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Xylose-derived thionocarbamates as a synthetic handle towards a functional platform of sugar-based polymers 将木糖衍生的硫代氨基甲酸酯作为糖基聚合物功能平台的合成工具
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-07-15 DOI: 10.1039/d4py00540f
James R. Runge, Bethan Davies, Antoine Buchard
The derivatisation of D-xylose with potassium thiocyanate is presented as a versatile synthetic handle towards functional synthetic carbohydrate polymers. The reactivity of the resulting 1,3-oxazolidine-2-thione (OZT) group with alkyl bromides is ubiquitous and, herein, has been exploited to synthesise seven bio-derived monomers with different pendant functionalities. These monomers were polymerised with dithiols to yield functional poly(ester-thioethers) with a broad spectrum of properties. From a single non-functionalised OZT-polymer, a variety of post-polymerisation modification approaches are possible to functionalise the materials with different pendant groups. These results present a novel simple methodology to tailor the properties of synthetic carbohydrate polymers to different applications.
D-xylose 与硫氰酸钾的衍生化是实现功能性合成碳水化合物聚合物的一种多功能合成方法。由此产生的 1,3-噁唑烷-2-硫酮(OZT)基团与烷基溴化物的反应性无处不在,本文利用这种反应性合成了七种具有不同悬垂官能团的生物衍生单体。这些单体与二硫醇聚合后可生成具有多种特性的功能性聚酯硫醚。从单一的非官能化 OZT 聚合物出发,可以采用多种聚合后改性方法,用不同的悬垂基团对材料进行官能化。这些成果提供了一种新颖简单的方法,可根据不同的应用定制合成碳水化合物聚合物的特性。
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引用次数: 0
Blue Light-emitting Conjugated Polymer with Low Modulus and Better EL Spectra Stability 具有低模量和更好 EL 光谱稳定性的蓝光发光共轭聚合物
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-07-12 DOI: 10.1039/d4py00180j
Huaqiang Gong, Wenxin Huang, Wenyu Chen, Lu-Bing Bai, Xinyu Liang, Yingying Zheng, Qingqing Lu, Rui Gao, Yamin Han, Zhiqiang Zhuo, Xiang An, Jin-Yi Lin, Wei Huang
Intrinsic stretchable light-emitting conjugated polymers (LCPs) with low modulus play an increasingly significant roles in flexible or skin-like displays. In this work, we focuse on investigating the optoelectronic and mechanical properties of polyfluorene-based blue LCPs, of which the polymer side chains were straight alkyl chains (octyl) and branched alkyl chains (2-hexyldecyl). Comparatively, the solution processed film of polymer with branched alkyl chains performed substantially improved photoluminescence quantum yield (PLQY) from 18.9% to 46.5%. Benefiting from the internal plasticization of branched alkyl chains, the elastic modulus of polymer film reduced from 350 Mpa to 180 Mpa, confirming the validity of enhancing alkyl/π ratio in lowering film stiffness and necessity for characterzing the intrinsic mechanical properties. Finally, polymer light-emitting diodes (PLED) that performed stable blue emitting was achieved with the polyfluorene-based LCPs functionalized by branched alkyl chains. Overall, these observations manifest the feasibility of side-chain branching in tuning the mechanical properties of LCPs, and provide a deep insights for developing intrinsic stretchable semiconductors.
