European Polymer Journal最新文献_第4页

Photoresponsive and UCST-Type thermoresponsive block Copolymer-Based composite micelles for Dual-Stimuli-Triggered selective and programmable release 用于双刺激触发选择性和可编程释放的光响应和ucst型热响应嵌段共聚物复合胶束

IF 6.3 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2025-12-24 DOI: 10.1016/j.eurpolymj.2025.114472

Ruizhen Zhang , Chengwen Jin , Pengjie Xie , Tao Chen

The coordinated release of multiple substances presents a significant technical challenge, primarily due to their distinct release kinetics and potential intermolecular interactions. To address this, we developed a composite nanoreactor and strategically selected two hydrophobic fluorescent dyes, Coumarin 102 and Nile Red, as model payloads. Firstly, a photoresponsive block copolymer, P(DMA₅₀-b-SPMA₆₀) (P1), containing carbamate spiropyran methacrylate units, and a thermoresponsive block copolymer with an Upper Critical Solution Temperature (UCST), P(DMA₅₀-b-SBMA₄₈) (P2), were synthesized via reversible addition-fragmentation chain transfer (RAFT) polymerization. These copolymers self-assembled into micelles, which encapsulated Coumarin 102 and Nile Red within the hydrophobic cores of P1 and P2, respectively. The individual stimulus-responsive release profiles were monitored via fluorescence spectroscopy. Composite nanoreactors were then prepared by physical blending the two loaded micelle types. The stability of the composite system was verified by fluorescence spectroscopy, transmission electron microscopy (TEM), and differential scanning calorimetry (DSC). Upon exposure to specific stimuli (light or temperature), selective release of the respective hydrophobic molecules was achieved: UV irradiation triggered a 80% release of Coumarin 102 from M3 micelles, while heating above the UCST induced a 75% release of Nile Red from M4 micelles. The composite micelles thus integrate multiple orthogonal stimulation responses with precise selective release control, offering a promising platform for advanced controlled-release applications in nanotechnology and biotechnology.

多种物质的协同释放是一项重大的技术挑战，主要是由于它们不同的释放动力学和潜在的分子间相互作用。为了解决这个问题，我们开发了一个复合纳米反应器，并策略性地选择了两种疏水荧光染料香豆素102和尼罗河红作为模型有效载荷。首先，采用可逆加成-破碎链转移（RAFT）聚合法制备了氨基甲酸酯-螺吡喃-甲基丙烯酸酯单元的光响应嵌段共聚物P(DMA50-b-SPMA60) （P1）和具有较高临界溶液温度（UCST）的热响应嵌段共聚物P(DMA50-b-SBMA48) （P2）。这些共聚物自组装成胶束，分别包裹香豆素102和尼罗红在P1和P2的疏水核心内。通过荧光光谱法监测个体刺激响应释放谱。然后通过物理共混制备了两种负载胶束类型的复合纳米反应器。通过荧光光谱、透射电子显微镜（TEM）和差示扫描量热法（DSC）验证了复合体系的稳定性。在暴露于特定刺激（光或温度）下，实现了各自疏水分子的选择性释放：紫外线照射触发M3胶束释放80%的香豆素102，而高于UCST的加热诱导M4胶束释放75%的尼罗红。因此，复合胶束将多种正交刺激反应与精确的选择性释放控制相结合，为纳米技术和生物技术的先进控释应用提供了一个有前途的平台。

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引用次数: 0

Orthogonal imine and disulfide exchange in a biobased covalent adaptable network: toward healable and recyclable thermosets 正交亚胺和二硫交换在一个生物基共价适应性网络：朝着可治疗和可回收的热固性

IF 6.3 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2025-12-24 DOI: 10.1016/j.eurpolymj.2025.114473

