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Preparation and Application of Poly(Arylamine Ketone) materials for Electrochromism and Lithium-ion Batteries
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-04-08 DOI: 10.1016/j.polymer.2025.128379
Huilin Shen, Qilin Wang, Yuntao Han, Shuo Yang, Yixuan Liu, Zheng Chen, Zhenhua Jiang
The investigation of electrochemical materials with multiple functions is steadily growing. By joining ketone groups to triphenylamine structures via a two-step C-N coupling procedure, PAEK-CzTPAs multiple function copolymers were prepared and used in the electrochromic and battery fields. When the PAK-CzTPA polymer is applied to the electrochromic field, the transmission change has a small attenuation even after 600 s. PAK-CzTPA polymer as cathode active material with a theoretical specific capacity of 122.9 mAh/g, PAK-CzTPA cathode capacity is about 90.0 mAh/g after 50 cycles with 87.9% capacity retention at 0.2 C current density. 6F-PAEK-CzTPA20 cathode reach 164.0 mAh/g at 0.1 C current density after 50 cycles with 85.0% coulombic efficiency that itself as binder is applied to ternary (NCM811) electrode. Materials with the ability to store energy, exhibit electrochromic characteristics and perform other physical tasks of materials with a wide range of potential uses that could increase energy efficiency, save an important quantity of resources and make the system more sustainable overall.
对具有多种功能的电化学材料的研究正在稳步发展。通过两步 C-N 偶联程序将酮基连接到三苯胺结构上,制备出 PAEK-CzTPAs 多种功能共聚物,并将其应用于电致变色和电池领域。PAK-CzTPA 聚合物作为阴极活性材料,理论比容量为 122.9 mAh/g,在 0.2 C 电流密度下,PAK-CzTPA 阴极容量在 50 个循环后约为 90.0 mAh/g,容量保持率为 87.9%。6F-PAEK-CzTPA20 阴极在 0.1 C 电流密度下循环 50 次后达到 164.0 mAh/g,库仑效率为 85.0%,其本身作为粘合剂应用于三元(NCM811)电极。具有储能、电致变色特性和执行其他物理任务能力的材料具有广泛的潜在用途,可提高能源效率,节约大量资源,并使系统在整体上更具可持续性。
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引用次数: 0
Diffusion-Limited Free Radical Mechanisms in Peroxide-Initiated Crosslinking of Low-Density Polyethylene
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-04-08 DOI: 10.1016/j.polymer.2025.128376
Kai Shang, Jiacai Li, Yifan Wu, Shihang Wang, Yang Feng, Shengtao Li
There have been many attempts to describe the kinetics of the peroxide-initiated crosslinking of low-density polyethylene (LDPE). However, these kinetic models have not comprehensively captured the free radical behavior during LDPE crosslinking. In this study, the evolution of the reduced reaction rate (Rr), derived from the mechanistic kinetic model, is employed to gain detailed insight into free radical behaviors in LDPE during crosslinking. The curve of Rr over time, which follows a bell shape, demonstrates that the complexity of the crosslinking chemistry incorporates diffusional limitation, leading to ineffective free radical terminations. When combined with structural characterization of functional trans-vinylene groups and hydroxyl groups of antioxidants, our analysis highlights a diffusion-limited mechanism associated with a continuous decrease in the effective consumption of peroxide and a sequential increase in radical scavenging. These observations are a result of the intramolecular disproportionation induced by the cage effect in peroxides and the unimolecular termination of LDPE radicals by antioxidants during network formation, respectively. Consequently, a refined kinetic model is proposed, which accounts for the effect of diffusional limitation on free radical terminations, thereby providing an accurate description of the LDPE crosslinking process. This comprehensive understanding of free radical crosslinking mechanisms in LDPE will facilitate the precise control and optimization of the properties of this reaction.
