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Sonochemical Nitroxide-Mediated Polymerization: Harnessing Sonochemistry for Polymer Synthesis. 声化学氮氧化物介导的聚合反应:利用声化学进行聚合物合成。
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-11-13 DOI: 10.1002/marc.202400732
Christophe Pauly, Lisa Schlichter, Bart Jan Ravoo, Armido Studer

In polymer science, mechanochemistry is emerging as a powerful tool for materials science and molecular synthesis, offering novel avenues for controlled polymerization and post-synthetic modification. Building upon the previous research, nitroxide-mediated polymerization (NMP) is merged with mechanochemistry through the design of nitroxide-based mechanophore macroinitiators, pioneering the first instance of a sonochemical nitroxide-mediated-type polymerization. As NMP usually requires high temperatures, this study demonstrates that a sonochemical NMP-type process allows polymerization under reduced temperatures down to 55 °C. Moreover, depending on the nature of the employed monomers, gelated networks are obtained, demonstrating the adaptability of the mechanophore system. This study elucidates the potential of mechanochemistry in polymer synthesis, offering insights into manipulating polymerization kinetics and advancing materials science applications.

在聚合物科学领域,机械化学正成为材料科学和分子合成的有力工具,为受控聚合和合成后改性提供了新的途径。在前人研究的基础上,通过设计基于硝基氧化物的机械骨架大引发剂,将硝基氧化物介导聚合(NMP)与机械化学相结合,开创了声化学硝基氧化物介导型聚合的先河。由于 NMP 通常需要较高的温度,这项研究表明,声化学 NMP 型工艺可以在低至 55 °C 的温度下进行聚合。此外,根据所使用单体的性质,还可获得凝胶状网络,这证明了机械发泡体系的适应性。这项研究阐明了机械化学在聚合物合成中的潜力,为操纵聚合动力学和推进材料科学应用提供了见解。
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引用次数: 0
Photo-Accelerated Synthesis of Oligo(triazole amide)s. 光促进寡(三唑酰胺)合成。
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-11-13 DOI: 10.1002/marc.202400759
Alexandros Petropoulos, Laurence Charles, Jean-Michel Becht, Michael Schmitt, Jacques Lalevée, Jean-François Lutz

A photo-assisted process is explored for improving the synthesis of oligo(triazole amide)s, which are prepared by solid phase synthesis using a repeated cycle of two reactions: amine-carboxylic acid coupling and copper-catalyzed azide-alkyne cycloaddition (CuAAC). The improvement of the second reaction is investigated herein. A catalytic system involving Cu(II)Cl2, N,N,N',N″,N″-pentamethyldiethylenetriamine (PMDETA) and a titanocene photoinitiator is explored for reducing the reaction time of CuAAC. This catalyst is first tested on a model reaction involving phenylacetylene and ethyl azidoacetate in DMSO. The kinetics of these model experiments are monitored by 1H NMR in the presence of different concentrations of the photoinitiator. It is found that 30 mol% of photoinitiator leads to quantitative reactions in only 8 min. These conditions are then applied to the solid phase synthesis of oligo(triazole amide)s, performed on a glycine-loaded Wang resin. The backbone of the oligomers is constructed using 6-heptynoic acid and 1-amino-11-azido-3,6,9-trioxaundecane as submonomers. Due to slow reagent diffusion, the CuAAC step required more time in the solid phase than in solution. Yet, one hour only is necessary to achieve quantitative CuAAC on the resin, which is twice as fast as previously-reported conditions. Using these optimized conditions, oligo(triazole amide)s of different length are prepared.

我们探索了一种光助工艺来改进寡(三唑酰胺)的合成,该工艺是通过固相合成法制备的,使用了两个反应的重复循环:胺-羧酸偶联反应和铜催化叠氮-炔环加成反应(CuAAC)。本文对第二个反应的改进进行了研究。为了缩短 CuAAC 的反应时间,研究人员探索了一种由 Cu(II)Cl2、N,N,N',N″,N″-五甲基二乙烯三胺(PMDETA)和二茂钛光引发剂组成的催化体系。该催化剂首先在涉及苯乙炔和叠氮乙酸乙酯在二甲基亚砜中的模型反应中进行了测试。在存在不同浓度光引发剂的情况下,通过 1H NMR 对这些模型实验的动力学进行了监测。结果发现,30 摩尔% 的光引发剂只需 8 分钟就能产生定量反应。然后,这些条件被应用于寡聚(三唑酰胺)的固相合成,合成是在含甘氨酸的王氏树脂上进行的。低聚物的骨架是用 6-庚炔酸和 1-氨基-11-叠氮-3,6,9-三氧杂十一烷作为亚单体构建的。由于试剂扩散速度较慢,CuAAC 步骤在固相中所需的时间比在溶液中长。然而,在树脂上实现定量 CuAAC 只需一小时,比以前报告的条件快了一倍。利用这些优化条件,制备出了不同长度的寡聚(三唑酰胺)。
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引用次数: 0
Advances in Self-Healing Perovskite Solar Cells Enabled by Dynamic Polymer Bonds. 通过动态聚合物键实现自愈合过氧化物太阳能电池的进展。
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-11-13 DOI: 10.1002/marc.202400630
Qisong Yuan, Juxiang Chen, Chengyu Shi, Xiangrong Shi, Chenyu Sun, Bo Jiang

