{"title":"Solvent-Free, UV-Curable Cellulosic Adhesives Engineered via a Supramolecular Eutectic Platform for Robust Adhesion.","authors":"Ren'ai Li, Anqi Zhao, Hanyu Jiang, Lizi Li, Xueren Qian","doi":"10.1002/marc.70449","DOIUrl":"https://doi.org/10.1002/marc.70449","url":null,"abstract":"<p><p>Cellulose-based adhesives offer sustainable alternatives to petroleum-derived products but face bottlenecks regarding organic solvent reliance, slow curing efficiency, and moisture sensitivity. Here, a solvent-free, UV-curable cellulosic adhesive (UCA) is developed via a supramolecular-covalent hybrid strategy. Utilizing a cellulose acetate butyrate/thymol eutectic platform, multi-component functionalization with silane, photoactive acrylic moieties, and fluorinated monomer yields a transparent, photocurable prepolymer. The cured UCA exhibits a lap-shear strength of 6.73 MPa on PMMA, high optical transparency, and broad temperature tolerance. Synergistic surface hydrophobicity, interfacial coupling, and dense photocrosslinking impart strong water resistance, retaining 5.86 MPa shear strength after 3-day water immersion and 5.12 MPa after 1 h in 100°C boiling water. The adhesive also withstands strong acids, bases, and organic solvents. This work provides a practical route for engineering high-performance bio-based adhesives.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e70449"},"PeriodicalIF":4.1,"publicationDate":"2026-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149101869","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":"Programming Stress Relaxation and Creep in Low-Molecular-Weight Self-Assembled Hydrogels Through Polymer Incorporation.","authors":"Ipsita Sahu, Kirti Nasir, Priyadarshi Chakraborty","doi":"10.1002/marc.70444","DOIUrl":"https://doi.org/10.1002/marc.70444","url":null,"abstract":"<p><p>Mechanical property characterization of supramolecular viscoelastic materials, particularly low-molecular-weight gelator (LMWG)-derived hydrogels, has predominantly relied on small-amplitude oscillatory shear (SAOS) measurements, although these experiments probe network dynamics only at short timescales and fail to capture the full spectrum of network rearrangements that drive bulk mechanical behavior. A key challenge is unveiling how transient non-covalent interactions in LMWGs and covalent polymeric components collectively modulate viscoelasticity across multiple timescales. Herein, we investigate an LMWG-polymer hybrid hydrogel to demonstrate how the progressive integration of a covalent polymer into a self-assembled network regulates the bulk mechanical response, using short-timescale SAOS and long-timescale stress-relaxation and creep/creep-recovery experiments. Notably, frequency-sweep and stress-relaxation measurements reveal that the storage modulus and characteristic relaxation time exhibit distinct sensitivities to polymer concentration, with comparable stiffnesses occurring alongside noticeably different relaxation times in the intermediate polymer composition range. Creep/Creep-recovery measurements further show enhanced resistance to irreversible deformation and improved elastic recovery at low polymer loadings, whereas higher polymer concentrations primarily promote faster recovery dynamics through a transition from dual to single retardation behavior. These findings demonstrate that polymer incorporation can differentially modulate the stiffness and relaxation dynamics of LMWG-derived supramolecular networks, providing a framework for tuning viscoelastic behavior across multiple timescales.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e70444"},"PeriodicalIF":4.1,"publicationDate":"2026-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149101872","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":"Cross-Hierarchical Analysis of Self-Oscillating Polymer Materials Through Activation Energy.","authors":"Zhouna Tang, Takafumi Enomoto, Ryo Yoshida","doi":"10.1002/marc.70448","DOIUrl":"https://doi.org/10.1002/marc.70448","url":null,"abstract":"<p><p>In chemically driven soft materials, polymer architecture can shape how chemical reactions are transduced into material-level dynamic behavior. However, the relationship between polymer architecture and the resulting dynamics remains insufficiently understood. Here, using Arrhenius analysis, we perform a cross-hierarchical comparison of the temperature dependence of Belousov-Zhabotinsky (BZ) reaction-driven oscillatory dynamics across three structurally related systems: molecular Ru(bpy)<sub>3</sub>Cl<sub>2</sub>, a linear self-oscillating polymer (SOP), and a self-oscillating microgel (SOMG). In these systems, Ru(bpy)<sub>3</sub> complex is present in solution as a molecular catalyst or covalently incorporated into either a linear polymer or a crosslinked microgel network. The resulting