人们曾多次尝试描述过氧化物引发的低密度聚乙烯(LDPE)交联动力学。然而,这些动力学模型并没有全面捕捉到低密度聚乙烯交联过程中的自由基行为。在本研究中,利用机械动力学模型推导出的还原反应速率(Rr)的演变来详细了解交联过程中低密度聚乙烯中的自由基行为。Rr 随时间变化的曲线呈钟形,表明交联化学的复杂性包含了扩散限制,从而导致自由基的无效终止。结合功能性反乙烯基团和抗氧化剂羟基的结构特征,我们的分析强调了一种与过氧化物有效消耗量持续减少和自由基清除量依次增加有关的扩散限制机制。这些观察结果分别是由于过氧化物中的笼效应引起的分子内比例失调,以及网络形成过程中抗氧化剂对低密度聚乙烯自由基的单分子终止。因此,我们提出了一个完善的动力学模型,该模型考虑了自由基终止的扩散限制效应,从而准确地描述了 LDPE 的交联过程。对低密度聚乙烯中自由基交联机理的全面了解将有助于精确控制和优化该反应的特性。
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引用次数: 0
Itaconic acid: from monomer properties to radical homo-polymerization in water
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-04-07 DOI: 10.1016/j.polymer.2025.128365
Angela Giunta, Paul Bouyssoux, Frédéric Becquart, Jean-Charles Majesté, Fabien Dutertre
Itaconic acid (ITA) is a promising renewable chemical building block. Previous research on its radical homo-polymerization in aqueous media has shown slow kinetics, low conversion, and low molecular weight polymers. In this paper, we demonstrate the impact of the intrinsic properties of itaconic acid on its polymerization conditions. Specifically, the role of the degree of ionization (α) on its structure, solubility, and reactivity towards radical polymerization in water was investigated. The results indicate that the highest solubility in water occurs when itaconic acid is half-deprotonated. At a given concentration, the reaction rate and final molecular weight decrease as the degree of ionization increases, presumably due to electrostatic effects and hydrophobic/hydrophilic variations. Despite lower reactivity, full conversion can be achieved in a relatively short time with the half-deprotonated form of itaconic acid, because the polymerization can be achieved at higher monomer concentrations. These experimental findings are further supported by computational simulations of the monomer's structure and reactivity.
衣康酸(ITA)是一种前景广阔的可再生化学构件。以往对其在水介质中进行自由基均聚的研究表明,其动力学速度慢、转化率低、聚合物分子量低。在本文中,我们展示了衣康酸的内在特性对其聚合条件的影响。具体来说,我们研究了电离度 (α)对其结构、溶解度以及在水中进行自由基聚合反应的作用。结果表明,当衣康酸处于半去质子化状态时,其在水中的溶解度最高。在给定浓度下,反应速率和最终分子量随着电离程度的增加而降低,这可能是由于静电效应和疏水/亲水变化造成的。尽管半脱质子形式的衣康酸反应活性较低,但由于可以在较高的单体浓度下实现聚合,因此可以在相对较短的时间内实现完全转化。对单体结构和反应活性的计算模拟进一步证实了这些实验结果。
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引用次数: 0
Antimicrobial anticorrosive silicone resin coating with high adhesion and excellent mechanical properties 抗菌防腐硅树脂涂层,具有高附着力和优异的机械性能
IF 4.1 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-04-07 DOI: 10.1016/j.polymer.2025.128366
Lixin Sun , Dong Tian , Kaiming Zhang , Yahui Wu , Yanan Sun , Yujie Jiang , Chuanhui Gao , Lei Liu , Yuetao Liu
Silicone resin is increasingly recognized for its applications in anti-fouling and anti-corrosion coatings. However, its inherent limitations such as low strength, poor mechanical properties, and weak substrate adhesion, hinder its widespread application. This study introduces a novel antibacterial and anticorrosive silicone resin coating characterized by excellent mechanical properties, and strong adhesion. By modifying natural rosin with KH 560, we successfully synthesized a novel rosin modifier DAS and introduced it into methylphenylsilicone (MPSR) matrix through a hydrolysis-condensation method, producing antibacterial coatings with different DAS content (MPSR-x% DAS, x= 0, 3, 5, 7, 10). Especially the MPSR-7% DAS coating reached 98.9% against Staphylococcus aureus (S. aureus) and 94.5% against Escherichia coli (E. coli). In addition, in order to enhance the hardness and adhesion of the coating, a multifunctional siloxane crosslinker (MF-S) was introduced to form an MPSR-7% DAS-y coating. The MPSR-7%DAS-y (y= 2- 5) coating all achieved grade 1 adhesion, and the hardness of the MPSR-7%DAS-4 coating exceeded 6H. The higher crosslinking density of MF-S contributes to a denser coating and improves the long-term corrosion resistance of the coating. This study provides potential progress for the development of coatings with enhanced antifouling and anti-corrosion properties.
