European Polymer Journal最新文献_第2页

Degradation and in vivo evaluation of an innovative delayed release implant of medical grade poly(glycolide-co-trimethylene carbonate-co-ε-caprolactone) 创新型医用聚（乙二醇-三亚甲基碳酸酯-ε-己内酯）缓释植入物的降解和体内评估

IF 5.8 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2024-11-09 DOI: 10.1016/j.eurpolymj.2024.113569

Norman L. Ilich , Enoch Chan , M. Scott Taylor , Brian Gaerke , Sinduja Suresh , Damien G. Harkin , Flavia Medeiros Savi , Siamak Saifzadeh , Dietmar W. Hutmacher , Tim R. Dargaville

Delayed release implants are a potential method to deliver a therapeutic after a specified lag time. A reservoir implant fabricated by dip-coating allows facile loading of a payload designed to be injected subcutaneously with release controlled by the physicochemical properties of a soft biodegradable terpolymer, poly(glycolide-co-trimethylene carbonate-co-ε-caprolactone). A triphasic profile is achieved, consisting of a lag period (Phase 1) due to negligible terpolymer degradation preventing payload release. By 37 days (Phase 2) bulk erosion of the terpolymer reaches a state where payload begins to diffuse into the surrounding medium, accounting for 75 % of release and 20 % mass loss, indicating a combination of diffusion and erosion-mediated release. Lastly, Phase 3 is predominately diffusion-controlled as 20 % payload release is achieved with minimal mass loss of the polymer. In a rodent preclinical model, the terpolymer was well-integrated within host tissue with a balanced foreign body reaction. This study demonstrates the feasibility of using a unique medical grade poly(ester)-based polymer to develop a delayed release implant with excellent potential for translation. Prospective applications of this device include the delivery of sensitive payloads such as protein vaccines as polymer-payload interactions during manufacturing are avoided.

延迟释放植入物是一种在特定滞后时间后释放治疗药物的潜在方法。通过浸涂法制造的储层植入物可以方便地装载有效载荷，设计为皮下注射，释放量由可生物降解的软性三元共聚物--聚（乙二醇-共三亚甲基碳酸酯-共ε-己内酯）的物理化学特性控制。由于三元共聚物降解微乎其微，阻碍了有效载荷的释放，因此出现了一个滞后期（第 1 阶段）。到 37 天时（第 2 阶段），三元共聚物的大量侵蚀达到有效载荷开始向周围介质扩散的状态，占释放量的 75% 和质量损失的 20%，表明扩散和侵蚀介导的释放相结合。最后，第 3 阶段主要由扩散控制，有效载荷的释放量为 20%，聚合物的质量损失极小。在啮齿动物临床前模型中，三元共聚物与宿主组织很好地结合在一起，异物反应平衡。这项研究证明了使用一种独特的医用级聚酯聚合物来开发缓释植入物的可行性，具有很好的应用前景。这种装置的应用前景包括输送敏感的有效载荷，如蛋白质疫苗，因为在制造过程中避免了聚合物与有效载荷之间的相互作用。

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引用次数: 0

Balancing hydrophobicity and surface potential in bio-based bisfuran-containing polyamide coatings for enhanced long-term antibacterial efficacy and endotoxin adsorption 平衡生物基含双呋喃聚酰胺涂层的疏水性和表面电位，提高长期抗菌效果和内毒素吸附性

IF 5.8 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2024-11-09 DOI: 10.1016/j.eurpolymj.2024.113571

