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Organic Donor–Acceptor–Donor Trimers Nanoparticles Stabilized by Amphiphilic Block Copolymers for Photocatalytic Generation of H2 由两性嵌段共聚物稳定的有机供体-受体-供体三聚体纳米粒子用于光催化产生 H2
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-09-23 DOI: 10.1002/marc.202470036
Thiago R. Guimarães, Alisha Khan, Hynd Remita, Jean-Louis Bobet, Eric Cloutet

Front Cover: A versatile platform is developed for creating functional π-conjugated organic nanoparticles stabilized by amphiphilic block copolymers for green H2 photocatalytic generation. The donor–acceptor–donor trimers nanoparticles show enhanced photocatalytic activity (≈0.6 mmol g−1 h−1) for H2 production via water splitting. More details can be found in article 2400395 by Thiago R. Guimarães, Jean-Louis Bobet, Eric Cloutet, and co-workers.

封面:开发了一种多功能平台,用于创建由两性嵌段共聚物稳定的功能性π-共轭有机纳米粒子,以进行绿色 H2 光催化发电。供体-受体-供体三聚体纳米粒子显示出更强的光催化活性(≈0.6 mmol g-1 h-1),可通过水分离产生 H2。更多详情,请参阅 Thiago R. Guimarães、Jean-Louis Bobet、Eric Cloutet 及合作者撰写的文章 2400395。
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引用次数: 0
Masthead: Macromol. Rapid Commun. 18/2024 刊头:Macromol.Rapid Commun.18/2024
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-09-23 DOI: 10.1002/marc.202470037
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引用次数: 0
Synthesis of Amino Acid-Based Aromatic Poly(Ester Urea)s Using 4-Hydroxycinnamic Acid-Derived Diols. 使用 4-羟基肉桂酸衍生的二元醇合成基于氨基酸的芳香族聚(酯脲)。
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-09-23 DOI: 10.1002/marc.202400507
Ghezae Tekleab, Harm-Anton Klok

Amino acid-based poly(ester urea)s are an attractive class of polymers that are of interest for a variety of biomedical applications. Generally, amino acid-based poly(ester urea)s are prepared by polymerization of diamines, which are obtained from the corresponding amino acids and aliphatic diols. This article presents an alternative synthetic strategy that uses diamine monomers obtained from aromatic, 4-hydroxycinnamic acid-derived diols. A library of structurally related diamine monomers has been prepared by coupling l-leucine to 4-hydroxycinnamic acid-based diols that incorporate alkyl spacers of different lengths. The exploration of 4-hydroxycinnamic acid as a building block is interesting as it can be obtained from various biological resources, such as for example lignin, and thus provides an opportunity to take advantage of (under-utilized) bio-based renewables for the design of new polymer materials. These diamine monomers can be copolymerized in a solvent-free, one-pot, two-step process using dimethyl carbonate as an environmentally sustainable reagent to afford amino acid-based aromatic poly(ester urea) homo- and copolymers with thermal properties that can be tuned by varying the chemical structure of the diamine monomer, or via copolymerization of two different monomers.

氨基酸基聚(酯脲)是一类极具吸引力的聚合物,可用于多种生物医学领域。一般来说,氨基酸基聚(酯脲)是通过二胺聚合制备的,而二胺是从相应的氨基酸和脂肪族二元醇中获得的。本文介绍了另一种合成策略,即使用从芳香族 4-羟基肉桂酸衍生的二元醇中获得的二胺单体。通过将 l-亮氨酸与含有不同长度烷基间隔物的 4-羟基肉桂酸基二醇偶联,制备出了一个结构相关的二胺单体库。将 4-羟基肉桂酸作为构筑基块的探索非常有趣,因为它可以从各种生物资源(如木质素)中获得,从而为利用(未充分利用的)生物基可再生资源设计新型聚合物材料提供了机会。使用碳酸二甲酯作为环境可持续试剂,这些二胺单体可在无溶剂、一步法、两步法工艺中进行共聚,从而制备出氨基酸基芳香族聚(酯脲)均聚物和共聚物,其热性能可通过改变二胺单体的化学结构或两种不同单体的共聚来调整。
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引用次数: 0
End-To-End FRET Enabling Direct Measurement of Oligomer Chain Conformations and Molecular Weight in Reaction Solutions. 端到端 FRET 可直接测量反应溶液中的低聚物链构型和分子量。
IF 4.2 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-09-23 DOI: 10.1002/marc.202400627
Sara Valdez, Syba Ismail, Yuming Wang, Zhe Qiang

Förster resonance energy transfer (FRET) is an established tool for measuring distances between two molecules (donor and acceptor) on the nanometer scale. In the field of polymer science, the use of FRET to measure polymer end-to-end distances (Ree) often requires complex synthetic steps to label the chain ends with the FRET pair. This work reports an anthracene-functionalized chain-transfer agent for reversible addition-fragmentation chain-transfer (RAFT) polymerization, enabling the synthesized chains to be directly end-labeled with a donor and acceptor without the need for any post-polymerization functionalization. Noteworthily, this FRET method allows for chain conformation measurements of low molecular weight oligomers in situ, without any work-up steps. Using FRET to directly measure the average Ree of the oligomer chains during polymerization, the chain growth of methyl methacrylate, styrene, and methyl acrylate is investigated as a function of reaction time, including determining their degree of polymerization (DP). It is found that DP results from FRET are consistent with other established measurement methods, such as nuclear magnetic resonance (NMR) spectroscopy. Altogether, this work presents a broadly applicable and straightforward method to in situ characterize Ree of low molecular weight oligomers and their DP during reaction.