硅树脂在防污和防腐蚀涂料中的应用日益得到认可。然而,其固有的局限性,如强度低、机械性能差、基材附着力弱等,阻碍了它的广泛应用。本研究介绍了一种新型的抗菌防腐硅树脂涂料,具有优异的机械性能和较强的附着力。通过用 KH 560 对天然松香进行改性,我们成功合成了一种新型松香改性剂 DAS,并通过水解-缩合方法将其引入甲基苯基硅酮(MPSR)基体中,制备出不同 DAS 含量(MPSR-x% DAS,x= 0、3、5、7、10)的抗菌涂料。其中,MPSR-7% DAS 涂层对金黄色葡萄球菌(S. aureus)的抗菌率达到 98.9%,对大肠杆菌(E. coli)的抗菌率达到 94.5%。此外,为了增强涂层的硬度和附着力,还引入了一种多功能硅氧烷交联剂(MF-S),以形成 MPSR-7% DAS-y 涂层。MPSR-7%DAS-y(y= 2-5)涂层的附着力都达到了 1 级,MPSR-7%DAS-4 涂层的硬度超过了 6H。MF-S 较高的交联密度使涂层更致密,并提高了涂层的长期耐腐蚀性。这项研究为开发具有更强防污和防腐蚀性能的涂层提供了潜在的进展。
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引用次数: 0
A Comprehensive Review of Polyurethane: Properties, Applications and Future Perspectives
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-04-07 DOI: 10.1016/j.polymer.2025.128361
Shuang Wu, Shaoping Ma, Qinghua Zhang, Chao Yang
Polyurethane (PU), an important polymeric material, has been widely utilized in numerous fields since its initial synthesis in 1937, owning to its distinctive molecular structure and excellent properties. In order to better understand the properties of polyurethane products, various polyurethane materials, including polyurethane foams, elastomers, coatings, adhesives and functional polyurethanes are comprehensively reviewed, in terms of their structural characteristics, preparation procedures, performance attributes, application status and associated challenges. Furthermore, the future development direction of polyurethane is also discussed.
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引用次数: 0
Synthesis of Biobased Polyamides for Hot Melt Adhesives: Utilizing Renewable Dimer Acids and 1,5-Pentanediamine Monomers 热熔胶用生物基聚酰胺的合成:利用可再生二聚酸和 1,5-戊二胺单体
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-04-07 DOI: 10.1016/j.polymer.2025.128368
Guoquan Chen, Yan Chen, Jingqi Gong, Jiangyu Zhu, Yaxiong Tian, Yuanli Liu
Biobased polyamides (BPAs) are increasingly attractive alternatives to conventional petroleum-derived polymers, owing to their bio-renewable and environmentally friendly. Nonetheless, their practical applications are severely restricted by excessive prices, limited scalability, and poor mechanical-thermal properties. Herein, a series of copolyamides (COPAs) were successfully synthesized by the one-pot polycondensation using sebacic acid-1,10-decane-diamine salt, biobased dimer acid, and biobased 1,5-pentanediamine monomers as raw materials. The thermal analysis revealed that the COPAs exhibited high thermal stability and suitable melting points with a Tm of 71 ∼152 °C. The processing properties and strong tensile strength were enhanced up to 24 MPa. Thus, as hot melt adhesives, the COPA30 demonstrated an adhesion strength of 8.28 MPa, making them suitable for various substrates such as aluminum, wood and iron. Notably, the COPA50 only slightly swelled after being immersed in organic solutions at room temperature for 30 days, which exhibited a remarkable chemical resistance. This study presents a viable approach for developing BPA as hot melt adhesives with desirable performance, which future foster applications in a range of areas.
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引用次数: 0
Upgrading of cotton fabrics by ionic liquid dissolving joint with wet spinning for stretchable and weaveable fiber-based strain sensors
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-04-05 DOI: 10.1016/j.polymer.2025.128344
Wentong Zhang, Hengyi Cheng, Tao Zhang, Dan Yu, Wei Wang
With the advent of an aging society, researchers are highly interested in the development of wearable strain sensors because of its promising futures in motion detection, artificial intelligence, and healthcare. Nevertheless, its practical uses are still severely limited by its unpleasant design, low sensitivity, and poor wear comfort. In this paper, we propose to use green solvent of ionic liquid to dissolve and reuse cellulose from cotton fabrics, and by the above method cellulose/ionic liquid solution (CILS) is successfully prepared, followed with the addition of thermoplastic urethane (TPU) to improve mechanical properties and carbon nanotubes (CNTs) to provide conductivity through wet spinning technology. The fiber-based strain sensor (ILCCD-4) prepared by the wet spinning has high sensitivity (487), large tensile properties (385%), low detection limit (2%), excellent durability (3200 tensile cycles), and fast response time (200 ms). Based on these excellent sensing properties, the strain sensor can detect motion signals from various parts of the human body. The results show that the fiber-based strain sensor has excellent sensitivity, and sensing performance, proving it can be used for smart textiles, wearable strain sensors, and flexible strain sensors.
