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Introduction to hybrid inorganic–organic polymers 无机-有机杂化聚合物简介
IF 3.9 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-11-28 DOI: 10.1039/D5PY90139A
Saurabh S. Chitnis, Rebekka S. Klausen and Erin M. Leitao

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引用次数: 0
Graft length and density govern morphology and optoelectronic properties of poly(caprolactone)-graft-oligo(3-hexylthiophene)s 接枝长度和密度影响聚(己内酯)-接枝寡聚(3-己基噻吩)s的形貌和光电性能
IF 3.9 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-11-27 DOI: 10.1039/D5PY00815H
Yuhka Uda, Eddie Wai Chi Chan, Timothy Lambden, Scott T. Keene, Xin Sun, Zoran Zujovic, David Barker, Paul Midgley, George Malliaras and Jadranka Travas-Sejdic

Compositional modifications of conducting polymer-based graft copolymers enable precise tuning of their properties, including conductivity, degradation and opto-electrochemical properties. This work investigates how the composition of poly(caprolactone)-graft-oligo(3-hexylthiophene)s, (P(CL-co-AVL)-g-O3HT), previously shown to be degradable, effects the morphological and opto-electrochemical properties of the copolymers. Effect of different grafting density and the length of the O3HT grafts on the material's properties were investigated using a range of advanced techniques, such as, spectroelectrochemistry, cyclic voltammetry, 2D-GIXRD and 4D-STEM. Short O3HT grafts (n = 15) yielded amorphous copolymers, whereas longer grafts (n = 30, 40) produced semi-crystalline material with distinct crystalline and amorphous redox signatures. High grafting density promoted formation of interconnected nanoscale O3HT crystallites. Thermal annealing (40–60 °C) or trace acetonitrile (1 vol%) in casting solutions enhanced intrachain order and crystallization, and, in turn, enhanced optoelectronic properties of the high-density, long grafts copolymers. These findings establish structure–property relationship in conducting polymer-based graft copolymers, guiding their macromolecular design, including for transient electronics.

导电聚合物基接枝共聚物的成分修饰可以精确调整其性能,包括电导率、降解和光电化学性能。本研究研究了聚(己内酯)-接枝-寡聚(3-己基噻吩)s, (P(CL-co-AVL)-g-O3HT)的组成如何影响共聚物的形态和光电电化学性能,这些共聚物之前被证明是可降解的。利用光谱电化学、循环伏安法、2D-GIXRD和4D-STEM等先进技术研究了不同接枝密度和接枝长度对O3HT材料性能的影响。较短的O3HT接枝(n = 15)产生了非晶共聚物,而较长的接枝(n = 30, 40)产生了具有明显结晶和非晶氧化还原特征的半结晶材料。高接枝密度促进了互连纳米级O3HT晶体的形成。热退火(40-60°C)或在铸造溶液中添加微量乙腈(1 vol.%)可增强链内有序度和结晶性,进而增强高密度长接枝共聚物的光电性能。这些发现建立了导电聚合物基接枝共聚物的结构-性能关系,指导了它们的大分子设计,包括瞬态电子。
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引用次数: 0
Upcycling of PET waste: from one polymer to another polymer PET废弃物的升级回收:从一种聚合物到另一种聚合物
IF 3.9 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-11-26 DOI: 10.1039/D5PY00861A
Te Yang, Zhenjie Yang, Yulu Zhang, Chenyang Hu, Zhenbiao Xie, Zhiqiang Sun, Xuan Pang and Xuesi Chen

Polyethylene terephthalate (PET), a dominant polymer in global plastic production, faces critical recycling challenges due to its persistence in ecosystems and limitations of conventional mechanical/thermal recycling. Upcycling PET waste into value-added polymers represents a transformative approach toward a circular plastics economy. This review systematically examines innovative strategies for chemically converting post-consumer PET into novel polymeric materials, thereby bypassing the performance degradation typically associated with traditional recycling. Key pathways include (1) depolymerization into monomers (terephthalic acid, ethylene glycol) for repolymerization into high-purity PET or advanced polyesters (e.g., biodegradable or bio-based variants), (2) transformation into functional polymers such as polyurethanes, epoxy resins, and ion-exchange membranes via tailored catalytic processes, and (3) copolymerization/blending with biopolymers to enhance material properties. Breakthroughs in catalysts (enzymes, ionic liquids), solvent-free systems, and energy-efficient reactors are highlighted for improving the reaction selectivity and scalability. Despite progress, challenges persist in managing mixed plastic wastes, removing contaminants, and achieving cost parity with virgin polymers. Emerging trends, including enzymatic engineering and AI-guided monomer-to-polymer design, are proposed to address these barriers. By bridging molecular innovation with industrial feasibility, PET upcycling offers dual environmental and economic incentives to close the plastic lifecycle loop.