Liuqi Shi , Hong-Hui Shu , Zhiyuan Zhu , Cheng-Mei Liu , Jingyi Rao

To develop antimicrobial protective materials based on renewable polymers, we synthesized a series of bio-based bisfuran-based polyamide (bFPA) polymers with various functional groups, including allyl quaternary ammonium cations, decyl quaternary ammonium cations, and sulfonate betaine. These bFPA-based coating materials, featuring excellent thermal stability (>230 °C) and biocompatibility, were facilely fabricated on polyurethane (PU) substrates by blending and crosslinking with unsaturated aliphatic PU resin. By altering the combination of different functional groups in bFPA polymers, we controlled the hydrophilicity/hydrophobicity and surface charge properties of the bio-based coating. Compared to pure PU coatings, the bFPA-based coatings with moderate hydrophilicity/hydrophobicity and surface potential significantly reduced the adhesion of model protein and bacteria by approximately 70 % and >99 %, respectively, demonstrating outstanding anti-protein and anti-bacterial adhesion properties. Even after seven cycles of use, the coatings maintained the ability to kill ∼80 % and >99 % of Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus bacteria, respectively, indicating long-lasting antibacterial activity. Additionally, the optimized bFPA-based coatings effectively adsorbed ∼80 % of endotoxins from damaged Gram-negative bacteria through electrostatic interactions, thereby reducing the risk of inflammation and sepsis. The development of bio-based polyamide coatings with long-term antibacterial and endotoxin adsorption properties significantly advances their safe and reliable application of in the field of biomedical devices.

为了开发基于可再生聚合物的抗菌保护材料，我们合成了一系列具有不同官能团（包括烯丙基季铵盐、癸基季铵盐和磺酸甜菜碱）的生物基双氟呋喃基聚酰胺（bFPA）聚合物。通过与不饱和脂肪族聚氨酯树脂混合和交联，可在聚氨酯（PU）基材上方便地制造出这些基于 bFPA 的涂层材料，它们具有优异的热稳定性（230 °C）和生物相容性。通过改变双酚A聚合物中不同官能团的组合，我们控制了生物基涂层的亲水性/疏水性和表面电荷特性。与纯聚氨酯涂层相比，亲水性/疏水性和表面电位适中的 bFPA 基涂层能显著降低模型蛋白质和细菌的附着力，降幅分别约为 70% 和 99%，显示出出色的抗蛋白质和抗细菌附着性能。即使在使用七个周期后，涂层仍能分别杀死 80% 和 99% 的革兰氏阴性大肠杆菌和革兰氏阳性金黄色葡萄球菌，这表明涂层具有持久的抗菌活性。此外，优化的生物基聚酰胺涂层通过静电相互作用，有效吸附了 80% 的受损革兰氏阴性细菌的内毒素，从而降低了炎症和败血症的风险。具有长期抗菌和内毒素吸附特性的生物基聚酰胺涂层的开发，大大推进了其在生物医学设备领域安全可靠的应用。

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引用次数: 0

Facile synthesis of polyhedral oligomeric silsesquioxanes with excellent thermosetting, fibrous and crystalline properties 轻松合成具有优异热固性、纤维性和结晶性的多面体低聚硅倍半氧烷

IF 5.8 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2024-11-08 DOI: 10.1016/j.eurpolymj.2024.113568

Weiwei Zhang , Yukuan Niu , Wenchao Zhang , Rongjie Yang

The development of multifunctional polyhedral oligomeric silsesquioxanes (POSS) that are more serialized than traditional POSS is essential to reduce the economic investment and expand the category of high-performance POSS. This work employed a simple one-step method to synthesize a series of different physical states of methacryloxypropyl-phenyl POSS (AcPhPOSS). The FTIR, NMR and MS results showed that the products were mainly composed of regular T₈, T₁₀ and T₁₂ cage-like structures, and the outer periphery of the AcPhPOSS cage carried different proportions of flexible methacryloxypropyl (R₁) and rigid phenyl (R₂) groups. In addition, the curable, fibrous, and crystalline properties of liquid, semi-solid, and powder AcPhPOSS were studied through thermal curing, electrospinning, and crystallization methods, respectively. The results showed that AcPhPOSS in three different states, especially AcPhPOSS@1:0 (liquid), AcPhPOSS@1:3 (semi-solid) and AcPhPOSS@0:1 (powder), exhibited good thermal curing properties, fiber and crystallization, respectively. Hence, this work proposes a facile strategy for producing multifunctional materials with good curing properties, fiber-forming properties, and crystallinity, which have broad application potential in thermosetting resins, fiber materials, and single crystal materials.