佛斯特共振能量转移(FRET)是测量两个分子(供体和受体)之间纳米级距离的成熟工具。在聚合物科学领域,使用 FRET 测量聚合物端到端距离 (Ree) 通常需要复杂的合成步骤,以便用 FRET 对标记链端。这项研究报告了一种用于可逆加成-断裂链转移(RAFT)聚合的蒽功能化链转移剂,它能使合成的链直接用供体和受体进行末端标记,而无需任何聚合后功能化。值得注意的是,这种 FRET 方法可以原位测量低分子量低聚物的链构象,而无需任何加工步骤。利用 FRET 直接测量聚合过程中低聚物链的平均 Ree,研究了甲基丙烯酸甲酯、苯乙烯和丙烯酸甲酯的链增长与反应时间的函数关系,包括确定它们的聚合度(DP)。研究发现,通过 FRET 得出的聚合度结果与核磁共振 (NMR) 光谱等其他成熟的测量方法一致。总之,这项工作提出了一种广泛适用且简单直接的方法,可在反应过程中原位表征低分子量低聚物 Ree 及其聚合度。
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引用次数: 0
A Novel Curcumin-Loaded Nanoplatform Alleviates Osteoarthritis by Inhibiting Chondrocyte Ferroptosis 一种新型姜黄素载体纳米平台通过抑制软骨细胞铁凋亡缓解骨关节炎
IF 4.6 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-09-18 DOI: 10.1002/marc.202400495
Weibei Sheng, Aikang Li, Yaohang Yue, Qichang Wang, Fei Yu, Jian Weng, Jianjing Lin, Yingqi Chen, Hui Zeng, Deli Wang, Jun Yang, Peng Liu
Osteoarthritis (OA) is a chronic degenerative joint disease characterized by the degradation of articular cartilage. Recent studies have demonstrated that chondrocyte ferroptosis plays a crucial role in the progression of OA. Consequently, developing nanomedicines that suppress chondrocyte ferroptosis is a promising strategy for OA treatment. However, there are few reports on nanomedicines specifically targeting chondrocyte ferroptosis for OA therapy. In this study, Curcumin-loaded nanoparticles (Cur-NPs) are fabricated to suppress chondrocyte ferroptosis by regulating reactive oxygen species (ROS), ferrous ion (Fe2⁺), and Acyl-CoA Synthetase Long-Chain Family Member 4 (ACSL4) levels of chondrocyte. This is achieved by combining the functions of curcumin and an amphiphilic block copolymer with ROS scavenging and iron-chelating properties. The in vitro anti-ferroptotic effects of Cur-NPs are thoroughly investigated. The findings indicate that Cur-NPs decrease the expression of ferroptosis markers such as ROS, Fe2⁺, and ACSL4, while protecting the mitochondrial membrane potential of chondrocytes. Additionally, Cur-NPs attenuated lipid peroxidation in chondrocytes. Furthermore, Cur-NPs significantly reduced the expression of the catabolic factor Matrix Metallopeptidase 13 (MMP13) and increased the expression of the anabolic factor Collagen type II (Col II) in vitro. This study demonstrates that Cur-NPs exhibit enhanced chondroprotective effects through anti-ferroptotic actions, presenting a promising approach for inhibiting chondrocyte ferroptosis using bioactive nanomaterials in OA treatment.