This comprehensive review addresses the self-healing phenomenon in perovskite solar cells (PSCs), emphasizing the reversible reactions of dynamic bonds as the pivotal mechanism. The crucial role of polymers in both enhancing the inherent properties of perovskite and inducing self-healing phenomena in grain boundaries of perovskite films are exhibited. The review initiates with an exploration of the various stability problems that PSCs encounter, underscoring the imperative to develop PSCs with extended lifespans capable of self-heal following damage from moisture and mechanical stress. Owing to the strong compatibility brought by polymer characteristics, many additive strategies can be employed in self-healing PSCs through artful molecular design. These strategies aim to limit ion migration, prevent moisture ingress, alleviate mechanical stress, and enhance charge carrier transport. By scrutinizing the conditions, efficiency, and types of self-healing behavior, the review encapsulates the principles of dynamic bonds in the polymers of self-healing PSCs. The meticulously designed polymers not only improve the lifespan of PSCs through the action of dynamic bonds but also enhance their environmental stability through functional groups. In addition, an outlook on self-healing PSCs is provided, offering strategic guidance for future research directions in this specialized area.

这篇综述探讨了包晶体太阳能电池(PSCs)中的自愈现象,强调动态键的可逆反应是关键机制。文中展示了聚合物在增强包晶石固有特性和诱导包晶石薄膜晶界自修复现象中的关键作用。本综述首先探讨了 PSC 遇到的各种稳定性问题,强调了开发具有延长寿命的 PSC 的必要性,这种 PSC 在受到湿气和机械应力破坏后能够自我修复。由于聚合物特性具有很强的兼容性,因此可以通过巧妙的分子设计,在自愈型 PSC 中采用多种添加剂策略。这些策略旨在限制离子迁移、防止湿气侵入、减轻机械应力和增强电荷载流子传输。通过仔细研究自愈合行为的条件、效率和类型,本综述概括了自愈合 PSC 聚合物中的动态键原理。精心设计的聚合物不仅通过动态键的作用提高了 PSC 的寿命,还通过功能基团增强了其环境稳定性。此外,报告还对自愈合 PSC 进行了展望,为这一专业领域的未来研究方向提供了战略指导。
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引用次数: 0
Antimicrobial Peptide SAAP-148-Functionalized Hydrogels from Photocrosslinkable Polymers with Broad Antibacterial Activity. 具有广泛抗菌活性的光交联聚合物抗菌肽 SAAP-148 功能化水凝胶。
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-11-12 DOI: 10.1002/marc.202400785
Muhammad Atif, Gizem Babuççu, Martijn Riool, Sebastian Zaat, Ulrich Jonas

Antimicrobial peptides (AMPs) are promising alternatives to traditional antibiotics for treating skin wound infections. Nonetheless, their short half-life in biological environments restricts clinical applicability. Covalent immobilization of AMPs onto suitable substrates offers a comprehensive solution, creating contact-killing surfaces with long-term functionality. Here, a copolymer of poly[(hydroxy ethyl acrylamide)-co-(4-benzophenone acrylamide)-co-(pentafluorophenyl acrylate)-co-(ECOSURF EH-3 acrylate)], in short poly(HEAAm-co-BPAAm-co-PFPA-co-EH3A), is synthesized by free radical polymerization. Subsequent modification of active ester groups with the amine groups of SAAP-148, results in a copolymer, that is non-cytotoxic to human lung fibroblasts. UV photocrosslinking of the benzophenone units yields a polymer network that forms a hydrogel after swelling with aqueous medium. Both the SAAP-148-modified polymer in solution and the photocrosslinked hydrogels show good antimicrobial activity against strains of Escherichia coli, Staphylococcus aureus, Pseudomonas aeruginosa, and Acinetobacter baumannii, including multidrug-resistant strains, frequently found in wound infections. The covalent attachment of SAAP-148 prevents leaching, ensuring sustained antimicrobial activity for at least 48 h in diluted human blood plasma and 14 days in PBS. This prolonged retention of antimicrobial activity in human blood plasma significantly enhances its clinical potential. Overall, this study shows the potential of the AMP-functionalized photocrosslinkable polymer as antimicrobial wound dressings, providing an effective alternative to antibiotics.

