ACS Macro Letters最新文献_第2页

Correction to “Fabrication of Functional Polycatechol Nanoparticles” 更正“功能性聚儿茶酚纳米颗粒的制备”

IF 4.9

ACS Macro Letters Pub Date : 2026-10-20 Epub Date: 2026-10-09 DOI: 10.1021/acsmacrolett.6c00510

Xinhao Hu, Zhan Li, Zhen Yang, Fang Zhu, Weifeng Zhao, Gaigai Duan, Yiwen Li

引用次数: 0

Emergence of a Persistent Surface-Normal Dynamical Mode in Planar Polymer Brushes 平面聚合物电刷中持久表面法向动力模式的出现

IF 4.9

ACS Macro Letters Pub Date : 2026-10-20 Epub Date: 2026-09-18 DOI: 10.1021/acsmacrolett.6c00437

Ankit Saha, Michael J. A. Hore

{"title":"Emergence of a Persistent Surface-Normal Dynamical Mode in Planar Polymer Brushes","authors":"Ankit Saha, Michael J. A. Hore","doi":"10.1021/acsmacrolett.6c00437","DOIUrl":"10.1021/acsmacrolett.6c00437","url":null,"abstract":"Polymer graftingaffects chain relaxation dynamics inways thatcan strongly influence the physical properties of polymer nanocompositesand surface layers. Here, we performed energy-conserving dissipativeparticle dynamics (eDPD) simulations with proper orthogonal decomposition(POD) to investigate the dominant relaxation modes of planar polymerbrushes. While the dynamics parallel to the substrate remain largelyconsistent with classical Rouse behavior, the perpendicular dynamicscollapse into a single persistent, surface-localized mode that remainsremarkably robust across polymer chain lengths and grafting densities.We show that this mode can be represented by a localized exponentialcontribution together with a small number of low-order Rouse modes.While the spatial extent of the localized contribution increases withgrafting density, the local strength of the graft-induced perturbationbecomes approximately independent of grafting density once a brushis formed. Further analysis of the contour-resolved dynamical memoryconfirms that grafting produces increasingly anisotropic dynamicsthat extend farther along the polymer contour with increasing graftingdensity. These results provide a mechanistic framework for understandinghow grafting reorganizes polymer dynamics and identify a surface-localizeddynamical mode that may underlie the suppression of long-wavelengthRouse modes observed in neutron scattering experiments.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"15 10","pages":"1550–1557"},"PeriodicalIF":4.9,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149003548","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

Absence of Ionomer Peaks in X-ray Scattering Does Not Imply Absence of Nanophase Separation in Ionomers 在x射线散射中没有离子峰并不意味着离子中没有纳米相分离

IF 4.9

ACS Macro Letters Pub Date : 2026-10-20 Epub Date: 2026-09-22 DOI: 10.1021/acsmacrolett.6c00408

Amalie L. Frischknecht

引用次数: 0

Salt-Induced Nanoparticle Aggregation Decouples Mechanical Reinforcement and Ionic Transport in Polymer Nanocomposite Electrolytes 盐诱导的纳米粒子聚集解耦聚合物纳米复合电解质中的机械增强和离子传输

IF 4.9

ACS Macro Letters Pub Date : 2026-10-20 Epub Date: 2026-09-28 DOI: 10.1021/acsmacrolett.6c00362

Seunghan Yun, So Youn Kim

{"title":"Salt-Induced Nanoparticle Aggregation Decouples Mechanical Reinforcement and Ionic Transport in Polymer Nanocomposite Electrolytes","authors":"Seunghan Yun, So Youn Kim","doi":"10.1021/acsmacrolett.6c00362","DOIUrl":"10.1021/acsmacrolett.6c00362","url":null,"abstract":"We report a salt-responsivestrategy for mechanically reinforcingpolymer nanocomposite (PNC) electrolytes while retaining ionic conductivity(σdc) of neat polymers. In poly(ethylene glycol)(PEG) electrolytes containing negatively charged silica nanoparticles,dissociated Li+ or Na+ cations screen the silicasurfaces and induce particle aggregation. Polymer-ion-silica interactionsconvert the resulting aggregates into stress-bearing structures, increasingthe shear modulus by up to 106-fold depending on PEG molecularweight and particle size. In contrast, σdc remainscomparatively insensitive to silica incorporation. Temperature-dependentσdc is instead strongly influenced by PEG-salt crystallizationand segmental relaxation, indicating strong coupling to polymer dynamics.Vogel–Tammann–Fulcher analysis yields pseudo-activationenergies of approximately 10–11 kJ/mol, while the Vogel temperaturevaries more strongly with PEG molecular weight and cation chemistrythan with silica incorporation. These results identify salt-inducedparticle organization as a practical route to decouple mechanicalreinforcement from ionic transport in PNC electrolytes.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"15 10","pages":"1438–1443"},"PeriodicalIF":4.9,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149093010","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

