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Small dop of comonomer, giant shift of dynamics: α-methyl-regulated viscoelasticity of poly(methacrylamide) hydrogels 少量共聚物掺入,动力学巨变:α-甲基调节聚(甲基丙烯酰胺)水凝胶的粘弹性
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-23 DOI: 10.1016/j.giant.2024.100342
Xin Guan , Zhiheng Zhou , Xinzhen Fan , Wenchao Xu , Yijie Jin , Chuanzhuang Zhao
α-Methyl groups play significant roles in the regulation of water molecules within both small molecular systems and bio-macromolecular systems. Systematically studying the influence of α-methyl on the dynamics of water molecules within hydrogel systems is therefore worthwhile. In this study, we prepared a series of hydrogen-bonded (H-bonded) hydrogels with varying densities of α-methyl groups by copolymerizing methacrylamide (MAm) with its α-methyl-absent analogue, acrylamide (Am). Introducing a small amount of Am (≤6 mol%) into the polymer chain resulted in significant shifts in the viscoelasticity of the hydrogels. The hydrogels exhibit a “time-temperature-α-methyl equivalence”, meaning that introduction of α-methyl-absent monomer has effects similar to elevating temperature and prolonging observation time on the dynamic properties. Based on low-field nuclear magnetic resonance spectroscopy and Raman scattering, a “hydrophilic defects-assisted H-bonds dissociation” mechanism is proposed, depicting that the α-methyl-absent monomer can disturb the rearrangement of water molecules surrounding the polymer chain and accelerate chain dissociation. These findings enabled the copolymer hydrogels with functions such as fast self-healing and tunable interface adhesion.
在小分子体系和生物大分子体系中,α-甲基对水分子的调节都起着重要作用。因此,系统研究α-甲基对水凝胶体系中水分子动力学的影响是有价值的。在本研究中,我们通过甲基丙烯酰胺(MAm)与不含α-甲基的类似物丙烯酰胺(Am)共聚,制备了一系列具有不同α-甲基密度的氢键(H-键)水凝胶。在聚合物链中引入少量 Am(≤6 摩尔%)可显著改变水凝胶的粘弹性。水凝胶表现出 "时间-温度-α-甲基等效",即引入α-甲基缺失单体对动态特性的影响类似于升高温度和延长观察时间。基于低场核磁共振光谱和拉曼散射,提出了 "亲水缺陷辅助 H 键解离 "机理,说明α-甲基缺失单体可干扰聚合物链周围水分子的重排,加速链解离。这些发现使共聚物水凝胶具有快速自愈合和可调界面粘附性等功能。
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引用次数: 0
Binary blends of poly(lactic acid) and poly(methyl methacrylate) for high energy density and charge/discharge efficiency capacitors 用于高能量密度和充放电效率电容器的聚乳酸和聚甲基丙烯酸甲酯二元混合物
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-10 DOI: 10.1016/j.giant.2024.100340
Shuo Zhao , Le Zhou , Junshang Zhang, Yang Shen, Ce-Wen Nan

Polymer dielectrics are widely used in modern power electronics due to their high flexibility and high breakdown strength. However, the limited energy density of current polymer dielectrics limits their wider applications, and there is an urgent need to develop novel polymer dielectric materials. Poly(lactic acid) (PLA) is favored for biological applications due to its biocompatibility and biodegradability. In general, PLA has three optical isomers, namely poly(L-lactide) (PLLA), poly(D-lactide) (PDLA), and poly(DL-lactide) (PDLLA), but the investigation of their dielectric properties remains limited. In this study, a significant increase in energy storage density and charge/discharge efficiency in poly(methyl methacrylate) (PMMA) was achieved by incorporating isomers of PLA into PMMA. Experimental results indicate that the introduction of PLA creates a phase-separated structure within PMMA, and in particular, the introduction of the crystalline region significantly improved the breakdown strength (Eb). Finally, PLLA/PMMA 50/50 and PDLA/PMMA 50/50 exhibit the discharged energy densities of 8.55 J cm−3 and 8.18 J cm−3, respectively, with charge/discharge efficiencies of 89.6% and 90.9%. This work enables the achievement of all-organic dielectrics with high energy storage density and high efficiency through the construction of phase-separated structures and demonstrates the great potential of biodegradable polymers in electronic devices.