Yulu Wang , Fengxiang Cao , Gang Liu , Zhen Fang , Zhuhui Qiao

The development of biobased thermosetting materials has garnered considerable interest as a promising alternative to conventional thermosets, which are often constrained by permanent cross-linking and dependence on petroleum-derived feedstocks. Nevertheless, both traditional and bio-based thermosets frequently exhibit limitations in reprocessability and recyclability. In this study, a novel epoxy covalent adaptable network (CAN) incorporating dynamic dual-crosslinking bonds (D-DCB) was synthesized from lignin-derived vanillin (VA) and glycerol propoxylate triglycidyl ether (GPTE). Specifically, a trialdehyde monomer (TAM) was first prepared from VA and GPTE, which subsequently reacted with disulfide-containing compounds (4,4′-diaminodiphenyl disulfide and cystamine) to form bio-based CANs (namely, TAM-APDS and TAM-Cys, respectively). This network synergistically combines imine and disulfide bonds as dynamic covalent units. The imine bonds not only provide fundamental mechanical strength and structural stability but also contribute UV-shielding properties due to their conjugated structure. The disulfide bonds impart reprocessability, self-healing capability, and degradability-enabling rapid disulfide exchange reactions within 1 h using a thiol/ethanol solution at 60 °C. Lap-shear adhesion tests on various substrates demonstrated that the resulting CANs exhibit a high strength of approximately 7 MPa on iron substrates, highlighting their potential as high-performance sustainable adhesives.

生物基热固性材料的发展已经获得了相当大的兴趣，作为传统热固性材料的一种有希望的替代品，传统热固性材料通常受到永久交联和依赖石油衍生原料的限制。然而，传统热固性和生物基热固性经常在再加工性和可回收性方面表现出局限性。本研究以木质素基香兰素（VA）和丙氧基甘油三酯醚（GPTE）为原料，合成了一种新型的含动态双交联键的环氧共价自适应网络（CAN）。具体而言，首先由VA和GPTE制备三醛单体（TAM），然后与含二硫化合物（4,4 ' -二氨基二苯二硫和半胺）反应形成生物基can（分别为TAM- apds和TAM- cys）。这个网络协同结合亚胺和二硫键作为动态共价单位。亚胺键不仅提供了基本的机械强度和结构稳定性，而且由于其共轭结构，还具有屏蔽紫外线的性能。二硫键具有可再加工性、自愈性和可降解性，在60°C的硫醇/乙醇溶液中，在1小时内实现快速的二硫交换反应。在不同的基材上进行的剪切粘合测试表明，所得到的can在铁基材上表现出约7兆帕的高强度，突出了它们作为高性能可持续粘合剂的潜力。

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引用次数: 0

3D printing, biocompatibility and long-lasting antibacterial hydrogel with recognizing stimuli for electromyographic signal 3D打印，具有生物相容性和长效抗菌水凝胶，可识别肌电信号刺激

IF 6.3 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2025-12-24 DOI: 10.1016/j.eurpolymj.2025.114461

Ruijia Wang , Xijia Fu , Yibo Sun , Zhuang Li

Hydrogel sensors as an emerging representative of flexible electronic devices, have demonstrated significant application potential in fields such as biomedicine, wearable devices, and smart healthcare. However, the existing hydrogel sensors have the problem of bacterial growth while maintaining high sensitivity. This not only may pose an infection risk, but also significantly shortens the lifespan of the devices. Herein, a conductive antibacterial hydrogel sensor based on a polyvinyl alcohol-carboxymethyl cellulose (CMC) double-network structure was prepared by the freeze–thaw method. By introducing Polyhexamethylene biguanide hydrochloride (PHMB), the hydrogel is endowed with antibacterial properties and long-term stability against both gram-positive and gram-negative bacteria. Hydrogels possess remarkable toughness and elasticity, enabling the construction and printing of complex three-dimensional structures. The hydrogel sensor can accurately capture human movement signals such as finger bending as well as vocalization, and sensitively detect weak electromyographic signals. The hydrogel sensors with antibacterial properties, anti-fatigue performance and rapid response capabilities provide important theoretical support for the research and development of new generation intelligent medical devices and their applications in health monitoring.

