ACS Macro Letters最新文献

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Programmable Macrocyclic Enoate-Mediated Regioselective ROMP for Sequence-Controlled Polymer Synthesis 序列控制聚合物合成的可编程大环烯酸酯介导的区域选择性ROMP
IF 5.8
ACS Macro Letters Pub Date : 2025-07-23 DOI: 10.1021/acsmacrolett.5c00468
Ying Wang, Yiyang Liang, Jianhua Tang, Xin Min, Zhenyang Luo, Ye Sha
{"title":"Programmable Macrocyclic Enoate-Mediated Regioselective ROMP for Sequence-Controlled Polymer Synthesis","authors":"Ying Wang, Yiyang Liang, Jianhua Tang, Xin Min, Zhenyang Luo, Ye Sha","doi":"10.1021/acsmacrolett.5c00468","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00468","url":null,"abstract":"Entropy-driven ring-opening metathesis polymerization (ED-ROMP) of macrocyclic olefins with built-in sequence information has emerged as a powerful strategy for synthesizing sequence-controlled polymers. However, conventional cyclic templates often require intricate synthetic procedures to achieve high regio- and stereospecificity. Leveraging the inherent selectivity of olefin cross-metathesis between acrylates and terminal olefins, we developed an easily accessible macrocyclic olefin template featuring an enoate motif. The information within the sequence-defined cyclic enoate monomer can be precisely encoded via an iterative stepwise growth approach. The resulting sequence-controlled polymers, with tunable sequence compositions, serve as an excellent model system for investigating how specific monomer sequences influence the polymer physical properties. This work expands the library of sequence-programmable macrocyclic monomers compatible with a tail-to-head-type polymerization strategy, offering a versatile and efficient platform for precision macromolecular engineering.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"46 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144684854","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
Cryo-EM Visualization of Intermolecular π-Electron Interactions within π-Conjugated Peptidic Supramolecular Polymers. π共轭肽超分子聚合物分子间π-电子相互作用的低温电镜观察。
IF 5.8
ACS Macro Letters Pub Date : 2025-07-21 DOI: 10.1021/acsmacrolett.5c00360
Shane T Rich-New,Runlai Wang,Ayisha Zia,Fengbin Wang,John D Tovar
{"title":"Cryo-EM Visualization of Intermolecular π-Electron Interactions within π-Conjugated Peptidic Supramolecular Polymers.","authors":"Shane T Rich-New,Runlai Wang,Ayisha Zia,Fengbin Wang,John D Tovar","doi":"10.1021/acsmacrolett.5c00360","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00360","url":null,"abstract":"The self-assembly of \"π-peptides\" - molecules with π-electron cores substituted with two or more oligopeptide chains - brings organic electronic function into biologically relevant nanomaterials. π-Peptides assemble into fibrillar nanomaterials as driven by enthalpic peptide-based hydrogen bonding networks and pi-core-based quadrupolar interactions. A large body of spectroscopic, morphological and computational studies informs on the nature of the self-assembly process and the resulting nanostructures, but detailed structural information has remained elusive. Inspired by the recent use of cryogenic electron microscopy (cryo-EM) to provide high-resolution structures for synthetic peptide nanomaterials, we present here the use of cryo-EM to offer ca. 3 Å resolution of π-peptide nanomaterial assemblies, visualizing for the first time the nature of the intermolecular π-core electronic interactions responsible for energy transport through these supramolecular materials.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"96 1","pages":"1100-1106"},"PeriodicalIF":5.8,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669582","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
Stiffening and Toughening Rigid Polymers Through Controllable Stress Concertation Induced by Hard-Hard Dual Nanophases. 硬-硬双纳米相诱导的可控应力集中对刚性聚合物的增强和增韧。
IF 5.8
ACS Macro Letters Pub Date : 2025-07-21 DOI: 10.1021/acsmacrolett.5c00376
Xing Li,Bohan Lv,Haitang Wang,Xuhui Zhang,Jing Huang,Ting Li,Shibo Wang,Weifu Dong
