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Recycling of human teeth for piezoelectric energy harvesting 回收人类牙齿用于压电能量采集
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-13 DOI: 10.1016/j.giant.2024.100333
Yuanyuan Yin , Shuaijie Liu , Yuehui Wang , Sihan Yang , Min Ding , Xiaohui Xu , Wei Ji , Jinlin Song

In the human body, non-centrosymmetric biological structures exhibit piezoelectric effect across from microscopic biomolecular building blocks to macroscopic tissues and organs. However, the fabrication of piezoelectric devices from discarded natural tissues and organs has rarely been exploited for energy harvesting applications. Herein, the extracted human teeth were recycled as an active layer in a piezoelectric nanogenerator for power generation. Due to the piezoelectric effect of enamel and dentin, a human teeth-based sandwiched piezoelectric nanogenerator was fabricated, producing high and stable power outputs with an open-circuit voltage of approximately 0.9 V under an external force at 60 N. Furthermore, the high mechanical durability of the piezoelectric nanogenerator was also verified after 1600 pressing-and-releasing cycles without noticeable output degradation. Notably, for the first time, a light-emitting diode (LED) was illuminated by the human teeth-based piezoelectric device. This work exemplifies a sustainable strategy to recycle the extracted human teeth by fabricating a piezoelectric nanogenerator for energy harvesting, providing inspiration for converting waste into wealth toward green energy in bionanotechnology.

在人体中,从微观的生物分子构件到宏观的组织和器官,非中心对称的生物结构都表现出压电效应。然而,利用废弃的天然组织和器官制造压电器件用于能量收集应用的情况还很少见。在这里,拔出的人类牙齿被回收利用,作为压电纳米发电机的活性层用于发电。由于珐琅质和牙本质的压电效应,基于人类牙齿的夹层压电纳米发电机被制造出来,在 60 N 的外力作用下产生高且稳定的功率输出,开路电压约为 0.9 V。值得注意的是,基于人类牙齿的压电装置首次点亮了发光二极管(LED)。这项工作体现了一种可持续的策略,即通过制造用于能量收集的压电纳米发电机来回收利用拔出的人类牙齿,为仿生技术中的绿色能源提供了变废为宝的灵感。
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引用次数: 0
Unraveling the nanostructures and self-assembly behavior of perfluorosulfonic acid in water/ethanol solvent: Effect of EW and side-chain chemistry 揭示全氟磺酸在水/乙醇溶剂中的纳米结构和自组装行为:EW和侧链化学性质的影响
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-13 DOI: 10.1016/j.giant.2024.100332
Jingnan Song , Suyan Wang , Wutong Zhao , Bonan Hao , Ming Zhang , Yecheng Zou , Gang Wei , Jia Liu , Guangying Chen , Huan Ren , Xuefei Wu , Xuesong Jiang , Yongfeng Zhou , Feng Liu , Yongming Zhang

The perfluorosulfonic acid (PFSA) ionomers are key materials for proton exchange membranes (PEMs) and catalyst layers (CLs). Their morphology is profoundly influenced by the chain assembly behavior of PFSA in dispersions. Hence, we combine the characterization techniques of dynamic light scattering (DLS), small-angle X-ray scattering (SAXS), and cryo-transmission electron microscopy (Cryo-TEM) to study the nanostructures of PFSA dispersions, and provide a structure model for diverse PFSA ionomers in water/ethanol solvent. It is seen that PFSA ionomers self-assembly into a rod-like particle in dilute dispersion. As the concentration increases, the primary rod aggregates gradually assemble into a swollen- or Gaussian-network structure. Beyond this feature, we see that different PFSA ionomers show different nanostructures in dispersion. For the long-side-chain (LSC) PFSA ionomers, the 800-LSC PFSA tends to form monodisperse rod-like aggregates that is in a highly ordered arrangement with a rod diameter of 3.16 nm and a length of 28.72 nm. As the equivalent weight (EW) increases to 960, the poor solubility of the main chains in water/ethanol solvents leads to the “end-to-end” assemblies of the primary rod particles and dendritic secondary aggregates. The short-side-chain (SSC) PFSA ionomer that shares the same backbone with 960-LSC PFSA exhibit remarkable mono-dispersity and ordered arrangement of rod-like aggregates in water/ethanol solvents due to the strong electrostatic repulsion.