随着老龄化社会的到来,可穿戴式应变传感器在运动检测、人工智能和医疗保健领域的发展前景广阔,因此研究人员对可穿戴式应变传感器的开发产生了浓厚的兴趣。然而,由于设计不美观、灵敏度低、佩戴舒适度差等原因,其实际用途仍然受到严重限制。本文提出使用绿色溶剂离子液体来溶解和再利用棉织物中的纤维素,并通过上述方法成功制备出纤维素/离子液体溶液(CILS),随后通过湿法纺丝技术添加热塑性聚氨酯(TPU)来改善机械性能,并添加碳纳米管(CNT)来提供导电性。湿法纺丝制备的纤维应变传感器(ILCCD-4)具有灵敏度高(487)、拉伸性能大(385%)、检测限低(2%)、耐用性好(3200 次拉伸循环)和响应时间快(200 毫秒)等特点。基于这些出色的传感特性,应变传感器可以检测到来自人体各个部位的运动信号。研究结果表明,纤维应变传感器具有出色的灵敏度和传感性能,可用于智能纺织品、可穿戴应变传感器和柔性应变传感器。
{"title":"Upgrading of cotton fabrics by ionic liquid dissolving joint with wet spinning for stretchable and weaveable fiber-based strain sensors","authors":"Wentong Zhang, Hengyi Cheng, Tao Zhang, Dan Yu, Wei Wang","doi":"10.1016/j.polymer.2025.128344","DOIUrl":"https://doi.org/10.1016/j.polymer.2025.128344","url":null,"abstract":"With the advent of an aging society, researchers are highly interested in the development of wearable strain sensors because of its promising futures in motion detection, artificial intelligence, and healthcare. Nevertheless, its practical uses are still severely limited by its unpleasant design, low sensitivity, and poor wear comfort. In this paper, we propose to use green solvent of ionic liquid to dissolve and reuse cellulose from cotton fabrics, and by the above method cellulose/ionic liquid solution (CILS) is successfully prepared, followed with the addition of thermoplastic urethane (TPU) to improve mechanical properties and carbon nanotubes (CNTs) to provide conductivity through wet spinning technology. The fiber-based strain sensor (ILCCD-4) prepared by the wet spinning has high sensitivity (487), large tensile properties (385%), low detection limit (2%), excellent durability (3200 tensile cycles), and fast response time (200 ms). Based on these excellent sensing properties, the strain sensor can detect motion signals from various parts of the human body. The results show that the fiber-based strain sensor has excellent sensitivity, and sensing performance, proving it can be used for smart textiles, wearable strain sensors, and flexible strain sensors.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"12 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782881","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
Machine Learning-Driven Constructing Relationship between Processing and Mechanical Properties of TPV: a view of one Stacking Model
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-04-05 DOI: 10.1016/j.polymer.2025.128359
Zhi Zhang, Lifeng Ma, Longhao Li, Chengyuan He, Chunxiao Li
Thermoplastic vulcanizate (TPV) exhibit excellent processability and mechanical properties, making them widely applicable in industrial fields. Their mechanical properties,including tensile strength, fracture toughness, and hardness, play a crucial role in determining their suitability for various applications. However, due to the numerous factors influencing the mechanical properties of TPV, the traditional trial-and-error experimental approach not only would consume significant resources but also fail to provide a comprehensive and quantitative understanding of the relationship between the processing parameters and its mechanical performance. To address this challenge, this study has developed one novel stacking model to achieve one high-precision prediction for tensile strength, elongation at break, and Shore hardness for TPV, thereby accelerating the experimental and development process of TPV. Additionally, SHapley Additive exPlanations (SHAP) feature analysis has been employed to interpret the black-box characteristics of the stacking model, revealing how different features influence the overall mechanical performance of TPV. Finally, bivariate dependence plots have been generated to establish the specific mechanisms governing the relationship between TPV processing parameters and mechanical properties. This study would provide an effective approach for guiding TPV experimentation while offering a more efficient method for optimizing TPV performance.