水凝胶传感器作为柔性电子器件的新兴代表，在生物医药、可穿戴设备、智能医疗等领域显示出巨大的应用潜力。然而，现有的水凝胶传感器在保持高灵敏度的同时存在细菌生长的问题。这不仅可能造成感染风险，而且还会大大缩短设备的使用寿命。采用冻融法制备了一种基于聚乙烯醇-羧甲基纤维素（CMC）双网络结构的导电抗菌水凝胶传感器。通过引入聚六亚甲基双胍盐酸盐（PHMB），该水凝胶对革兰氏阳性菌和革兰氏阴性菌均具有抗菌性能和长期稳定性。水凝胶具有显著的韧性和弹性，可以构建和打印复杂的三维结构。水凝胶传感器可以准确捕捉人体运动信号，如手指弯曲和发声，并灵敏地检测微弱的肌电信号。具有抗菌性能、抗疲劳性能和快速响应能力的水凝胶传感器为新一代智能医疗器械的研发及其在健康监测中的应用提供了重要的理论支持。

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引用次数: 0

Shape memory polymers: From materials to emerging biomedical applications 形状记忆聚合物：从材料到新兴的生物医学应用

IF 6.3 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2025-12-23 DOI: 10.1016/j.eurpolymj.2025.114460

Nusrat Hassan Khan , Mohamed Sultan Mohamed Ali , Mohammed Nazibul Hasan

Shape Memory Polymers (SMPs) have emerged as adaptable and promising biomaterials in biomedical engineering, enabling innovative solutions for minimally invasive procedures and personalized therapies. This review presents a comprehensive overview of SMPs, focusing on their unique shape memory effects, tuneable material properties, and emerging biomedical applications. Unlike previous reviews that primarily focused on performance enhancement through conductive fillers or crosslinking strategies, this work highlights both the tailored modification of SMP characteristics and their functional integration within biomedical contexts. Key SMP types, such as poly(lactic acid), polycaprolactone, polyurethane, poly(methyl methacrylate) and bile acid-based polymers are critically evaluated with respect to their biocompatibility, biodegradability, and responsiveness to external stimuli. Moreover, biomedical applications such as controlled drug delivery, vascular stenting, dental devices, and tissue engineering are also discussed, with particular attention to recent advances and persisting challenges. Furthermore, the review identifies essential considerations for SMP selection, including mechanical robustness, physiological compatibility, and regulatory requirements. By synthesizing current developments and outlining emerging research directions, this article provides a framework to guide both researchers and clinicians in leveraging the full potential of SMPs for next-generation biomedical devices and therapeutic platforms.

形状记忆聚合物（SMPs）已成为生物医学工程中适应性强、前景广阔的生物材料，为微创手术和个性化治疗提供了创新的解决方案。这篇综述介绍了SMPs的全面概述，重点是其独特的形状记忆效应，可调谐的材料特性，以及新兴的生物医学应用。与之前主要关注通过导电填料或交联策略提高性能的综述不同，这项工作强调了SMP特征的定制修改及其在生物医学背景下的功能整合。关键的SMP类型，如聚乳酸、聚己内酯、聚氨酯、聚甲基丙烯酸甲酯和胆汁酸基聚合物的生物相容性、生物可降解性和对外部刺激的反应性进行了严格评估。此外，生物医学应用，如控制药物输送，血管支架植入，牙科设备和组织工程也进行了讨论，特别关注最近的进展和持续的挑战。此外，该综述确定了SMP选择的基本考虑因素，包括机械稳健性、生理相容性和监管要求。通过综合当前的发展和概述新兴的研究方向，本文提供了一个框架，以指导研究人员和临床医生充分利用SMPs的下一代生物医学设备和治疗平台的潜力。

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引用次数: 0

Triethoxysilyl group containing amidophosphonates and amidophosphates and polysilsesquioxanes based on them: synthesis and non-conventional luminescent properties 含偕胺膦酸酯、偕胺膦酸酯和基于它们的聚硅氧烷的三乙氧基硅氧基：合成及其非常规发光性能

