Macromolecular Chemistry and Physics最新文献

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Luminescent Hybrid Material Based on the Europium(III)–β‐Diketone Complex Doped with Smectite 基于掺杂了 Smectite 的铕(III)-β-二酮配合物的发光混合材料

IF 2.5 4区化学 Q3 POLYMER SCIENCE

Macromolecular Chemistry and Physics

Pub Date : 2024-09-12 DOI: 10.1002/macp.202400208

Rong Cao, Ryota Nishiyama, Kazuki Nakamura, Norihisa Kobayashi

Lanthanide‐containing organic–inorganic hybrid materials exhibit considerable potential for applications in optical devices. In this study, efficient luminescent hybrid materials are prepared by employing a straightforward doping method to mix the Eu(tta)3phen complex (tta = 2‐thenoyltrifluoroacetone, phen = 1,10‐phenanthroline) with a synthetic clay compound of hectorite (smectite). The comprehensive photophysical properties of dispersion solution containing the Eu(tta)3phen/smectite hybrid material are systematically investigated via ultraviolet‐visible absorption spectroscopy, luminescence spectra, luminescence lifetimes, and Judd–Ofelt analysis. The emission properties of the Eu(tta)3phen are enhanced by its interaction with smectite. Furthermore, the interaction suppressed the molecular vibration of Eu(tta)3phen, resulting in elevated luminescence intensity and quantum efficiency. Moreover, a highly luminescent and transparent polymeric film is prepared by incorporating Eu(tta)3phen/smectite hybrid material into a polymer (PMMA) matrix. With the addition of the smectite compound, the transparency and surface smoothness of the polymeric film are improved. Consistent with the solution state, smectite enhanced the luminescence intensity of Eu(tta)3phen in the film state. This strategy presents a novel opportunity for high‐luminescence imaging devices.

含镧系元素的有机-无机杂化材料在光学设备中的应用潜力巨大。本研究采用简单的掺杂方法，将 Eu(tta)3phen 复合物（ta = 2-噻酰基三氟丙酮，phen = 1,10-菲罗啉）与合成的蛭石粘土化合物（smectite）混合，制备了高效的发光杂化材料。通过紫外-可见吸收光谱、发光光谱、发光寿命和 Judd-Ofelt 分析，系统地研究了含有 Eu(tta)3phen/smectite 混合材料的分散溶液的综合光物理特性。Eu(ta)3phen的发射特性因其与闪长岩的相互作用而增强。此外，相互作用抑制了 Eu(tta)3phen 的分子振动，从而提高了发光强度和量子效率。此外，通过在聚合物（聚甲基丙烯酸甲酯）基体中加入 Eu（ta）3phen/smectite 混合材料，制备出了一种高发光和透明的聚合物薄膜。添加了smectite化合物后，聚合物薄膜的透明度和表面光滑度都得到了改善。与溶液状态一致的是，在薄膜状态下，埃辉石增强了 Eu(tta)3phen 的发光强度。这一策略为高发光成像设备提供了新的机遇。

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引用次数: 0

Functionalized Polyisobutylene and Polyisobutylene‐Based Block Copolymers by Mechanistic Transformation from Cationic to Radical Process 通过从阳离子到自由基过程的机理转变获得功能化聚异丁烯和聚异丁烯基嵌段共聚物

IF 2.5 4区化学 Q3 POLYMER SCIENCE

Macromolecular Chemistry and Physics

Pub Date : 2024-09-10 DOI: 10.1002/macp.202400261

Yusra Bahar Cakir, Miraslau Makarevich, Mikalai Bohdan, Tugba Celiker, Maksim Hulnik, Irina V. Vasilenko, Baris Kiskan, Sergei V. Kostjuk

The strategy for the preparation of polyisobutylene‐based block copolymers via mechanistic transformation from cationic to radical polymerization is reported. This strategy involves the synthesis of 2‐bromo‐2‐methylpropanoyl‐terminated difunctional polyisobutylene macroinitiator (BiBB‐PIB‐BiBB) via consecutive cationic polymerization, in situ preparation of hydroxyl‐terminated polyisobutylene and its acylation by 2‐bromo‐2‐methylpropanoyl bromide. The Mn2(CO)10−triggered photo‐induced radical polymerization of styrene in bulk using this macroinitiator leads to the formation of multiblock copolymer, while predominantly triblock copolymer is generated during the polymerization of methyl methacrylate. The possibility to functionalize the polyisobutylene by pyrene via photo‐induced radical addition of 1‐bromomethyl pyrene in the presence of Mn2(CO)10 is also demonstrated in this work.