骨关节炎(OA)是一种以关节软骨退化为特征的慢性退行性关节疾病。最近的研究表明,软骨细胞铁突变在 OA 的发展过程中起着至关重要的作用。因此,开发能抑制软骨细胞铁突变的纳米药物是治疗 OA 的一种前景广阔的策略。然而,有关专门针对软骨细胞铁突变的纳米药物用于治疗 OA 的报道却很少。本研究制作了姜黄素载体纳米粒子(Cur-NPs),通过调节软骨细胞的活性氧(ROS)、亚铁离子(Fe2⁺)和乙酰辅酶长链家族成员4(ACSL4)水平来抑制软骨细胞的铁突变。这是通过结合姜黄素和一种具有清除 ROS 和螯合铁特性的两性嵌段共聚物的功能实现的。研究人员对 Cur-NPs 的体外抗骨质疏松作用进行了深入研究。研究结果表明,Cur-NPs 在保护软骨细胞线粒体膜电位的同时,还能降低 ROS、Fe2⁺ 和 ACSL4 等铁变态反应标志物的表达。此外,Cur-NPs 还能减轻软骨细胞的脂质过氧化反应。此外,Cur-NPs 还能在体外明显减少分解因子基质金属肽酶 13(MMP13)的表达,并增加合成代谢因子 II 型胶原(Col II)的表达。这项研究表明,Cur-NPs 通过抗软骨凋亡作用增强了软骨保护效果,为利用生物活性纳米材料抑制软骨细胞软骨凋亡治疗 OA 提供了一种前景广阔的方法。
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引用次数: 0
Polymer Single-Chain Nanoparticles: Shaping Solid Surfactants 聚合物单链纳米颗粒:塑造固体表面活性剂
IF 4.6 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-09-18 DOI: 10.1002/marc.202400393
Shuailong Li, Shuyi Sun, Jiaqiu Luo, Zhiqin Xia, Yaxin Wang, Thomas P. Russell, Shaowei Shi, Zhenzhong Yang
Polymer single-chain nanoparticles (SCNPs) have found a wide range of applications spanning catalysts, sensors and nanomedicine. The generation of structured SCNPs from star-shaped polymers with diverse architectures and functionalities affords a new avenue to expand the emerging research area. The large-scale synthesis of structured SCNPs is described by the electrostatics-mediated intramolecular crosslinking of three types of 3-armed star-shaped polymers (T-P4VP, T-PS-b-P4VP, and T-P4VP-b-PS), whose configuration is tunable from spherical to cage-shaped to dumbbell-shaped and star-shaped. The structured SCNPs are amphiphilic and can be used as solid surfactants to stabilize different types of emulsions.
聚合物单链纳米粒子(SCNPs)在催化剂、传感器和纳米医学等领域有着广泛的应用。从具有不同结构和功能的星形聚合物中生成结构化 SCNPs 为拓展这一新兴研究领域提供了新途径。结构化 SCNPs 的大规模合成是通过静电介导的三种三臂星形聚合物(T-P4VP、T-PPS-b-P4VP 和 T-P4VP-b-PS)的分子内交联来实现的。这些结构化的 SCNPs 具有两亲性,可用作固体表面活性剂来稳定不同类型的乳液。
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引用次数: 0
Probing the Linear-to-Plastic Transition in Polymer Nanocomposites via Atomistic Simulations: The Role of Interphases 通过原子模拟探索聚合物纳米复合材料的线性到弹性转变:相间的作用
IF 4.6 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-09-18 DOI: 10.1002/marc.202400612
Hilal Reda, Panayiota Katsamba, Anthony Chazirakis, Vagelis Harmandaris
Polymer nanocomposites have found ubiquitous use across diverse industries, attributable to their distinctive properties and enhanced mechanical performance compared to conventional materials. Elucidating the elastic-to-plastic transition in polymer nanocomposites under diverse mechanical loads is paramount for the bespoke design of materials with desired mechanical attributes. In the current work, the elastic-to-plastic transition is probed in model systems of polyethylene oxide (PEO) and silica, SiO2, nanoparticles, through detailed atomistic molecular dynamics simulations. This comprehensive, multi-scale analysis unveils pivotal markers of the elastic-to-plastic transition, highlighting the quintessential role of microstructural and regional heterogeneities in density, strain, and stress fields, featuring the polymer-nanoparticle interphase region. At the atomic level, the behavior of polymer chains interacting with nanoparticle surfaces is traced, differentiating between free and adsorbed chains, and identifying the microscopic origins of the linear-to-plastic transition. The mechanical behavior of subregions are characterized within the PEO/SiO2 nanocomposites, focusing on the interphase and bulk-like polymer areas, probing stress heterogeneities and their decomposition into various force contributions. At the inception of plasticity, a disruption is discerned in isotropy of the polymeric density field, the emergence of low-density regions, and microscopic voids/cavities within the polymer matrix concomitant with a transition of adsorbed chains to free. The yield strain also emerges as an inflection point in the local versus global strain diagram, demarcating the elastic limit, and the plastic regime shows pronounced strain heterogeneities. The decomposition of the atomic Virial stress into bonded and non-bonded interactions indicates that the rigidity of the material is primarily governed by non-bonded interactions, significantly influenced by the volume fraction of the nanoparticle. These findings emphasize the importance of the microstructural and micromechanical environment at the polymer-nanoparticle interface on the linear-to-plastic transition, which is of great importance in the design of nanocomposite materials with advanced mechanical properties.