聚合物电介质具有高柔韧性和高击穿强度,因此被广泛应用于现代电力电子设备中。然而,目前聚合物电介质的能量密度有限,限制了其更广泛的应用,因此迫切需要开发新型聚合物电介质材料。聚乳酸(PLA)因其生物相容性和生物可降解性,在生物应用中备受青睐。一般来说,聚乳酸有三种光学异构体,即聚(L-乳酸)(PLLA)、聚(D-乳酸)(PDLA)和聚(DL-乳酸)(PDLLA),但对它们介电性能的研究仍然有限。在本研究中,通过在聚甲基丙烯酸甲酯(PMMA)中加入聚乳酸异构体,实现了聚甲基丙烯酸甲酯(PMMA)储能密度和充放电效率的显著提高。实验结果表明,聚乳酸的引入在 PMMA 中产生了相分离结构,尤其是晶体区的引入显著提高了击穿强度(Eb)。最后,PLLA/PMMA 50/50 和 PDLA/PMMA 50/50 的放电能量密度分别为 8.55 J cm-3 和 8.18 J cm-3,充放电效率分别为 89.6% 和 90.9%。这项工作通过构建相分离结构实现了高储能密度和高效率的全有机电介质,展示了生物可降解聚合物在电子器件中的巨大潜力。
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引用次数: 0
The effect of dynamic cross-links and mesogenic groups on the swelling and collapse of polymer gels 动态交联和介原基团对聚合物凝胶溶胀和崩解的影响
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-10 DOI: 10.1016/j.giant.2024.100341
Daniil E. Larin , Andrey V. Shibaev , Ch.-Y. Liu , Alexander V. Emelyanenko

The polymer gels containing dynamic cross-links and mesogenic groups are among the key candidates for the development of soft actuators and detectors, displays, sensors and other programmable and self-healing materials. In this article, firstly, the collapse of polymer networks with irreversible cross-links in the presence of a dynamic cross-linker is investigated by means of Flory-type theory. It is shown that, at not a very poor solvent quality (near the theta-conditions), the swelling ratio for a gel containing irreversible and dynamic cross-links is less than for a gel with irreversible cross-links only, whereas at poor or good solvent qualities sizes of these gels are close to each other. The number of dynamic cross-links monotonically increases with worsening the solvent quality. The gel contraction can be also achieved by increasing the dynamic cross-linker concentration, which allows one to change the transition point in a wide range of solvent conditions. Secondly, polymer networks containing irreversible and dynamic cross-links and incorporating mesogenic side groups is studied using the Maier–Saupe theory. With decreasing in the temperature, the continuous transition from a swollen to collapsed state occurs. With further increase in the temperature, the swelling ratio discontinuously decreases and the nematic order parameter sharply increases from zero to a value ​​close to one. By increasing the dynamic cross-linker concentration, the swelling-to-collapse transition and, then, the isotropic-nematic transition are observed. A phase diagram of the gel is constructed and, depending on the dynamic cross-linker concentration and temperature, the swollen gel with the zero nematic order parameter, the collapsed gel with the zero nematic order parameter, and the collapsed gel with the nematic ordering can be formed. A growth of the length of the mesogenic side group leads to an increase in the area of ​​existence of the collapsed gel with the nematic ordering in the phase diagram. The obtained theoretical results are in agreement with corresponding experimental data from the literature.

