dielectric constant, superhydrophobic), the inner layer composed of wool (hygroscopic, skin-friendly), and a middle layer embedded with silver-plated nylon (SPN) conductive yarns forming a flexible electrode array. Benefiting from its asymmetric design, this material exhibits excellent triboelectric performance (open-circuit voltage of 37 V, short-circuit current of 58 nA), breathability (341.9 mm/s), and mechanical durability (over 1000 cycles). Through modification with a polyacrylic acid coating, the PTFE side demonstrates superhydrophobicity (contact angle > 150°) and self-cleaning capabilities. In practical applications, this e-skin can accurately monitor the bending angle of the elbow joint (30°∼120°, R² = 0.979) and recognize sliding gestures through differences in voltage waveforms. Additionally, it can drive commercial electronic devices and charge capacitors (4.7 µF capacitor charged to 4.5 V within 100 s). This study provides a scalable textile-based solution for developing comfortable and durable self-driven electronic skin, suitable for human-computer interaction and health monitoring applications.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00464"},"PeriodicalIF":4.2,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144673538","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mechanically Strong Functionalized-BNNS/PVA Composite Hydrogels with Excellent Thermal Conductivities","authors":"Junliang Zhang,&nbsp;Chenyang Tang,&nbsp;Qingqing Kong,&nbsp;Kunpeng Ruan,&nbsp;Yongqiang Guo,&nbsp;Jiangtao Wang,&nbsp;Junwei Gu","doi":"10.1002/marc.202500416","DOIUrl":"10.1002/marc.202500416","url":null,"abstract":"<div>\u0000 \u0000 <p>Polyvinyl alcohol (PVA) hydrogels exhibit superior viscoelasticity, flexibility, and biocompatibility and have been widely utilized in wearable devices, flexible electronics, and electronic packaging. However, their low thermal conduction ability and poor mechanical performance limit their further applications and development for the high integration and multifunctionality of flexible electronics and wearables. Herein, BNNS-OH/PVA composite hydrogels containing oriented structure were fabricated via directional freezing, salting-out, and stretching, applying PVA hydrogel as matrix and hydroxyl boron nitride nanosheets (BNNS-OH) as thermal-conductive fillers. The oriented BNNS-OH/PVA composite hydrogel containing 9 wt.% of BNNS-OH exhibited appreciably improved in-plane thermal conductivity (<i>λ</i>) of 3.13 W/(m·K) when stretched by 3.5 times, enhanced by 210% compared to 1.01 W/(m·K) for the unstretched hydrogel and 502% compared to 0.52 W/(m·K) for pure PVA hydrogel made applying freeze–thaw (FT) method. Additionally, the oriented BNNS-OH/PVA composite hydrogels exhibited superior elastic modulus, tensile strength, and toughness of 20 MPa, 18.8 MPa, and 9.9 MJ/m³, respectively, to 0.07 MPa, 0.4 MPa, and 0.32 MJ/m³ of pure FT PVA hydrogel.</p>\u0000 </div>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":"46 19","pages":""},"PeriodicalIF":4.3,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144673539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Molecular Dynamics Simulation of Cross-linked Epoxy Resins: Past and Future","authors":"Satoru Yamamoto,&nbsp;Keiji Tanaka","doi":"10.1002/marc.202570041","DOIUrl":"https://doi.org/10.1002/marc.202570041","url":null,"abstract":"<p><b>Front Cover</b>: Epoxy resins are cured by the reaction between epoxy and amine compounds to form a three-dimensional network. To better understand the curing process and crosslinking structure of epoxy resins, a treasure hunt using molecular dynamics simulations is conducted. More details can be found in article 2400978 by Satoru Yamamoto and Keiji Tanaka.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":"46 14","pages":""},"PeriodicalIF":4.2,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/marc.202570041","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144647228","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}