IF 6.3 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2025-12-23 DOI: 10.1016/j.eurpolymj.2025.114469

Ivan A. Strelkov , Tatiana P. Gerasimova , Sergey A. Katsyuba , Artemiy G. Shmelev , Elmira A. Vasilieva , Ayrat R. Khamatgalimov , Radis R. Gainullin , Kirill V. Kholin , Almaz A. Zagidullin

Unconventional luminescence caused by hindered intra- and intermolecular mobility of molecules is of great research interest in science and technology. However, the lack of data on the effect of the structure of such compounds on the process of aggregation-induced emission and the underdevelopment of existing synthetic approaches make these studies difficult. We have developed new non-classical luminophores based on amidophosphonate and amidophosphate containing polysilsesquioxanes obtained by a simple two-stage synthetic route: monomers were obtained by nucleophilic substitution reactions at the P(V) atom, and the corresponding polymers were obtained by hydrolytic polymerization. Luminescent properties of both monomers and polymers were described, and it was shown that luminescence by cluster aggregation is also characteristic of low-molecular luminophores.

由于分子在分子内和分子间的迁移受阻而引起的非常规发光是目前科学技术研究的热点。然而，由于缺乏这些化合物的结构对聚集诱导发射过程的影响的数据，以及现有合成方法的不发达，使得这些研究变得困难。我们开发了基于偕胺膦酸盐和含偕胺磷酸酯的聚硅氧烷的新型非经典发光基团，通过简单的两阶段合成路线：在P(V)原子上通过亲核取代反应得到单体，通过水解聚合得到相应的聚合物。描述了单体和聚合物的发光特性，表明簇聚集发光也是低分子发光团的特征。

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引用次数: 0

Facile synthesis and high-efficient separation of low-entanglement fraction from heterogeneous entangled ultrahigh molecular weight polyethylene for solvent-free fabrication of high-performance tapes 非均相缠结超高分子量聚乙烯低缠结率的快速合成和高效分离，用于无溶剂制备高性能胶带

IF 6.3 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2025-12-23 DOI: 10.1016/j.eurpolymj.2025.114452

Zhi Li , Jincheng Xia , Yilun Hu , Wenjing Zhao , Wei Hong , Weizhong Yuan

Solvent-free solid-state fabrication of ultrahigh molecular weight polyethylene (UHMWPE) products with high strength and modulus properties such as fibers or films has emerged as a significant research area. Commonly, solvent-free preparation of high-performance UHMWPE films relies on low entanglement UHMWPE resins. To date, low-entanglement UHMWPE (LE-UHMWPE) could only be synthesized through single-site catalysts or specially modified Ziegler-Natta catalysts; however, these approaches remain limited in commercial viability due to elevated production costs associated with their low catalytic activity. In this study, LE-UHMWPE resin was successfully prepared using a conventional Ziegler-Natta catalyst combined with a post-polymerization extraction process. The LE-UHMWPE resin, serving as the core component of the original UHMWPE (O-UHMWPE) resin, was successfully isolated through a process analogous to peeling an egg. The normalized molecular chain entanglement density of the resin was reduced from 74.2% prior to treatment to 40.7% after the extraction procedure. Experimental results demonstrated that LE-UHMWPE extracted under a 10% solid content exhibited higher crystallinity (74.7%) compared to O-UHMWPE (66.8%). Compared to O-UHMWPE resin, LE-UHMWPE resin demonstrated the ability to undergo solid-state processing at temperatures below its melting point. Through solid-state stretching molding conducted below the melting temperature, the processed LE-UHMWPE tapes achieved a crystallinity of 91.5%, along with tensile strength and modulus values of 1.3 GPa and 68.0 GPa, respectively. These findings indicate that the combination of conventional high-activity Ziegler-Natta slurry polymerization with a straightforward post-treatment methodology enables efficient production of low-entanglement UHMWPE resin. The continuous integration of Ziegler-Natta catalytic polymerization with extraction treatment for UHMWPE could offer a cost-effective approach to the large-scale production of high-performance UHMWPE. Furthermore, this study contributes to challenging the long-held belief that conventional Ziegler-Natta catalysts are unsuitable for the synthesis of LE-UHMWPE.