抗菌肽(AMPs)是治疗皮肤伤口感染的传统抗生素的理想替代品。然而,它们在生物环境中的半衰期较短,限制了其临床应用。将 AMPs 共价固定在合适的基底上提供了一种全面的解决方案,可形成具有长期功能性的接触杀菌表面。本文通过自由基聚合合成了聚[(羟乙基丙烯酰胺)-co-(4-苯甲酮丙烯酰胺)-co-(五氟苯基丙烯酸酯)-co-(ECOSURF EH-3 丙烯酸酯)]共聚物,简称聚(HEAAm-co-BPAAm-co-PFPA-co-EH3A)。活性酯基团与 SAAP-148 的胺基团随后发生改性,从而产生了一种对人类肺纤维母细胞无细胞毒性的共聚物。二苯甲酮单元经紫外线光交联后形成聚合物网络,在水介质中溶胀后形成水凝胶。溶液中的 SAAP-148 改性聚合物和光交联水凝胶对大肠杆菌、金黄色葡萄球菌、铜绿假单胞菌和鲍曼不动杆菌(包括伤口感染中常见的耐多药菌株)都具有良好的抗菌活性。SAAP-148 的共价附着可防止浸出,确保在稀释的人体血浆中至少能保持 48 小时的抗菌活性,在 PBS 中至少能保持 14 天的抗菌活性。这种在人体血浆中的长期抗菌活性大大提高了其临床应用潜力。总之,这项研究显示了 AMP 功能化光交联聚合物作为抗菌伤口敷料的潜力,为抗生素提供了一种有效的替代品。
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引用次数: 0
A Hyperbranched Phosphorus/Nitrogen/Silicon-Containing Polymer as a Multifunctional Additive for Epoxy Resins. 作为环氧树脂多功能添加剂的超支化含磷/氮/硅聚合物
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-11-11 DOI: 10.1002/marc.202400801
Qian Zhong, Siqi Huo, Cheng Wang, Guofeng Ye, Qi Zhang, Hao Wang, Zhitian Liu

High-performance, versatile epoxy resins (EPs) are used in a variety of fields, but the manufacture of transparent, fireproof, and strong EPs remains a major challenge. The hyperbranched, multifunctional flame retardant (DSi) is prepared by using diethanolamine, polyformaldehyde, diphenylphosphine oxide, and phenyltrimethoxysilane as raw materials in this work. When the additional amount of DSi is only 2 wt.%, the EP-DSi2 sample reaches a vertical burning (UL-94) V-0, and its limiting oxygen index (LOI) is 32.8%. When the content of DSi is 3 wt.%, the peak heat release rate (PHRR) and total smoke production (TSP) of EP-DSi samples are 43.8% and 21.4% lower than those of EP. The good compatibility of DSi and EP endows EP-DSi with high transparency, and the hyperbranched structure of DSi makes EP-DSi have obviously enhanced mechanical strength and toughness. The enhanced fire safety of EP-DSi is mainly due to the promoting carbonization and radical quenching effects of DSi. This paper offers a comprehensive design concept aimed at creating high-performance epoxy resins with good optical, mechanical, and flame-retardant properties, which have broad application prospects.

高性能、多功能环氧树脂(EPs)被广泛应用于各个领域,但透明、防火、高强度 EPs 的制造仍是一大挑战。本研究以二乙醇胺、聚甲醛、二苯基氧化膦和苯基三甲氧基硅烷为原料,制备了超支化多功能阻燃剂(DSi)。当 DSi 的添加量仅为 2 wt.%时,EP-DSi2 样品的垂直燃烧(UL-94)达到 V-0,其极限氧指数(LOI)为 32.8%。当 DSi 含量为 3 wt.% 时,EP-DSi 样品的峰值放热率 (PHRR) 和总产烟量 (TSP) 比 EP 样品分别低 43.8% 和 21.4%。DSi 和 EP 的良好相容性赋予 EP-DSi 高透明度,而 DSi 的超支化结构则使 EP-DSi 的机械强度和韧性明显增强。EP-DSi 防火安全性的提高主要得益于 DSi 的促进碳化和自由基淬火作用。本文提出了一种全面的设计理念,旨在创造出具有良好光学、机械和阻燃性能的高性能环氧树脂,其应用前景十分广阔。
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引用次数: 0
Chemical and Solvent-Based Recycling of DGEBA-Based Epoxy Thermoset and Carbon-Fiber Reinforced Epoxy Composite Utilizing Imine-Containing Secondary Amine Hardener. 利用含亚胺的仲胺固化剂对基于 DGEBA 的环氧热固性和碳纤维增强环氧复合材料进行化学和溶剂回收。
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-11-09 DOI: 10.1002/marc.202400678
Özgün Dağlar, Tankut Türel, Christos Pantazidis, Željko Tomović