具有低模量的本征可拉伸发光共轭聚合物(LCP)在柔性或类似皮肤的显示器中发挥着越来越重要的作用。在这项工作中,我们重点研究了以聚芴为基础的蓝色 LCP 的光电和机械性能,其中聚合物侧链包括直链烷基(辛基)和支链烷基(2-己基癸基)。相比之下,具有支化烷基链的聚合物溶液加工薄膜的光致发光量子产率(PLQY)从 18.9% 大幅提高到 46.5%。得益于支化烷基链的内部塑化,聚合物薄膜的弹性模量从 350 兆帕降至 180 兆帕,这证实了提高烷基/π 比率在降低薄膜刚度方面的有效性,以及表征内在机械特性的必要性。最后,通过支化烷基链功能化的聚芴基低粘度聚氯乙烯实现了聚合物发光二极管(PLED)的稳定蓝色发光。总之,这些观察结果表明了侧链分支在调整 LCP 机械性能方面的可行性,并为开发本征可拉伸半导体提供了深刻的见解。
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引用次数: 0
Synthesis of a sulfonamide functionalized poly(styrene oxide) and illustration of a potential post-polymerization strategy 磺酰胺功能化聚(氧化苯乙烯)的合成及潜在后聚合策略说明
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-07-10 DOI: 10.1039/d4py00460d
Marina Wittig, Philipp Pfändner, Bernhard Rieger
In the first part of our work, we demonstrate a design concept for the functionalization of styrene oxide (SO) with a sulfonamide protecting group. A (1S,2S)-(+)-[1,2-cyclohexanediamino-N,N′-bis(3,5-di-t-butylsalicylidene)]-chromium(III)chloride ((salen)Cr(III)) catalyst polymerizes the end grouped epoxide via ring-opening-polymerization (ROP) into the respective polyether backbone. Absolute molecular weights of the resulting homopolymers range between 14.2 to 113 kg mol−1 with a polymer stability up to 300 °C and a glass transition temperature (Tg) of around 68–73 °C. The synthesis is completed by showing a possible post-polymerization modification of the functionalized poly(styrene oxide) (PSO). By adding the polymer to a lithium methoxide solution, a new reactive group in the form of a free sulfonate moiety can be generated. This method enables the transition towards a lithium sulfonated PSO that shows a thermal stability up to 300 °C and a Tg in the range of 18–20 °C.
在工作的第一部分,我们展示了用磺酰胺保护基团对氧化苯乙烯(SO)进行官能化的设计理念。(1S,2S)-(+)-[1,2-环己烷二氨基-N,N′-双(3,5-二叔丁基水杨酰)]-氯化铬(III)((salen)Cr(III))催化剂通过开环聚合(ROP)将端基环氧化物聚合到相应的聚醚骨架中。所得均聚物的绝对分子量在 14.2 至 113 kg mol-1 之间,聚合物稳定性高达 300 ℃,玻璃化转变温度 (Tg) 约为 68-73 ℃。合成完成后,还展示了对功能化聚(氧化苯乙烯)(PSO)进行聚合后改性的可能性。将聚合物添加到甲醇锂溶液中,可以生成游离磺酸基形式的新活性基团。这种方法可使锂磺化 PSO 转变为热稳定性高达 300 ℃、Tg 在 18-20 ℃ 范围内的聚苯乙烯氧化物。
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引用次数: 0
Oxygen-tolerant, Eosin Y mediated synthesis of protein-polymer biohybrids and protein-coated polymer nanoparticles 耐氧、以曙红 Y 为介质合成蛋白质聚合物生物混合物和蛋白质涂层聚合物纳米粒子
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-07-10 DOI: 10.1039/d4py00407h
Errika Voutyritsa, Thomai Lazou, Jonida Bushi, Stavroula Margaritaki, Myrto Charitaki, Sune M. Christensen, Nikos Hatzakis, Kelly Velonia
To avoid metal catalysts used in conventional approaches, an Eosin Y/TEMED mediated, photoinduced polymerization of vinyl monomers was optimized for the synthesis of protein-polymer conjugates. This oxygen-tolerant, photoinduced approach allowed to graft a series of hydrophobic, hydrophilic and responsive polymers with quantitative protein macroinitiator consumption. CALB bioconjugates were also synthesized and found to retain part of the parent protein activity for extended periods of time. Notably, when BSA was used in the absence of initiator, protein-coated nanoparticles were shown to form during emulsion polymerization.
