ACS Macro Letters最新文献

Regulation of Sol Viscosity and Gel Elasticity in Thermoresponsive Polyrotaxane Block Copolymers via Tunable Macrocycle Coverage 热响应性聚轮烷嵌段共聚物溶胶粘度和凝胶弹性的可调大环覆盖调控

IF 5.8

ACS Macro Letters Pub Date : 2026-11-10 DOI: 10.1021/acsmacrolett.6c00529

Yingfei Wang,Jinhan Chen,Chenhuan Long,Qi Zhu,Fuxiang Li,Chaoying Wu,Wenjian Zhang,Enxu Liu,Yunyan Qiu,Kang Cai,Aspen X.-Y. Chen,Dengke Shen

{"title":"Regulation of Sol Viscosity and Gel Elasticity in Thermoresponsive Polyrotaxane Block Copolymers via Tunable Macrocycle Coverage","authors":"Yingfei Wang,Jinhan Chen,Chenhuan Long,Qi Zhu,Fuxiang Li,Chaoying Wu,Wenjian Zhang,Enxu Liu,Yunyan Qiu,Kang Cai,Aspen X.-Y. Chen,Dengke Shen","doi":"10.1021/acsmacrolett.6c00529","DOIUrl":"https://doi.org/10.1021/acsmacrolett.6c00529","url":null,"abstract":"Thermoresponsive polymers often face a trade-off between low sol viscosity and high gel elasticity because interchain entanglements contribute differently to the two states. Here, we report PNIPAM-b-PEG-b-PNIPAM-based polyrotaxane block copolymers with precisely controlled coverage of cyclodextrin-derived macrocycles. Macrocycle coverage is regulated during threading through kinetic regulation by terminal ATRP initiator groups and thermodynamic regulation by cyclodextrin derivatization, followed by ATRP end-capping. In 20 wt % aqueous solutions, copolymers bearing 22 and 32 macrocycles per chain exhibit apparent viscosities of ∼1% and ∼0.1% of the nonthreaded control, respectively; the resulting gels show storage moduli above 3000 Pa and >900-fold modulus enhancement from 25 to 40 °C, with thermal hysteresis decreasing as macrocycle coverage increases. These results suggest that macrocycles dynamically slide along the PEG segment in the sol state and may translocate during gelation, forming mobile rigid domains that modulate backbone accessibility for interchain entanglement.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"30 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374633","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Real-Time Tracking of Mitochondrial O2•– and Polarity Fluctuations in Ferroptosis via a Polysiloxane-Supported Dual-Channel Fluorescent Probe 通过聚硅氧烷支持的双通道荧光探针实时跟踪铁下垂中线粒体O2•-和极性波动

IF 5.8

ACS Macro Letters Pub Date : 2026-11-07 DOI: 10.1021/acsmacrolett.6c00507

Lu Wang,Xinze Xi,Alessandro Palmieri,Yujing Zuo

引用次数: 0

Deciphering the Manifestations of Topological Imprints in Low-Entangled Polymer 解读低纠缠聚合物中拓扑印迹的表现

IF 5.8

ACS Macro Letters Pub Date : 2026-10-31 DOI: 10.1021/acsmacrolett.6c00471

Aakash Sharma,Ameur Louhichi,Margarita Kruteva,Dieter Richter,Sanjay Rastogi

引用次数: 0

Adaptive Polymer Networks: A Leap from Smart to Life-Like Systems 自适应聚合物网络：从智能到类生命系统的飞跃