聚对苯二甲酸乙二醇酯(PET)是全球塑料生产中的主要聚合物,由于其在生态系统中的持久性和传统机械/热回收的局限性,面临着严峻的回收挑战。将PET废物升级为增值聚合物代表了迈向循环塑料经济的变革方法。本综述系统地研究了将消费后PET化学转化为新型聚合物材料的创新策略,从而绕过了通常与传统回收相关的性能退化。关键途径包括:(1)解聚成单体(对苯二甲酸,乙二醇),再聚合成高纯度PET或高级聚酯(例如,可生物降解或生物基变体),(2)通过定制的催化工艺转化为功能性聚合物,如聚氨酯,环氧树脂和离子交换膜,以及(3)与生物聚合物共聚/共混以增强材料性能。在催化剂(酶、离子液体)、无溶剂体系和节能反应器方面的突破突出了反应选择性和可扩展性的提高。尽管取得了进展,但在管理混合塑料废物、去除污染物以及实现与原生聚合物同等成本方面仍然存在挑战。新兴趋势,包括酶工程和人工智能引导的单体到聚合物设计,被提出来解决这些障碍。通过将分子创新与工业可行性相结合,PET升级回收为关闭塑料生命周期循环提供了双重环境和经济激励。
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引用次数: 0
A precursor-dependent distinctive polymerization process controls the optoelectronic properties of graphitic carbon nitride photocatalyst 依赖前驱体的独特聚合过程控制着氮化石墨碳光催化剂的光电性能
IF 3.9 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-11-26 DOI: 10.1039/D5PY01003A
Simon Joyson Galbao, Sherlin Samantha Menezes, Syeda Reha Khadri and Dharmapura H. K. Murthy

Due to its metal-free polymeric nature, ease of synthesis using low-cost earth-abundant precursors and tunable optoelectronic properties, graphitic carbon nitride (GCN) is extensively used in solar fuel production. Despite two decades of extensive research, the fundamentals of the thermal polymerization process leading to the formation of GCN are inadequately understood. In this work, we employ cyanamide (CYN) and dicyandiamide (DCDA) precursors and systematically reveal the polymerization mechanism. Though CYN has half the amount of C and N compared with DCDA, it yielded virtually similar structural properties and a similar degree of conjugation that determines the energetic difference for π-to-π* fundamental (optical) transitions and photoexcited lifetimes. Detailed complementary analysis using thermal methods, along with quantifying the amount of NH3 released using the temperature-programmed desorption technique, offered unique insights into the polymerization process. Unlike previous notions, the results unambiguously demonstrate that GCN formation need not always release NH3 as a result of a thermal condensation reaction. Rather, it is possible that molecular rearrangement (dimerization and/or cyclization) of intermediate condensates can also play a major role in the formation of melamine, which is found to be an important intermediate. The obtained mechanistic insights into the thermodynamics of the polymerization process and its impact on optoelectronic properties and photoelectrochemical performance will aid the rational design of GCN to enhance the efficiency of solar energy conversion.

由于其不含金属的聚合物性质,易于使用低成本的富土前驱体合成和可调谐的光电性能,石墨氮化碳(GCN)被广泛用于太阳能燃料的生产。尽管进行了二十年的广泛研究,但对导致GCN形成的热聚合过程的基本理解尚不充分。在这项工作中,我们采用氰胺(CYN)和双氰胺(DCDA)前体,系统地揭示了聚合机理。虽然CYN的C和N含量是DCDA的一半,但它产生了几乎相似的结构性质,共轭度决定了π到π*基本(光学)跃迁和光激发寿命之间的能量差异。使用热方法进行详细的互补分析,并使用温度程序解吸技术定量释放NH3的量,为聚合过程提供了独特的见解。与之前的概念不同,结果明确表明GCN的形成并不总是需要释放NH3作为热缩合反应的结果。相反,中间凝聚物的分子重排(二聚化和/或环化)也可能在三聚氰胺的形成中起主要作用,三聚氰胺被发现是一种重要的中间体。深入了解聚合过程的热力学机理及其对光电性能和电化学性能的影响,有助于合理设计GCN以提高太阳能转换效率。
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引用次数: 0
Efficient catechol functionalization of high oleic sunflower oil for the preparation of fully biobased and extrudable acetal CANs 高含油向日葵油的高效儿茶酚功能化制备全生物基和可挤压缩醛罐
IF 3.9 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-11-25 DOI: 10.1039/D5PY00927H
Timo Sehn, Mickaël Du Fraysseix, Cédric Le Coz, Emmanuel Ibarboure, Michael A. R. Meier and Audrey Llevot