apparent activation energies E<sub>a, app</sub> are used to quantify the overall temperature dependence of their oscillatory dynamics. In the SOP, the redox and coacervation/dissolution oscillations exhibit similar E<sub>a, app</sub> values, indicating that periodic liquid-liquid phase separation had only a limited effect on the overall temperature dependence. In contrast, in the SOMG, the flocculation/dispersion oscillation exhibits a substantially higher E<sub>a, app</sub> than the redox oscillation. Moreover, the relative order of E<sub>a, app</sub> between the SOP and SOMG is reversed between the redox and structural oscillatory modes. These results indicate that E<sub>a, app</sub> is modulated by both the underlying polymer architecture and the architecture-dependent structural dynamics accompanying BZ-driven oscillations.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e70448"},"PeriodicalIF":4.1,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149101907","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}
Seyed Rasoul Mousavi, Samaneh Salkhi Khasraghi, Mohammad Arjmand
{"title":"Multifunctional Hybrid Rubber Nanocomposites With Enhanced Durability and Electrothermal Performance.","authors":"Seyed Rasoul Mousavi, Samaneh Salkhi Khasraghi, Mohammad Arjmand","doi":"10.1002/marc.70445","DOIUrl":"https://doi.org/10.1002/marc.70445","url":null,"abstract":"<p><p>Rubber materials for demanding environments require high wear resistance, reliable frictional behavior, and stable performance over a wide temperature range. Electrothermal functionality is also required for temperature regulation in cold conditions. However, incorporating electrothermal capability without compromising mechanical and tribological performance remains challenging. In this work, pre-intercalated molybdenum disulfide (MoS<sub>2</sub>) nanosheets were synthesized and modified by substituting molybdenum atoms with isolated iron (Fe) atoms to tailor interfacial interactions. The engineered nanosheets were hybridized with conductive carbon nanotubes to establish a synergistic filler network within an acrylonitrile butadiene rubber/butadiene rubber blend. Structural and morphological analyses confirmed successful Fe substitution and improved compatibility of MoS<sub>2</sub> with the matrix. The resulting hybrid nanocomposite exhibited substantial mechanical reinforcement, with tensile strength and modulus increasing by 146% and 169%, respectively, relative to the neat blend. Enhanced wear resistance was accompanied by increased friction: weight loss decreased by nearly 25%, while the coefficient of friction increased by approximately 12%. Additionally, the hybrid system demonstrated effective electrothermal performance, heating from -40°C to a stable temperature of 29°C at only 5 V within 90 s. Overall, this multifunctional nanocomposite simultaneously enhances mechanical, tribological, and electrothermal performance, offering a promising strategy for durable and temperature-responsive rubber materials.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e70445"},"PeriodicalIF":4.1,"publicationDate":"2026-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149079056","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}
Yongkang Pang, Min Wang, Sarah Fasbender, Martin Jäger, Bernd Strehmel, Zhonghua Tang, Xiongfei Luo
{"title":"Metal Polyphenol Network Enables Photo-ATRP Under Blue Light.","authors":"Yongkang Pang, Min Wang, Sarah Fasbender, Martin Jäger, Bernd Strehmel, Zhonghua Tang, Xiongfei Luo","doi":"10.1002/marc.70443","DOIUrl":"https://doi.org/10.1002/marc.70443","url":null,"abstract":"<p><p>Photo-ATRP commonly relies on petrochemical-derived ligands and copper-based catalytic systems, which is misaligned with green-chemistry principles. Here, 4-hydroxychalcone is used as a building block and functionalized amino groups through a Mannich reaction, then self-assembled with FeBr<sub>3</sub> to form a metal-polyphenol network (MPN). Under 420 nm visible-light irradiation, the MPN effectively mediates photo-ATRP, reaching a maximum monomer conversion of 67.4%. The resulting polymers exhibit a dispersity of Đ < 1.5, with values down to 1.3, indicating a certain control of polymerization. Using the PMMA-Br macroinitiator, synthesis of block copolymers comprising methyl methacrylate (MMA), benzyl methacrylate (BMA), and styrene (St) successfully succeeded. Notably, polymers exhibiting a dispersity of Đ < 1.5 were obtained even without degassing, while chain-end fidelity was available. In addition, a FeCl<sub>3</sub>-catalyzed photo-ATRP system is demonstrated. Overall, this work provides an operationally simple approach to light-controlled radical polymerization using Fe catalysts with bio-based ligands.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e70443"},"PeriodicalIF":4.1,"publicationDate":"2026-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149068729","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}