Aqueous Ring-Opening Metathesis Polymerization for Water-Soluble Polymer Materials 水溶性高分子材料的开环复分解聚合

IF 4.9

ACS Macro Letters Pub Date : 2026-10-20 Epub Date: 2026-10-09 DOI: 10.1021/acsmacrolett.6c00488

Wangmeng Hou, Haoyu Zhang, Fuxianzi Gao, Yi Shi, Chenlu He

{"title":"Aqueous Ring-Opening Metathesis Polymerization for Water-Soluble Polymer Materials","authors":"Wangmeng Hou, Haoyu Zhang, Fuxianzi Gao, Yi Shi, Chenlu He","doi":"10.1021/acsmacrolett.6c00488","DOIUrl":"10.1021/acsmacrolett.6c00488","url":null,"abstract":"Aqueousring-opening metathesis polymerization (ROMP) has beenrecognized as an environmentally friendly and promising approach forsynthesizing water-soluble polymer materials. However, the inevitabledecomposition of Grubbs catalysts in aqueous media restricts aqueousROMP with a low synthetic efficacy and poor control. Over the pastfew decades, substantial progress has been made in understanding themechanisms behind catalyst decomposition in aqueous solution. Buildingon these insights, several advanced aqueous ROMP strategies have beendeveloped, significantly facilitating the preparation of water-solublepolymer materials, including topological polymers, nanostructuredpolymer nano-objects, and polymer–protein bioconjugates. Encouragingly,these strategies have significantly lowered the barrier for researcherslacking a catalyst synthesis background, making aqueous ROMP a moreaccessible and user-friendly route to such materials. This Viewpointfocuses on the mechanisms of catalyst decomposition, highlights representativecases of aqueous ROMP from the past decade, and discusses the futureprospects for this promising field.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"15 10","pages":"1414–1421"},"PeriodicalIF":4.9,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151450","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

Positional Isomerism: A Molecular Switch for Substantial Modulation of Polymer Mechanics 位置同分异构：高分子力学实质性调制的分子开关

IF 4.9

ACS Macro Letters Pub Date : 2026-10-20 Epub Date: 2026-10-12 DOI: 10.1021/acsmacrolett.6c00458

Chengna Yang, Guoquan Liu, Ruixue Bai, Xinli Jing

{"title":"Positional Isomerism: A Molecular Switch for Substantial Modulation of Polymer Mechanics","authors":"Chengna Yang, Guoquan Liu, Ruixue Bai, Xinli Jing","doi":"10.1021/acsmacrolett.6c00458","DOIUrl":"10.1021/acsmacrolett.6c00458","url":null,"abstract":"Positional isomerism, a universal structural regulationstrategyin nature, achieves precise control over biological functions throughminute variations in substituent positions on a molecular backbone.Despite its extensive application in small-molecule chemistry, thesystematic introduction of positional isomerism as the sole structuralvariable into polymer main chains remains unexplored. Herein, inspiredby biological systems, we employ three isomeric aromatic diols, 1,2-,1,3-, and 1,4-benzenedimethanol (o-, m-, and p-BDM) as chain extenders to synthesize threethermoplastic polyurethanes with identical chemical composition, differingonly in the substitution pattern on the aromatic ring. The para-substitutedpolyurethane (p-PU) exhibits a tensile strength of13.1 MPa, an elongation at break of 2016%, and a toughness of 151.8MJ/m3, representing a 7.7-fold increase in tensile strengthand a 19.2-fold increase in toughness over its ortho-substituted counterpart(o-PU, with a tensile strength of 1.7 MPa, an elongationat break of 604%, and a toughness of 7.9 MJ/m3), whilethe meta-substituted polyurethane (m-PU) shows intermediatevalues (tensile strength: 7.4 MPa; elongation at break: 1271%; toughness:47.0 MJ/m3). Combined characterization using small-angleX-ray scattering (SAXS), density functional theory (DFT) calculations,and molecular dynamics simulations reveals that the para isomer, withminimal steric hindrance, promotes ordered hydrogen bonding and π–πstacking within hard segments, inducing the most well-defined microphase-separatedmorphology among the three isomers. This work demonstrates the feasibilityof positional isomerism as an independent dimension for tuning polymerproperties and offers a molecular design strategy for precisely modulatingmechanical performance without altering chemical composition.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"15 10","pages":"1602–1609"},"PeriodicalIF":4.9,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151995","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