{"title":"Stiffening and Toughening Rigid Polymers Through Controllable Stress Concertation Induced by Hard-Hard Dual Nanophases.","authors":"Xing Li,Bohan Lv,Haitang Wang,Xuhui Zhang,Jing Huang,Ting Li,Shibo Wang,Weifu Dong","doi":"10.1021/acsmacrolett.5c00376","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00376","url":null,"abstract":"Rigid polymers generally face the rigidity-extensibility trade-off due to the contradictory requirements for chain-segment movability. Herein, both the rigidity and extensibility of rigid poly(lactic acid) PLA are obviously improved based on the controllable stress concentration induced by hard-hard dual nanophases, overcoming the long-standing trade-off. Based on masterbatch method and short-term low-temperature annealing, nanodispersed CNTs and nanoscale PLA crystals are constructed in PLA to serve as rigid stress concentrators with small size and high quantity. With the designed hard-hard dual nanophases, the Young's modulus, elongation at break, and toughness of PLA are improved by 32%, 644%, and 776% respectively. The combined high improvement in rigidity and extensibility is unprecedented for PLA. The toughening mechanism is revealed to be that hard-hard dual nanophases can initiate plentiful small-sized microcracks and suppress the development of microcracks during continuous deformation. Besides, the high rigidity of hard-hard dual nanophases imparts PLA with a significantly improved rigidity. Moreover, dual-nanophase PLA also shows improved heat resistance and electrical conductivity. We envision that this work will enrich the theory of polymer toughening and contribute to the industrial preparation of polymers with excellent comprehensive performances.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"11 1","pages":"1107-1113"},"PeriodicalIF":5.8,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669580","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
Advanced Polymer Characterization: Modular Operations for Spectral Alignment by Iterative Compression (MOSAIC). 高级聚合物表征:迭代压缩(MOSAIC)光谱对准的模块化操作。
IF 5.8
ACS Macro Letters Pub Date : 2025-07-18 DOI: 10.1021/acsmacrolett.5c00385
Hanlin M Wang,Benjamin A Suslick,David J Lundberg,Jacob J Lessard,Zhenchuang Xu,Mary A Choy,Jeremiah A Johnson,Jeffrey S Moore
{"title":"Advanced Polymer Characterization: Modular Operations for Spectral Alignment by Iterative Compression (MOSAIC).","authors":"Hanlin M Wang,Benjamin A Suslick,David J Lundberg,Jacob J Lessard,Zhenchuang Xu,Mary A Choy,Jeremiah A Johnson,Jeffrey S Moore","doi":"10.1021/acsmacrolett.5c00385","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00385","url":null,"abstract":"Matrix-assisted laser desorption/ionization (MALDI) mass spectrometry encodes structural information across diverse homo- and copolymer ensembles, yet decrypting these spectra requires a systematic analytical approach. We introduce Modular Operations for Spectral Alignment by Iterative Compression (MOSAIC)─a general cipher algorithm that applies modular arithmetic to filter monomer-derived mass contributions and cluster MALDI peaks by nonconstitutional repeating units (non-CRUs). MOSAIC performs sequential modular operations using monomer mass differences as base units to compress complex spectral data, revealing end-group distributions and comonomer incorporation. As a demonstration, we applied MOSAIC to five copolymers formed by two different polymerization mechanisms. The resulting remainder-mass plots clearly resolve polymer homologs with distinct non-CRUs into visually apparent clusters, enabling intuitive assignment of mass spectral features.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"3 1","pages":"1094-1099"},"PeriodicalIF":5.8,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652752","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
Direct Observation of Short-Time Welding in UHMWPE Powders via X-ray Photon Correlation Spectroscopy and Magnetic Hyperthermia-Induced Sintering. 利用x射线光子相关光谱和磁热烧结直接观察超高分子量聚乙烯粉末的短时间焊接。
IF 5.8
ACS Macro Letters Pub Date : 2025-07-18 DOI: 10.1021/acsmacrolett.5c00388
Mathieu Salse,Guilhem P Baeza,Angelo Pommella,William Chèvremont,Victor Trillaud,Olivier Lame