为了避免传统方法中使用的金属催化剂,对乙烯基单体的 Eosin Y/TEMED 介导的光诱导聚合进行了优化,以合成蛋白质-聚合物共轭物。这种耐氧的光诱导方法可以在定量消耗蛋白质大引发剂的情况下接枝一系列疏水性、亲水性和反应性聚合物。我们还合成了 CALB 生物共轭物,并发现它们能在较长时间内保持母体蛋白质的部分活性。值得注意的是,在没有引发剂的情况下使用 BSA 时,乳液聚合过程中会形成蛋白质包覆的纳米颗粒。
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引用次数: 0
Anionic Polymerization of Phenyl-Substituted Isoprene Derivatives: Polymerization Behaviour and Cyclization-Enabled Fluorescence 苯基取代异戊二烯衍生物的阴离子聚合:聚合行为与环化荧光
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-07-10 DOI: 10.1039/d4py00601a
Moritz Rauschenbach, Laura Stein, Gregor Linden, Ramona Barent, Katja Heinze, Holger Frey
1,3-dienes are important monomers for the living anionic polymerization. However, phenyl-substituted diene monomer structures have been hardly investigated. Based on DFT-calculations and 13C NMR spectroscopy, a discrepancy in the reactivity of the two monomers 1-phenyl isoprene (1PhI) and 4-phenyl isoprene (4PhI) in the anionic polymerization is expected. Starting from a Wittig reaction including an optimized extraction procedure, the disubstituted 1,3-dienes resulted in polymers with different prevalence of 1,3-incorporation. The polymers have been characterized by 1H NMR spectroscopy and using different SEC conditions. Molecular weights up to 48.8 kg mol-1 with narrow dispersities (Đ ≤ 1.13) were achieved. The addition of the modifier THF led to an initial increase of vinyl-units as well as a loss of control for the polymerization of 4PhI. Increasing the THF concentration further resulted in a rather unusual decrease of the vinyl units and climaxed in more than 80% 1,4-units in pure THF. Copolymerizations with styrene (S) and isoprene (I), respectively, were tracked via in situ 1H NMR kinetics. The observed ideally random copolymerization of I and 1PhI as well as the gradient copolymers with S were further investigated via the synthesis of copolymers with a targeted Mn of 40 kg mol-1. In a subsequent reaction step, the homopolymers were cyclized using trifluoromethyl sulfonic acid inducing fluorescent properties. The different microstructure and substitution pattern of the original polymers differ in both emission maximum and quantum yields.
1,3 二烯是活阴离子聚合的重要单体。然而,对苯基取代二烯单体结构的研究却很少。根据 DFT 计算和 13C NMR 光谱分析,预计 1-苯基异戊二烯(1PhI)和 4-苯基异戊二烯(4PhI)这两种单体在阴离子聚合中的反应活性存在差异。从威蒂希反应(包括优化的萃取程序)开始,二取代的 1,3-二烯产生了具有不同 1,3 嵌合率的聚合物。这些聚合物通过 1H NMR 光谱和不同的 SEC 条件进行了表征。分子量最高可达 48.8 kg mol-1,分散度较窄(Đ≤ 1.13)。加入改性剂 THF 后,乙烯基单位开始增加,4PhI 的聚合也失去了控制。进一步增加 THF 浓度会导致乙烯基单位异常减少,最终在纯 THF 中 1,4 单位的比例超过 80%。通过原位 1H NMR 动力学分别跟踪了与苯乙烯(S)和异戊二烯(I)的共聚情况。通过合成目标 Mn 为 40 kg mol-1 的共聚物,进一步研究了 I 和 1PhI 的理想无规共聚以及与 S 的梯度共聚。在随后的反应步骤中,使用三氟甲基磺酸对均聚物进行环化,从而诱发荧光特性。原始聚合物的微观结构和取代模式不同,其发射最大值和量子产率也不同。
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引用次数: 0
The α-Diimine-based Conjugated Microporous Polymers as Heterogeneous Ligand for highly Efficient Palladium-Catalyzed Direct C-H Arylation α-二胺基共轭微孔聚合物作为异质配体用于高效钯催化直接 C-H 芳基化反应
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-07-09 DOI: 10.1039/d4py00539b
Chang-An Wang, Ya-Ru Wang, Mia Guo, Bing Han, Kun Nie, Yinfeng Han, Feng-Shou Liu
Direct C-H bond transformation has long been regarded as the "holy Grail of chemistry" in the field of organic synthesis. Significant progress in this area has been achieved with a variety of homogeneous transition-metal catalysts. However, few examples of heterogeneous catalysis of direct C-H bond transformation have been reported. In this work, we report a new type of α-diimine structure functionalized conjugated microporous polymers (DIM-CMP) used as ligand for heterogeneous catalysis, which shows high efficiency and recyclability for the Pd-catalyzed direct C-H arylation. These DIM-CMPs are distinguished by their exceptional stability, robust porous framework, and efficacious allocation of palladium active sites, all of which cumulatively contribute to their superior catalytic performance. The superior utility of DIM-Pd-CMP in catalysis was elucidated by the broad substrate scopes (32 examples, 82-98% yields), along with the tolerance of a variety of functional groups, good recyclability (6 times) and proven on a gram scale (10 mmol). Moreover, its utility has been highlighted in the synthesis of potentially bioactive molecule through sequential C-H arylation and Suzuki coupling. This innovative development is poised to significantly impact the synthesis of heterobiaryls, crucial constituents in a variety of natural products and pharmaceutical compounds, potentially revolutionizing catalysis in industrial applications and offering significant economic and environmental advantages.