IF 5.8

ACS Macro Letters Pub Date : 2026-10-27 DOI: 10.1021/acsmacrolett.6c00502

Destina E. Genc,Negar Rajabi,Hamed Shahsavan,Tayler S. Hebner

{"title":"Adaptive Polymer Networks: A Leap from Smart to Life-Like Systems","authors":"Destina E. Genc,Negar Rajabi,Hamed Shahsavan,Tayler S. Hebner","doi":"10.1021/acsmacrolett.6c00502","DOIUrl":"https://doi.org/10.1021/acsmacrolett.6c00502","url":null,"abstract":"Stimuli-responsive polymers are functional materials that convert environmental stimuli into programmed changes in material properties. The use of these soft materials in numerous applications, such as soft robotics and functional devices, is often founded on their ability to mimic the functions of biological systems. However, many of these stimuli-responsive polymers have been studied thus far as “smart” materials with predetermined, reversible responses that lack the dynamic adaptability that is characteristic of biological systems. Moving toward life-like “adaptable” responses will require thoughtful consideration of multifunctionality, integrated feedback loops, and out-of-equilibrium behavior in the programming of stimuli-responsive polymers. Notably, an immense design space for integrating these functionalities has been explored, providing tools for advancing the design of adaptive behavior in responsive polymer networks. In this Viewpoint, we discuss the broad range of tools that are currently accessible for programming stimuli-responsive behavior spanning from the molecular to the polymer network scale and with respect to macroscopic processing of the material. We discuss how these principles provide a foundation for incorporating increasingly life-like capabilities in stimuli-responsive materials, establishing a toolkit for transforming stimuli-responsive polymers from predictable smart materials into dynamic, adaptive materials that more closely emulate the functionality of biological systems.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"79 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2026-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149250968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Precise Engineering Poly(Glucose Acrylate)-b-Poly(Guanidine Thioctic Acid) Diblock Copolymers for Selective Killing of Drug-Resistant Gram-negative Bacteria 精确工程聚（葡萄糖丙烯酸酯）-b-聚（胍硫辛酸）二嵌段共聚物选择性杀灭耐药革兰氏阴性菌

IF 5.8

ACS Macro Letters Pub Date : 2026-10-27 DOI: 10.1021/acsmacrolett.6c00430

Bing Han,Gangfeng Li,Jian Song,Tengjiao Wang,Peng Li

{"title":"Precise Engineering Poly(Glucose Acrylate)-b-Poly(Guanidine Thioctic Acid) Diblock Copolymers for Selective Killing of Drug-Resistant Gram-negative Bacteria","authors":"Bing Han,Gangfeng Li,Jian Song,Tengjiao Wang,Peng Li","doi":"10.1021/acsmacrolett.6c00430","DOIUrl":"https://doi.org/10.1021/acsmacrolett.6c00430","url":null,"abstract":"Drug-resistant Gram-negative bacteria remain difficult to eradicate owing to their complex and lipopolysaccharide-rich outer membranes. Guanidinium-containing polymers offer a promising membrane-active strategy, combining potent bactericidal activity, preferential interactions with anionic Gram-negative membranes and a low propensity to induce resistance. However, their therapeutic translation is hampered by nonspecific cytotoxicity and limited aqueous solubility. The incorporation of glycosyl pendants may mitigate this through their biocompatibility. However, the inherent polydispersity of natural polysaccharides poses challenges to investigating how glycosyl pendants modulate copolymer performance and how the block ratio can be precisely tuned. Herein, we report a controllable strategy to construct poly(glucose acrylate)-b-poly(guanidine thioctic acid) diblock copolymers termed p(Glum-b-GTAn), by combining reversible addition-fragmentation chain-transfer (RAFT) polymerization with thiol-initiated disulfide exchange polymerization. Precise tuning of the glycosyl-to-guanidinium block ratio (m = 20, n = 10) enabled a systematic balance of antibacterial potency, hemocompatibility, and cytocompatibility. Meanwhile, p(Glu20-b-GTA10) exhibited selective killing of extended-spectrum β-lactamase-producing Escherichia coli (ESBL-E. coli) over methicillin-resistant Staphylococcus aureus (MRSA), negligible resistance development during serial passaging, and effective in vivo antibacterial efficacy in an ESBL-E. coli-induced murine peritonitis model. This work establishes precise engineering of p(Glum-b-GTAn) as a promising strategy for structural optimization of guanidinium-containing diblock copolymers with reduced toxicity and retained antibacterial activity, effectively addressing Gram-negative infections.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"5 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2026-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149250970","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Water Vapor Stability of Silyl Ether Bonds in Silicone Elastomers 有机硅弹性体中硅醚键的水蒸气稳定性