{"title":"Direct Observation of Short-Time Welding in UHMWPE Powders via X-ray Photon Correlation Spectroscopy and Magnetic Hyperthermia-Induced Sintering.","authors":"Mathieu Salse,Guilhem P Baeza,Angelo Pommella,William Chèvremont,Victor Trillaud,Olivier Lame","doi":"10.1021/acsmacrolett.5c00388","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00388","url":null,"abstract":"We aim to elucidate the time scale over which welding between ultrahigh molecular weight polyethylene (UHMWPE) grains occurs by monitoring the dynamics of iron nanoparticles located at their interfaces, using X-ray photon correlation spectroscopy (XPCS). Within just one min above the melting point, we observe abnormally fast nanoparticle dynamics that emphasize the rapidity of the sintering mechanism, being key for the processing of long-chains polymers, as compared to the much slower chains re-entanglement shown by Yang et al. (Macromolecules, 2024, 57 (18), 8779-8792), resulting in UHMWPE thermodynamic equilibrium. The XPCS results are corroborated by in situ SEM imaging and supported by a theoretical model describing pore resorption, together offering a comprehensive view of early stage dynamics in weakly entangled polymers. To further validate our findings, experiments performed under conventional conduction heating are replicated using induction heating, where iron nanoparticles serve as localized nanoheaters through \"magnetic hyperthermia\", yielding consistent conclusions.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"109 1","pages":"1088-1093"},"PeriodicalIF":5.8,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652753","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
Low-Bandgap Organic Conjugated Copolymers with Ultra-Broadband Optical Limiting Properties Extending to Near-Infrared-II. 低带隙有机共轭共聚物的超宽带光学限制性能扩展到近红外ii。
IF 5.8
ACS Macro Letters Pub Date : 2025-07-17 DOI: 10.1021/acsmacrolett.5c00362
Jiang Wang,Peiran Wang,Yunfei Li,Xiaowei Cheng,Shuyun Zhou,Shuai Han,Jibin Sun,Chenghua Sun
{"title":"Low-Bandgap Organic Conjugated Copolymers with Ultra-Broadband Optical Limiting Properties Extending to Near-Infrared-II.","authors":"Jiang Wang,Peiran Wang,Yunfei Li,Xiaowei Cheng,Shuyun Zhou,Shuai Han,Jibin Sun,Chenghua Sun","doi":"10.1021/acsmacrolett.5c00362","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00362","url":null,"abstract":"Developing organic conjugated copolymers with an intramolecular charge transfer (ICT) system is an efficient strategy for expanding their applications but is still a challenge for broadband optical limiting (OL). Herein, three thiadiazoloquinoxaline (TQ)-based donor-acceptor (D-A) type copolymers P1, P2, and P3 with different electron-donating groups of thiophene, bithiophene, and di(thiophen-2-yl)ethene, respectively, were reported. Copolymers exhibit low bandgaps of 0.70-0.83 eV attributed to their extended π-conjugation and strong ICT. Interestingly, these copolymers display the nonlinear optical response of reversed saturable absorption (RSA) extending from the visible to near-infrared-II region. P3 exhibits the most excellent RSA property with a nonlinear absorption coefficient (β) value of 17.8 cm GW-1, over double that of P1 and P2. Consequently, P3 displays the most remarkable OL ability with a limiting threshold (Fth) of 8.9 J cm-2 under a laser wavelength of 1600 nm. This study provides a new strategy for developing ultra-broadband OL materials based on well-identified D-A copolymers.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"276 1","pages":"1081-1087"},"PeriodicalIF":5.8,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144645896","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
Engineered Probiotics for Colitis Therapy by Improving Intestinal Colonization and Scavenging ROS. 工程益生菌通过改善肠道定植和清除ROS治疗结肠炎。
IF 5.8
ACS Macro Letters Pub Date : 2025-07-17 DOI: 10.1021/acsmacrolett.5c00295
Siyuan Yuan,Xiaomei Dai,Yuqin Zou,Menglin Huang,Xue Yang,Feng Gao
{"title":"Engineered Probiotics for Colitis Therapy by Improving Intestinal Colonization and Scavenging ROS.","authors":"Siyuan Yuan,Xiaomei Dai,Yuqin Zou,Menglin Huang,Xue Yang,Feng Gao","doi":"10.1021/acsmacrolett.5c00295","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00295","url":null,"abstract":"Probiotics hold significant promise for treating colitis, but their application remains challenging because of insufficient colonization and survival against colorectal oxidative stress. Herein, engineered probiotics were prepared to enhance probiotics' colonization and scavenge the overexpressed reaction oxygen species (ROS) at the site of colitis. First, primary amino groups on the Lactobacillus rhamnosus (LAB) surface were converted to free thiols by a simple one-step imidoester reaction. Then, we used thiol-initiated ring-opening cascade of dithiolanes to prepare a class of structurally dynamic microgels on the LAB surface (LAB-gel) by reacting alpha-lipoic acid (LA) and sodium thioctate (LANa). Finally, a lipid bilayer was coated on the surface of the LAB-gel to improve the stability of the microgel in gastric juice. Engineered probiotics survived an oxidative stress insult (100 μM H2O2) and were able to effectively colonize the colon. Furthermore, engineered probiotics could significantly uptake by macrophages and scavenge intracellular ROS. Engineered probiotics with enhanced colonization and ROS scavenging activity showed promising therapeutic effects on colitis.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"37 1","pages":"1075-1080"},"PeriodicalIF":5.8,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144645974","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