开发比传统 POSS 更系列化的多功能多面体低聚硅倍半氧烷（POSS）对于减少经济投资和扩大高性能 POSS 的种类至关重要。本研究采用简单的一步法合成了一系列不同物理状态的甲基丙烯酰氧基丙基苯基 POSS（AcPhPOSS）。傅立叶变换红外光谱、核磁共振和质谱结果表明，产物主要由规则的 T8、T10 和 T12 笼状结构组成，AcPhPOSS 笼的外围带有不同比例的柔性甲基丙烯酰氧基丙基（R1）和刚性苯基（R2）。此外，还分别通过热固化法、电纺丝法和结晶法研究了液态、半固态和粉末 AcPhPOSS 的可固化性、纤维性和结晶性。结果表明，三种不同状态的 AcPhPOSS，特别是 AcPhPOSS@1:0（液态）、AcPhPOSS@1:3（半固态）和 AcPhPOSS@0:1（粉末），分别具有良好的热固化性能、纤维性能和结晶性能。因此，本研究提出了一种简便的策略来生产具有良好固化性能、纤维成型性能和结晶性的多功能材料，在热固性树脂、纤维材料和单晶材料方面具有广泛的应用潜力。

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引用次数: 0

Studies on preparation of silicon-containing polyester via ring-opening polymerization and new type of elastomers derived from the resulting diols 通过开环聚合法制备含硅聚酯以及由所得二元醇衍生出的新型弹性体的研究

IF 5.8 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2024-11-08 DOI: 10.1016/j.eurpolymj.2024.113570

Zedong He , Hao Zhang , Ju Xie , Ti Zhou , Jie Zhang

Silicon-containing polyesters represent a novel class of polymers that integrate silicone and polyester units within their main chain. Polysiloxanes typically consist of flexible chain segments, while polyesters are characterized by their rigidity. The combination of these two components in the main chain offers the potential for tunable properties across a broad range. For the first time, a new organosilicon cyclic ester monomer (Si-Mon) was synthesized using a pseudo-high dilution condensation method. Both theoretical and experimental studies confirm that the ring-opening reaction site of Si-Mon is the ester group, rather than the Si-O-Si bond. Silicon-containing polyesters (SiPET-Series 1) with molecular weights exceeding 20,000 Da were efficiently and rapidly synthesized at room temperature, utilizing benzyl alcohol as the initiator and t-BuP₄ as the catalyst. Organosilicon polyester diols (SiPET-Series 2) with varying molecular weights were produced using 1,4-benzenedimethanol as the initiator. Additionally, a new type of organosilicon polyester elastomer (SiPET-E) was developed by employing SiPET-Series 2 as the base gum and (2,4,6-trioxotriazine-1,3,5(2H,4H,6H)- triyl)tris(hexamethylene)isocyanate (THDI) as the crosslinking agent. The stress–strain behavior of SiPET-E is influenced by the molecular weight of SiPET-Series 2. Notably, SiPET-E exhibits remarkable properties; for instance, it demonstrates superelastic characteristics when the molecular weight of SiPET-Series 2 is 13,000 g/mol, achieving a tensile strength of 2.56 MPa and an elongation at break of 776 % without the use of reinforcing fillers.

含硅聚酯是一类新型聚合物，其主链中集成了硅氧烷和聚酯单元。聚硅氧烷通常由柔性链段组成，而聚酯则以刚性为特征。主链中这两种成分的结合为实现广泛的可调特性提供了可能。我们首次采用假高稀释缩合法合成了一种新型有机硅环酯单体（Si-Mon）。理论和实验研究都证实，Si-Mon 的开环反应位点是酯基，而不是 Si-O-Si 键。利用苯甲醇作为引发剂，t-BuP4 作为催化剂，在室温下高效、快速地合成了分子量超过 20,000 Da 的含硅聚酯（SiPET-系列 1）。使用 1,4-苯二甲醇作为引发剂，生产出了不同分子量的有机硅聚酯二元醇（SiPET 系列 2）。此外，以 SiPET 系列 2 为基胶，以(2,4,6-三氧三嗪-1,3,5(2H,4H,6H)-三基)三(六亚甲基)异氰酸酯 (THDI) 为交联剂，开发了一种新型有机硅聚酯弹性体 (SiPET-E)。SiPET-E 的应力应变行为受 SiPET-Series 2 分子量的影响。值得注意的是，SiPET-E 具有显著的特性，例如，当 SiPET-Series 2 的分子量为 13,000 g/mol 时，它表现出超弹性特性，在不使用增强填料的情况下，拉伸强度达到 2.56 MPa，断裂伸长率达到 776%。