含有动态交联和介原基团的聚合物凝胶是开发软致动器和探测器、显示器、传感器以及其他可编程和自修复材料的主要候选材料之一。本文首先通过弗洛里型理论研究了具有不可逆交联的聚合物网络在动态交联剂存在时的塌缩。研究表明,在溶剂质量不是很差的情况下(接近θ条件),含有不可逆交联和动态交联的凝胶的溶胀率小于仅含有不可逆交联的凝胶,而在溶剂质量较差或较好的情况下,这些凝胶的尺寸则相互接近。动态交联的数量随着溶剂质量的恶化而单调增加。增加动态交联剂的浓度也可以实现凝胶收缩,从而在多种溶剂条件下改变过渡点。其次,我们利用 Maier-Saupe 理论研究了含有不可逆动态交联和介源侧基的聚合物网络。随着温度的降低,出现了从膨胀状态到塌缩状态的连续转变。随着温度的进一步升高,膨胀率不连续地降低,向列有序参数从零急剧上升到接近于 1 的值。通过增加动态交联剂浓度,可以观察到从膨胀到塌陷的转变,然后是各向同性-向列转变。根据动态交联剂浓度和温度的不同,可以形成向列有序参数为零的膨胀凝胶、向列有序参数为零的塌缩凝胶和向列有序的塌缩凝胶。介生侧基长度的增加会导致相图中存在向列有序塌缩凝胶的区域增大。获得的理论结果与文献中的相应实验数据一致。
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引用次数: 0
Systematic anode engineering enabling universal efficiency improvements in organic solar cells 系统化阳极工程可普遍提高有机太阳能电池的效率
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-30 DOI: 10.1016/j.giant.2024.100338
Kwok Kiu Tsang , Han Yu , Joshua Yuk Lin Lai , Ho Ming Ng , Chung Hang Kwok , Wenzhao Xiong , Huawei Hu , He Yan

Anode modification and optimization is crucial towards improving performance of organic solar cells (OSCs). PEDOT:PSS is the most common choice as a hole transport layer (HTL) material, but suffers from issues including low conductivity. In this work, three alkyl amine derivatives - methylamine hydrochloride (MA), ethylamine hydrochloride (EA) and propylamine hydrochloride (PA) are doped into the commercially available Al 4083 PEDOT:PSS to form PEDOT:PSS-MA, PEDOT:PSS-EA and PEDOT:PSS-PA, as modified HTLs. All these modified HTLs exhibit improved chemical and electrical properties including work functions (WF), conductivities and charge carrier motilities. The alkyl amine doping shows compatibility in both Small Molecular Acceptors and All-Polymer OSCs. With PEDOT:PSS-MA demonstrates a highest PCE of 18.49 % compared to the 17.84 % of OSC devices prepared with pristine PEDOT:PSS with the PM6:L8-BO system, while PM6:PY-IT all-polymer OSCs improve PCE from 14.53 % to 15.22 %. AFM characterizations reveal that the introduction of the dopants have smoothened the surface morphology of spin-coated HTL films, which contributes towards more efficient charge extraction. In summary, this study not only presents a method of improving OSC efficiencies, but also provides insight and further possible directions towards anode optimization of OSCs.

阳极改性和优化对提高有机太阳能电池(OSC)的性能至关重要。PEDOT:PSS 是最常用的空穴传输层(HTL)材料,但存在导电率低的问题。在这项工作中,三种烷基胺衍生物--甲胺盐酸盐(MA)、乙胺盐酸盐(EA)和丙胺盐酸盐(PA)被掺杂到市售的 Al 4083 PEDOT:PSS 中,形成 PEDOT:PSS-MA、PEDOT:PSS-EA 和 PEDOT:PSS-PA 作为改性 HTL。所有这些改性 HTL 都具有更好的化学和电气性能,包括功函数(WF)、电导率和电荷载流子运动。烷基胺掺杂显示了小分子受体和全聚合物 OSC 的兼容性。与使用原始 PEDOT:PSS 和 PM6:L8-BO 系统制备的 17.84% 的 OSC 器件相比,PEDOT:PSS-MA 的 PCE 最高达 18.49%,而 PM6:PY-IT 全聚合物 OSC 的 PCE 则从 14.53% 提高到 15.22%。原子力显微镜表征显示,掺杂剂的引入使旋涂 HTL 薄膜的表面形貌更加平滑,这有助于提高电荷萃取的效率。总之,这项研究不仅提出了一种提高 OSC 效率的方法,还为优化 OSC 的阳极提供了深入的见解和更多可能的方向。
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引用次数: 0
Thermal response color-tunable electroluminescent device for real-time visual temperature monitoring 用于实时视觉温度监测的热响应彩色可调电致发光装置
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-28 DOI: 10.1016/j.giant.2024.100339
Xiaohui Sun , Jiuyue Zhang , Xu Li , Xuelei Gong , Debin Kong , Linjie Zhi

Alternating current electroluminescent (ACEL) devices have attracted tremendous attention due to their significant applications in bioinspired electronics, smart wearables, and human-machine interfaces. However, it still faces limitations in real-time visual temperature sensing. Herein, a universal strategy is established to achieve real-time temperature dynamic visualization by integrating a thermochromic layer through a simple spin coating procedure. Such elaborate integration permits the device to display a wide array of luminous colors and achieve high-contrast color transitions in response to ambient temperature variations. More importantly, a quantitative relationship can be established between the temperatures and the luminous color changes. This advancement not only enhances multi-color emission capabilities but also enables the display of diverse information, marking a significant stride in the development of dynamic temperature sensing in ACEL devices.