全氟磺酸(PFSA)离子聚合物是质子交换膜(PEM)和催化剂层(CL)的关键材料。它们的形态深受分散体中 PFSA 链组装行为的影响。因此,我们结合动态光散射(DLS)、小角 X 射线散射(SAXS)和低温透射电子显微镜(Cryo-TEM)等表征技术来研究 PFSA 分散体的纳米结构,并提供了水/乙醇溶剂中各种 PFSA 离子聚合物的结构模型。结果表明,PFSA 离子聚合物在稀释分散液中自组装成杆状颗粒。随着浓度的增加,初级棒状聚集体逐渐组装成膨胀或高斯网状结构。除了这一特征外,我们还发现不同的 PFSA 离子聚合物在分散过程中呈现出不同的纳米结构。对于长侧链(LSC)PFSA 离子聚合物,800-LSC PFSA 倾向于形成单分散棒状聚集体,这种聚集体呈高度有序排列,棒状直径为 3.16 纳米,长度为 28.72 纳米。当等效重量(EW)增加到 960 时,由于主链在水/乙醇溶剂中的溶解性较差,导致主杆状颗粒和树枝状次级聚集体 "端对端 "地组装在一起。与 960-LSC PFSA 具有相同主链的短侧链(SSC)PFSA 离子聚合物由于具有很强的静电排斥力,在水/乙醇溶剂中表现出显著的单分散性和杆状聚集体的有序排列。
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引用次数: 0
Organic photovoltaic materials with near-infrared II-region response 具有近红外 II 区响应的有机光伏材料
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-13 DOI: 10.1016/j.giant.2024.100334
Lei Li , Tengfei Li , Yuze Lin

Organic photovoltaic materials have been widely used in organic solar cells (OSCs) and organic photodetectors (OPDs) systems, owing to their numerous advantages such as low cost, light weight, high structural tunability, and ease of solution processing. Among these materials, near-infrared (NIR)-responsive materials, especially those with NIR II-region (1000–1700 nm) response, are crucial in the construction of tandem OSCs and semitransparent OSCs to achieve high power conversion efficiency and high light utilization efficiency, respectively. Meanwhile, OPDs with NIR II-region response show great application potential in industrial, military, and medical fields. In recent years, some progress has been made in the development of organic photovoltaic materials and devices with NIR II-region response. This review provides an overview of the design strategies for NIR organic photovoltaic materials, followed by a classification and summary of representative organic NIR II-region responsive materials and their performance in OSCs and OPDs. Lastly, we conclude with an outlook on the development of organic photovoltaic materials with NIR II-region response.

有机光伏材料具有成本低、重量轻、结构可调性高、易于溶液处理等诸多优点,已被广泛应用于有机太阳能电池(OSC)和有机光电探测器(OPD)系统中。在这些材料中,近红外(NIR)响应材料,尤其是具有近红外 II 区(1000-1700 nm)响应的材料,对于构建串联 OSC 和半透明 OSC 以实现高功率转换效率和高光利用效率至关重要。同时,具有近红外 II 区响应的 OPD 在工业、军事和医疗领域具有巨大的应用潜力。近年来,具有近红外 II 区响应的有机光伏材料和器件的开发取得了一些进展。本综述概述了近红外有机光伏材料的设计策略,随后对具有代表性的近红外 II 区响应有机材料及其在 OSC 和 OPD 中的性能进行了分类和总结。最后,我们对具有近红外 II 区响应的有机光伏材料的发展进行了展望。
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引用次数: 0
Surface-induced orientation of liquid crystal phases 表面诱导的液晶相定向
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-01 DOI: 10.1016/j.giant.2024.100324
Wantae Kim , Dae Seok Kim , Dong Ki Yoon

