ACS Macro Letters最新文献_第3页

Preparation, Characterization, and Self-Assembly of P3HT-Based Janus Fibers via a Crystallization-Driven Self-Assembly Process. 基于p3ht的Janus纤维的制备、表征和自组装的结晶驱动自组装工艺。

IF 5.8

ACS Macro Letters Pub Date : 2025-09-09 DOI: 10.1021/acsmacrolett.5c00525

Boyang Shi,Chengcheng Zhou,Xinyu Wang,Ding Shen,Guowei Wang

{"title":"Preparation, Characterization, and Self-Assembly of P3HT-Based Janus Fibers via a Crystallization-Driven Self-Assembly Process.","authors":"Boyang Shi,Chengcheng Zhou,Xinyu Wang,Ding Shen,Guowei Wang","doi":"10.1021/acsmacrolett.5c00525","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00525","url":null,"abstract":"Poly(3-hexylthiophene) (P3HT)-based complex topological copolymers have attracted a great deal of attention for their unique electrical and optical properties. In this contribution, the P3HT-based Janus fibers with controlled lengths were innovatively prepared by sequential crystallization-driven self-assembly (CDSA) of poly(p-tert-butylstyrene)-b-polyisoprene-b-poly(3-hexylthiophene) (PtBS-b-PI-b-P3HT) triblock copolymer, cross-linking of the interlayer PI region, and dissociation of fibers in good solvent. The comprehensive characterizations showed that the PtBS/P3HT Janus fibers have nearly half the width of PtBS-b-PI-b-P3HT fibers and fiber lengths close to or slightly shorter than those of PtBS-b-PI-b-P3HT fibers, indicating that the Janus fibers with adjustable lengths could be prepared in a large window range. Furthermore, the PtBS/P3HT Janus fibers could re-self-assemble into average 2- or 4-aggregates in selective solvent. The work provided a general strategy to produce P3HT-based or analogous π-conjugated polymer-based Janus fibers, which is hoped to facilitate the applications of π-conjugated polymers in advanced materials.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"37 1","pages":"1367-1374"},"PeriodicalIF":5.8,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145017994","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

Introducing Disulfide Bonds into Polyester Biomaterials via Nucleophilic Thiol-yne Polymerization. 通过亲核硫醇炔聚合将二硫键引入聚酯生物材料。

IF 5.8

ACS Macro Letters Pub Date : 2025-09-08 DOI: 10.1021/acsmacrolett.5c00427

Daniele Giannantonio,Meltem Haktaniyan,Arianna Brandolese,Maria C Arno,Andrew P Dove

{"title":"Introducing Disulfide Bonds into Polyester Biomaterials via Nucleophilic Thiol-yne Polymerization.","authors":"Daniele Giannantonio,Meltem Haktaniyan,Arianna Brandolese,Maria C Arno,Andrew P Dove","doi":"10.1021/acsmacrolett.5c00427","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00427","url":null,"abstract":"Polyesters are a widely used class of biomaterials thanks to their (bio)degradability and tunable thermomechanical properties. Introducing dynamic disulfide bonds into their backbone enables them to be degraded through different routes and also imparts self-healing properties. However, while numerous polymerization protocols exist with which to introduce disulfide bonds into linear polymers, these methods lack the versatility needed to produce materials with diverse thermomechanical properties. In this work, nucleophilic thiol-yne polymerization was employed to synthesize polymers with a controllable amount of disulfide bonds in the backbone. The crystallinity and, hence, the thermomechanical properties of these polymers were tuned through the variation of different parameters such as disulfide bond content, polymer backbone conformational features (i.e., E/Z isomerism), and monomer combinations. Moreover, polymer degradability was confirmed by leveraging the reversible disulfide bonds in the presence of chemical stimuli. Finally, the cytocompatibility of these polymers was demonstrated, suggesting their potential use as polymeric biomaterials.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"47 1","pages":"1359-1366"},"PeriodicalIF":5.8,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145017995","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

Achieving PLA with Excellent Heat Resistance and Transparency via Synergistic Nucleation Effect Assisted by Hydrogen Bonding 通过氢键辅助的协同成核效应，获得具有优异耐热性和透明性的聚乳酸。