长期以来,直接 C-H 键转化一直被视为有机合成领域的 "化学圣杯"。利用各种均相过渡金属催化剂在这一领域取得了重大进展。然而,有关 C-H 键直接转化的异相催化实例却鲜有报道。在这项工作中,我们报告了一种新型的 α-二亚胺结构官能化共轭微孔聚合物(DIM-CMP),这种聚合物用作异相催化的配体,在 Pd 催化的直接 C-H 芳基化反应中表现出高效率和可回收性。这些 DIM-CMP 具有优异的稳定性、坚固的多孔框架和有效的钯活性位点分配,所有这些都有助于提高它们的催化性能。DIM-Pd-CMP 在催化方面的优越性体现在其广泛的底物范围(32 个实例,82-98% 的产率)、对多种官能团的耐受性、良好的可回收性(6 次)以及经证实的克级规模(10 毫摩尔)。此外,它在通过顺序 C-H 芳基化和铃木偶联合成潜在生物活性分子方面的作用也得到了强调。这一创新发展将对杂环丁烷的合成产生重大影响,而杂环丁烷是多种天然产品和医药化合物的重要成分,有可能彻底改变工业应用中的催化反应,并带来显著的经济和环境优势。
{"title":"The α-Diimine-based Conjugated Microporous Polymers as Heterogeneous Ligand for highly Efficient Palladium-Catalyzed Direct C-H Arylation","authors":"Chang-An Wang, Ya-Ru Wang, Mia Guo, Bing Han, Kun Nie, Yinfeng Han, Feng-Shou Liu","doi":"10.1039/d4py00539b","DOIUrl":"https://doi.org/10.1039/d4py00539b","url":null,"abstract":"Direct C-H bond transformation has long been regarded as the \"holy Grail of chemistry\" in the field of organic synthesis. Significant progress in this area has been achieved with a variety of homogeneous transition-metal catalysts. However, few examples of heterogeneous catalysis of direct C-H bond transformation have been reported. In this work, we report a new type of α-diimine structure functionalized conjugated microporous polymers (DIM-CMP) used as ligand for heterogeneous catalysis, which shows high efficiency and recyclability for the Pd-catalyzed direct C-H arylation. These DIM-CMPs are distinguished by their exceptional stability, robust porous framework, and efficacious allocation of palladium active sites, all of which cumulatively contribute to their superior catalytic performance. The superior utility of DIM-Pd-CMP in catalysis was elucidated by the broad substrate scopes (32 examples, 82-98% yields), along with the tolerance of a variety of functional groups, good recyclability (6 times) and proven on a gram scale (10 mmol). Moreover, its utility has been highlighted in the synthesis of potentially bioactive molecule through sequential C-H arylation and Suzuki coupling. This innovative development is poised to significantly impact the synthesis of heterobiaryls, crucial constituents in a variety of natural products and pharmaceutical compounds, potentially revolutionizing catalysis in industrial applications and offering significant economic and environmental advantages.","PeriodicalId":100,"journal":{"name":"Polymer Chemistry","volume":null,"pages":null},"PeriodicalIF":4.6,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141561203","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Patchy Stereocomplex Micelles as Efficient Compatibilizers for Polymer Blends 作为聚合物混合物高效相容剂的斑状立体络合胶束
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-07-09 DOI: 10.1039/d4py00449c
Roman Schaller, Marius Schmidt, Kristian Schweimer, Holger Schmalz