Epoxy systems are essential in numerous industrial applications due to their exceptional mechanical properties, thermal stability, and chemical resistance. Yet, recycling epoxy networks and reinforcing materials in epoxy composites remains challenging, raising environmental concerns. The critical challenge is the recovery of well-defined molecules upon depolymerization. To address these issues, an innovative strategy is developed utilizing imine-containing secondary amine hardener (M1). The reaction of M1 with DGEBA produced high-performance epoxy thermoset P1, which exhibits Young's modulus of 2.18 GPa and tensile strength of 63.4 MPa, and excellent stability in neutral aqueous conditions. Upon carbon-fiber reinforcement, Young's modulus and tensile strength are significantly elevated to 10.99 GPa and 328.3 MPa, respectively. The reactive secondary amine functionalities enabled the tailored network to display a well-defined growth pattern, yielding only well-defined molecules and intact carbon fibers upon acidic depolymerization. Consequently, the recycled polymers retained properties identical to those of P1. Notably, it is discovered that despite the cross-linked nature of the epoxy networks, complete dissolution in dichloromethane facilitated straightforward solvent-based recycling, allowing the recovery of undamaged carbon fibers and an epoxy thermoset with properties matching the virgin material. Presented novel monomer design and approach showcased two important and efficient recycling options for epoxy systems.

环氧系统因其卓越的机械性能、热稳定性和耐化学性,在众多工业应用中都是必不可少的。然而,环氧树脂复合材料中环氧树脂网络和增强材料的回收利用仍然具有挑战性,引发了环境问题。关键的挑战在于如何在解聚时回收定义明确的分子。为了解决这些问题,我们开发了一种利用含亚胺的仲胺固化剂(M1)的创新策略。M1 与 DGEBA 反应生成了高性能环氧热固性材料 P1,其杨氏模量为 2.18 GPa,拉伸强度为 63.4 MPa,在中性水溶液条件下具有出色的稳定性。碳纤维增强后,杨氏模量和拉伸强度分别显著提高到 10.99 GPa 和 328.3 MPa。活性仲胺官能团使定制网络显示出明确的生长模式,在酸性解聚时只产生明确的分子和完整的碳纤维。因此,再生聚合物保留了与 P1 相同的特性。值得注意的是,尽管环氧网络具有交联性质,但在二氯甲烷中完全溶解后,可直接进行溶剂回收,从而回收未损坏的碳纤维和具有与原始材料相匹配特性的环氧热固性材料。所介绍的新型单体设计和方法展示了环氧系统的两种重要而高效的回收方案。
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引用次数: 0
Enhanced Emission in Polyelectrolyte Assemblies for the Development of Artificial Light-Harvesting Systems and Color-Tunable LED Device. 为开发人工光收集系统和色彩可调 LED 设备而增强聚电解质组件的发射。
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-11-09 DOI: 10.1002/marc.202400752
Qunpeng Duan, Xiuxiu Li, Zhiying Wu, Shihao Lin, Rong Zeng, Tangxin Xiao

Artificial light-harvesting systems (LHSs) are of growing interest for their potential in energy capture and conversion, but achieving efficient fluorescence in aqueous environments remains challenging. In this study, a novel tetraphenylethylene (TPE) derivative, TPEN, is synthesized and co-assembled with poly(sodium 4-styrenesulfonate) (PSS) to enhance its fluorescence via electrostatic interactions. The resulting PSS⊃TPEN network significantly increased blue emission, which is further harnessed by an energy-matched dye, 4,7-di(2-thienyl)benzo[2,1,3]thiadiazole (DBT), to produce an efficient LHS with yellow emission. Moreover, this system is successfully applied to develop color-tunable light-emitting diode (LED) devices. The findings demonstrate a cost-effective and environmentally friendly approach to designing tunable luminescent materials, with promising potential for future advancements in energy-efficient lighting technologies.