IF 5.2

ACS Macro Letters Pub Date : 2025-09-05 DOI: 10.1021/acsmacrolett.5c00413

Wu Guo, Jian Yang, Tongrui Zhang and Li Li*,

{"title":"Achieving PLA with Excellent Heat Resistance and Transparency via Synergistic Nucleation Effect Assisted by Hydrogen Bonding","authors":"Wu Guo, Jian Yang, Tongrui Zhang and Li Li*, ","doi":"10.1021/acsmacrolett.5c00413","DOIUrl":"10.1021/acsmacrolett.5c00413","url":null,"abstract":"Typically, specific amide nucleating agents (NAs) that can form nanofibrous networks by self-assembly are vital to achieve poly(l-lactic acid) (PLA) with good heat resistance and transparency. However, the long time required for self-assembly during rapid cooling results in a narrow crystallization window for induced PLA, thus requiring a combination of high annealing temperature and a long annealing time. Herein, a synergistic nucleation strategy was introduced to address this challenge, i.e., adopting hexanedioic,1,6-bis (2-benzoyl hydrazide) (TMC) to induce the self-assembly of a N,N-ethylenebis(12-hydroxystearamide) (EBH) nanofibrous network at higher temperature via hydrogen bonding, then promoting the crystallization of PLA via the nucleating effect of EBH nanofibers. In this way, PLA crystals could be induced earlier during the rapid cooling process, resulting in higher crystallinity and smaller crystals. And driven by this synergistic nucleation effect of TMC and EBH, the annealing time of PLA at 85 °C was greatly shortened to 90 s. The accelerated annealing on PLA effectively increased its heat deflection temperature (HDT) to 96.6 °C, and the formation of refined crystals respectively improved its light transmission at 600 nm from 21% to 70% and impact strength from 3.2 to 7.8 kJ/m2. This work would offer a universal approach for accelerating the crystallization rate of NAs for PLA and simultaneously widen the application fields of PLA products.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 9","pages":"1352–1358"},"PeriodicalIF":5.2,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144995739","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

Unlocking Ring-Opening Polymerization of Glycidyl Propargyl Ether via Lewis Pair Organocatalysts 路易斯对有机催化剂解锁缩水甘油丙炔醚开环聚合。

IF 5.2

ACS Macro Letters Pub Date : 2025-09-05 DOI: 10.1021/acsmacrolett.5c00486

Byungwoo Yoo, Jinsu Baek and Byeong-Su Kim*,

{"title":"Unlocking Ring-Opening Polymerization of Glycidyl Propargyl Ether via Lewis Pair Organocatalysts","authors":"Byungwoo Yoo, Jinsu Baek and Byeong-Su Kim*, ","doi":"10.1021/acsmacrolett.5c00486","DOIUrl":"10.1021/acsmacrolett.5c00486","url":null,"abstract":"Alkyne groups provide exceptional versatility for functionalization in macromolecular systems. However, the controlled anionic ring-opening polymerization (AROP) of epoxide monomers bearing terminal alkynes remains challenging due to the lability of alkynes under strongly basic conditions. Herein, we present a controlled AROP of glycidyl propargyl ether enabled by Lewis pair organocatalysis, employing a phosphazene base and triethylborane. This catalytic system suppresses undesired interactions with the acidic alkyne proton, allowing precise control over the polymerization degree (25–100) with narrow dispersity (Đ < 1.1) and high initiation efficiency in the synthesis of poly(glycidyl propargyl ether). Moreover, this method yields diverse polymer architectures, including diblock copolymers via atom transfer radical polymerization and triblock copolymers using a macroinitiator strategy. Post-polymerization modification is demonstrated through Cu-catalyzed azide–alkyne cycloaddition and thiol–yne reactions. We envision that this approach significantly broadens access to alkyne-functionalized AROP systems and paves the way for their use in diverse applications.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 9","pages":"1344–1351"},"PeriodicalIF":5.2,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144995741","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

Side-Chain Poly[2]rotaxane-Toughened Graphene Films 侧链聚[2]轮烷增韧石墨烯薄膜。

IF 5.2

ACS Macro Letters Pub Date : 2025-09-04 DOI: 10.1021/acsmacrolett.5c00459

Mengling Yang, Guoquan Liu, Wenbin Wang, Shaolei Qu, Zhiwei Fan, Zhaoming Zhang, Li Yang*, Chunyu Wang* and Xuzhou Yan*,