Surface-compartmentalized polymer micelles (Janus and patchy micelles) have gained increasing attention as their unique properties open the way for various applications. While Janus micelles have been extensively studied, e.g. as compatibilizers in polymer blends, there are hardly any reports on the use of patchy micelles. In this study, we show that spherical micelles with a polylactide stereocomplex (SC) core and a patch-like microphase separated polystyrene/poly(tert-butyl methacrylate) (PS/PtBMA) corona are efficient compatibilizers for highly immiscible PS/PtBMA blends. The patchy SC micelles, prepared by stereocomplex-driven self-assembly (SCDSA) of enantiomeric diblock copolymers, improved the homogeneity of the blends and led to a significant reduction of the PS droplet size. We further employed SCDSA to selectively incorporate a fluorescent dye inside the SC micelle core without changing the shape or chemistry of the patchy corona. This allows the use of confocal scanning fluorescence microscopy to localize the patchy SC micelles, being predominantly assembled at the PS/PtBMA blend interface. Interestingly, the reduction in PS droplet size was comparable for blends compatibilized with patchy SC micelles and Janus micelles, but only for patchy SC micelles a monomodal droplet size distribution could be achieved. The outstanding interfacial activity of the patchy SC micelles can be attributed to their adaptive corona structure, resulting in a selective swelling/collapse of the respective miscible/immiscible corona patches at the blend inter¬face.
表面分隔的聚合物胶束(简纳斯胶束和斑块状胶束)因其独特的性质为各种应用开辟了道路,因而受到越来越多的关注。人们对 Janus 胶束进行了广泛的研究,例如将其用作聚合物混合物的相容剂,但几乎没有关于斑块状胶束用途的报道。在这项研究中,我们发现以聚乳酸立体络合物(SC)为核心、聚苯乙烯/聚甲基丙烯酸叔丁酯(PS/PtBMA)为副边的球形胶束是高度不相溶的 PS/PtBMA 混合物的高效相容剂。通过对映体二嵌段共聚物的立体共聚物驱动自组装(SCDSA)制备的斑块状 SC 胶束改善了共混物的均匀性,并显著减小了 PS 液滴的尺寸。我们进一步利用 SCDSA 将荧光染料选择性地加入 SC 胶束核心,而不改变斑状电晕的形状或化学性质。这样就可以使用共焦扫描荧光显微镜来定位主要聚集在 PS/PtBMA 混合界面上的斑块状 SC 胶束。有趣的是,与斑块状 SC 胶束和 Janus 胶束相容的共混物的 PS 液滴尺寸减小程度相当,但只有斑块状 SC 胶束才能实现单模态液滴尺寸分布。斑块状 SC 胶束出色的界面活性可归因于其自适应性的电晕结构,这种结构可使混溶/不混溶电晕斑块在混合界面上有选择地膨胀/塌陷。
{"title":"Patchy Stereocomplex Micelles as Efficient Compatibilizers for Polymer Blends","authors":"Roman Schaller, Marius Schmidt, Kristian Schweimer, Holger Schmalz","doi":"10.1039/d4py00449c","DOIUrl":"https://doi.org/10.1039/d4py00449c","url":null,"abstract":"Surface-compartmentalized polymer micelles (Janus and patchy micelles) have gained increasing attention as their unique properties open the way for various applications. While Janus micelles have been extensively studied, e.g. as compatibilizers in polymer blends, there are hardly any reports on the use of patchy micelles. In this study, we show that spherical micelles with a polylactide stereocomplex (SC) core and a patch-like microphase separated polystyrene/poly(<em>tert</em>-butyl methacrylate) (PS/P<em>t</em>BMA) corona are efficient compatibilizers for highly immiscible PS/P<em>t</em>BMA blends. The patchy SC micelles, prepared by stereocomplex-driven self-assembly (SCDSA) of enantiomeric diblock copolymers, improved the homogeneity of the blends and led to a significant reduction of the PS droplet size. We further employed SCDSA to selectively incorporate a fluorescent dye inside the SC micelle core without changing the shape or chemistry of the patchy corona. This allows the use of confocal scanning fluorescence microscopy to localize the patchy SC micelles, being predominantly assembled at the PS/P<em>t</em>BMA blend interface. Interestingly, the reduction in PS droplet size was comparable for blends compatibilized with patchy SC micelles and Janus micelles, but