Liquid crystal (LC) phases have been used in various self-assembly technologies owing to their stimuli-responsive characteristics. Especially, orientation-controlled LC structures on and in surfaces are extensively studied in physics, chemistry, and materials science because they can be used in patterning applications beyond the conventional LC display. The key idea in recent development is to control the surface anchoring condition between the substrate and LC materials. Specifically, defects in the LC phases have been introduced as an effective lithographic tool for fabricating distinguished patterns. In this review, the bulk and surface-induced structures of LC materials are overviewed to show the relationship between the surface characteristics of the substrates and the elastic properties of LC materials. The two main themes are (1) orientation control, which can be achieved by micro- and nano-confinement using solid and fluid substrates, and (2) the application of LC materials as optoelectronics and sensors. Finally, the review discusses the defect structures of LC materials fabricated on flexible substrates and their possible applications.

液晶(LC)相因其刺激响应特性而被用于各种自组装技术。特别是表面上和表面中的取向控制液晶结构,在物理学、化学和材料科学领域得到了广泛的研究,因为它们可用于传统液晶显示之外的图案化应用。近期发展的关键思路是控制基底和低浓材料之间的表面锚定条件。具体来说,液相色谱相中的缺陷已被引入作为一种有效的光刻工具,用于制作杰出的图案。本综述概述了液相色谱材料的主体结构和表面诱导结构,以说明基底表面特性与液相色谱材料弹性特性之间的关系。两大主题是:(1) 取向控制,可通过使用固体和流体基底进行微米和纳米压制来实现;(2) 低浓材料在光电和传感器方面的应用。最后,综述讨论了在柔性基底上制造的液相色谱材料的缺陷结构及其可能的应用。
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引用次数: 0
Silica gel-supported Pd nanocatalyst: Efficient Mizoroki-Heck reactions and sustainable Ozagrel synthesis 硅胶支撑的钯纳米催化剂:高效的 Mizoroki-Heck 反应和可持续的 Ozagrel 合成
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-01 DOI: 10.1016/j.giant.2024.100326
Shaheen M. Sarkar , Md Lutfor Rahman

We developed a cost-effective silica gel-supported palladium nanocatalyst in a three-step reactions process. Initially, silica gel (60–120 mesh) underwent amino group functionalization using 3-aminopropyltriethoxysilane, leading to the formation of a Schiff base through a reaction with the 1,10-phenanthroline-2,9-dicarboxaldehyde ligand. Subsequently, palladium nanocatalyst was introduced to the silica matrix ligand in the presence of palladium salt and hydrazine hydrate, resulting in the formation of the silica gel-supported Schiff-base palladium nanocatalyst (Si@SBPdNPs 3). Successful functionalization of the silica matrix was confirmed using various spectroscopic techniques. FT-IR spectra demonstrated the incorporation of organic moieties onto the silica surface, while SEM images revealed the modified spherical shape of the silica gel. TEM and XRD analyses confirmed the presence of palladium on the silica matrix. ICP and EDX measurements validated the anchoring of 0.55 mmol/g of palladium to the catalyst. Additionally, XPS analysis showed the complexation of Pd(0) with the organic ligand on the silica matrix, confirming the successful integration of palladium into the system. This nanocatalyst demonstrated outstanding performance in Mizoroki-Heck reactions, yielding high product outputs in the cross-coupling of various aryl halides and olefins under mild conditions. Additionally, the nanocatalyst was effectively utilized in synthesizing Ozagrel, a thromboxane A2 synthesis inhibitor used for treating noncardioembolic stroke patients. Remarkably, the catalyst demonstrated excellent reusability, maintaining high productivity across five consecutive cycles, underscoring its economic and sustainable potential for industrial applications.