人工光收集系统(LHS)因其在能量捕获和转换方面的潜力而日益受到关注,但在水环境中实现高效荧光仍具有挑战性。本研究合成了一种新型四苯基乙烯(TPE)衍生物 TPEN,并将其与聚(4-苯乙烯磺酸钠)(PSS)共同组装,通过静电相互作用增强其荧光。由此产生的 PSS⊃TPEN 网络可显著增加蓝色发射,能量匹配染料 4,7-二(2-噻吩基)苯并[2,1,3]噻二唑(DBT)可进一步利用该网络产生具有黄色发射的高效 LHS。此外,该系统还被成功应用于开发颜色可调的发光二极管(LED)器件。研究结果表明,设计可调谐发光材料是一种既经济又环保的方法,未来有望推动节能照明技术的发展。
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引用次数: 0
Sequence-Controlled Copolymerization of Structurally Well-Defined Multinuclear Zinc Acrylate Complexes and Styrene. 结构明确的多核丙烯酸锌络合物与苯乙烯的序列控制共聚。
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-11-09 DOI: 10.1002/marc.202400742
Takanori Iwasaki, Gaito Suehisa, Ryo Mandai, Kyoko Nozaki

The copolymerization of two or more monomers produces polymeric materials with unique properties that cannot be achieved with homopolymers. However, precise control over the polymer sequence remains challenging because the sequence is determined by the inherent reactivity of comonomers. Therefore, only limited methods using modified monomers or supramolecular interactions are reported. In this study, the sequence control of acrylate-styrene copolymerization using multinuclear zinc complexes is reported. The copolymerization of the zinc acrylate complex with a polymeric sheet-like structure and styrene in benzene affords a copolymer with a higher content of acrylate triad than calculated for the statistical random model, whereas tetranuclear zinc acrylate (TZA) affords a copolymer with fewer adjacent acrylate sequences. The copolymer with a higher content of acrylate triad exhibits a lower glass transition temperature because of the higher mobility of the longer polystyrene segments. These results highlight the promise of multinuclear zinc acrylate complexes as monomers for sequence-controlled copolymerization.

两种或两种以上单体共聚产生的聚合物材料具有均聚物无法达到的独特性能。然而,由于共聚单体的固有反应性决定了聚合物的序列,因此精确控制聚合物序列仍然具有挑战性。因此,目前报道的使用改性单体或超分子相互作用的方法非常有限。本研究报告了利用多核锌配合物控制丙烯酸酯-苯乙烯共聚的序列。具有聚合片状结构的丙烯酸酯锌络合物与苯乙烯在苯中共聚,可得到丙烯酸酯三元组含量高于统计随机模型计算值的共聚物,而四核丙烯酸酯锌(TZA)可得到相邻丙烯酸酯序列较少的共聚物。丙烯酸酯三元组含量较高的共聚物显示出较低的玻璃化转变温度,这是因为较长的聚苯乙烯段具有较高的流动性。这些结果凸显了多核丙烯酸锌配合物作为序列控制共聚单体的前景。
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引用次数: 0
Masthead: Macromol. Rapid Commun. 21/2024 刊头:Macromol.Rapid Commun.21/2024
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-11-08 DOI: 10.1002/marc.202470045
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引用次数: 0
Solidification of Polyurethane Model Foams via Catalyst Drainage from a Secondary Foam 通过催化剂从二次泡沫中排出实现聚氨酯模型泡沫的固化
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-11-08 DOI: 10.1002/marc.202470044
Manon Jouanlanne, Antoine Egelé, Wiebke Drenckhan, Jean Farago, Aurélie Hourlier-Fargette

Front Cover: The generation of model monodisperse polyurethane foams with controlled morphology is achieved via the drainage from a secondary foam containing catalyst into a first foam produced without catalyst, and the homogeneity and reproducibility of the final foams is revealed via detailed structural characterization using X-ray microtomography. More details can be found in article 2400254 by Aurélie Hourlier-Fargette and co-workers.

封面:通过将含有催化剂的二次泡沫排入不含催化剂的一次泡沫中,生成了具有可控形态的单分散聚氨酯泡沫模型,并利用 X 射线显微层析技术进行了详细的结构表征,从而揭示了最终泡沫的均匀性和可重复性。更多详细信息,请参阅 Aurélie Hourlier-Fargette 及其合作者撰写的文章 2400254。
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引用次数: 0
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Macromolecular Rapid Communications
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