交变电流电致发光(ACEL)器件因其在生物启发电子学、智能可穿戴设备和人机界面中的重要应用而备受关注。然而,它在实时视觉温度传感方面仍然面临着局限性。在本文中,通过简单的旋涂过程集成热致变色层,建立了实现实时温度动态可视化的通用策略。这种精心设计的集成使设备能够显示多种发光颜色,并根据环境温度变化实现高对比度的颜色转换。更重要的是,可以在温度和发光颜色变化之间建立定量关系。这一进步不仅增强了多色发光能力,还能显示各种信息,标志着 ACEL 器件在动态温度传感方面取得了重大进展。
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引用次数: 0
Giant molecule acceptors for high performance polymer solar cells 用于高性能聚合物太阳能电池的巨分子受体
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-22 DOI: 10.1016/j.giant.2024.100336
Hongmei Zhuo , Beibei Qiu , Xiaojun Li , Zhi-Guo Zhang , Yongfang Li

Giant molecule acceptors (GMAs) are composed of two or more narrow bandgap small molecule acceptors (SMAs) subunits connected by conjugated or non-conjugated linking units, which possesses the advantages of the SMAs with broad absorption, appropriate electronic energy levels and fixed molecular weight (with good photovoltaic performance reproducibility), and the polymerized SMAs (PSMAs) with good film-forming property and high morphology stability and photo-stability. So that the GMAs are promising for future commercial application in polymer solar cells (PSCs). Therefore, the GMAs have attracted great attention recently. In this review, we will briefly introduce the development of the narrow bandgap SMAs, especially the A-DA’D-A structured SMAs, and the PSMAs. Then we will focus on the recent research progress of the GMAs, including the synthetic method of GMAs and the effect of number of the SMA subunits on the photovoltaic performance of the GMAs. Finally, we present our perspectives and offer a concise outlook on the further advancement of the GMAs.

巨分子受体(GMAs)由两个或多个窄带隙小分子受体(SMAs)亚基通过共轭或非共轭连接单元连接而成,它具有 SMAs 的宽吸收、适当的电子能级和固定分子量(具有良好的光伏性能重现性),以及聚合 SMAs(PSMAs)的良好成膜性、高形态稳定性和光稳定性等优点。因此,GMAs 在聚合物太阳能电池(PSCs)中的商业应用前景广阔。因此,最近 GMAs 引起了极大的关注。在本综述中,我们将简要介绍窄带隙 SMA 的发展,尤其是 A-DA'D-A 结构 SMA 和 PSMA。然后,我们将重点介绍 GMAs 的最新研究进展,包括 GMAs 的合成方法以及 SMA 子单元数量对 GMAs 光伏性能的影响。最后,我们将提出自己的观点,并对 GMAs 的进一步发展进行简要展望。
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引用次数: 0
Recent progress in gel polymer electrolyte for lithium metal batteries 用于锂金属电池的凝胶聚合物电解质的最新进展
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-22 DOI: 10.1016/j.giant.2024.100337
Changxing Han , Xiong Shui , Guansheng Chen , Gaojie Xu , Jun Ma , Shanmu Dong , Shitao Wang , Xinhong Zhou , Zili Cui , Lixin Qiao , Guanglei Cui

Lithium metal batteries (LMBs) with high energy density have been deemed as one of the promising alternatives to alleviate the “range anxiety” of current electric vehicles based on traditional lithium-ion batteries. However, LMBs using traditional liquid electrolytes (LEs) are always facing serious lithium dendrite growth and electrolyte leakage issues, which could usually cause serious safety concerns. Solid polymer electrolytes (SPEs) with high mechanical stability could suppress the lithium dendrites to some extent, however, they are suffering from low ionic conductivity and inferior interfacial contact with electrodes. Gel polymer electrolytes (GPEs) combining the advantages of traditional LEs and SPEs could be a promising choice to alleviate above issues. In this review, we systematically summarized and clarified very recent progress of various advanced GPEs for LMBs, which is mainly focusing on the advancement of different polymer matrices used for GPE-based LMBs as well as the development of methodologies for the preparation of GPEs. In addition, we also provide a perspective aiming at inspiring new ideas and directions to design reliable GPEs for advancing the performance of LMBs and boosting their practical application.