我们通过三步反应过程开发出了一种具有成本效益的硅胶支撑钯纳米催化剂。首先,硅胶(60-120 目)使用 3-aminopropyltriethoxysilane 进行氨基官能化,通过与 1,10-菲罗啉-2,9-二甲醛配体反应形成希夫碱。随后,在钯盐和水合肼的存在下,将纳米钯催化剂引入硅胶基质配体,形成了硅胶支撑的希夫碱纳米钯催化剂()。使用各种光谱技术确认了硅胶基质的成功功能化。傅立叶变换红外光谱显示了有机分子在二氧化硅表面的结合,而扫描电镜图像则显示了硅胶的改性球形。TEM 和 XRD 分析证实了二氧化硅基体上钯的存在。ICP 和 EDX 测量证实催化剂上锚定了 0.55 mmol/g 的钯。此外,XPS 分析表明钯与二氧化硅基体上的有机配体发生了络合反应,证实钯成功地融入了该体系。这种纳米催化剂在 Mizoroki-Heck 反应中表现出卓越的性能,在温和条件下,各种芳基卤化物和烯烃的交叉偶联反应中产生了大量产物。此外,该纳米催化剂还被有效地用于合成 Ozagrel(一种血栓素 A2 合成抑制剂,用于治疗非心肌栓塞性中风患者)。值得注意的是,该催化剂具有极佳的可重复使用性,可在连续五个循环中保持高生产率,这凸显了其在工业应用中的经济性和可持续发展潜力。
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引用次数: 0
3D printing of reprogrammable liquid crystal elastomers with exchangeable boronic ester bonds 具有可交换硼酸酯键的可再编程液晶弹性体的三维打印技术
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-31 DOI: 10.1016/j.giant.2024.100331
Xinzi Yu , Changyue Liu , Liqian Wang , Tianyu Li , Lingxin Yuan , Jiping Yang , Rui Xiao , Zhijian Wang

Liquid crystal elastomers (LCEs) are a kind of soft actuating materials with large reversible deformation ability, which can work as the “motor” to exhibit complex deformations and drive the locomotion of soft robots. The deformation of LCEs depends on the three-dimensional (3D) shape of whole structure and alignment patterns of mesogens. Various methods have been employed to fabricate the LCE structure with desired shapes and mesogen alignments. However, conventional 3D printed LCEs require continuous thermal energy input to maintain their actuated shapes. The LCEs cannot be reprocessed and reprogrammed once cured. Herein, we introduce dynamic boronic ester bonds into the ink, with which the printed LCE structures are capable of being reprogrammed from polydomain into monodomain state and vice versa. We further explore the effects of printing parameters and content of dynamic covalent bonds on the actuation performance and reprogramming ability. The actuated shape could be well predicted with finite element method. The dynamic printable LCEs developed here offer new strategy and large design space for LCE structures.

液晶弹性体(LCE)是一种具有较大可逆形变能力的软执行材料,可作为 "马达 "产生复杂形变,驱动软机器人运动。LCE 的变形取决于整体结构的三维(3D)形状和介质的排列模式。人们采用了各种方法来制造具有所需形状和中原排列的 LCE 结构。然而,传统的三维打印 LCE 需要持续输入热能以保持其驱动形状。LCE 固化后无法进行再加工和再编程。在此,我们在油墨中引入了动态硼酸酯键,这样打印出的 LCE 结构就能从多域状态重新编程为单域状态,反之亦然。我们进一步探讨了印刷参数和动态共价键含量对致动性能和重编程能力的影响。用有限元方法可以很好地预测驱动形状。本文开发的动态可印刷 LCE 为 LCE 结构提供了新的策略和广阔的设计空间。
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引用次数: 0
Conformation-assisted solid-solid phase transition of LiTFSI electrolyte salt and the lithium ion coordination LiTFSI 电解质盐的构象辅助固固相变与锂离子配位
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-29 DOI: 10.1016/j.giant.2024.100330
Ziwei Lai , Donglei You , Wei Wei , Huiming Xiong