报告介绍了通过阳离子聚合到自由基聚合的机理转变制备聚异丁烯基嵌段共聚物的策略。该策略包括通过连续阳离子聚合合成 2-溴-2-甲基丙酰基封端的双官能团聚异丁烯大引发剂（BiBB-PIB-BiBB），原位制备羟基封端的聚异丁烯，并用 2-溴-2-甲基丙酰基溴对其进行酰化。使用这种大引发剂，Mn2(CO)10 引发的苯乙烯块体光引发自由基聚合可形成多嵌段共聚物，而在甲基丙烯酸甲酯聚合过程中则主要生成三嵌段共聚物。这项工作还证明了在 Mn2(CO)10 的存在下，通过光诱导自由基加成 1-溴甲基芘，用芘对聚异丁烯进行官能化的可能性。

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引用次数: 0

Masthead: Macromol. Chem. Phys. 17/2024 刊头：Macromol.Chem.17/2024

IF 2.5 4区化学 Q3 POLYMER SCIENCE

Macromolecular Chemistry and Physics

Pub Date : 2024-09-08 DOI: 10.1002/macp.202470035

引用次数: 0

Front Cover: Macromol. Chem. Phys. 17/2024 封面：Macromol.Chem.17/2024

IF 2.5 4区化学 Q3 POLYMER SCIENCE

Macromolecular Chemistry and Physics

Pub Date : 2024-09-08 DOI: 10.1002/macp.202470034

引用次数: 0

Solid‐State NMR Exploration of Factors for Enhancement of Hole Mobility by Introduction of Poly(styrene) Into Poly(3‐hexylthiophene) 固态核磁共振探究在聚(3-己基噻吩)中引入聚(苯乙烯)增强孔迁移率的因素

IF 2.5 4区化学 Q3 POLYMER SCIENCE

Macromolecular Chemistry and Physics

Pub Date : 2024-08-30 DOI: 10.1002/macp.202400225

Riku Takahashi, Eri Tomita, Shinpei Mukadeyama, Shinji Kanehashi, Kenji Ogino

Solid‐state cross‐polarization magic angle spinning (CPMAS) 13C NMR is employed to examine the morphological factors that contribute to the enhanced hole mobility observed in poly(3‐hexylthiophene) (P3HT) by the introduction of electrically inert poly(styrene) (PSt). Chain mobilities of crystalline and amorphous phases in the P3HT domain are evaluated utilizing T1C (13C spin‐lattice relaxation time in the laboratory frame). The crystallinity of P3HT component is estimated based on the spectral editing method through T1ρH (1H spin‐lattice relaxation time in the rotating frame) filtered CPMAS. Moreover, the miscibility of P3HT crystalline and P3HT amorphous domains is estimated. These results suggest the formation of the rigid amorphous (short‐range ordered amorphous) in a block copolymer (P3HT‐block‐PSt). An increase in the proportion of the crystallite and proximate presence of each crystallite in a blend sample of P3HT with PSt (P3HT‐blend‐PSt) are also indicated. Enhanced mobility is attributed to the larger portion of rigid amorphous domain for P3HT‐block‐PSt, and to higher crystalline content for P3HT‐blend‐PSt.