{"title":"Side-Chain Poly[2]rotaxane-Toughened Graphene Films","authors":"Mengling Yang, Guoquan Liu, Wenbin Wang, Shaolei Qu, Zhiwei Fan, Zhaoming Zhang, Li Yang*, Chunyu Wang* and Xuzhou Yan*, ","doi":"10.1021/acsmacrolett.5c00459","DOIUrl":"10.1021/acsmacrolett.5c00459","url":null,"abstract":"Graphene-based films are highly valued for their superior conductivity, thermal stability, and mechanical strength, yet their brittleness and low ductility limit their full potential. Current toughening strategies for graphene-based composites mainly focus on interfacial reinforcement between polymers and graphene substrates. However, research on energy dissipation arising from the intrinsic properties of polymers remains limited. Herein, we develop a toughened graphene film (PRrGO) incorporating side-chain poly[2]rotaxane (PR) bearing anthracene units, where both interfacial reinforcement and intramolecular motion contribute to energy dissipation, greatly upgrading the film’s mechanical properties. Results show that PRrGO films exhibit a tensile strength of 183 MPa, strain at break of 20.9%, Young’s modulus of 896 MPa, and toughness of 17.2 MJ/m3, which are 4.27, 2.37, 1.25, and 8.33 times higher than those of original rGO films, respectively, while significantly outperforming conventional polymer-modified graphene films (CrGO). Molecular dynamics simulations reveal a synergistic toughening mechanism: the intramolecular motion of side-chain [2]rotaxane units and the π–π interactions with graphene nanosheets. This study exploits the application of PRs in graphene engineering and provides unique insights into enhancing the performance of two-dimensional materials.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 9","pages":"1336–1343"},"PeriodicalIF":5.2,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990973","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

Tuning Anisotropic Swelling in a Liquid Crystalline Polyester–Polyethylene Glycol Hydrogel via Large Strain and Annealing 通过大应变和退火调节液晶聚酯-聚乙二醇水凝胶的各向异性膨胀。

IF 5.2

ACS Macro Letters Pub Date : 2025-09-03 DOI: 10.1021/acsmacrolett.5c00454

Shasha Li, Yahui Wang, Hongjing Yao and Rong Yang*,

{"title":"Tuning Anisotropic Swelling in a Liquid Crystalline Polyester–Polyethylene Glycol Hydrogel via Large Strain and Annealing","authors":"Shasha Li, Yahui Wang, Hongjing Yao and Rong Yang*, ","doi":"10.1021/acsmacrolett.5c00454","DOIUrl":"10.1021/acsmacrolett.5c00454","url":null,"abstract":"The anisotropic swelling behavior of hydrogels can be controlled by the alignment of their molecular chains. In this work, we report a strategy to precisely control the anisotropic swelling direction of hydrogels by leveraging a rationally designed liquid crystalline polymer in combination with large strain and annealing. A liquid crystalline polyester–polyethylene glycol random block copolymer (LCP-b-PEG) is synthesized via one-pot polycondensation. The LCP block serves three key roles: a physical network, anisotropic skeleton, and nucleation agent. Under large strain, the molecular chains of the LCP block orient and extend, losing their nucleating capacity. Consequently, the PEG molecular chains align under strain and form lamellae perpendicular to the stretching direction. Following annealing, the extended LCP molecular chains refold, with the stacked pendant phenyl groups acting as row nuclei, inducing the PEG chains to form lamellae parallel to the stretching direction. This strategy not only enables precise control over swelling behavior but also facilitates versatile actuation modes, allowing the liquid crystalline hydrogel actuator to perform tasks such as grabbing, hugging, crawling, and climbing.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 9","pages":"1329–1335"},"PeriodicalIF":5.2,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144960103","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

Linear Polyethylene with Ketone Groups for Photodegradability: Higher Efficiency with Side-Chain Carbonyls than In-Chain 具有酮基的线性聚乙烯光降解性：侧链羰基比内链羰基效率更高。

IF 5.2

ACS Macro Letters Pub Date : 2025-09-03 DOI: 10.1021/acsmacrolett.5c00476

Haobo Yuan, Kohei Takahashi, Shintaro Nakagawa, Naoko Yoshie and Kyoko Nozaki*,

引用次数: 0

Sterically Engineered Polymeric HTM with Suppressed Torsion for High-Efficiency and Long-Lifetime Solution-Processed OLEDs 抑制扭转的立体工程聚合物HTM用于高效长寿命溶液处理oled