Herein, we introduce the synthesis of fully renewable and extrudable high oleic sunflower oil-based acetal containing covalent adaptable networks (CANs) via a catalyst and solvent-free click-like reaction between a bio-based polyol and divinyl ether, i.e. 1,4-cyclohexanedimethanol divinyl ether. High oleic sunflower oil was therefore first converted into the respective polyol via a simple H2SO4 catalyzed Friedel–Crafts alkylation using catechol within 30 minutes at 120 °C. After subsequent structural characterization of the polyol, acetal containing CANs showing high cross-linking densities, fast stress relaxation, and excellent malleability were synthesized without releasing any small-molecule byproducts. The presence of the catechol moiety is particularly interesting, as the presence of an adjacent phenolic group induces neighboring group participation effects and accelerates exchange reaction rates. The dynamic behavior of the new cross-linked materials was confirmed by stress relaxation measurements at different temperatures as well as by their reprocessability via compression molding and extrusion. Additionally, the materials were degraded under weak acidic conditions, and the starting biobased polyol was recovered in a yield of 72%, thus enabling a closed-loop chemical recycling of this monomer.

本文介绍了一种生物基多元醇和二乙烯基醚(即1,4-环己二甲醇二乙烯基醚)之间通过无催化剂和无溶剂的键合反应,合成了完全可再生和可挤压的含有共价适应性网络(can)的高油基向日葵油基缩醛。因此,高油分葵花籽油首先在120°C下通过简单的H2SO4催化的Friedel-Crafts烷基化反应在30分钟内转化为相应的多元醇。在对多元醇进行后续结构表征后,合成了具有高交联密度、快速应力松弛和优异延展性的缩醛型can,且不释放任何小分子副产物。儿茶酚部分的引入特别有趣,因为相邻酚基的存在诱导邻基参与效应并加速交换反应速率。通过不同温度下的应力松弛测量以及通过压缩成型和挤压的再加工性,证实了新型交联材料的动态行为。此外,该材料在弱酸性条件下被降解,初始生物基多元醇的回收率为72%,从而实现了该单体的闭环化学循环。
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引用次数: 0
Diversity-oriented route to functional covalent triazine frameworks 以多样性为导向的功能性共价三嗪框架
IF 3.9 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-11-24 DOI: 10.1039/D5PY00872G
Catherine Mollart, Ellena Sherrett, Patrick Heasman, Michael J. G. Peach, Adam Rowling, Lewis J. Beck, Ellie Varley, David Seed and Abbie Trewin

An alternative route to synthesise TCNQ-CTF by using trifluoromethanesulfonic (TFMS) acid catalysis is presented, in comparison to a previously reported ZnCl2-catalysed synthesis. The new synthetic route yields a polymer with additional structural diversity compared to the previously reported material. The composition of the framework is rationalised by ‘artificial’ acid-catalysed synthesis of TCNQ-CTF, together with a novel approach to structural feature identification, with a range of alternative structural features appearing that were not present in the previously reported polymer formed by ZnCl2 catalysis. These results will inform the design of new CTF materials with additional functionality and broader applications.

与之前报道的zncl2催化合成相比,提出了一种利用三氟甲烷磺酸(TFMS)酸催化合成TCNQ-CTF的替代途径。与先前报道的材料相比,新的合成路线产生了具有额外结构多样性的聚合物。框架的组成通过“人工”酸催化合成TCNQ-CTF来合理化,以及一种新的结构特征识别方法,出现了一系列替代结构特征,这些特征在以前报道的由ZnCl2催化形成的聚合物中不存在。这些结果将为具有附加功能和更广泛应用的新型CTF材料的设计提供信息。
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引用次数: 0
Preparation and performance characterization of block cross-linked copolymers PCaPE(Br) and PCaPE(I) via RAFT polymerization and quaternization reaction RAFT聚合和季铵化反应制备嵌段交联共聚物PCaPE(Br)和PCaPE(I)及其性能表征
IF 3.9 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-11-22 DOI: 10.1039/D5PY01036E
Chaoyue Shan, Haohao Zhang, Yan Gao, Hui Wang, Li Han, Yuanyuan Du, Wen He, Mingyuan Pang, Xing Gao and Yen Leng Pak