Qianyu Cai, Till Paha, Marianne Armbruster, André Jung, Eli Zysman-Colman, Andreas-Neil Unterreiner, Michael A R Meier
{"title":"Conjugation-Length Dependent Interplay Between Charge Transfer and Locally Excited States in Sequence-Defined Donor-Acceptor Substituted Oligo(Phenylene Ethynylene)s.","authors":"Qianyu Cai, Till Paha, Marianne Armbruster, André Jung, Eli Zysman-Colman, Andreas-Neil Unterreiner, Michael A R Meier","doi":"10.1002/marc.70442","DOIUrl":"https://doi.org/10.1002/marc.70442","url":null,"abstract":"<p><p>Oligo(para-phenylene ethynylene)s (OPEs) serve as well-defined model compounds to understand electronic effects in conjugated macromolecules. Here, we report a sequence-defined series of OPEs capped with a di-tert-butylcarbazole (DtBCz) donor and a triphenyltriazine (Trz) acceptor to investigate how the donor-acceptor distance along a conjugated OPE backbone governs charge-transfer properties. Using an iterative synthetic strategy, the OPE length was extended stepwise, providing a molecularly highly defined platform to investigate length-dependent excited-state evolution. The lowest excited-state character was examined by steady-state absorption and photoluminescence spectroscopy, Lippert-Mataga analysis, time-resolved photoluminescence (TRPL) spectroscopy, transient absorption (TA) spectroscopy, and quantum-chemical calculations. Shorter OPE sequences (PE0 and PE1) exhibit stronger charge-transfer (CT) dominant behavior, reflected by clear donor-acceptor coherence in transition-density analyses and pronounced solvatochromism. With increasing OPE length (PE2 and PE3), locally excited (LE) contributions become more prominent, leading to hybridized LE and CT (HLCT) states which is further supported by TA and TRPL spectroscopy. The observed CT-to-HLCT evolution highlights the importance of precise backbone length control for rationally tuning excited-state properties in conjugated macromolecules.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e70442"},"PeriodicalIF":4.1,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149023445","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}
Polyxeni P. Angelopoulou, Jong K. Keum, Marti Checa, Peter V. Bonnesen, Yangyang Wang, Amit K. Naskar, Georgios Sakellariou, Kunlun Hong, Logan T. Kearney
{"title":"Functionalization Enhanced Phase Separation in PS-b-PVP Derived Polyzwitterionic Block Copolymers","authors":"Polyxeni P. Angelopoulou, Jong K. Keum, Marti Checa, Peter V. Bonnesen, Yangyang Wang, Amit K. Naskar, Georgios Sakellariou, Kunlun Hong, Logan T. Kearney","doi":"10.1002/marc.70328","DOIUrl":"10.1002/marc.70328","url":null,"abstract":"<div>\u0000 \u0000 <p>Block copolymers with strong tendency for block demixing have attracted significant attention especially for applications in microelectronics and membranes. Enabling technological advances in these areas critically depends on access to well-defined nanostructures with dimensions near or below 10 nm. Block copolymers bearing polyzwitterionic segments are a promising class of materials for phase separation due to their ion association-induced phase segregation which bestow high-<i>χ</i>. In this work, the synthesis of parent poly(styrene)-<i>block</i>-poly(vinylpyridine) (PS-<i>b</i>-PVP) block copolymers that are subsequently modified to the targeted poly(styrene)-<i>block</i>-poly(vinylpyridine carboxybetaine) using a two-step modification scheme is presented. We study the thermophysical and phase separation properties of the parent, polyelectrolyte intermediate and the final polyzwitterionic block copolymers. Ultra-small, periodic nanostructures with half-spacing as low as 5.3 nm are obtained from the polyzwitterionic copolymers. This work demonstrates a scalable synthetic methodology to access pH responsive polyzwitterions and establishes connectivity between polymer design attributes and phase separation behavior for neutral-<i>block</i>-polyzwitterionic copolymers.</p>\u0000 </div>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":"47 18","pages":""},"PeriodicalIF":4.1,"publicationDate":"2026-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148337025","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}
Ting Li, Jie Fang, Dongdong Xia, Zhiyun Hu, Qian Xie, Yuefeng Zhang, Yu Xie, Weiwei Li, Lang Jiang, Chaowei Zhao