无溶剂固态制造具有高强度和模量性能的超高分子量聚乙烯（UHMWPE）产品，如纤维或薄膜，已成为一个重要的研究领域。通常，高性能超高分子量聚乙烯薄膜的无溶剂制备依赖于低缠结超高分子量聚乙烯树脂。迄今为止，低纠缠度超高分子量聚乙烯（LE-UHMWPE）只能通过单位点催化剂或特殊改性的Ziegler-Natta催化剂合成；然而，这些方法的商业可行性仍然有限，因为它们的催化活性低，生产成本高。在本研究中，采用传统的Ziegler-Natta催化剂结合聚合后萃取工艺成功制备了LE-UHMWPE树脂。LE-UHMWPE树脂作为原始UHMWPE （O-UHMWPE）树脂的核心成分，通过类似于剥鸡蛋的过程成功分离。树脂的归一化分子链纠缠密度由处理前的74.2%降至提取后的40.7%。实验结果表明，固含量为10%时，LE-UHMWPE的结晶度为74.7%，高于O-UHMWPE的66.8%。与O-UHMWPE树脂相比，LE-UHMWPE树脂能够在低于其熔点的温度下进行固态加工。在熔融温度以下进行固态拉伸成型，制备的LE-UHMWPE带结晶度达到91.5%，抗拉强度和模量分别达到1.3 GPa和68.0 GPa。这些发现表明，将传统的高活性Ziegler-Natta浆料聚合与简单的后处理方法相结合，可以高效地生产低缠结的超高分子量聚乙烯树脂。将Ziegler-Natta催化聚合与萃取处理相结合，为大规模生产高性能超高分子量聚乙烯提供了一条经济有效的途径。此外，该研究有助于挑战长期以来认为传统的齐格勒-纳塔催化剂不适合合成LE-UHMWPE的观点。

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引用次数: 0

Advanced polymer-based thermal interface materials: A review on matrix optimization and filler engineering for superior performance 先进聚合物基热界面材料：性能优越的基体优化和填料工程研究进展

IF 6.3 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2025-12-22 DOI: 10.1016/j.eurpolymj.2025.114468

Miao Yin , Munan Qiu , Youmeng Yuan , Chuxuan Zhu , Wenqi Zou , Biao Yang

The rapid advancement of 5G communication, artificial intelligence, and high-power electronics highlights the critical importance of efficient thermal management for reliable device operation. In this context, thermal interface materials (TIMs) perform the critical function of displacing microscopic air pockets at interfaces, thereby establishing an efficient pathway for heat dissipation. Polymer-based TIMs have attracted considerable interest owing to the excellent interfacial conformity, electrical insulation, and ease of processing. However, their development is constrained by a fundamental conflict between the intrinsically low thermal conductivity of polymers and the requirement for low modulus, which is often compromised by the high filler loadings to enhance heat transport ability. This review systematically surveys recent advances aimed at resolving this challenge. We first introduce the heat transfer mechanism and simulation method of polymer-based TIMs, followed by a summary of the classification according to physical state. The core discussion is then articulated through two pivotal, complementary approaches: polymer matrix optimization and filler engineering. Matrix optimization focuses on improving thermal conductivity and tailoring mechanical properties via molecular design, while also covering innovative processing techniques and sustainable material development. In parallel, filler engineering is explored through surface modification, hybrid systems, and the construction of two-dimensional oriented fillers and three-dimensional filler networks to establish efficient thermal pathways. Finally, key challenges and future research opportunities for the development of advanced polymer-based TIMs are highlighted. It is anticipated that this review can provide guidance for the design of high-performance polymer-based TIMs suitable for a wide range of applications in high-density integration and flexible electronics.