与传统材料相比,聚合物纳米复合材料具有独特的性能和更强的机械性能,因此在各行各业得到了广泛应用。阐明聚合物纳米复合材料在不同机械载荷下的弹塑性转变,对于定制设计具有所需机械属性的材料至关重要。在目前的研究工作中,通过详细的原子分子动力学模拟,在聚环氧乙烷(PEO)和二氧化硅(SiO2)纳米颗粒模型系统中探究了弹性到塑性的转变。这种全面、多尺度的分析揭示了弹性到塑性转变的关键标志,突出了微结构和密度、应变和应力场区域异质性的重要作用,其特点是聚合物-纳米粒子相间区域。在原子层面上,对聚合物链与纳米粒子表面相互作用的行为进行了追踪,区分了自由链和吸附链,并确定了线性到塑性转变的微观起源。对 PEO/SiO2 纳米复合材料内部各子区域的机械行为进行了表征,重点是相间和块状聚合物区域,探究应力异质性及其分解为各种力的贡献。在塑性开始时,聚合物密度场的各向同性被打破,出现了低密度区域,聚合物基体中出现了微观空洞,同时吸附链过渡到自由链。屈服应变也是局部应变与全局应变图中的一个拐点,是弹性极限的分界点,塑性体系显示出明显的应变异质性。将原子维里亚尔应力分解为成键和非成键相互作用表明,材料的刚性主要受非成键相互作用的支配,而纳米粒子的体积分数对其影响很大。这些发现强调了聚合物-纳米粒子界面的微结构和微机械环境对线性到塑性转变的重要性,这对设计具有先进机械性能的纳米复合材料具有重要意义。
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引用次数: 0
Preparation of Hierarchical Porous Monoliths With High Surface Areas by a Solvent Knitting Strategy 用溶剂编织法制备高表面积的分层多孔单晶体
IF 4.6 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-09-18 DOI: 10.1002/marc.202400494
Zicheng Zhong, Xiaojie Peng, Hui Gao, Irshad Hussain, Xiaoyan Wang, Bien Tan
Hierarchical porous hypercrosslinked monoliths (PolyHIPE-HCP) with ultrahigh specific surface areas are prepared via a solvent knitting strategy. Compared to previous work, the solvent knitting strategy is carried out in a relatively low air-controlled atmosphere with gradient heating starting from low temperature while using DCM (Dichloromethane) as both a solvent and a cross-linker, allowing for a slow and controlled cross-linking process, thereby achieving a BET surface area ranging from 514 to 728 m2 g−1. Scanning electron microscopy (SEM) shows that the knitting process does not affect the presence of macroporous structure in the PolyHIPE. With the introduction of mesopores and micropores, these hierarchical porous monoliths exhibit significant potential for applications in gas adsorption and water treatment. Hence, a universal, simple and low-cost method to synthesize polymeric monoliths with hierarchically porous structure and higher surface area is proposed, which has fascinating prospects in industrialization.
