Sébastien Berruée, Jean-Michel Guigner, Cécile Huin, Jan Patrick Calupitan, Laurent Bouteiller, Lydia Sosa Vargas, Jutta Rieger
{"title":"Direct Assembly of Micrometer-Long Polymeric Cylinders in Water via Supramolecular Sticker Engineering.","authors":"Sébastien Berruée, Jean-Michel Guigner, Cécile Huin, Jan Patrick Calupitan, Laurent Bouteiller, Lydia Sosa Vargas, Jutta Rieger","doi":"10.1002/marc.202500478","DOIUrl":"https://doi.org/10.1002/marc.202500478","url":null,"abstract":"<p><p>We report a direct, solvent-free method to produce micrometer-length, well-organized polymer nanocylinders in water. To achieve this, a hydrophilic poly(N,N-dimethylacrylamide) (PMDAc) was functionalized at one chain-end with a perylene diimide (PDI) sticker using RAFT polymerization. Two PDI RAFT agents were prepared and studied: one featuring two tri(ethylene glycol) (TEG) units at the PDI bay-positions and one without. The corresponding PDI-PDMAc conjugates spontaneously self-assembled in water, driven by π-π interactions made of H-aggregates, and showed a morphological evolution from cylinders to spheres when increasing the polymer chain length. The introduction of TEG units was found to be important to avoid the clustering of nanocylinders or the formation of ill-defined assemblies, which were observed in the TEG-free system. Moreover, we found that the PDI-TEG<sub>2</sub>-PDMAc with degrees of polymerization (DP<sub>n</sub>) below 24 self-assembled into micrometer-long nanocylinders. By heating the aqueous polymer solution, this process can be accelerated and is accompanied by a large increase in viscosity. Fluorescence spectroscopy revealed an excimer emission signal for the PDI polymers in water, with a higher emission for cylinders, suggesting better organization within the PDI H-aggregates. This strategy provides a sustainable approach for developing functional nanomaterials with precise morphological control, eliminating organic solvents and complex processing.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00478"},"PeriodicalIF":4.3,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144843890","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":"Polymerization-Induced Self-Assembly for the Synthesis of Multi-Responsive Micelles Hydrogel and its Versatile Applications.","authors":"Linjie Yang, Hanfeng Liu, Junhui Gong, Jianfeng Xie, Jianqiang Zhang, Xinrui Zhang, Xianqiang Pei, Qihua Wang, Yaoming Zhang","doi":"10.1002/marc.202500545","DOIUrl":"https://doi.org/10.1002/marc.202500545","url":null,"abstract":"<p><p>Poly(N-isopropyl acrylamide) (PNIPAM) is well-known for its lower critical solution temperature (LCST) and widely studied as thermo-responsive micelles for various applications. However, the synthesis of micelles with precise structures often involves complex process. Herein, we developed a novel multi-responsive micelles hydrogel GBN, which was prepared by combining the polymerization-induced self-assembly (PISA) of poly(N-isopropyl acrylamide)-poly (glycerol methacrylate) (PGMA<sub>x</sub>-PNIPAM) and B─O crosslinking the micelles. The yielded micelles with stable worm-like structures, easily form a hydrogel through significant entanglement. The thermo-responsiveness of these micelles facilitates a reversible gel-sol transition, accompanied by changes in transparency, making them suitable for thermal management in smart window applications. Additionally, the glucose responsiveness associated with the dynamic B─O bonds address the incompatibility of PNIPAM's LCST temperature for drug release applications. Importantly, we discovered that the GNB hydrogel can also function as sealing material; its thermo-responsiveness enables the formation of liquid gaskets that uniformly fill rough surfaces. In its gel state, it exhibits stable load-bearing capacity, sealing strength, and consistent friction coefficients, making it applicable in both static and dynamic sealing scenarios to tackle sealing challenges in extreme environments. Thus, this work offers a novel approach for fabricating stimulus-responsive materials, broadening the application scope of PNIPAM in various fields.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00545"},"PeriodicalIF":4.3,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144843895","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}
Muhammad Haseeb Iqbal, Julio Zelaya, Quy Ong, Francesco Stellacci, Joerg Lahann
{"title":"Lyotropy as a Design Consideration for Ultra-Small Protein Nanoparticles via Electrohydrodynamic Jetting.","authors":"Muhammad Haseeb Iqbal, Julio Zelaya, Quy Ong, Francesco Stellacci, Joerg Lahann","doi":"10.1002/marc.202500533","DOIUrl":"https://doi.org/10.1002/marc.202500533","url":null,"abstract":"<p><p>Protein-based nanoparticles offer tailored bioactivity and biodegradability that are distinct from their synthetic polymeric counterparts. Precise engineering of physical properties, especially size, of nanoparticles using electrohydrodynamic (EHD) jetting is a crucial factor that defines the fate of delivery systems in nanomedicine. Herein, we establish a systematic understanding that leads to the preparation of human serum albumin (HSA) nanoparticles with sizes as small as 50 nm. Interestingly, the addition of salt at very low concentrations, around 1-5 mm, combined with EHD process parameters, can result in narrow distributions of particle sizes that are consistently below 100 nm. At a given concentration, i.e., 2 mm, anions modulate the particle diameters that follow the Hofmeister Series as SO<sub>4</sub> <sup>2-</sup> < CO<sub>3</sub> <sup>2-</sup> < H<sub>2</sub>PO<sub>4</sub> <sup>-</sup> < Cl<sup>-</sup> < I<sup>-</sup>. This size reduction is primarily due to increased solution conductivity and interfacial charge density induced by salt ions during the EHD jetting process. High mobility ions compensate for the higher surface energy required to produce ultra-small nanoparticles. Tight control over the size and distribution of ultra-small nanoparticles may be critical for targeted drug delivery, as it can influence nanoparticle tropism or affect their cellular uptake.