{"title":"Machine Learning-Driven Constructing Relationship between Processing and Mechanical Properties of TPV: a view of one Stacking Model","authors":"Zhi Zhang, Lifeng Ma, Longhao Li, Chengyuan He, Chunxiao Li","doi":"10.1016/j.polymer.2025.128359","DOIUrl":"https://doi.org/10.1016/j.polymer.2025.128359","url":null,"abstract":"Thermoplastic vulcanizate (TPV) exhibit excellent processability and mechanical properties, making them widely applicable in industrial fields. Their mechanical properties,including tensile strength, fracture toughness, and hardness, play a crucial role in determining their suitability for various applications. However, due to the numerous factors influencing the mechanical properties of TPV, the traditional trial-and-error experimental approach not only would consume significant resources but also fail to provide a comprehensive and quantitative understanding of the relationship between the processing parameters and its mechanical performance. To address this challenge, this study has developed one novel stacking model to achieve one high-precision prediction for tensile strength, elongation at break, and Shore hardness for TPV, thereby accelerating the experimental and development process of TPV. Additionally, SHapley Additive exPlanations (SHAP) feature analysis has been employed to interpret the black-box characteristics of the stacking model, revealing how different features influence the overall mechanical performance of TPV. Finally, bivariate dependence plots have been generated to establish the specific mechanisms governing the relationship between TPV processing parameters and mechanical properties. This study would provide an effective approach for guiding TPV experimentation while offering a more efficient method for optimizing TPV performance.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"20 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782880","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
Enhancement of the thermal conductivity and mechanical properties of low-k epoxy resin by UIO-66@CNT nanocomposites
IF 4.1 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-04-05 DOI: 10.1016/j.polymer.2025.128362
Ruihong Ning , Yuyu Zhao , Mengyuan Xie , Hao Chen , Haiping Xu , Jingrong Wang , Dandan Yang
Epoxy resin (EP) is commonly used to reduce the dielectric constant and dielectric loss by incorporating appropriate fillers, addressing issues such as slow signal transmission and signal delay in smart terminals employed in ultra-large-scale integrated (ULSI) circuits under harsh operating conditions. Ensuring excellent mechanical properties and thermal conductivity is also essential to extending the service life of these components. In this work, the effects of carbon nanotubes (CNTs) modified through the in-situ growth of the two-dimensional hybrid material UIO-66 on the epoxy resin matrix (UCNT/EP) in terms of thermal, mechanical, and dielectric properties were investigated. The results indicated that the dielectric constant of the 1.0 wt% UCNT/EP composite decreased by 4.9 % at 102 Hz compared with the original matrix, while the dielectric loss remained below 0.025 in the frequency range of 102–107 Hz. At a filler content of 2.0 wt%, the bending strength and flexural modulus of the composite reached 142.7 MPa and 3356.1 MPa, respectively. Additionally, the thermal conductivity of the composites exhibited a substantial increase of 226 %, and the char formation rate was improved at 700 °C.
{"title":"Enhancement of the thermal conductivity and mechanical properties of low-k epoxy resin by UIO-66@CNT nanocomposites","authors":"Ruihong Ning ,&nbsp;Yuyu Zhao ,&nbsp;Mengyuan Xie ,&nbsp;Hao Chen ,&nbsp;Haiping Xu ,&nbsp;Jingrong Wang ,&nbsp;Dandan Yang","doi":"10.1016/j.polymer.2025.128362","DOIUrl":"10.1016/j.polymer.2025.128362","url":null,"abstract":"<div><div>Epoxy resin (EP) is commonly used to reduce the dielectric constant and dielectric loss by incorporating appropriate fillers, addressing issues such as slow signal transmission and signal delay in smart terminals employed in ultra-large-scale integrated (ULSI) circuits under harsh operating conditions. Ensuring excellent mechanical properties and thermal conductivity is also essential to extending the service life of these components. In this work, the effects of carbon nanotubes (CNTs) modified through the in-situ growth of the two-dimensional hybrid material UIO-66 on the epoxy resin matrix (UCNT/EP) in terms of thermal, mechanical, and dielectric properties were investigated. The results indicated that the dielectric constant of the 1.0 wt% UCNT/EP composite decreased by 4.9 % at 10<sup>2</sup> Hz compared with the original matrix, while the dielectric loss remained below 0.025 in the frequency range of 10<sup>2</sup>–10<sup>7</sup> Hz. At a filler content of 2.0 wt%, the bending strength and flexural modulus of the composite reached 142.7 MPa and 3356.1 MPa, respectively. Additionally, the thermal conductivity of the composites exhibited a substantial increase of 226 %, and the char formation rate was improved at 700 °C.</div></div>","PeriodicalId":405,"journal":{"name":"Polymer","volume":"326 ","pages":"Article 128362"},"PeriodicalIF":4.1,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143784723","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
Inelastic and Quasielastic Neutron Scattering on Polynorbornenes with Bulky Carbocyclic Side groups.