通过溶剂编织策略制备了具有超高比表面积的分层多孔超交联单片(PolyHIPE-HCP)。与之前的工作相比,溶剂编织策略是在相对较低的空气控制气氛中进行的,从低温开始梯度加热,同时使用 DCM(二氯甲烷)作为溶剂和交联剂,使交联过程缓慢而可控,从而实现了 514 至 728 m2 g-1 的 BET 表面积。扫描电子显微镜(SEM)显示,编织过程不会影响 PolyHIPE 中大孔结构的存在。随着中孔和微孔的引入,这些分层多孔单体在气体吸附和水处理方面展现出巨大的应用潜力。因此,我们提出了一种通用、简单、低成本的方法来合成具有分层多孔结构和更高比表面积的聚合物单片,该方法具有广阔的工业化前景。
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引用次数: 0
Organization of A2-Type Active Composite Nanorods A2 型活性复合纳米棒的组织结构
IF 4.6 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-09-18 DOI: 10.1002/marc.202400563
Fenglin Li, Yajing Yang, Zhendong Wen, Dayin Sun, Yilan Ye, Zhenzhong Yang
Nanorods as building blocks are promising to construct functional superstructures. A paramagnetic Fe3O4-based composite nanorod is large-scale synthesized from the poly(2-vinylpyridine) (P2VP) side chain grafted polymer bottlebrush by electrostatics-mediated intramolecular crosslinking via metallic coordination. Ultrasonication-assisted fracturing of the composite nanorod derives the corresponding A2-type composite nanorods whose two ends are active with the metallic coordinated P2VP exposed. The active ends are prone to connection upon feeding ligands (acidic or alkaline) or metallic ions to trigger the organization of the A2-type nanorods toward functional superstructures. Their microstructure is tunable from linear nanowires to branches, which is dependent on the valent state of the assistant chemicals. The report method is easily extended to derive a family of A2-type active nanorods with varied compositions and functions which are capable to organize functional nanomaterials with tunable microstructure.
以纳米棒为构件构建功能超结构大有可为。通过金属配位,在静电介导的分子内交联作用下,从聚(2-乙烯基吡啶)(P2VP)侧链接枝聚合物bottlebrush大规模合成了顺磁性Fe3O4基复合纳米棒。在超声波辅助下,复合纳米棒发生断裂,从而得到相应的 A2 型复合纳米棒,其两端是活性的,金属配位的 P2VP 暴露在外。活性末端在加入配体(酸性或碱性)或金属离子后容易发生连接,从而引发 A2 型纳米棒向功能超结构组织。它们的微观结构从线性纳米线到分支都是可调的,这取决于辅助化学物质的价态。报告中的方法很容易扩展到一系列具有不同成分和功能的 A2- 型活性纳米棒,它们能够组织具有可调微观结构的功能纳米材料。
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引用次数: 0
Stretchable and Elastic Triboelectric Nanogenerator with Liquid-Metal Grid–Patterned Single Electrode for Wearable Energy-Harvesting Devices 用于可穿戴能量收集设备的带有液态金属网格图案单电极的可伸缩弹性三电纳米发电机
IF 4.6 3区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-09-16 DOI: 10.1002/marc.202400321
Yuwen Wei, Priyanuj Bhuyan, Qingshi Zhang, Sihyun Kim, Yejin Bae, Mukesh Singh, Sungjune Park
Triboelectric nanogenerators (TENGs) have garnered significant attention as efficient energy-harvesting systems for sustainable energy sources in the field of self-powered wearable devices. Various conductive materials are used to build wearable devices, among which, gallium-based liquid metal (LM) is a preferred electrode owing to its fluidity and metallic conductivity even when strained. In this study, a stretchable, elastic, and wearable triboelectric nanogenerator is designed using a single electrode fabricated by embedding LM grid patterns into a stretchable silicone substrate through a two-step spray-coating process. Contrary to conventional double-electrode TENG that is challenging to integrate to human body, the LM grid-patterned single-electrode TENG (LMG-SETENG) has a simplified design and provides more flexibility. The LMG-SETENG can generate voltages of up to 100 V via triboelectrification upon contact with the human body, even under various degrees of strain, owing to the fluidity of the LM electrode. The generated energy can be utilized as a sustainable energy source to power various small appliances. Moreover, the proposed LMG-SETENG can be utilized in soft robotics, electronic skin, and healthcare devices.
作为自供电可穿戴设备领域可持续能源的高效能量收集系统,三电纳米发电机(TENGs)备受关注。各种导电材料被用于制造可穿戴设备,其中镓基液态金属(LM)因其流动性和金属导电性(即使在拉伸时)而成为首选电极。本研究设计了一种可拉伸、有弹性和可穿戴的三电纳米发电机,它采用单电极制造,通过两步喷涂工艺将 LM 网格图案嵌入可拉伸硅基板。传统的双电极 TENG 难以与人体集成,与之相反,LMG 网格图案单电极 TENG(LMG-SETENG)设计简化,灵活性更高。由于 LM 电极的流动性,LMG-SETENG 与人体接触后,即使在不同程度的应变下,也能通过三电化产生高达 100 V 的电压。产生的能量可作为可持续能源为各种小家电供电。此外,拟议的 LMG-SETENG 还可用于软机器人、电子皮肤和医疗保健设备。
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引用次数: 0
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Macromolecular Rapid Communications
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