5G通信、人工智能和大功率电子设备的快速发展凸显了高效热管理对设备可靠运行的至关重要性。在这种情况下，热界面材料（TIMs）发挥了取代界面上微观气穴的关键作用，从而建立了有效的散热途径。聚合物基TIMs由于其优异的界面一致性、电绝缘性和易于加工而引起了相当大的兴趣。然而，它们的发展受到聚合物固有的低导热性和低模量要求之间的根本冲突的制约，而低模量要求往往被高填料负载以增强热传递能力所损害。本综述系统地调查了旨在解决这一挑战的最新进展。本文首先介绍了聚合物基TIMs的传热机理和模拟方法，然后总结了基于物理状态的TIMs分类。然后通过两个关键的，互补的方法来阐述核心讨论：聚合物基质优化和填料工程。矩阵优化的重点是通过分子设计来提高导热性和定制机械性能，同时也涵盖了创新的加工技术和可持续的材料开发。同时，填料工程通过表面改性、混合系统、二维定向填料和三维填料网络的构建来探索，以建立有效的热路径。最后，强调了先进聚合物基TIMs发展的关键挑战和未来的研究机会。期望本文的研究成果能够为高密度集成和柔性电子领域的高性能聚合物基TIMs的设计提供指导。

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引用次数: 0

Smart pH-responsive hydrogels: A versatile tool for addressing public health challenges in diagnostic and therapeutic applications 智能ph响应水凝胶：在诊断和治疗应用中解决公共卫生挑战的多功能工具

IF 6.3 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2025-12-21 DOI: 10.1016/j.eurpolymj.2025.114466

Jige Yuan , Yi Wang , Xiaoxia Kang , Conglin Guo , Haiwei ji , Li Wu , Yuling Qin

Hydrogels have garnered substantial attention in biomedical and public health applications due to their high water content, tunable physicochemical properties, excellent biocompatibility, and capacity for functional modification. Among them, pH-responsive hydrogels represent a notably promising category of “smart” materials, which can undergo significant physical or chemical changes in response to slight variations in environmental pH. This inherent responsiveness allows for their application in real-time monitoring and targeted therapy, thereby addressing the key limitations of conventional diagnostic and therapeutic approaches, including poor sensitivity, lack of real-time feedback, non-specific drug release, and systemic side effects. In the field of public health, alterations in pH often serve as critical indicators of pathological states, such as wound infection, food spoilage, and the acidic tumor microenvironment. While traditional methods for pH detection or pH-triggered drug delivery face challenges in terms of portability, continuous monitoring, selectivity, and adaptability to dynamic physiological conditions, pH-responsive hydrogels offer a versatile platform that can be engineered for specific public health scenarios. However, their broader application is constrained by several challenges, including the need for precise response range tuning, stability under physiological conditions, long-term biocompatibility, and scalable fabrication. This review systematically summarizes recent advances in the design and application of pH-responsive hydrogels in public health, with a focus on diagnostic tools (e.g., wound pH monitoring, food freshness detection, disease biomarker sensing) and therapeutic strategies (e.g., antimicrobial wound dressings, tumor-targeted drug delivery, tissue engineering). Unlike prior reviews that often emphasize material synthesis or single applications, this work uniquely integrates public health perspectives, highlighting how hydrogel design can be tailored to address real-world detection and treatment challenges. We further discuss current limitations and future directions, aiming to provide insightful guidance for the rational development of pH-responsive hydrogels that can be effectively translated into public health practice.