具有高能量密度的锂金属电池(LMB)被认为是缓解当前基于传统锂离子电池的电动汽车 "续航焦虑 "的有前途的替代品之一。然而,使用传统液态电解质(LE)的锂金属电池始终面临着严重的锂枝晶生长和电解质泄漏问题,通常会引发严重的安全隐患。固态聚合物电解质(SPE)具有较高的机械稳定性,可在一定程度上抑制锂枝晶的产生,但其离子电导率较低,与电极的界面接触性较差。凝胶聚合物电解质(GPEs)结合了传统锂离子电解质和固相锂离子电解质的优点,是缓解上述问题的一个很有前景的选择。在这篇综述中,我们系统地总结并阐明了各种用于 LMB 的先进 GPE 的最新进展,主要集中在用于基于 GPE 的 LMB 的不同聚合物基质的进步以及 GPE 制备方法的发展。此外,我们还提供了一个视角,旨在启发设计可靠 GPE 的新思路和新方向,以提高 LMB 的性能并促进其实际应用。
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引用次数: 0
Backbone engineering and side group manipulation in covalent organic frameworks for overall solar-driven hydrogen peroxide production 共价有机框架中的骨架工程和侧基操作,用于太阳能驱动的过氧化氢整体生产
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-20 DOI: 10.1016/j.giant.2024.100335
Ying Zhang , Hangxun Xu

Covalent Organic Frameworks (COFs) have emerged as highly promising materials for the photocatalytic production of hydrogen peroxide (H2O2) due to their exceptional structural tunability, robust frameworks, and high porosity. The efficient overall photosynthesis of H2O2 hinges on the simultaneous occurrence of the oxygen reduction reaction (ORR) and water oxidation reaction (WOR). This review introduces recent progress in developing key approaches such as backbone engineering and the incorporation of side groups to facilitate these critical reaction pathways. For example, innovative COF designs, such as spatially separating redox centers, have demonstrated significant improvements in photocatalytic performance. Moreover, the introduction of thioether-decorated triazine-based COFs and hexavalent triphenylene knots has led to remarkable H2O2 production rates. Furthermore, this review also addresses the challenges associated with the practical implementation of COFs, including their stability under operational conditions and the necessity for innovative reactor designs. The future prospects of COFs in sustainable chemical synthesis are also discussed, emphasizing their potential for COFs to revolutionize H2O2 production through green and sustainable methodologies. This review aims to provide valuable insights into the design and development of high-performance COF photocatalysts, paving the way for their practical applications in the sustainable production of value-added chemicals.

共价有机框架(COFs)因其卓越的结构可调性、坚固的框架和高孔隙率,已成为极具前景的光催化生产过氧化氢(H2O2)的材料。H2O2 的高效整体光合作用取决于氧还原反应(ORR)和水氧化反应(WOR)的同时发生。本综述介绍了在开发骨架工程和加入侧基等关键方法以促进这些关键反应途径方面的最新进展。例如,创新的 COF 设计(如在空间上分离氧化还原中心)已在光催化性能方面取得显著改善。此外,硫醚装饰的三嗪基 COF 和六价三苯结的引入也带来了显著的 H2O2 产率。此外,本综述还探讨了与 COFs 实际应用相关的挑战,包括 COFs 在操作条件下的稳定性以及创新反应器设计的必要性。还讨论了 COFs 在可持续化学合成中的未来前景,强调 COFs 通过绿色和可持续方法彻底改变 H2O2 生产的潜力。本综述旨在为高性能 COF 光催化剂的设计和开发提供有价值的见解,为其在可持续生产高附加值化学品方面的实际应用铺平道路。
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引用次数: 0
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
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