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引用次数: 0

Mechanically robust, self-healing and stretchable electromagnetic shielding materials based on multi-component dynamic bonded polyurethane elastomer 基于多组分动态粘合聚氨酯弹性体的机械坚固、自修复和可拉伸电磁屏蔽材料

IF 5.8 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2024-11-07 DOI: 10.1016/j.eurpolymj.2024.113556

Zongyi Zheng , Jiaji Zhu , Huagao Fang , Jiewu Cui , Yong Zhang , Yunsheng Ding

Stretchable self-healing electromagnetic interference (EMI) shielding materials can automatically restore their original performance after mechanical damage, and can still maintain over 20 dB EMI shielding effectiveness (EMI SE) under tensile state. In this work, a series of highly stretchable self-healing polyurethane elastomer PUBNS-X was prepared by introducing dynamic disulfide bonds, boronic ester bonds and boron-nitrogen coordination (B-N) on the polyurethane main chain. It was found that B-N coordination significantly increased the elongation at break and the tensile strength. The high dynamic reversibility of boronic ester, disulfide bond and B-N coordination bond synergistically endowed PUBNS-X with excellent temperature-triggered self-healing properties. The mechanical properties of PUBNS-X can be restored to more than 90 % at 60 °C. The pre-assembled silver nanowires (AgNWs) conductive network was then introduced into the polyurethane surface by taking advantage of the fluidity of the dynamically bonded polyurethane backbone to obtain a series of stretchable self-healing electromagnetic shielding composites (AgNWs/PUBNS-Y). The results showed that the EMI SE of AgNWs/PUBNS-Y can reach ∼55 dB, and the conductivity can be restored to 82 % of the original value after healing at 60 °C. The investigation of the electromagnetic interference shielding performance of composites under different strains showed that the EMI SE of AgNWs/PUBNS-3 can still maintain 20 dB under 90 % strain. These composites will have broad potential applications in the fields of flexible wearable electronic products, bionic intelligent materials and soft robots.

可拉伸自愈合电磁干扰（EMI）屏蔽材料可在机械损伤后自动恢复原有性能，在拉伸状态下仍能保持 20 分贝以上的 EMI 屏蔽效能（EMI SE）。在这项工作中，通过在聚氨酯主链上引入动态二硫键、硼酸酯键和硼氮配位（B-N），制备了一系列高拉伸自修复聚氨酯弹性体 PUBNS-X。研究发现，B-N 配位显著提高了断裂伸长率和拉伸强度。硼酸酯、二硫键和 B-N 配位键的高动态可逆性协同赋予了 PUBNS-X 优异的温度触发自修复性能。在 60 °C 时，PUBNS-X 的机械性能可恢复到 90% 以上。然后，利用动态键合聚氨酯骨架的流动性，将预组装的银纳米线（AgNWs）导电网络引入聚氨酯表面，得到了一系列可拉伸的自修复电磁屏蔽复合材料（AgNWs/PUBNS-Y）。结果表明，AgNWs/PUBNS-Y 的电磁干扰 SE 可达到 ∼55 dB，在 60 °C 下愈合后导电率可恢复到原始值的 82%。对复合材料在不同应变下的电磁干扰屏蔽性能的研究表明，AgNWs/PUBNS-3 的 EMI SE 在 90% 的应变下仍能保持 20 dB。这些复合材料将在柔性可穿戴电子产品、仿生智能材料和软机器人等领域具有广阔的应用前景。

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引用次数: 0

Visible-light-switchable glass transition temperatures and optical actuation in crosslinked fluoroazopolymers 可见光可切换玻璃化转变温度和交联氟唑聚合物中的光学致动作用

IF 5.8 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2024-11-06 DOI: 10.1016/j.eurpolymj.2024.113563