水凝胶由于其高含水量、可调节的物理化学性质、优异的生物相容性和功能修饰能力，在生物医学和公共卫生应用中获得了大量关注。其中，ph响应水凝胶代表了一个非常有前途的“智能”材料类别，它可以对环境ph的轻微变化做出显著的物理或化学变化。这种固有的响应性允许它们在实时监测和靶向治疗中应用，从而解决了传统诊断和治疗方法的关键局限性，包括灵敏度差、缺乏实时反馈、非特异性药物释放、还有全身的副作用。在公共卫生领域，pH值的改变通常是病理状态的关键指标，如伤口感染、食物腐败和酸性肿瘤微环境。虽然传统的pH检测或pH触发药物递送方法在便携性、连续监测、选择性和对动态生理条件的适应性方面面临挑战，但pH响应水凝胶提供了一个多功能平台，可以针对特定的公共卫生场景进行设计。然而，它们的广泛应用受到几个挑战的限制，包括需要精确的响应范围调谐，生理条件下的稳定性，长期生物相容性和可扩展的制造。本文系统总结了pH响应水凝胶在公共卫生领域的设计和应用的最新进展，重点介绍了诊断工具（如伤口pH监测、食品新鲜度检测、疾病生物标志物传感）和治疗策略（如抗菌伤口敷料、肿瘤靶向药物输送、组织工程）。与以往强调材料合成或单一应用的综述不同，这项工作独特地整合了公共卫生观点，强调了如何定制水凝胶设计来解决现实世界的检测和治疗挑战。我们进一步讨论了目前的局限性和未来的发展方向，旨在为ph响应水凝胶的合理开发提供有洞察力的指导，从而有效地转化为公共卫生实践。

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引用次数: 0

Synthesis and vat-photopolymerization of hydrogen bonding-rich eugenol-based benzoxazine resins for 4D printing of shape memory polymers 形状记忆聚合物4D打印用富氢键丁香酚基苯并恶嗪树脂的合成及光聚合

IF 6.3 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2025-12-20 DOI: 10.1016/j.eurpolymj.2025.114465

Nuttinan Boonnao , Minwook Jeon , Krittapas Charoensuk , Ibrahim Lawan , Cheol-Hee Ahn , Sarawut Rimdusit

This work presents a novel strategy for developing a UV-curable bio-based eugenol-derived benzoxazine resin for 4D printing of shape-memory polymers (SMPs) via vat photopolymerization (VPP). The methacrylate group of 2-isocyanatoethyl methacrylate (IEM) was grafted onto the benzoxazine monomer through an isocyanate–hydroxyl reaction, introducing urethane linkages and a methacrylate functional group that enhances hydrogen bonding, improves chain segmental mobility, and imparts UV-reactive functionality. The resulting photoreactive resin exhibits moderate viscosity (25.0 Pa·s at 25 °C and at a shear rate of 30 s⁻¹) and high UV reactivity. After dual UV/thermal curing, the polymer shows high stiffness (storage modulus 2.2 GPa), thermal stability (T_d5 = 256 °C), and excellent shape memory performance, with shape fixity and shape recovery ratios ∼ 99 % over 30 cycles. In comparison with conventional benzoxazine-based SMPs, the developed 4D printing SMPs polymer also supports larger temporary shape deformation. Structure–property analyses using solubility testing and DMA indicate a relatively low crosslink density (gel content 56.6 %), suggesting that the thermo-mechanical and shape memory performance primarily arises from the dense hydrogen bonding network within the dual-cured polymer. This study establishes a molecular-design strategy for hydrogen-bonding-rich UV-curable benzoxazine systems and demonstrates the critical role of hydrogen bonding in governing the thermo-mechanical and shape memory properties. The 4D-printed structures produced in this work exhibit large deformation capability and excellent shape memory stability, highlighting their potential for durable and flexible high-performance 4D printing applications.