IF 5.8

ACS Macro Letters Pub Date : 2026-10-26 DOI: 10.1021/acsmacrolett.6c00375

Brian M. Jun,Thomas J. McCarthy

引用次数: 0

Preferential Ion Solvation Drives Divergent Miscibility in Polyether Blend Electrolytes 优先离子溶剂化驱动聚醚共混电解质的分散性混相

IF 5.8

ACS Macro Letters Pub Date : 2026-10-26 DOI: 10.1021/acsmacrolett.6c00451

Yongxin Lei,Chao Fang

{"title":"Preferential Ion Solvation Drives Divergent Miscibility in Polyether Blend Electrolytes","authors":"Yongxin Lei,Chao Fang","doi":"10.1021/acsmacrolett.6c00451","DOIUrl":"https://doi.org/10.1021/acsmacrolett.6c00451","url":null,"abstract":"Polymer blending provides a promising route for designing high-performance solid-state electrolytes. Coarse-grained molecular dynamics simulations of binary polyether blends formed by PEO/P(2EO-MO), PEO/P(EO-MO), and P(EO-MO)/P(2EO-MO) mixed with LiTFSI salt reproduce an experimentally observed miscibility sequence. PEO/P(2EO-MO) blends phase-separate at low salt concentrations and mix at high salt concentrations. The effective Flory–Huggins interaction parameters, evaluated via the random phase approximation, transition from critical value in the phase-separated regime to negative in the high-salt miscible regime. This behavior arises from preferential PEO solvation at low salt concentrations and coordination saturation at higher concentrations, which equalizes solvation and promotes ion bridging to restore miscibility. Similar re-entrant mixing is predicted for PEO/P(EO-MO), whereas the mismatched solvation capability and the absence of coordination saturation in P(EO-MO)/P(2EO-MO) sustains phase separation. These findings establish a molecular understanding of how selective ion solvation governs blend miscibility and provide a rational basis for electrolyte design with tailored phase morphology.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"43 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2026-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149248571","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Acrylate-Scavenging Beads Enable High-Throughput Purification of Copolymer Libraries 丙烯酸酯清除珠使高通量纯化共聚物库

IF 5.8

ACS Macro Letters Pub Date : 2026-10-24 DOI: 10.1021/acsmacrolett.6c00480

Alice Y. Wang,Zejie Guo,Trinity A. Blackmon,Roshiny Roy Thomas,Seth E. Chislea,Zhiyao Yang,Ruishi Lei,Junfeng Chen

{"title":"Acrylate-Scavenging Beads Enable High-Throughput Purification of Copolymer Libraries","authors":"Alice Y. Wang,Zejie Guo,Trinity A. Blackmon,Roshiny Roy Thomas,Seth E. Chislea,Zhiyao Yang,Ruishi Lei,Junfeng Chen","doi":"10.1021/acsmacrolett.6c00480","DOIUrl":"https://doi.org/10.1021/acsmacrolett.6c00480","url":null,"abstract":"High-throughput polymer science provides new opportunities to accelerate materials discovery. Acrylate copolymerization provides rapid access to diverse polymer libraries but requires equally rapid, parallel purification to remove unreacted monomers. Here, we report low-cost thiol-functionalized acrylate-scavenging beads (Beads-SH), prepared in two steps from a commercial ion-exchange resin, that efficiently remove residual acrylates through thiol-Michael addition. The beads achieved near-quantitative removal of diverse small-molecule acrylates within 12 h and remained effective in both organic solvents and water. Size-restricted access to the reactive sites within the beads minimized polymer adsorption and side reactions, with no measurable changes in polymer composition, molar mass, or dispersity. As a proof of concept, Beads-SH were used in a microplate format to purify a 72-member library of amphiphilic acrylate copolymers and evaluate polymer-mediated modulation of enzyme activity. This inexpensive, practical, and accessible strategy enables rapid purification of polyacrylate libraries for high-throughput materials discovery.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"13 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2026-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149241513","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Acoustic Field-Assisted Nanoparticle Ordering in Poly(ethylene oxide) Nanocomposites 声场辅助聚环氧乙烷纳米复合材料中纳米粒子的排序