only for patchy SC micelles a monomodal droplet size distribution could be achieved. The outstanding interfacial activity of the patchy SC micelles can be attributed to their adaptive corona structure, resulting in a selective swelling/collapse of the respective miscible/immiscible corona patches at the blend inter¬face.","PeriodicalId":100,"journal":{"name":"Polymer Chemistry","volume":null,"pages":null},"PeriodicalIF":4.6,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141566083","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
3D printing hydrogel network regulation based on macroinitiator induced rapid photoATRP 基于大引发剂诱导快速光引发剂的三维打印水凝胶网络调控
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-07-09 DOI: 10.1039/d4py00365a
Menghan Si, Mengjie Zhou, Wenjie Zhang, Ge Shi, Yanjie He, Xiaoguang Qiao, Weihua Fan, Xinchang Pang
Although 3D printing can easily control the macroscopic structure of printed subjects based on the digital modeling, the control of micro-structure of polymer network was still a challenge. Herein, we report the using of macroinitiator induced rapid photoATRP to regulate the 3D printed hydrogel network. This approach consists of synthesizing of macroinitiator through CDs catalyzed photoATRP, and photocuring in the same pot by subsequent adding of crosslinker. By varying the chain length of the macroinitiator, we demonstrated the effect of physical entanglements of on the formation of hydrogel, as well as the mechanical property and swelling ratio. All the 3D printing objects with different macroinitiators exhibited outstanding print resolution. With PNIPAM macroinitiator, the printed hydrogel shows the characteristics of temperature-sensitive response. Overall, the findings of this work enable an interesting platform for control the mechanical property and functional of 3D printing hydrogel.
虽然基于数字建模,3D 打印可以轻松控制打印对象的宏观结构,但聚合物网络微观结构的控制仍是一个挑战。在此,我们报告了利用大引发剂诱导快速光ATPRP来调控3D打印水凝胶网络的方法。这种方法包括通过 CDs 催化光固化反应合成大引发剂,然后在同一锅中加入交联剂进行光固化。通过改变大引发剂的链长,我们证明了物理缠结对水凝胶形成的影响,以及对机械性能和膨胀率的影响。所有使用不同大引发剂的三维打印对象都表现出了出色的打印分辨率。使用 PNIPAM 大引发剂打印出的水凝胶具有温度敏感响应的特点。总之,这项研究成果为控制三维打印水凝胶的机械性能和功能提供了一个有趣的平台。
{"title":"3D printing hydrogel network regulation based on macroinitiator induced rapid photoATRP","authors":"Menghan Si, Mengjie Zhou, Wenjie Zhang, Ge Shi, Yanjie He, Xiaoguang Qiao, Weihua Fan, Xinchang Pang","doi":"10.1039/d4py00365a","DOIUrl":"https://doi.org/10.1039/d4py00365a","url":null,"abstract":"Although 3D printing can easily control the macroscopic structure of printed subjects based on the digital modeling, the control of micro-structure of polymer network was still a challenge. Herein, we report the using of macroinitiator induced rapid photoATRP to regulate the 3D printed hydrogel network. This approach consists of synthesizing of macroinitiator through CDs catalyzed photoATRP, and photocuring in the same pot by subsequent adding of crosslinker. By varying the chain length of the macroinitiator, we demonstrated the effect of physical entanglements of on the formation of hydrogel, as well as the mechanical property and swelling ratio. All the 3D printing objects with different macroinitiators exhibited outstanding print resolution. With