Single crystal growth and characterization of the lithium bis(trifluoromethyl sulfonyl)imide (LiTFSI), the most common electrolyte salt for lithium-ion batteries, have been performed and succeeded in unraveling the atomic structures of its different crystalline phases. The structures of two crystalline phases (phase I: orthorhombic, Pccn; phase II: monoclinic, P21/c) have been determined through temperature-dependent X-ray crystallography of the LiTFSI single crystal on heating, and the solid-solid phase transformation between phase I and phase II has been dictated. Interestingly, a conformational change of TFSI⁻ from transoid to cisoid has been discovered during the transition from phase I to phase II, which has been further confirmed by the temperature-dependent Raman spectroscopy. The coordination of Li⁺ with the TFSI⁻ ions of different conformations has been also elucidated in the polymorphic crystalline structures. The solid-solid phase transformation of the first-order leads to the cracking of the LiTFSI crystal, probably along the lithium-ion or the fluorine-rich layer in phase II. In the molten state, the coexistence of the transoid conformation and the cisoid conformation is found in the TFSI⁻ ions, affirming the recent observation in the concentrated non-crystalline state. This work is anticipated to shed light on the (de)solvation and the transport of lithium ions in complex fluids encompassing LiTFSI electrolyte solutions from the structural aspects.

对锂离子电池最常见的电解质盐--双(三氟甲基磺酰基)亚胺锂(LiTFSI)进行了单晶生长和表征,并成功揭示了其不同晶相的原子结构。通过对 LiTFSI 单晶加热时的温度依赖性 X 射线晶体学分析,确定了两种结晶相(I 相:正交相;II 相:单斜相)的结构,并确定了 I 相和 II 相之间的固-固相转变。有趣的是,在从 I 相到 II 相的转变过程中,发现了 TFSI- 从 到 的构象变化,温度依赖性拉曼光谱进一步证实了这一点。在多晶体结构中,还阐明了不同构象的 Li⁺ 与 TFSI- 离子的配位关系。一阶固-固相变导致锂-TFSI 晶体开裂,可能是沿着锂离子层或第二阶段的富氟层开裂。在熔融状态下,TFSI- 离子中发现了构象与构象共存的现象,这肯定了最近在浓缩非晶态下的观察结果。这项工作有望从结构方面揭示锂离子在包括 LiTFSI 电解质溶液在内的复杂流体中的(去)溶解和传输。
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引用次数: 0
Morphology evolution of lipid nanoparticle discovered by small angle neutron scattering 小角中子散射发现脂质纳米粒子的形态演变
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-25 DOI: 10.1016/j.giant.2024.100329
Yuqing Li , Changli Ma , Zehua Han , Weifeng Weng , Sicong Yang , Zepeng He , Zheqi Li , Xiaoye Su , Taisen Zuo , He Cheng

The structure of mRNA lipid nanoparticles (LNPs) is still under debate, with different studies presenting varying morphological characteristics, significantly hindering their biomedical potential. A typical formulation process of mRNA LNPs involves three steps: initial rapid mixing of lipids in an ethanol phase and mRNA in an acidic aqueous phase, followed by the swift removal of ethanol, and finally adjusting the solution to a neutral environment. In this study, we utilize Small Angle Neutron Scattering (SANS) with contrast matching to reveal the kinetic pathway-dependent of mRNA LNPs morphology. We find that the formulation process of the Moderna COVID-19 vaccine is controlled by a competition between aggregation and microphase separation, dictating the diverse morphologies observed in mRNA LNPs. The first step leads to the formation of polydisperse spherical droplets with an average diameter of 42±6.0 nm in an acidic ethanol aqueous solution. Ethanol removal initiates both aggregation and internal microphase separation, resulting in a polydisperse core-shell structure with an average diameter of 48±3.7 nm. Heptadecan-9-yl 8-((2-hydroxyethyl) (6-oxo-6-(undecyloxy) hexyl) amino) octanoate (SM-102) binds to mRNA via electrostatic interaction to form a reverse-wormlike micelle structure inside. The 1,2-Distearoyl-sn‑glycero-3-phosphocholine (DSPC) and PEG-lipid are just in the shell and cholesterol acting as a filler throughout the core-shell structure. Upon transitioning to a neutral environment, SM-102 loses its charge and neither the periphery nor the reverse-wormlike micelle can maintain their stabilities, leading to further aggregation and microphase separation. The average diameter of core-shell structure turns to be 66±5.2 nm. In the actual formulation process of the Moderna COVID-19 vaccine, steps 2 and 3 occur simultaneously, and the competition between aggregation and microphase separation determines the final morphology. These findings offer crucial insights into optimizing the morphology of mRNA LNPs, thereby facilitating advancements in vaccine development and mRNA vaccine delivery technologies.