Reversible addition–fragmentation chain transfer (RAFT) polymerization enables precise regulation of polymer chain growth and active center distribution. This study adopted a two-step approach with RAFT polymerization followed by quaternization to synthesize antibacterial materials, specifically tunable porous polymers PCaPE(Br) and PCaPE(I). The work focused on the structure–activity relationship between RAFT-derived block structures and the antibacterial properties of these materials. RAFT-mediated polymerization precisely controlled the block copolymer precursor PE-PDE, which is PEMA-b-P(DMAEA-co-EGDMA), and this control facilitated the subsequent formation of ordered porous structures. When the molar ratio of poly(ethyl methacrylate) (PEMA) to ethylene glycol dimethacrylate (EGDMA) was set to 1 : 6, the final quaternized products PCaPE2(Br) and PCaPE2(I) exhibited porous and fluffy microstructures. These microstructures were characterized by large specific surface area and high porosity. This structure, combined with uniformly distributed quaternary ammonium salt groups from the quaternization of N,N-dimethylaminoethyl acrylate (DMAEA) tertiary amine groups, enhanced the contact between antibacterial active sites and bacteria as well as antibacterial efficacy. PCaPE(Br) and PCaPE(I) showed excellent broad-spectrum antibacterial activity against E. coli and S. aureus. They also maintained good reusability with over 95% activity retention after five cycles. Such advantages support their prospects in biomedicine, agricultural antibacterials and wastewater treatment.

可逆加成-破碎链转移(RAFT)聚合可以精确调节聚合物链的生长和活性中心的分布。本研究采用RAFT聚合-季铵化两步法合成抗菌材料,特别是可调多孔聚合物PCaPE(Br)和PCaPE(I)。研究了raft衍生的块结构与这些材料的抗菌性能之间的构效关系。raft介导的聚合精确地控制了嵌段共聚物前体PE-PDE,即pma -b- p (DMAEA-co-EGDMA),这种控制促进了随后有序多孔结构的形成。当聚甲基丙烯酸乙酯(PEMA)与乙二醇二甲基丙烯酸酯(EGDMA)的摩尔比为1:6时,最终季铵化产物PCaPE2(Br)和PCaPE2(I)呈现多孔和蓬松的微观结构。这些微观结构具有比表面积大、孔隙率高的特点。这种结构与N,N-二甲氨基丙烯酸乙酯(DMAEA)叔胺基季铵化形成的均匀分布的季铵盐基结合,增强了抗菌活性位点与细菌的接触,提高了抗菌效果。PCaPE(Br)和PCaPE(I)对大肠杆菌和金黄色葡萄球菌具有良好的广谱抗菌活性。它们还保持了良好的可重用性,在5个周期后保持了95%以上的活动留存率。这些优势支持了它们在生物医学、农业抗菌剂和废水处理方面的前景。
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引用次数: 0
Effect of ionization by proton transfer on propagation rate coefficients: a PLP-SEC study of methacrylic acid-amine monomers 质子转移电离对繁殖速率系数的影响:甲基丙烯酸-胺单体的PLP-SEC研究
IF 3.9 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-11-21 DOI: 10.1039/D5PY01000D
Samuel Wierzbicki, Szczepan Bednarz and Igor Lacík

Previously, we reported the dependence of the propagation rate coefficient (kp) for methacrylic acid (MAA) and sodium methacrylate (MAANa) on monomer concentration, degree of ionization, and temperature (I. Lacík, L. Učňová, S. Kukučková, M. Buback, P. Hesse and S. Beuermann, Macromolecules, 2009, 42, 7753–7761). In this study, we extend this work to investigate the ionization of MAA via a proton transfer mechanism in the presence of primary isobutylamine (IBA) and tertiary triethylamine (TEA), which differ in their affinity for the carboxylic proton. An advantage of these systems lies in their solubility in both water and non-polar solvents due to the presence of a hydrophobic group in the cation moiety. NMR and FTIR spectroscopy showed that complete proton transfer occurs for both monomers in water, and for MAA-IBA in DMSO. In contrast, MAA-TEA forms a hydrogen-bonded molecular complex in DMSO. The Kamlet–Taft α parameter was determined as a measure of the hydrogen bond donor ability of these systems. The kp values for these MAA-amine monomers were determined in water and DMSO over a monomer concentration range of 0.45–1.82 mol L−1 and a temperature range of 20–60 °C, using pulsed laser polymerization coupled with size-exclusion chromatography. In both solvents, the kp values for MAA-IBA are lower than those for MAA-TEA, with the difference being modest in water (up to a factor of 2) and more pronounced in DMSO (up to a factor of 4). The influence of monomer concentration on kp is less significant than for MAANa. Activation energies, EA(kp), increase from 19.3 ± 1.5 and 17.8 ± 0.3 kJ mol−1 in water to 28.2 ± 1.6 and 26.9 ± 1.7 kJ mol−1 in DMSO for MAA-IBA and MAA-TEA, respectively. The pre-exponential factor ∼0.9 × 106 L mol−1 s−1 is similar for both monomers in water and is increased by an order of magnitude in DMSO. These results demonstrate that kp depends on monomer speciation and a complex interplay between electrostatic, hydrogen bonding, and hydrophobic interactions.