PNIPAM macroinitiator, the printed hydrogel shows the characteristics of temperature-sensitive response. Overall, the findings of this work enable an interesting platform for control the mechanical property and functional of 3D printing hydrogel.","PeriodicalId":100,"journal":{"name":"Polymer Chemistry","volume":null,"pages":null},"PeriodicalIF":4.6,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141561493","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Aggregation-induced emission polydithioacetal with pendant tetraphenylethtlene groups for Hg2+ detection and removal 用于检测和去除 Hg2+ 的带有四苯乙烯基团的聚合诱导发射聚二硫乙缩醛
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-07-09 DOI: 10.1039/d4py00226a
Yu Gu, Jianjian Zhu, Xingyu Yuan, Siyong Li, Zhongxiang Zhao, Yanbing Lu
The development of responsive polymers with the ability to detect and quantitatively separate toxic ions is a challenge for chemical research. Combined with the excellent fluorescence performance of aggregation-induced emission (AIE) tetraphenylethtlene (TPE) in aggregation state and the high selectivity of dithioacetal groups to Hg2+, a versatile one-pot polycondensation strategy was utalized to construct amphiphilic AIE polydithioacetal PTA-TPE containing dithioacetal units in the main chain for the detection and removal of Hg2+ in aqueous solutions. PTA-TPE showed high selectivity and sensitivity to Hg2+ with a detection limit of 10.81 nM in aqueous PBS buffer (pH 7.4). Moreover, PTA-TPE removed Hg2+ from aqueous 1.0 ppm Hg2+ solution with removal rates over 80.0 % in both acidic and alkaline media. The maximum adsorption at low concentration Hg2+ was 124.3 mg/g. Therefore, this amphiphilic fluorescence polymer can not only be applied to detect Hg2+, but also to separate and remove mercury from water environments.
开发具有检测和定量分离有毒离子能力的响应性聚合物是化学研究中的一项挑战。结合聚合诱导发射(AIE)四苯乙烯(TPE)在聚合态下的优异荧光性能和二硫代乙醛基团对 Hg2+ 的高选择性,利用多功能一锅缩聚策略,构建了主链中含有二硫代乙醛单元的两亲 AIE 聚二硫乙醛 PTA-TPE,用于检测和去除水溶液中的 Hg2+。PTA-TPE 对 Hg2+ 具有很高的选择性和灵敏度,在水性 PBS 缓冲液(pH 值为 7.4)中的检测限为 10.81 nM。此外,PTA-TPE 还能去除 1.0 ppm Hg2+ 水溶液中的 Hg2+,在酸性和碱性介质中的去除率均超过 80.0%。低浓度 Hg2+ 的最大吸附量为 124.3 毫克/克。因此,这种两亲性荧光聚合物不仅可用于检测 Hg2+,还可用于分离和去除水环境中的汞。
{"title":"Aggregation-induced emission polydithioacetal with pendant tetraphenylethtlene groups for Hg2+ detection and removal","authors":"Yu Gu, Jianjian Zhu, Xingyu Yuan, Siyong Li, Zhongxiang Zhao, Yanbing Lu","doi":"10.1039/d4py00226a","DOIUrl":"https://doi.org/10.1039/d4py00226a","url":null,"abstract":"The development of responsive polymers with the ability to detect and quantitatively separate toxic ions is a challenge for chemical research. Combined with the excellent fluorescence performance of aggregation-induced emission (AIE) tetraphenylethtlene (TPE) in aggregation state and the high selectivity of dithioacetal groups to Hg2+, a versatile one-pot polycondensation strategy was utalized to construct amphiphilic AIE polydithioacetal PTA-TPE containing dithioacetal units in the main chain for the detection and removal of Hg2+ in aqueous solutions. PTA-TPE showed high selectivity and sensitivity to Hg2+ with a detection limit of 10.81 nM in aqueous PBS buffer (pH 7.4). Moreover, PTA-TPE removed Hg2+ from