关于 mRNA 脂质纳米粒子(LNPs)的结构仍存在争议,不同的研究呈现出不同的形态特征,极大地阻碍了其生物医学潜力的发挥。mRNA LNPs 的典型配制过程包括三个步骤:首先将乙醇相中的脂质与酸性水相中的 mRNA 快速混合,然后迅速去除乙醇,最后将溶液调整至中性环境。在本研究中,我们利用小角中子散射(SANS)与对比度匹配揭示了 mRNA LNPs 形态的动力学路径依赖性。我们发现,Moderna COVID-19 疫苗的配制过程受控于聚集和微相分离之间的竞争,这决定了在 mRNA LNPs 中观察到的不同形态。第一步是在酸性乙醇水溶液中形成平均直径为 42±6.0 nm 的多分散球形液滴。移除乙醇后,会产生聚集和内部微相分离,从而形成平均直径为 48±3.7 nm 的多分散核壳结构。Heptadecan-9-yl 8-((2-hydroxyethyl) (6-oxo-6-(undecyloxy) hexyl) amino) octanoate(SM-102)通过静电作用与 mRNA 结合,在内部形成反向蠕虫状胶束结构。1,2-二硬脂酰-sn-甘油-3-磷酸胆碱(DSPC)和 PEG-脂质只是在外壳中,胆固醇在整个核壳结构中充当填充物。在过渡到中性环境时,SM-102 会失去电荷,外围和反向蠕虫状胶束都无法保持稳定,导致进一步聚集和微相分离。核壳结构的平均直径为 66±5.2 nm。在 Moderna COVID-19 疫苗的实际配制过程中,第 2 步和第 3 步同时进行,聚集和微相分离之间的竞争决定了最终的形态。这些发现为优化 mRNA LNPs 的形态提供了重要启示,从而促进了疫苗开发和 mRNA 疫苗递送技术的进步。
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引用次数: 0
Dual role of epoxidized soybean oil (ESO) as plasticizer and chain extender for biodegradable polybutylene succinate (PBS) formulations 环氧化大豆油(ESO)作为可生物降解聚丁二酸丁二醇酯(PBS)配方的增塑剂和扩链剂的双重作用
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-23 DOI: 10.1016/j.giant.2024.100328
Rosa Turco , Salvatore Mallardo , Domenico Zannini , Arash Moeini , Martino Di Serio , Riccardo Tesser , Pierfrancesco Cerruti , Gabriella Santagata

This work reports the effect of 1–5 wt% epoxidized soybean oil (ESO) addition on the thermal, mechanical, and morphological properties of polybutylene succinate (PBS). ESO acts as a chain extender as well as a mild plasticizer of PBS. N-methylimidazole (NMI) is used as a catalyst to promote the reaction between PBS and ESO, and thermal, rheological, and spectroscopic analyses demonstrate increased viscoelastic properties, compatibility, crystallinity and thermal stability of the melt reacted formulations. In the presence of NMI, storage modulus (G’) values two orders of magnitude higher than that of pure PBS are achieved, confirming the completion of the chain extension reaction. A drastic refinement of the biphasic structure of the blend is observed, with the formation of a homogenous structure where ESO is well incorporated into the matrix. Finally, tensile tests reveal enhanced mechanical performance in the blends reacted in the presence of NMI. These findings pave the way for the development of a versatile family of materials which could find potential application in sustainable biodegradable packaging.