此前,我们报道了甲基丙烯酸(MAA)和甲基丙烯酸钠(MAANa)的增殖速率系数(kₚ)与单体浓度、电离度和温度的关系(Macromolecules 2009, 42, 7753-7761)。在这项研究中,我们扩展了这项工作,研究了在伯异丁胺(IBA)和叔三乙胺(TEA)存在下,MAA通过质子转移机制的电离,这两种物质对羧基质子的亲和力不同。这些体系的优点在于它们在水和非极性溶剂中的溶解度,这是由于阳离子部分中存在疏水性基团。核磁共振和红外光谱分析表明,单体在水中和MAA-IBA在DMSO中均发生完全质子转移。相反,MAA-TEA在DMSO中形成氢键分子络合物。确定了Kamlet-Taft α参数作为衡量这些体系氢键供体能力的指标。在水和DMSO中测定了这些maa -胺单体的kₚ值,其浓度范围为0.45-1.82 mol L⁻¹,温度范围为20-60 °C。在两种溶剂中,MAA-IBA的kₚ值都低于MAA-TEA,在水中的差异不大(高达2倍),而在DMSO中的差异更明显(高达4倍)。单体浓度对kₚ的影响不如MAANa显著。MAA-IBA和MAA-TEA的活化能,EA(kp),分别从水的19.3±1.5和17.8±0.3 kJ mol -毒发展到DMSO的28.2±1.6和26.9±1.7 kJ mol -毒发展。指数前因子~0.9 x 106 L mol(⁻¹s)在水中是相似的,在DMSO中增加了一个数量级。这些结果表明,kₚ取决于单体形态和静电、氢键和疏水相互作用之间的复杂相互作用。
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引用次数: 0
Polyimidazolium amphiphilic dendrimers on thiacalix[4]arene and gallic acid platforms via copper-free click chemistry: synthesis, self-assembly and DNA binding 巯基芳烃和没食子酸平台上的聚咪唑类两亲树状大分子:合成、自组装和DNA结合
IF 3.9 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-11-19 DOI: 10.1039/D5PY00984G
Ilshat M. Bogdanov, Angelina A. Fedoseeva, Anastasiya A. Glukhova, Elza D. Sultanova, Timur A. Mukhametzyanov, Vladimir G. Evtugyn, Svetlana E. Solovieva, Vladimir A. Burilov and Igor S. Antipin

A divergent synthetic scheme based on copper-free click chemistry was used to obtain two types of bromine-containing dendrimers with a thiacalix[4]arene or gallic acid core. These dendrimers were then terminated with cationic imidazolium groups via the Menshutkin reaction to obtain a series of amphiphilic dendrimers. The critical aggregation concentrations of the dendrimers were determined using three different probes. It was demonstrated that the solubilization capacity with respect to the hydrophobic Orange OT substrate logically increases with the transition from the second to the third generation, whereas the first generation does not solubilize the dye. In the case of the thiacalix[4]arene core, the most compact aggregates (approximately 80 nm) were obtained in the second generation. In the case of gallic acid, the most compact aggregates (approximately 30 nm) were obtained in the second and third generations, with the third generation forming the most monodisperse particles. Steady-state and time-resolved fluorescence spectroscopy revealed that the third generation on both the gallic acid and thiacalix[4]arene platforms interacts most effectively with calf thymus DNA, displacing ethidium bromide. The addition of third-generation dendrimers causes DNA compaction, forming particles measuring approximately 70–120 nm, and results in surface recharging to +40 mV. Since the CD data show that the addition of dendrimers results in DNA ordering (transition to the C-form), the obtained second- and third-generation dendrimers are promising as potential matrices for stabilization, storage, or delivery of nucleic acids in future studies.