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00533"},"PeriodicalIF":4.3,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144843894","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":"Self-Healing and Reprocessable Polyurethane Elastomer with Triple Dynamic Crosslinked Networks.","authors":"Xingyu Mou, Yiqin Guo, Xuejun Lai, Jianping Ding, Hongqiang Li, Xingrong Zeng","doi":"10.1002/marc.202500509","DOIUrl":"https://doi.org/10.1002/marc.202500509","url":null,"abstract":"<p><p>Chemically crosslinked polyurethane materials with excellent mechanical properties have attracted considerable attention, yet recyclability is still challenging. Herein, a self-healing and reprocessable polyurethane (PU) elastomer with triple dynamic networks was synthesized through the addition reactions of methylenediphenyldiisocyanate with polyetheramine, protocatechualdehyde, and tris(2-aminoethyl) amine, as well as the incorporation of Fe<sup>3+</sup> ions. Owing to the formation of microphase-separated structure and triple dynamic networks including hydrogen bonds, Fe<sup>3+</sup>-catechol coordination, and imine bonds, the obtained PU elastomer exhibited excellent mechanical properties with a tensile strength of 6.40 MPa, elongation at break of 1838%, toughness of 51.16 MJ m<sup>-</sup> <sup>3</sup> and fracture energy of 154.91 kJ m<sup>-</sup> <sup>2</sup>. Importantly, the PU elastomer possessed not only high healing efficiency of 96.6% after healing at 60°C for 24 h, but also superior reprocessability with a tensile strength retention rate of 75.6% after three reprocessing cycles. Besides, owing to residual phenolic hydroxyl groups in unreacted PA, the PU elastomer also exhibited outstanding thermal-oxidative aging resistance. The findings in this work conceivably stand out as a new methodology for the preparation of functional and high-performance elastomers.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00509"},"PeriodicalIF":4.3,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144843896","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":"Low-Hysteresis Cellulose-Based Hydrogels for Strain Detecting.","authors":"Xia Sun, Fanghan Luo, Feng Jiang","doi":"10.1002/marc.202500521","DOIUrl":"https://doi.org/10.1002/marc.202500521","url":null,"abstract":"<p><p>Hydrogels are promising materials for wearable and flexible electronics, yet combining low mechanical hysteresis with high renewable content remains a key challenge. Here, we report a cellulose-based hydrogel with low hysteresis, enabled by incorporating dialcohol nanocellulose (DANC) into a polyacrylamide (PAAM) network. The flexible, hydroxyl-rich DANC chains form abundant reversible hydrogen bonds with the PAAM matrix, allowing the hydrogel to achieve an unprecedented cellulose content of ∼15 wt.% while maintaining stretchability and mechanical robustness. The PAAM/DANC hydrogels display low mechanical hysteresis and high durability during 1000 cyclic strains, with stable mechanical and sensing performance. In addition, the hydrogels exhibit reliable strain sensitivity with a gauge factor of 1.1 and consistent signal output under varying strains. Finally, we demonstrate their potential in wearable strain sensing by detecting complex human motions. This work presents a sustainable strategy to design high-performance cellulose-based hydrogels, advancing their application in next-generation wearable electronics.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00521"},"PeriodicalIF":4.3,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144843893","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}
Suraj Aswale, Hyerin Kang, Aruna Kumar Mohanty, Hanyoung Kim, Yerin Jang, Minsung Kim, Heung Bae jeon, Hong Y. Cho, Hyun-jong Paik
{"title":"Various Topological Poly(tert-butyl acrylate)s and Their Impacts on Thermal and Solution Properties","authors":"Suraj Aswale, Hyerin Kang, Aruna Kumar Mohanty, Hanyoung Kim, Yerin Jang, Minsung Kim, Heung Bae jeon, Hong Y. Cho, Hyun-jong Paik","doi":"10.1002/marc.70002","DOIUrl":"https://doi.org/10.1002/marc.70002","url":null,"abstract":"<p><b>Front Cover</b>: Topologically diverse poly(t-butyl acrylate)s including linear, tetra-arm, cyclic, and 8-shaped architectures, are synthesized via ARGET ATRP and CuAAC click chemistry. Despite similar molar masses, distinct thermal and solution behaviors are observed. These findings highlight the critical role of topology in tuning polymer properties for applications in adhesives, nanomaterials, etc. More details can be found in article 2401043 by Hong Y. Cho, Hyun-jong Paik, and co-workers.\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 15","pages":""},"PeriodicalIF":4.3,"publicationDate":"2025-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/marc.70002","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144833194","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}