本研究采用固态交叉偏振魔角旋光（CPMAS）13C NMR 技术来研究通过引入电惰性聚（苯乙烯）（PSt）而在聚（3-己基噻吩）（P3HT）中观察到的空穴迁移率增强的形态因素。利用 T1C（实验室框架中的 13C 自旋晶格弛豫时间）评估了 P3HT 域中结晶相和无定形相的链迁移率。通过 T1ρH（旋转框架中的 1H 自旋晶格弛豫时间）滤波 CPMAS，利用光谱编辑法估算了 P3HT 成分的结晶度。此外，还估算了 P3HT 结晶畴和 P3HT 非晶畴的可混溶性。这些结果表明在嵌段共聚物（P3HT-block-PSt）中形成了刚性无定形（短程有序无定形）。在 P3HT 与 PSt 的共混样品（P3HT-blend-PSt）中，结晶体比例的增加和每个结晶体的近似存在也表明了这一点。流动性的增强归因于 P3HT 块状-PSt 中刚性无定形域的比例增大，以及 P3HT 混合物-PSt 中晶体含量的增加。

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引用次数: 0

Aggregation‐Induced Emission Near‐Infrared (NIR)‐II‐Conjugated Polymers Coupled With Nonconjugated Segments for NIR‐II Fluorescence Imaging–Guided NIR‐II Photothermal Therapy 聚合诱导发射的近红外 (NIR)-II 共轭聚合物与非共轭段耦合，用于 NIR-II 荧光成像引导的 NIR-II 光热疗法

IF 2.5 4区化学 Q3 POLYMER SCIENCE

Macromolecular Chemistry and Physics

Pub Date : 2024-08-29 DOI: 10.1002/macp.202400268

Zixin Hu, Jiarong He, Chenhang Xi, Sicheng Xu, Qingming Shen, Pengfei Chen, Pengfei Sun, Quli Fan

The development of conjugated polymer–based water‐soluble nanoparticles for near‐infrared‐II (NIR‐II) fluorescence (FL; 1000–1700 nm)‐guided photothermal therapy holds promise in advancing cancer treatment. However, excessive nonradiative decay leads to almost complete quenching of conjugated polymers’ fluorescence. Therefore, a critical challenge is to suppress nonradiative decay while maintaining high‐quality fluorescence imaging and excellent photothermal conversion efficiency. In this study, a series of NIR‐II‐conjugated polymers with aggregation‐induced emission (AIE) effects are designed and synthesized using the Stille coupling reaction. The dual enhancement strategy of modulating the AIE units and introducing non‐conjugated backbone into the polymer backbone resulted in BCT1 with a high αAIE value of 3.27. BCT1 nanoparticles exhibit excellent NIR‐II fluorescence, a high photothermal conversion efficiency of 70.51%, and a tenfold enhancement in fluorescence compared with BT1. Both in vitro and in vivo experiments validated their good biocompatibility and outstanding performance in NIR‐II fluorescence imaging for accurately determining the location of tumors. This study provides a novel strategy and method for designing and developing multifunctional conjugated polymers for NIR‐II fluorescence imaging–guided photothermal therapy.

开发基于共轭聚合物的水溶性纳米粒子，用于近红外-II（NIR-II）荧光（FL；1000-1700 纳米）引导的光热疗法，有望推动癌症治疗。然而，过度的非辐射衰变会导致共轭聚合物的荧光几乎完全熄灭。因此，如何在抑制非辐射衰变的同时保持高质量的荧光成像和出色的光热转换效率是一项严峻的挑战。本研究利用 Stille 偶联反应设计并合成了一系列具有聚集诱导发射（AIE）效应的 NIR-II 共轭聚合物。通过调节 AIE 单元和在聚合物骨架中引入非共轭骨架的双重增强策略，得到了αAIE 值高达 3.27 的 BCT1。BCT1 纳米粒子具有优异的近红外-II 荧光性能，光热转换效率高达 70.51%，与 BT1 相比，荧光增强了 10 倍。体外和体内实验均验证了其良好的生物相容性和在近红外-II荧光成像中的出色表现，可用于准确确定肿瘤位置。这项研究为设计和开发用于近红外-II 荧光成像引导的光热疗法的多功能共轭聚合物提供了一种新的策略和方法。