Electrostatic Compatibilization of Amorphous and Semicrystalline Immiscible Polymer Blends. 非晶和半晶非混相聚合物共混物的静电增容。
IF 5.1
ACS Macro Letters Pub Date : 2025-07-15 Epub Date: 2025-06-27 DOI: 10.1021/acsmacrolett.5c00294
Haley K Beech, Kseniia M Karnaukh, Madeleine E Miyamoto, KeRay Chen, Jerrick Edmund, Javier Read de Alaniz, Craig J Hawker, Rachel A Segalman
{"title":"Electrostatic Compatibilization of Amorphous and Semicrystalline Immiscible Polymer Blends.","authors":"Haley K Beech, Kseniia M Karnaukh, Madeleine E Miyamoto, KeRay Chen, Jerrick Edmund, Javier Read de Alaniz, Craig J Hawker, Rachel A Segalman","doi":"10.1021/acsmacrolett.5c00294","DOIUrl":"10.1021/acsmacrolett.5c00294","url":null,"abstract":"<p><p>The rapid accumulation of plastic waste underscores the urgent need for effective recycling strategies, yet conventional approaches are hindered by the immiscibility of chemically dissimilar polymers, which phase-separate upon blending and yield poor material properties. This study demonstrates a versatile strategy for electrostatic compatibilization, utilizing acid-base proton transfer between minimally functionalized polymers. Waste-derived polystyrene (PS) was successfully modified with <4 mol % acid groups, while amorphous polybutadiene (PBD) was functionalized with <6 mol % diethylamino base groups and subsequently hydrogenated to yield semicrystalline polyethylene (PE) with the same functionalization level as the PBD. In both cases, blending with functionalized PS produced optically transparent, mechanically robust films. Notably, increasing charge density from 1.0 to 3.5 mol % significantly reduced domain sizes, indicating enhanced compatibilization, while increasing PS molecular weight from 28 to 470 kDa led to a three-order-of-magnitude increase in toughness. In PE/PS blends, the preservation of crystallinity during melt reprocessing was achieved by maintaining low functionalization levels, demonstrating compatibility without sacrificing critical material properties. These findings establish electrostatic compatibilization as a powerful, scalable platform for creating high-performance materials from chemically diverse and mixed plastic waste streams.</p>","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":" ","pages":"969-975"},"PeriodicalIF":5.1,"publicationDate":"2025-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144504118","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
IF 5.1
ACS Macro Letters Pub Date : 2025-07-15
Hantao Zhou, Jesus Guillen Campos, Rishabh Tennankore, Wenwen Xu, Yunfeng Hu, Javier Read de Alaniz* and Ryan C. Hayward*, 
{"title":"","authors":"Hantao Zhou,&nbsp;Jesus Guillen Campos,&nbsp;Rishabh Tennankore,&nbsp;Wenwen Xu,&nbsp;Yunfeng Hu,&nbsp;Javier Read de Alaniz* and Ryan C. Hayward*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 7","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":5.1,"publicationDate":"2025-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmacrolett.5c00206","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144623020","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
IF 5.1
ACS Macro Letters Pub Date : 2025-07-15
Zeyi Yan, Jingjing Xiao, Weijie Zhang, Yuxiang Zhang, Lei Liu, Bo Zhang* and Anchao Feng*, 
{"title":"","authors":"Zeyi Yan,&nbsp;Jingjing Xiao,&nbsp;Weijie Zhang,&nbsp;Yuxiang Zhang,&nbsp;Lei Liu,&nbsp;Bo Zhang* and Anchao Feng*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 7","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":5.1,"publicationDate":"2025-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmacrolett.5c00269","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144623022","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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