Hatice Mutlu, Bercis Pektas, C Remzi Becer, Azra Kocaarslan
{"title":"Green and Sustainable Chemistry Approaches on Azide-Based Click Reactions in Polymer Science.","authors":"Hatice Mutlu, Bercis Pektas, C Remzi Becer, Azra Kocaarslan","doi":"10.1002/marc.202500171","DOIUrl":"https://doi.org/10.1002/marc.202500171","url":null,"abstract":"<p><p>Click Chemistry, particularly the azide-alkyne cycloaddition (AAC) reaction, has revolutionized polymer chemistry, enabling precise and efficient synthesis of advanced functional materials. With its high regioselectivity, mild reaction conditions, and versatility, AAC reactions align closely with the principles of Green and Sustainable Chemistry. However, the core principles of Click Chemistry, particularly its compatibility with Green Chemistry ideals-such as reduced waste, high atom economy, and mild reaction conditions-remain insufficiently emphasized in the context of polymer chemistry. The review evaluates current limitations in AAC-particularly the challenges associated with hazardous azide reagents and reliance on non-renewable resources-and explores innovative solutions, including greener catalysts, solvent-free systems, and the incorporation of renewable feedstocks. Additionally, the review presents a comparison of activation methods, spanning thermal, catalytic, metal-free, and strain-promoted pathways, to highlight their respective advantages and trade-offs in sustainability. Practical applications of AAC in polymer design are discussed, showcasing its role in creating materials with tailored properties such as thermal stability, bioactivity, and electronic functionality. This analysis provides a roadmap for future research to optimize AAC for sustainability without compromising its effectiveness in materials design.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00171"},"PeriodicalIF":4.3,"publicationDate":"2025-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144787922","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":"Correction: Structural and Property Characterizations of Dual-Responsive Core–Shell Tecto Dendrimers for Tumor Penetration and Gene Delivery Applications","authors":"","doi":"10.1002/marc.202500596","DOIUrl":"10.1002/marc.202500596","url":null,"abstract":"<p>Junjie Liu, Xiaoyu Wang, Xiaolei Li, et al., <i>Macromol. Rapid Commun</i>. <b>2024</b>, 45, 2400251, https://doi.org/10.1002/marc.202400251.</p><p>The authors regret that the original version of our paper contained an incorrect picture in Figure 7A, where the image of “N/P = 5” in the P-Glu/Cas9-PD-L1 group was mistakenly replaced with the P-Gal/Cas9-PD-L1 image during data organization. The corrected Figure 7 is shown below. This correction does not affect the validity of the original discussion, interpretation, and conclusion presented in this paper. The authors sincerely apologize to the Journal and its readers for the confusion that may have caused.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":"46 16","pages":""},"PeriodicalIF":4.3,"publicationDate":"2025-08-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/marc.202500596","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774392","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}
Warisha Mehmood, Muhammad Gulraiz Tanvir, Kamran Amin, Zhixiang Wei
{"title":"Designing Solution-Processable Covalent Organic Frameworks: Opportunities and Challenges.","authors":"Warisha Mehmood, Muhammad Gulraiz Tanvir, Kamran Amin, Zhixiang Wei","doi":"10.1002/marc.202500328","DOIUrl":"https://doi.org/10.1002/marc.202500328","url":null,"abstract":"<p><p>Since their discovery, numerous covalent organic frameworks (COFs) have been reported, showcasing unique properties that make them materials of choice for a wide range of applications. COFs have gained significant attention due to their fascinating characteristics, such as tunable pore structures, customizable functionality, and high crystallinity. Despite substantial progress in this field, the widespread application of COFs remains limited due to challenges in large-scale synthesis, issues with repeatability, and poor solubility, which hinder their processability. We propose that the lack of solution processability represents the most significant challenge hindering the application of COFs across various fields. Recognizing the importance of this issue and aiming to highlight the challenges in this direction, we have summarized the available data and previous attempts made to address these limitations. This review provides an insightful analysis of the current issues and future challenges, while also proposing strategies to overcome these challenges. The review not only summarizes all the relevant issues but also aims to inspire researchers to investigate these challenges in greater detail.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e00328"},"PeriodicalIF":4.3,"publicationDate":"2025-08-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774393","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}