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引用次数: 0

[NVim]Br and Poly([NVim]Br-Co-AM): Synthesis and Effects on Inhibiting Clay Swelling and Dispersion and the Mechanisms [NVim]Br 和 Poly([NVim]Br-Co-AM)：合成、对抑制粘土膨胀和分散的作用及其机理

IF 2.5 4区化学 Q3 POLYMER SCIENCE

Macromolecular Chemistry and Physics

Pub Date : 2024-08-29 DOI: 10.1002/macp.202400141

Lan Li, Yanjun Ren, Rugang Yao, Hong Yang

To solve the downhole problems correlated with clay hydration swelling and dispersion under high-temperature conditions, a 1-aminoethyl-3-vinylimidazolium bromide ([NVim]Br) and a [NVim]Br/acrylamide copolymer (poly([NVim]Br-co-AM)) are synthesized and used as inhibitors. The molecular structures of [NVim]Br and poly([NVim]Br-co-AM) are characterized by FT-IR and ¹H-NMR. The inhibition properties of [NVim]Br and poly([NVim]Br-co-AM) are evaluated by free swelling and dispersion tests, linear swelling, hot roll recovery experiments and thermogravimetric analyses.The inhibition mechanisms were revealed by X-ray diffraction, zeta potential, wettability analysis and ESEM observation. The results showed that both [NVim]Br and poly([NVim]Br-co-AM) has significantly superior inhibition performance compared with the common inhibitors KCl, polyether amine D230 and polyquaternium-7. Both [NVim]Br and poly([NVim]Br-co-AM) can resist 250 °C. [NVim]Br performed excellently in inihibiting both crystalline and osmotic swelling, which depended on the strong electrostatic adsorption and hydrogen bonds of imidazole cations and primary amine in [NVim]⁺. Poly([NVim]Br-co-AM) exerted excellent inhibition by minimizing osmotic swelling, reducing hydrophilicity and increasing clay bonding. The results are important for understanding the rational design of novel efficient inhibitors for drilling high-temperature shale formation.

为了解决高温条件下与粘土水化膨胀和分散相关的井下问题，合成了 1-氨基乙基-3-乙烯基咪唑溴化物（[NVim]Br）和[NVim]Br/丙烯酰胺共聚物（poly([NVim]Br-co-AM)），并将其用作抑制剂。傅立叶变换红外光谱和 1H-NMR 对 [NVim]Br 和 poly([NVim]Br-co-AM) 的分子结构进行了表征。通过 X 射线衍射、ZETA 电位、润湿性分析和 ESEM 观察揭示了[NVim]Br 和 poly([NVim]Br-co-AM) 的抑制机理。结果表明，与常见的抑制剂 KCl、聚醚胺 D230 和聚季铵盐-7 相比，[NVim]Br 和聚（[NVim]Br-co-AM）的抑制性能明显优于它们。[NVim]Br和聚（[NVim]Br-co-AM）都能耐受 250 °C。[NVim]Br在抑制结晶膨胀和渗透膨胀方面表现出色，这取决于[NVim]+中咪唑阳离子和伯胺的强静电吸附和氢键。聚（[NVim]Br-co-AM）通过最大限度地减少渗透膨胀、降低亲水性和增加粘土键来发挥出色的抑制作用。这些结果对于合理设计用于钻探高温页岩层的新型高效抑制剂具有重要意义。

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引用次数: 0

Fabrication and Characterization of Carrageenan-Biopolymer Composite Microneedles for Interstitial Fluid Collection 用于间质液体收集的卡拉胶-生物聚合物复合微针的制作与特性分析