Composition Distribution-Dependent Miscibility of Amphiphilic Random Copolymer Mixtures in Water 两亲性无规共聚物混合物在水中的组成分布相关性研究

IF 5.8

ACS Macro Letters Pub Date : 2026-10-20 DOI: 10.1021/acsmacrolett.6c00477

Jimin Yoo,Hiroyuki Kono,Takaya Terashima,Myungeun Seo

{"title":"Composition Distribution-Dependent Miscibility of Amphiphilic Random Copolymer Mixtures in Water","authors":"Jimin Yoo,Hiroyuki Kono,Takaya Terashima,Myungeun Seo","doi":"10.1021/acsmacrolett.6c00477","DOIUrl":"https://doi.org/10.1021/acsmacrolett.6c00477","url":null,"abstract":"Random copolymers intrinsically possess chain-by-chain composition distributions that originate from sequence heterogeneity. Yet they can form macroscopically homogeneous materials and develop intriguing, higher-order self-assembled structures at microscopic levels. Here, we investigate the miscibility and self-assembly behaviors of model amphiphilic random copolymer mixtures in water as a function of composition distributions. We systematically vary the compositional distribution width (σ) and the fraction of the central composition (wR55) by mixing presynthesized random copolymers with different weight ratios. Increasing σ drives a phase transition from homogeneously coassembled, bilayer-folded lamellar mesophases to macrophase-separated, self-sorted states. Introducing a central composition to broadly distributed multinary blends restores macroscopic homogeneity and ordered coassembly, effectively mediating compatibility between compositionally disparate chains. While alternating copolymers with uniform composition distribution do not undergo bilayer folding, the lyotropic mesophase can persist in a ternary blend even under strong shear, suggesting opportunities to use composition distributions as a design parameter of soft matter.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"73 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221526","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

Hydrophobic Monomer Incorporation Tunes the pH Responsivity of Polycationic Brushes 疏水单体掺入调节聚阳离子刷的pH响应

IF 4.9

ACS Macro Letters Pub Date : 2026-10-20 Epub Date: 2026-09-25 DOI: 10.1021/acsmacrolett.6c00398

Adam P. Humpal, Pethuel Ofori, Alexander Dhupar, Ramya Kumar

{"title":"Hydrophobic Monomer Incorporation Tunes the pH Responsivity of Polycationic Brushes","authors":"Adam P. Humpal, Pethuel Ofori, Alexander Dhupar, Ramya Kumar","doi":"10.1021/acsmacrolett.6c00398","DOIUrl":"10.1021/acsmacrolett.6c00398","url":null,"abstract":"We tune the pH-responsiveswelling response of polycationicbrushesvia the incorporation of hydrophobic repeat units. Careful compositionaltuning realizes apparent brush pKa values,which we term pK*a, between 5.0 and 5.7. Further, we observedmonotonic decreases in pK*a with an increase in hydrophobic monomerincorporation. Although brush pK*a was readily tuned with composition,the cooperativity of deprotonation was influenced only by polycationidentity and not hydrophobic monomer incorporation. Interestingly,hydrophobicity-driven pK*a decreases were observed exclusivelyfor brushes and not untethered, compositionally matched polymers,suggesting that confining polymers in the form of nanoparticle-tetheredbrushes might grant more fine-tuned control over pH-responsivity thanthe tunability offered by free polymers alone. We readily reproducedpK*a trends from planar substrates to nanoparticle-tethered brushes,potentiating applications in intracellular pH sensing and nucleicacid delivery that demand precise pKa tuning.We will apply pK*a-tuned brush-grafted nanoparticles to overcomeintracellular barriers that have previously hindered free polymers.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"15 10","pages":"1491–1497"},"PeriodicalIF":4.9,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149050169","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