Youfeng Yue

Nature has provided significant inspiration for designing polymer materials that can move in response to light, with many examples of such materials created, especially using ultraviolet (UV) light as an external stimulus. However, it is essential to design materials that can regulate the mechanical properties of polymers through visible light stimulation and macroscale movement under visible light exposure. Here, we have developed a polymer film chemically crosslinked with fluorinated azobenzenes, which produces a strong mechanical response when exposed to green or blue light in air. The film exhibits visible-light-switchable mechanical properties and directional bending due to the photoisomerization of azo chromophores in the crosslinked polymer networks. The thin film also changes their optical transparency upon visible light irradiation. This work offers insights into the development of responsive polymer materials and photomechanical materials, advancing the realization of self-propelled machines and soft robotics powered by visible light.

大自然为设计能随光移动的聚合物材料提供了重要灵感，并创造了许多此类材料的实例，尤其是利用紫外线（UV）作为外部刺激。然而，必须设计出能够通过可见光刺激调节聚合物机械特性的材料，并在可见光照射下实现宏观运动。在这里，我们开发了一种与氟化偶氮苯化学交联的聚合物薄膜，当它暴露在空气中的绿光或蓝光下时，会产生强烈的机械响应。由于交联聚合物网络中的偶氮发色团发生了光异构化，这种薄膜具有可在可见光下切换的机械特性和方向性弯曲。在可见光照射下，薄膜的光学透明度也会发生变化。这项研究为开发响应性聚合物材料和光机械材料提供了新的视角，推动了以可见光为动力的自走式机器和软机器人的实现。

引用次数: 0

Multifunctional performance of gallic acid in biodegradable food packaging films and coatings: Mechanisms, developments, applications, and horizons 没食子酸在可生物降解食品包装薄膜和涂料中的多功能表现：机理、发展、应用和前景

IF 5.8 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2024-11-06 DOI: 10.1016/j.eurpolymj.2024.113559

Behnam Bahramian , Reza Abedi-Firoozjah , Narges Kiani-Salmi , Asghar Azizian , Nazli Dorud , Seyyed Mohammad Ali Noori , Mohammad Hashemi , Elham Assadpour , Milad Tavassoli , Ehsan Sadeghi , Fuyuan Zhang , Seid Mahdi Jafari

There is an increasing interest in the development of degradable and biopolymeric food packaging films (FPFs) based on green ingredients and strategies. To enhance the performance of these films, modifications can be made to the biopolymer molecules, or additives can be incorporated, such as nanomaterials, crosslinkers, bioactive compounds, and other polymers. The use of green compounds is an effective method to improve the performance of degradable FPFs, with gallic acid (GA) being a widely used natural green compound in various biopolymeric films. This review provides an in-depth analysis of GA chemistry and discusses the different types of biopolymeric FPFs crosslinked by GA. Furthermore, it summarizes the recent applications of GA crosslinked biopolymeric FPFs/coatings for food preservation. The comprehensive improvement of biopolymeric films due to GA crosslinking is evident, with the effect on the films’ properties dependent on the concentration of GA and reaction state. The cross-linking of GA with polymer molecules increases the cohesion of the polymer network, with physical and chemical covalent crosslinking being the two main types of cross-linking. Notably, biopolymeric FPFs/coatings crosslinked by GA have demonstrated remarkable effectiveness in preserving fresh foods.

人们对基于绿色成分和策略开发可降解和生物聚合物食品包装薄膜（FPF）的兴趣与日俱增。为提高这些薄膜的性能，可对生物聚合物分子进行改性，或加入添加剂，如纳米材料、交联剂、生物活性化合物和其他聚合物。使用绿色化合物是提高可降解 FPF 性能的有效方法，其中没食子酸（GA）是一种广泛应用于各种生物聚合物薄膜的天然绿色化合物。本综述深入分析了没食子酸的化学性质，并讨论了由没食子酸交联的不同类型的生物聚合物 FPF。此外，它还总结了 GA 交联生物聚合物 FPFs/ 涂层在食品保鲜方面的最新应用。GA 交联对生物聚合物薄膜的全面改善是显而易见的，对薄膜性能的影响取决于 GA 的浓度和反应状态。GA 与聚合物分子的交联增加了聚合物网络的内聚力，物理交联和化学共价交联是两种主要的交联方式。值得注意的是，由 GA 交联的生物聚合物 FPF/涂层在保鲜食品方面表现出了显著的功效。