IF 5.2

ACS Macro Letters Pub Date : 2025-09-01 DOI: 10.1021/acsmacrolett.5c00477

Jingzhi Zhang, Zizheng Tong, Shunyu Wang, Hong Meng and Hao Yan*,

{"title":"Sterically Engineered Polymeric HTM with Suppressed Torsion for High-Efficiency and Long-Lifetime Solution-Processed OLEDs","authors":"Jingzhi Zhang, Zizheng Tong, Shunyu Wang, Hong Meng and Hao Yan*, ","doi":"10.1021/acsmacrolett.5c00477","DOIUrl":"10.1021/acsmacrolett.5c00477","url":null,"abstract":"Achieving both high efficiency and operational stability in solution-processed organic light-emitting diodes (OLEDs) remains a significant challenge due to charge imbalance and the limited structural robustness of polymeric hole transport layers (HTLs). Herein, we report a sterically engineered polymer HTM, TFPHS, designed by incorporating a bulky 1-methyl-4-phenylnaphthalene side group into a TFB-derived conjugated backbone. This structural modification enhances backbone rigidity, suppresses dihedral torsion, and enables balanced hole and electron transport. Devices employing TFPHS exhibit a peak external quantum efficiency of 24% and an extended LT95 lifetime of over 215 h at 1000 cd m–2, substantially outperforming TFB-based counterparts. In-situ Raman spectroscopy, supported by density functional theory (DFT) calculations, reveals that improved photochemical stability stems from the inhibited reorganization of triphenylamine segments. Additionally, TFPHS films display improved morphology and wettability, facilitating a uniform emissive layer formation. This work establishes a clear structure–property–performance relationship and offers a rational design strategy for high-performance polymer semiconductors in solution-processed OLEDs and other optoelectronic applications.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 9","pages":"1314–1322"},"PeriodicalIF":5.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144931016","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

Rapid Preparation of D-A Microporous Polyimides via Domino Polymerization for Photocatalytic Hydrogen Peroxide Production 光催化过氧化氢用多米诺聚合快速制备D-A微孔聚酰亚胺

IF 5.2

ACS Macro Letters Pub Date : 2025-08-29 DOI: 10.1021/acsmacrolett.5c00484

Kaiyu Xiong, Xiaogeng Lin, Shijun Li, Xingyu Ma, Mingxuan Zhang and Lei Li*,

引用次数: 0

Scalable Preparation of Well-Defined Hierarchical Colloidal Materials by Heterogeneous Orthogonal RAFT Polymerization in Water 非均相正交RAFT聚合在水中可扩展制备层次明确的胶体材料

IF 5.2

ACS Macro Letters Pub Date : 2025-08-28 DOI: 10.1021/acsmacrolett.5c00500

Zuobao Zheng, Chaojian Luo, Li Zhang and Jianbo Tan*,

{"title":"Scalable Preparation of Well-Defined Hierarchical Colloidal Materials by Heterogeneous Orthogonal RAFT Polymerization in Water","authors":"Zuobao Zheng, Chaojian Luo, Li Zhang and Jianbo Tan*, ","doi":"10.1021/acsmacrolett.5c00500","DOIUrl":"10.1021/acsmacrolett.5c00500","url":null,"abstract":"Hierarchical assembly of nanosized building blocks has emerged as an effective strategy for the bottom-up fabrication of functional materials with a wide range of potential applications, but large-scale production of well-defined hierarchical colloidal materials still remains challenging. In this study, cross-linked block copolymer micelles with reversible addition–fragmentation chain transfer (RAFT) groups at the interface were prepared by orthogonal RAFT-mediated polymerization-induced self-assembly (PISA) of hydroxypropyl methacrylate (HPMA) in water. These micelles were then used as building blocks for the polymerization-induced hierarchical self-assembly (PIHSA) of N-isopropylacrylamide (NIPAM) in water. We demonstrated that the presence of RAFT groups at the interface of micelles could promote the PIHSA process that enables the preparation of hierarchical colloidal materials with higher-order structures (e.g., vesicles). Careful monitoring the PIHSA process revealed some intermediate structures that provide mechanistic insights into the formation of hierarchical colloidal materials. This study provides a scalable and environmentally benign approach to prepare hierarchical colloidal materials with a diverse set of complex structures.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 9","pages":"1299–1306"},"PeriodicalIF":5.2,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144931065","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