采用一种基于无铜键合化学的发散合成方案,得到了两种芯部为硫杯[4]芳烃或没食子酸的含溴树状大分子。这些树状大分子通过Menshutkin反应被阳离子咪唑基终止,得到一系列两亲性树状大分子。用三种不同的探针确定了树状大分子的临界聚集浓度。结果表明,从第二代过渡到第三代,疏水橙色OT底物的增溶能力合乎逻辑地增加,而第一代不增溶染料。在第二代的情况下,获得了最致密的聚集体(约80 nm)。以没食子酸为例,第二代和第三代获得了最致密的聚集体(约30纳米),第三代形成了最单分散的颗粒。稳态和时间分辨荧光光谱显示,第三代没食子酸和硫代芳烃平台与小牛胸腺DNA相互作用最有效,取代溴化乙啶。第三代树状大分子的加入导致DNA压实,形成约70 - 120nm的颗粒,并导致表面充电至+ 40mv。由于CD数据表明,添加树状大分子导致DNA排序(过渡到c型),因此所获得的第二代和第三代树状大分子有望在未来的研究中作为稳定、储存或递送核酸的潜在基质
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引用次数: 0
A new amorphous dithienocyclopentapyrene-benzothiadiazole (PyDT-BT) polymer with high-mobility and strong red light emission 新型高迁移率、强红光发射的非晶态二噻吩环五apyrene苯并噻唑(PyDT-BT)聚合物
IF 3.9 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-11-19 DOI: 10.1039/D5PY00990A
Tianrui Zhang, Honglei Li, Jichao Jiang, Jidong Zhang, Hongkun Tian and Lixiang Wang

Due to the contradictory molecular design principles required to achieve both high mobility and strong luminescence, the development of polymer semiconductors that simultaneously possess these characteristics remains a significant challenge. To address this issue, the development of structurally innovative conjugated polymers is highly desired. Herein, two dithienocyclopentapyrene (PyDT) donor units with either centro- or axial-symmetry were designed and synthesized, and subsequently copolymerized with a benzothiadiazole (BT) acceptor to afford cs-PyDT-BT and as-PyDT-BT. The resulting polymers exhibit pronounced position- and molecular-weight-dependent characteristics. Specifically, cs-PyDT-BT displays low crystallinity and a nearly amorphous microstructure, yet achieves higher charge-carrier mobility and intense red emission (∼670 nm) relative to its counterpart as-PyDT-BT, which shows higher crystallinity, lower mobility, and a red-shifted emission (∼690 nm). Furthermore, the influence of molecular weight was systematically investigated for cs-PyDT-BT. As the molecular weight increased, the film-state photoluminescence quantum yield (PLQY) gradually decreased, with the maximum value reaching 22%, while the highest mobility of 1 cm2 V−1 s−1 was obtained at a medium Mn of approximately 100 kDa. This molecular design strategy provides new insights for developing next-generation conjugated polymers that combine strong luminescence with high mobility, thereby advancing multifunctional integrated polymeric materials.

由于实现高迁移率和强发光所需的相互矛盾的分子设计原则,同时具有这些特性的聚合物半导体的发展仍然是一个重大的挑战。为了解决这一问题,迫切需要开发结构创新的共轭聚合物。本文设计并合成了两个中心对称或轴对称的二噻吩环五apyrene (PyDT)给体单元,并与苯并噻唑(BT)受体共聚得到cs-PyDT-BT和as-PyDT-BT。所得聚合物表现出明显的位置和分子量依赖特性。具体来说,cs-PyDT-BT具有较低的结晶度和接近无定形的微观结构,但相对于具有较高结晶度、较低迁移率和红移发射(~690 nm)的as-PyDT-BT, cs-PyDT-BT具有较高的载流子迁移率和强红移发射(~670 nm)。此外,系统地研究了分子量对cs-PyDT-BT的影响。随着分子量的增加,膜态光致发光量子产率(PLQY)逐渐降低,最大值可达22%,而迁移率最高的1 cm²V⁻¹s⁻¹在约100 kDa的介质中得到。这种分子设计策略为开发结合强发光和高迁移率的下一代共轭聚合物提供了新的见解,从而推动了多功能集成聚合物材料的发展。
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引用次数: 0
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