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引用次数: 0

Intrinsic self-healing Polyurethanes: Advances, Applications, and future prospects 内在自愈合聚氨酯：进展、应用和未来展望

IF 5.8 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2024-11-06 DOI: 10.1016/j.eurpolymj.2024.113566

Roham Ghanbari , Azam Serajian , Shahla Ataei , Ehsan Nazarzadeh Zare

Polyurethane (PU), a versatile and widely used polymer, has garnered significant research attention due to its intrinsic properties such as extended lifetime and durability, with diverse applications, ranging from clothing to industrial components. Self-healing mechanisms in PU primarily rely on intrinsic and extrinsic driving forces, in which the intrinsic process got sough after because of its reversible features. The intrinsic mechanism can be categorized into reversible covalent bonds (e.g., Diels-Alder reactions and disulfide bonds,) and dynamic non-covalent interactions (e.g., hydrogen bonds and ionic bonds). These mechanisms enable the spontaneous reconfiguration and healing of the polymer structure. Furthermore, the integration of new functional groups into PU structures introduces additional properties such as shape memory, degradability, and biocompatibility, broadening the scope of applications, particularly in flexible sensors and biomedical engineering. This paper delves into the self-healing mechanisms of PU, its functional integration, and potential applications in emerging fields such as coatings, adhesives, photo-thermal conversion, and biomedical devices, highlighting the challenges and future prospects in the development of self-healing PUs. Through a synthesis of recent studies, this article also discusses the balance between self-healing capabilities and mechanical properties, proposing new research directions for enhancing the efficacy and utility of self-healing PUs.

聚氨酯（PU）是一种用途广泛的聚合物，因其固有的特性（如延长使用寿命和耐用性）而备受研究关注，其应用范围从服装到工业部件不一而足。聚氨酯的自愈合机制主要依赖于内在和外在驱动力，其中内在过程因其可逆性而受到追捧。内在机制可分为可逆共价键（如 Diels-Alder 反应和二硫键）和动态非共价相互作用（如氢键和离子键）。这些机制使聚合物结构能够自发地重新配置和修复。此外，将新的功能基团整合到聚氨酯结构中还能带来额外的特性，如形状记忆、可降解性和生物相容性，从而拓宽了应用范围，尤其是在柔性传感器和生物医学工程方面。本文深入探讨了聚氨酯的自愈合机理、功能集成以及在涂料、粘合剂、光热转换和生物医学设备等新兴领域的潜在应用，重点介绍了自愈合聚氨酯的发展挑战和未来前景。本文还通过对最新研究的综述，探讨了自愈合能力与机械性能之间的平衡问题，为提高自愈合聚氨酯的功效和实用性提出了新的研究方向。

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引用次数: 0

Disparity between rate and selectivity in the controlled synthesis of gradient conjugated copolymers 梯度共轭共聚物受控合成中速率与选择性之间的差异

IF 5.8 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2024-11-06 DOI: 10.1016/j.eurpolymj.2024.113562

Annelien Van Oosten , Florian Matz , Valentina Parravicini , Thomas Christian Jagau , Guy Koeckelberghs

In this report, a one-pot synthesis of gradient copolymers is attempted employing Kumada catalyst transfer condensative polymerization (KCTCP). The hypothesis that a more reactive monomer is preferentially being built into the chain at the beginning, while the slower reacting monomer is only being built into the chain at the end due to it being in excess, is investigated. The monomer rate constants are influenced by the usage of differently sized sidechains (octyl versus 3-octyldodecyl) and nucleophilicity of the monomers (thiophene versus selenophene). Nonetheless, while the rate constants differ by a factor 2, no selectivity is obtained. The cause thereof is further investigated by increasing the sterical crowdedness around the catalyst-complex by employing a 4-substituted monomer, the polymerization of which also gave rise to random copolymers. Accompanied by density functional theory calculations of the geometry and Gibbs free energy, it is concluded that the distance between the nickel catalyst and the polymer chain is much smaller compared to the distance between the catalyst and the incoming monomer. This results in different polymerization rates (depending on the polymer-nickel complex), while having no selectivity for one incoming monomer over the other.