IF 4.6 2区 化学 Q2 POLYMER SCIENCE Pub Date : 2025-04-05 DOI: 10.1016/j.polymer.2025.128358
Paulina Szymoniak, Mohamed A. Kolmangadi, Martin Böhning, Nicolas R. De Souza, Fanni Juranyi, Reiner Zorn, Andreas Schönhals
This study investigates the molecular mobility and vibrational properties of polynorbornenes with bulky carbocyclic side groups using inelastic and quasielastic neutron scattering techniques. The polymers, synthesized via metathesis and addition polymerization, exhibit varying degrees of microporosity, which significantly influences their gas separation performance. By inelastic neutron scattering experiments, it could be shown that all considered polymers have excess contributions to the low frequency vibrational density of states known as the Boson peak. The maximum frequency of the Boson peak correlates to the microporosity of the polymers. This correlation supports the sound wave interpretation of the Boson peak, suggesting that the microporous structure enhances the compressibility of the material at a microscopic length scale. The molecular mobility, particularly the methyl group rotations, was characterized using elastic scans and quasielastic neutron scattering. The study revealed a temperature-dependent relaxation process, with the onset of molecular fluctuations observed around 200 K for the polymer containing methyl groups. For the polymer having no methyl groups only elastic scattering is observed. The methyl group rotation was analyzed in terms of a jump diffusion in a threefold potential with three equivalent energy minima. This leads to an almost correct description of the q dependence of the elastic incoherent scattering function when the number of hydrogen nuclei undergoing the methyl group rotation is considered. It was further evidenced that the fraction of methyl undergoing the methyl group rotation increases with increasing temperature.
{"title":"Inelastic and Quasielastic Neutron Scattering on Polynorbornenes with Bulky Carbocyclic Side groups.","authors":"Paulina Szymoniak, Mohamed A. Kolmangadi, Martin Böhning, Nicolas R. De Souza, Fanni Juranyi, Reiner Zorn, Andreas Schönhals","doi":"10.1016/j.polymer.2025.128358","DOIUrl":"https://doi.org/10.1016/j.polymer.2025.128358","url":null,"abstract":"This study investigates the molecular mobility and vibrational properties of polynorbornenes with bulky carbocyclic side groups using inelastic and quasielastic neutron scattering techniques. The polymers, synthesized via metathesis and addition polymerization, exhibit varying degrees of microporosity, which significantly influences their gas separation performance. By inelastic neutron scattering experiments, it could be shown that all considered polymers have excess contributions to the low frequency vibrational density of states known as the Boson peak. The maximum frequency of the Boson peak correlates to the microporosity of the polymers. This correlation supports the sound wave interpretation of the Boson peak, suggesting that the microporous structure enhances the compressibility of the material at a microscopic length scale. The molecular mobility, particularly the methyl group rotations, was characterized using elastic scans and quasielastic neutron scattering. The study revealed a temperature-dependent relaxation process, with the onset of molecular fluctuations observed around 200 K for the polymer containing methyl groups. For the polymer having no methyl groups only elastic scattering is observed. The methyl group rotation was analyzed in terms of a jump diffusion in a threefold potential with three equivalent energy minima. This leads to an almost correct description of the q dependence of the elastic incoherent scattering function when the number of hydrogen nuclei undergoing the methyl group rotation is considered. It was further evidenced that the fraction of methyl undergoing the methyl group rotation increases with increasing temperature.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"59 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782879","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
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Polymer
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