本研究提出了一种新型的紫外光固化生物基丁香酚衍生苯并恶嗪树脂，用于通过还原光聚合（VPP）进行形状记忆聚合物（SMPs）的4D打印。2-异氰基甲基丙烯酸乙酯（IEM）的甲基丙烯酸基团通过异氰酸-羟基反应接枝到苯并恶嗪单体上，引入氨基甲酸乙酯键和甲基丙烯酸官能团，增强氢键，提高链段迁移率，并赋予紫外线反应官能团。所得光反应树脂具有中等粘度（25°C时为25.0 Pa·s，剪切速率为30 s−1）和高紫外反应性。在双UV/热固化后，聚合物表现出高刚度（存储模量2.2 GPa）、热稳定性（Td5 = 256°C）和优异的形状记忆性能，在30次循环中具有形状固定性和形状恢复率~ 99%。与传统的苯并恶嗪基SMPs相比，所开发的4D打印SMPs聚合物还支持更大的临时形状变形。使用溶解度测试和DMA进行的结构性能分析表明，交联密度相对较低（凝胶含量56.6%），表明热机械和形状记忆性能主要来自双固化聚合物内部致密的氢键网络。本研究建立了一种富氢键的紫外光固化苯并恶嗪体系的分子设计策略，并证明了氢键在控制热力学和形状记忆性能中的关键作用。在这项工作中生产的4D打印结构表现出大的变形能力和优异的形状记忆稳定性，突出了它们在耐用和灵活的高性能4D打印应用中的潜力。

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引用次数: 0

Self-assembling nanoscale platforms for curcumin delivery using cerebroprotein hydrolysate/crown ether/quaternary ammonium salts/phospholipid: pH-responsive release, in vivo targeting real-time monitoring and visualization analysis 脑蛋白水解物/冠醚/季铵盐/磷脂自组装纳米级姜黄素递送平台：ph响应释放，体内靶向实时监测和可视化分析

IF 6.3 2区化学 Q1 POLYMER SCIENCE

European Polymer Journal

Pub Date : 2025-12-20 DOI: 10.1016/j.eurpolymj.2025.114457

Pei Su , Tiantian Chai , Zhenning Wang , Mengtong Zhang , Chichong Lu , Guofan Jin

The aim of this study is to provide a way to create new drug delivery strategies for the poor bioavailability and stability of curcumin. Distearyl phosphatidylcholine (DSPC) and cerebroprotein hydrolysate were employed to facilitate curcumin administration. Abundant experimental results demonstrate that the synthesized polymer exhibits favorable fluorescence properties. The polymer prepared in this research presents as spherical nanoparticles. Precise measurements reveal that its optimal particle size is 392.3 nm, and the surface is densely populated with negative charges. Such a surface charge distribution effectively promotes the release of drugs within the organism. Through in − depth in vitro release experiments and comprehensive mouse gastrointestinal tract studies, it has been clearly demonstrated that the polymer is in full compliance with the intestinal release and absorption characteristics essential for oral drugs. Through cell imaging techniques, it was observed that in the in vivo environment, the target substance presents a high level of exposure. The cytotoxicity test results showed that the prepared polymer had a remarkable inhibition effect on cancer cells, and the inhibition rate reached about 70 %. In-vivo and gastrointestinal imaging in mice showed that after oral administration, the synthesized polymer was released in the stomach, then enriched at the colon tumor site via the intestine and stayed in the tumor microenvironment for long. Therefore, this innovative design has important prospects in drug delivery mechanism research and cancer treatment.

本研究旨在为姜黄素生物利用度和稳定性较差的现状提供一种新的给药策略。采用二硬脂酰磷脂酰胆碱（DSPC）和脑蛋白水解物促进姜黄素给药。大量的实验结果表明，合成的聚合物具有良好的荧光性能。本研究制备的聚合物表现为球形纳米颗粒。精确测量表明，其最佳粒径为392.3 nm，表面密集分布着负电荷。这种表面电荷分布有效地促进了药物在机体内的释放。通过深入的体外释放实验和全面的小鼠胃肠道研究，已经清楚地证明该聚合物完全符合口服药物所必需的肠道释放和吸收特性。通过细胞成像技术观察到，在体内环境中，靶物质呈现出高水平的暴露。细胞毒性试验结果表明，所制备的聚合物对癌细胞具有显著的抑制作用，抑制率达到70%左右。小鼠体内和胃肠道成像显示，口服给药后，合成的聚合物在胃中释放，然后通过肠道在结肠肿瘤部位富集，并在肿瘤微环境中停留较长时间。因此，这种创新设计在药物传递机制研究和癌症治疗中具有重要的前景。

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