本报告尝试采用 Kumada 催化剂转移冷凝聚合法 (KCTCP) 单锅合成梯度共聚物。我们研究了这样一种假设，即反应性较强的单体在开始时优先被加入链中，而反应性较弱的单体由于过量而只在末端被加入链中。单体速率常数受到不同大小侧链（辛基与 3-辛基十二烷基）的使用和单体亲核性（噻吩与硒吩）的影响。然而，虽然速率常数相差 2 倍，但却没有获得选择性。通过使用 4 取代单体增加催化剂复合物周围的立体拥挤度，进一步研究了其原因。通过对几何形状和吉布斯自由能的密度泛函理论计算得出结论，镍催化剂与聚合物链之间的距离比催化剂与进入的单体之间的距离要小得多。这导致了不同的聚合速率（取决于聚合物-镍复合物），同时对一种进入的单体没有选择性。

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引用次数: 0

pH and light-triggered shape transformation of block copolymer particles in emulsion droplets 乳液液滴中嵌段共聚物颗粒在 pH 值和光线触发下的形状变化

IF 5.8 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2024-11-05 DOI: 10.1016/j.eurpolymj.2024.113561

Dan Ji, Yaping Wang, Mengqing Luo, Zihao Zhang, Xiaohua Chang, Yutian Zhu

Dual-responsive shape-transformable block copolymer (BCP) particles have arisen great attentions because of their tunable physical and chemical characteristics triggered by external stimuli. Herein, we developed a simple yet effective strategy to realize pH and light dual-triggered shape-switchable BCP particles through the co-assembly of BCPs with photo-responsive additive 4-hydroxyazobenzene (Azo-OH) within the evaporation emulsion droplets. The formation of hydrogen bonding interactions between the Azo-OH and 4-vinylpyridine (4VP) unit increases the volume fraction of P4VP domain, in turn leading to a morphological transition of the particles from onions to pupas by tuning the Azo-OH content. Subsequent light-induced trans–cis transition of the Azo unit induces the enhancement of the hydrophilicity of the P4VP domains, giving rise to internal shape transitions of the BCP particles from pupas to onions with P4VP at the outmost-layer. Furtherly, since the hydrogen bonds between Azo-OH and 4VP group are sensitive to pH, the interfacial properties of the emulsion droplets and the assembled structures are tuned through adjusting the environment pH of the aqueous solution, causing the formation of various particle shape, including pupas, raspberries, and onions. This work offers a promising method to engineer the microstructures of polymeric assemblies, which may attract more attention on the applications of the stimuli-responsive particles.

双响应形状可变嵌段共聚物（BCP）颗粒因其在外部刺激下可调的物理和化学特性而备受关注。在此，我们开发了一种简单而有效的策略，通过在蒸发乳液液滴中共同组装含有光响应添加剂 4-羟基偶氮苯（Azo-OH）的嵌段共聚物，实现 pH 和光双重触发的形状可变嵌段共聚物颗粒。偶氮-OH 与 4-乙烯基吡啶（4VP）单元之间形成的氢键相互作用增加了 P4VP 结构域的体积分数，进而通过调节偶氮-OH 的含量实现了颗粒从洋葱到蛹的形态转变。随后，光诱导的偶氮单元反式-顺式转变会增强 P4VP 结构域的亲水性，从而导致 BCP 粒子的内部形状从蛹转变为洋葱，P4VP 位于最外层。此外，由于 Azo-OH 和 4VP 基团之间的氢键对 pH 值很敏感，因此可通过调节水溶液环境的 pH 值来调整乳液液滴和组装结构的界面特性，从而形成不同的颗粒形状，包括蛹、树莓和洋葱。这项工作提供了一种很有前景的方法来设计聚合物组装体的微结构，可能会引起人们对刺激响应粒子应用的更多关注。

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