aqueous 1.0 ppm Hg2+ solution with removal rates over 80.0 % in both acidic and alkaline media. The maximum adsorption at low concentration Hg2+ was 124.3 mg/g. Therefore, this amphiphilic fluorescence polymer can not only be applied to detect Hg2+, but also to separate and remove mercury from water environments.","PeriodicalId":100,"journal":{"name":"Polymer Chemistry","volume":null,"pages":null},"PeriodicalIF":4.6,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141561494","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Stereoregular polymerization of phenylacetylene by alkynyl and methyl rhodium(I) complexes with functionalized phosphine ligands: linear vs branched poly(phenylacetylene)s 带有功能化膦配体的炔基和甲基铑(I)络合物对苯乙炔的立体聚合:线性与支化聚苯乙炔
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2024-07-08 DOI: 10.1039/d4py00497c
Marta Angoy, M. Victoria Jiménez, Eugenio Vispe, Stepan Podzimek, Jesús J. Pérez-Torrente
The alkynyl [Rh(C≡C-Ph)(nbd){Ph2P(CH2)3Z}2] and [Rh(C≡C-Ph)(cod){Ph2P(CH2)3Z}] (cod = 1,5-cycloctadiene, nbd = 2,5-norbornadiene) and methyl complexes [Rh(CH3)(cod){Ph2P(CH2)3Z}] featuring functionalized phosphine ligands (Z = NMe2, OEt) have been prepared. These complexes efficiently catalyze the polymerization of phenylacetylene in the absence of base to afford stereoregular poly(phenylacetylene)s of high molar mass. Polymer characterization by SEC-MALS and A4F-MALS revealed a bimodal molar mass distribution due to the presence of a high molar mass polymer fraction. The diene ligand in the alkynyl complexes influences the morphology of the polymers. The poly(phenylacetylene)s prepared with the square-planar alkynyl complexes [Rh(C≡C-Ph)(cod){Ph2P(CH2)3Z}] having cod as diene are linear, whereas that catalysts [Rh(C≡C-Ph)(nbd){Ph2P(CH2)3Z}2] with nbd as diene afford PPAs with a fraction of high molar mass branched polymer. However, neither the catalytic performance nor the PPA morphology is affected by the donor function of the functionalized phosphine ligand (-NMe2 or -OEt). The alkynyl complexes having nbd as the diene ligand, [Rh(C≡C-Ph)(nbd){Ph2P(CH2)3Z}2], are much more active than the square-planar alkynyl and methyl complexes having cod as diene. These catalysts polymerize phenylacetylene at faster rate than catalyst [Rh(C≡C-Ph)(nbd)(PPh3)2] bearing a non-functionalized phosphine ligand and afford polymers of much higher molecular weight.
炔基[Rh(C≡C-Ph)(nbd){Ph2P(CH2)3Z}2]和[Rh(C≡C-Ph)(cod){Ph2P(CH2)3Z}](cod = 1,5-环辛二烯,nbd = 2、5-降冰片二烯)和以功能化膦配体(Z = NMe2、OEt)为特征的甲基配合物 [Rh(CH3)(cod){Ph2P(CH2)3Z}]。这些配合物在无碱条件下能有效催化苯乙炔的聚合反应,生成高摩尔质量的立体配位聚苯乙炔。通过 SEC-MALS 和 A4F-MALS 进行的聚合物表征显示,由于存在高摩尔质量的聚合物部分,聚合物的摩尔质量呈双峰分布。炔基配合物中的二烯配体会影响聚合物的形态。使用以 cod 为二烯的方形平面炔基配合物 [Rh(C≡C-Ph)(cod){Ph2P(CH2)3Z}] 制备的聚苯乙炔是线性的,而使用以 nbd 为二烯的催化剂 [Rh(C≡C-Ph)(nbd){Ph2P(CH2)3Z}2] 制备的聚苯乙炔则含有一部分高摩尔质量的支化聚合物。然而,催化性能和 PPA 形态均不受官能化膦配体的供体功能(-NMe2 或 -OEt)的影响。以 nbd 作为二烯配体的炔基配合物 [Rh(C≡C-Ph)(nbd){Ph2P(CH2)3Z}2],比以 cod 作为二烯的方形平面炔基和甲基配合物活性要高得多。与含有非官能化膦配体的催化剂[Rh(C≡C-Ph)(nbd)(PPh3)2]相比,这些催化剂聚合苯乙炔的速度更快,并能生成分子量高得多的聚合物。
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引用次数: 0
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Polymer Chemistry
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