{"title":"Benzimidazole-Fused A-D-A’-D-A Type Non-Fullerene Acceptors for Efficient Organic Solar Cells","authors":"Ting Li, Jie Fang, Dongdong Xia, Zhiyun Hu, Qian Xie, Yuefeng Zhang, Yu Xie, Weiwei Li, Lang Jiang, Chaowei Zhao","doi":"10.1002/marc.70368","DOIUrl":"10.1002/marc.70368","url":null,"abstract":"<div>\u0000 \u0000 <p>The molecular engineering of the A-D-A’-D-A type non-fullerene acceptors (NFAs) at the core has generated a diverse of high-performance acceptor materials. Recently, transformation of the benzothiadiazole (BT) core to benzimidazole (Im), which is a widely used unit in constructing functional framework, cluster or carbene based materials, has been explored with a series of Im-based NFAs, which displayed attractive optoelectronic properties. However, the more general synthetic route remains necessary for further exploration of this kind of NFAs. Herein, we applied the typical approach for Im structures by using o-benzoquinone and aldehyde in the presence of ammonium acetate yielding the target NFAs effectively, and three new Im-based acceptors were obtained by adjusting the hanging groups with benzene, 4-fluorobenzene and 3.5-difluorobenzene. These NFAs displayed tunable molecular dipole moments, UV–vis absorption, and frontier energy levels. When used as the guest acceptor in the PM6:BTP-eC9 based organic solar cells, the fluorinated NFAs can effectively improve the device efficiency to 19.48%, which is significantly higher than 18.42% of the binary control and also among top efficiencies for cells using Im-based NFAs. This work provides an effective protocol for Im-based NFAs with tunable molecular scaffolds and properties, which can be of great potential for optoelectronics.</p>\u0000 </div>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":"47 18","pages":""},"PeriodicalIF":4.1,"publicationDate":"2026-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148682920","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}
Ayça Tüter Semercioğlu, Gökhan Önder Aksu, Seda Keskin Avcı, Can Erkey
{"title":"MOF Triggered Gelation: A Novel Method for Preparation of MOF and Aerogel Composites","authors":"Ayça Tüter Semercioğlu, Gökhan Önder Aksu, Seda Keskin Avcı, Can Erkey","doi":"10.1002/marc.70396","DOIUrl":"10.1002/marc.70396","url":null,"abstract":"<div>\u0000 \u0000 <p>A novel method was developed to synthesize composites of Cu-BTC with alginate. The gelation was triggered by the open Cu metal centers which are coordinated to the BTC ligands. The resulting gel was dried supercritically to obtain the aerogel composite. Cu-BTC content in the composite was tuned in to the mass ratio of 1:2 to 2:1 and the resulting materials’ BET surface areas ranged between 450 and 1162 m<sup>2</sup>/g. The equilibrium uptake of CO<sub>2</sub> for AlgA/Cu-BTC (2:1), AlgA/Cu-BTC (1:1), and AlgA/Cu-BTC (1:2) at 1 bar and 298 K was determined as 0.132, 0.325, and 0.434 mmol g<sup>−1</sup>, respectively for a binary mixture of 15% CO<sub>2</sub>/85% N<sub>2</sub>. Uptake values determined by dynamic adsorption experiments were slightly lower than those obtained for single-component CO<sub>2</sub> conditions, which was attributed to competitive adsorption between CO<sub>2</sub> and N<sub>2</sub>. The simulated CO<sub>2</sub> adsorption isotherms slightly overestimated the experimental uptake values, which is consistent with the involvement of open Cu metal centers in the gelation of sodium alginate. This is the first time that a MOF is utilized as a gelation triggering agent and is likely to lead to the development of novel nanostructured alginate aerogel/gel composites of MOFs with divalent cation centers.</p>\u0000 </div>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":"47 18","pages":""},"PeriodicalIF":4.1,"publicationDate":"2026-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148696919","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}
Polyxeni P. Angelopoulou, Jong K. Keum, Marti Checa, Peter V. Bonnesen, Yangyang Wang, Amit K. Naskar, Georgios Sakellariou, Kunlun Hong, Logan T. Kearney
{"title":"Front Cover: Functionalization Enhanced Phase Separation in PS-b-PVP Derived Polyzwitterionic Block Copolymers","authors":"Polyxeni P. Angelopoulou, Jong K. Keum, Marti Checa, Peter V. Bonnesen, Yangyang Wang, Amit K. Naskar, Georgios Sakellariou, Kunlun Hong, Logan T. Kearney","doi":"10.1002/marc.70394","DOIUrl":"https://doi.org/10.1002/marc.70394","url":null,"abstract":"<p>Polyzwitterion-containing block copolymers (BCPs) are prepared from neutral poly(styrene)-<i>block</i>-poly(vinylpyridine) BCPs via a two-step synthetic procedure. The polyzwitterionic BCPs phase separate into well-ordered nanostructures with feature sizes down to 5.3 nm highlighting the strong tendency for block demixing in the system. More details can be found in the Research Article by Kunlun Hong, Logan T. Kearney, and co-workers (DOI: 10.1002/marc.70328).\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":"47 18","pages":""},"PeriodicalIF":4.1,"publicationDate":"2026-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/marc.70394","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149011607","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}