本研究报告介绍了添加 1-5 wt%环氧化大豆油(ESO)对聚丁二酸丁二醇酯(PBS)的热、机械和形态特性的影响。ESO 既是 PBS 的扩链剂,也是一种温和的增塑剂。N 甲基咪唑(NMI)被用作催化剂来促进 PBS 和 ESO 之间的反应,热学、流变学和光谱分析表明,熔融反应配方的粘弹性能、相容性、结晶度和热稳定性都有所提高。在 NMI 的存在下,存储模量(G')值比纯 PBS 高出两个数量级,这证明链延伸反应已经完成。共混物的双相结构得到了显著改善,形成了一种均匀的结构,其中 ESO 与基质结合得很好。最后,拉伸测试表明,在 NMI 存在的情况下反应的共混物具有更高的机械性能。这些发现为开发多功能材料系列铺平了道路,这些材料可能会应用于可持续生物降解包装。
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引用次数: 0
Generation and regularization of zigzag focal conic domains guided by thermodynamic-driven topological defect evolution 热力学驱动的拓扑缺陷演化引导之字形焦点圆锥域的生成和正则化
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1016/j.giant.2024.100327
Daoxing Luo , Jinbing Wu , Zhenghao Guo , Jingmin Xia , Wei Hu

Liquid crystals, as typical anisotropic building blocks, tend to self-assemble into various ordered architectures during distinct thermodynamic processes. Research on the underlying mechanisms and rules may drastically promote our understanding of complicated structures. Here, zigzag focal conic domains (ZFCDs) are generated in rapid cooling process under an antagonistic boundary condition. After several thermal cycles beneath the nematic-smectic (N-S) phase transition point, the ZFCDs are well regularized. We found that the dislocations associated with the rapid cooling play vital roles in the formation of ZFCDs. A strong interphase correlation between the zigzag ± 1/2 disclination pairs and ZFCDs is observed above the N-S phase transition point. The orientational order inheritance and topological invariance across the phase transition indicate that similar disclination pairs exist in ZFCDs. These disclination pairs facilitate the opposite tilt direction and a half-pitch lateral shift between neighboring focal conic domains (FCDs), thus forming ZFCDs. During thermal cycles, the thermal motion of molecules induces the regularization and elimination of defect cores, further resulting in the ordered ZFCDs. Via properly controlling the cooling rate, large-area ordered ZFCDs are achieved in a wide film thickness range after thermal cycles. This study enriches the knowledge on the topological defect guided architecture of liquid crystals and may pave the way for the generation and regularization of ordered self-assembled systems.

液晶作为典型的各向异性构件,往往会在不同的热力学过程中自组装成各种有序结构。对其基本机制和规则的研究可能会极大地促进我们对复杂结构的理解。在这里,"之 "字形焦点圆锥域(ZFCD)是在拮抗边界条件下的快速冷却过程中产生的。在向列-共晶(N-S)相变点下经过数次热循环后,ZFCD 得到了很好的规整。我们发现,与快速冷却相关的位错在 ZFCD 的形成过程中起着至关重要的作用。在N-S相变点上方,我们观察到人字形±1/2位错对和ZFCD之间存在很强的相间相关性。整个相变过程中的定向顺序继承性和拓扑不变性表明,ZFCDs 中也存在类似的披露对。这些分离对促进了相邻焦点圆锥畴(FCD)之间的相反倾斜方向和半间距横向移动,从而形成了 ZFCD。在热循环过程中,分子的热运动促使缺陷核心规整化和消除,从而进一步形成有序的 ZFCD。通过适当控制冷却速率,在热循环后的较宽薄膜厚度范围内实现了大面积有序 ZFCD。这项研究丰富了人们对液晶拓扑缺陷导向结构的认识,并可能为有序自组装系统的生成和规整化铺平道路。
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