Light- and Temperature-Programmed Block Copolymer Capsules with Tunable Shell Nanostructures 具有可调壳纳米结构的光和温度编程嵌段共聚物胶囊

IF 4.9

ACS Macro Letters Pub Date : 2026-10-20 Epub Date: 2026-09-06 DOI: 10.1021/acsmacrolett.6c00395

Zhengping Tan, Jinwoo Kim, Younghyeon Ahn, Jaeyoung Choi, Dong-Po Song, Yuesheng Li, Kang Hee Ku, Bumjoon J. Kim

{"title":"Light- and Temperature-Programmed Block Copolymer Capsules with Tunable Shell Nanostructures","authors":"Zhengping Tan, Jinwoo Kim, Younghyeon Ahn, Jaeyoung Choi, Dong-Po Song, Yuesheng Li, Kang Hee Ku, Bumjoon J. Kim","doi":"10.1021/acsmacrolett.6c00395","DOIUrl":"10.1021/acsmacrolett.6c00395","url":null,"abstract":"Polymercapsules capable of adopting distinct shell nanostructuresin response to external stimuli are attractive microcompartments forencapsulation, separation, and triggered release. Realizing such capsulesrequires orthogonal control, in which distinct stimuli independentlydefine the structural outcome. Here, we report a light- and temperature-programmedassembly strategy for hollow polystyrene-block-poly(4-vinylpyridine)(PS-b-P4VP) block copolymer (BCP) capsules with tunableshell nanostructures. The key to this dual responsiveness is a photocleavablethermoresponsive additive, in which an amide-based thermoresponsivebackbone sets the transition temperature and a photocleavable comonomerencodes the light response. During emulsion-confined assembly, photocleavageshifts the lower critical solution temperature of the additive andredistributes it between the aqueous and organic phases, selectingeither concentric lamellar or cylindrical shells at a given temperature.Replacing the poly(N-isopropylacrylamide) backbonewith poly(N-isopropylmethacrylamide) raises the operatingtemperature from 27 to 50 °C, whereas replacing the o-nitrobenzyl group with a coumarin unit shifts photoactivation from365 to 410 nm and reverses the direction of the light-driven morphologyselection. This modular design offers a versatile strategy for programmingBCP capsule shell morphologies under user-defined thermal and opticalconditions.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"15 10","pages":"1483–1490"},"PeriodicalIF":4.9,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148896031","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

Light-Programmed Reversible Valence Reconfiguration of Polymeric Colloidal Molecules 高分子胶体分子的光控可逆价态重构

IF 4.9

ACS Macro Letters Pub Date : 2026-10-20 Epub Date: 2026-09-11 DOI: 10.1021/acsmacrolett.6c00426

Hongzhu Lai, Yuying Huang, Li Jiang, Daoyong Chen

{"title":"Light-Programmed Reversible Valence Reconfiguration of Polymeric Colloidal Molecules","authors":"Hongzhu Lai, Yuying Huang, Li Jiang, Daoyong Chen","doi":"10.1021/acsmacrolett.6c00426","DOIUrl":"10.1021/acsmacrolett.6c00426","url":null,"abstract":"Polymericcolloidal molecules (CMs) with light-switchable compartmentalarchitectures and valences are attractive building blocks for reconfigurablecolloidal materials. Here, we report the stepwise and reversible light-inducedvalence reconfiguration of preformed AB2-type CMs. TheCMs were prepared by associating an amine-functionalized trans-azobenzene (t-AZO) with the PAA corona of poly(acrylicacid)-block-poly(vinylnaphthalene) (PAA-b-PVN) micelles, producing a PVN core (A) and two t-AZO-rich PAA corona compartments (B). Upon 365 nm UV irradiation,the AB2 CMs evolved successively into AB3- andAB4-rich states, whereas 470 nm visible-light irradiationdrove the reverse AB4/AB3/AB2 evolutionover repeated cycles. The reversible reconfiguration is attributedprimarily to photoisomerization-induced changes in AZO packing withinthe PAA corona, which regulate B compartment formation and number.The light-selected valence states further directed secondary assemblyinto linear chains, branched assemblies, and interconnected networks.Light therefore enables dynamic reprogramming of both the valenceof preformed CMs and the topology of their subsequent higher-orderassemblies.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"15 10","pages":"1544–1549"},"PeriodicalIF":4.9,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148933574","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