IF 2.5 4区化学 Q3 POLYMER SCIENCE

Macromolecular Chemistry and Physics

Pub Date : 2024-08-28 DOI: 10.1002/macp.202400160

Shreya Shashank Chauhan, Venkata Vamsi Krishna Venuganti

Identification of suitable polymeric materials to fabricate microneedles (MNs) for the collection of interstitial fluid (ISF) is a challenge. Here, characterization of different carrageenan-biopolymer composites for MN patch fabrication intended for ISF collection is reported. Systematic oscillatory rheological studies of composites containing iota-carrageenan mixed with alginate, gelatin, or pectin are performed to determine the linear viscoelastic region, gel point, tan delta, complex viscosity, and flow transition index. A polynomial equation is derived by relating flow transition index of biopolymer composites and compression strength of fabricated MNs. The biopolymer composite of iota-carrageenan and gelatin at 2% and 14%, respectively, and CaCl₂ crosslinker (80 mm) shows the greatest compression strength sufficient for MNs insertion into the excised porcine skin. MNs swell up on application in an agarose gel model and the ex vivo excised porcine skin model to collect 36 ± 5 and 14 ± 1 µL of fluid within 10 min, respectively. Taken together, it is demonstrated that rheological analysis can be performed to select suitable polymer composites that possess sufficient strength for the skin insertion and swellability for ISF collection.

寻找合适的聚合物材料来制造微针（MN）以收集组织间液（ISF）是一项挑战。本文报告了不同卡拉胶-生物聚合物复合材料的特性，这些复合材料可用于制造用于收集间质液的微针。对含有混有海藻酸、明胶或果胶的异卡拉胶的复合材料进行了系统的振荡流变学研究，以确定线性粘弹性区域、凝胶点、tan delta、复合粘度和流动转变指数。通过将生物聚合物复合材料的流动转变指数与制成的 MN 的压缩强度联系起来，得出了一个多项式方程。由分别为 2% 和 14% 的 iota-carrageenan 和明胶以及 CaCl2 交联剂（80 毫米）组成的生物聚合物复合材料显示出最大的压缩强度，足以将 MNs 插入切除的猪皮肤中。MNs 在琼脂糖凝胶模型和体外切除猪皮肤模型中应用时会膨胀，在 10 分钟内分别收集到 36 ± 5 µL 和 14 ± 1 µL 的液体。综上所述，可以通过流变分析来选择合适的聚合物复合材料，这些复合材料既要有足够的强度用于皮肤插入，又要有足够的膨胀性用于收集 ISF。

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引用次数: 0

Polymer Composite Electrolytes Membrane Consisted of Polyacrylonitrile Nanofibers Containing Lithium Salts: Improved Ion Conductive Characteristics and All‐Solid‐State Battery Performance 由含锂盐的聚丙烯腈纳米纤维组成的聚合物复合电解质膜：改善离子导电特性和全固态电池性能

IF 2.5 4区化学 Q3 POLYMER SCIENCE

Macromolecular Chemistry and Physics

Pub Date : 2024-08-28 DOI: 10.1002/macp.202400196

Yu Matsuda, Shun Nakazawa, Manabu Tanaka, Hiroyoshi Kawakami

Polymer electrolyte membranes with superior lithium‐ion (Li+) conductivity and sufficient electrochemical stability are desired for all‐solid‐state lithium‐ion batteries (ASS‐LIBs). This paper reports novel polymer composite membranes consisting of polyacrylonitrile (PAN) nanofibers (Nfs) containing lithium salts. It is first revealed that the lithium salt addition increases polar surface groups on the PAN nanofibers. Subsequently, the lithium salts‐containing PAN nanofiber (PAN/Li Nf) composite membrane affects the matrix poly(ethylene oxide) (PEO)/lithium bis(trifluoromethyl sulfonylimide) (LiTFSI) electrolyte to increase the numbers of Li+ with high mobility. Consequently, the PAN/Li Nf composite membrane shows relatively good ion conductivity (σ = 9.0 × 10−5 S cm−1) and a considerably large Li+ transference number (tLi+ = 0.41) at 60 °C, compared to the PEO/LiTFSI membrane without nanofibers. The 6Li solid‐state NMR study supports that the PAN/Li Nf bearing abundant polar nitrile groups at their surface enhances Li+ diffusion in the PEO‐based electrolyte membranes. The galvanostatic constant current cycling tests reveal that the PAN/Li Nf composite membrane possesses good electrochemical and mechanical stabilities. The ASS‐LIB consisting of the PAN/Li Nf composite membrane shows significantly improved charge and discharge cycling performances, promising future all‐solid‐state batteries.