IF 5.8

ACS Macro Letters Pub Date : 2026-10-23 DOI: 10.1021/acsmacrolett.6c00482

Vighnesh Pai,Sameer Rajendra Kalghatgi,Monika Król,Michele Valsecchi,Nicholas Mendez,Caroline Banks,Janne Ruokolainen,Alejandro J. Müller,Sanat K. Kumar,Linda S. Schadler

{"title":"Acoustic Field-Assisted Nanoparticle Ordering in Poly(ethylene oxide) Nanocomposites","authors":"Vighnesh Pai,Sameer Rajendra Kalghatgi,Monika Król,Michele Valsecchi,Nicholas Mendez,Caroline Banks,Janne Ruokolainen,Alejandro J. Müller,Sanat K. Kumar,Linda S. Schadler","doi":"10.1021/acsmacrolett.6c00482","DOIUrl":"https://doi.org/10.1021/acsmacrolett.6c00482","url":null,"abstract":"Prior work has shown that nanoparticle (NP) organization within the interlamellar regions of semicrystalline polymers can be achieved below a critical crystallization rate defined by an appropriate Péclet number, Pe = aG/D, where a is the characteristic NP transport distance, G is the crystal growth rate, and D is the NP diffusivity. NPs can redistribute ahead of the advancing crystallization front and become organized within the interlamellar regions with the most pronounced NP ordering occurring when Pe ≈ 1. We demonstrate, using small-angle X-ray scattering (SAXS) and electron microscopy, that the application of an external acoustic field increases the temperature range (i.e., the supercooling) over which NPs can be ordered by crystallization thereby shifting the kinetic boundary for crystallization-induced ordering and expanding the accessible processing window. Analysis using the Péclet-number framework indicates that acoustic excitation enhances effective NP transport relative to the advancing crystallization front. Acoustic excitation therefore provides a means of controlling NP morphology without substantially altering the bulk crystalline fraction or melting temperature of the polymer matrix.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"79 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2026-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149241584","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

When BAB Beats ABA ionomers: Architecture-Dependent Micelle Packing under Limited Intermicellar Connectivity 当BAB击败ABA离聚体：有限胶束连通性下的结构依赖胶束包装

IF 5.8

ACS Macro Letters Pub Date : 2026-10-21 DOI: 10.1021/acsmacrolett.6c00413

Chia-Chi Tsai,Jie Xu,Hanwen Fan,Yuemin Xin,Yuxiao Zhou,Shuyi Xie

{"title":"When BAB Beats ABA ionomers: Architecture-Dependent Micelle Packing under Limited Intermicellar Connectivity","authors":"Chia-Chi Tsai,Jie Xu,Hanwen Fan,Yuemin Xin,Yuxiao Zhou,Shuyi Xie","doi":"10.1021/acsmacrolett.6c00413","DOIUrl":"https://doi.org/10.1021/acsmacrolett.6c00413","url":null,"abstract":"In conventional ABA triblock copolymers, hard domains (A) often act as physical cross-links connected by a soft midblock (B), leading ABA architecture to be commonly associated with better mechanical performance than BAB analogues. Here, we propose a new design principle using triblock ionomers in which charged A blocks self-assemble into spherical ionic micelles dispersed within a polymer matrix. Surprisingly, BAB triblock ionomer exhibits higher modulus and markedly slower stress relaxation than compositionally analogous ABA triblock. Small-angle X-ray scattering and atomic force microscopy reveal that the BAB architecture produces a much higher density of smaller ionic micelles with substantially reduced intermicellar spacing. With both ABA and BAB show little-to-no intermicellar connectivity, the enhanced mechanical performance cannot be explained by conventional thermoplastic elastomer (TPE) theory. Instead, the dense micellar packing and the resulting cooperative structural relaxation play a critical role in governing the mechanical response. More broadly, this work demonstrates that self-assembled ionic domains can fundamentally alter the structure–property relationships of triblock copolymers and identifies micellar organization as an important design parameter for controlling the mechanics and thermomechanical stability of ionomer materials.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"12 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149225959","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0