全固态锂离子电池（ASS-LIB）需要具有卓越锂离子（Li+）传导性和足够电化学稳定性的聚合物电解质膜。本文报道了由含有锂盐的聚丙烯腈（PAN）纳米纤维（Nfs）组成的新型聚合物复合膜。研究首先发现，锂盐的添加增加了 PAN 纳米纤维上的极性表面基团。随后，含锂盐的 PAN 纳米纤维（PAN/Li Nf）复合膜影响了基质聚环氧乙烷（PEO）/双（三氟甲基磺酰亚胺）锂（LiTFSI）电解质，增加了具有高迁移率的 Li+ 数量。因此，与不含纳米纤维的 PEO/LiTFSI 膜相比，PAN/Li Nf 复合膜在 60 °C 时显示出相对较好的离子传导性（σ = 9.0 × 10-5 S cm-1）和相当大的 Li+ 转移数（tLi+ = 0.41）。6Li 固态核磁共振研究证明，表面含有大量极性腈基的 PAN/Li Nf 增强了 Li+ 在 PEO 基电解质膜中的扩散。电静态恒流循环测试表明，PAN/Li Nf 复合膜具有良好的电化学和机械稳定性。由 PAN/Li Nf 复合膜组成的 ASS-LIB 显著改善了充放电循环性能，有望成为未来的全固态电池。

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引用次数: 0

Fabrication of Cross‐Linked Polyimide Hollow Microspheres With Lightweight, Thermal Resistance and Controllable Size 制造轻质、耐热、尺寸可控的交联聚酰亚胺中空微球

IF 2.5 4区化学 Q3 POLYMER SCIENCE

Macromolecular Chemistry and Physics

Pub Date : 2024-08-28 DOI: 10.1002/macp.202400227

Yuntao Fu, Haichao Meng, Fenglin Wang, Huawei Zou, Yinfu Luo, Mei Liang, Peng Xie

Polyimide (PI) hollow microspheres possess lightweight and excellent thermal resistance, which are widely used in microreactors, catalysis, adsorption separation, high‐temperature insulation, and so on. In this manuscript, PI hollow microspheres are fabricated by constructing a crosslinked structure combined with gradient heating. The formation of PI hollow microspheres includes gas nucleation, expansion, and imidization. The PI hollow microspheres size is controlled by adjusting polyester ammonium salts size, and microspheres size is distributed in 309–956 µm. PI hollow microspheres have lightweight, excellent heat resistance and carbonization performance, bulk density, initial decomposition temperature, and weight residue at 800 °C is 87.3–178.6 kg m−3, 533.6 °C and 59.8%. The PI hollow microspheres have potential applications in high‐temperature resistant and multifunctional composite materials preparation. Moreover, this method is simple, efficient, and highly operable, which can be used for large‐scale production of PI hollow microspheres.

聚酰亚胺（PI）空心微球具有重量轻、耐热性好等特点，被广泛应用于微反应器、催化、吸附分离、高温绝缘等领域。在本手稿中，通过构建交联结构并结合梯度加热，制备了 PI 空心微球。PI 空心微球的形成过程包括气体成核、膨胀和酰亚胺化。通过调节聚酯铵盐的大小来控制 PI 空心微球的尺寸，微球尺寸分布在 309-956 微米之间。PI 空心微球具有轻质、优异的耐热性和碳化性能，体积密度、初始分解温度和 800 °C 时的残余重量分别为 87.3-178.6 kg m-3、533.6 °C 和 59.8%。该 PI 空心微球在制备耐高温和多功能复合材料方面具有潜在的应用前景。此外，该方法简单、高效、可操作性强，可用于 PI 空心微球的大规模生产。

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引用次数: 0

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