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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 : 2024-12-01 Epub 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
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 : 2024-12-01 Epub 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
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 : 2024-12-01 Epub 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
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 : 2024-12-01 Epub 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
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 : 2024-12-01 Epub 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
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 : 2024-12-01 Epub 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
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 : 2024-12-01 Epub 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
Nonlinear optical director reorientation in heliconical cholesteric liquid crystals: a brief review 螺旋胆甾型液晶中的非线性光学导向重新定向:简要回顾
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-01 Epub Date: 2024-06-28 DOI: 10.1016/j.giant.2024.100311
Liana Lucchetti , Giovanni Nava

Cholesteric liquid crystals, also known as chiral nematics, possess a right-angle helicoidal structure with pitch in the submicrometer and micrometer range. Although the possibility of getting optical reorientation in this kind of materials has been considered since the discovery of giant optical nonlinearity in nematic liquid crystals, a significant light-induced modulation of the helical structure has shown to be a challenging task. The recent experimental realization of a chiral phase with an oblique helicoidal structure, identified as the heliconical phase predicted by Meyer and DeGennes in 1968, offers the opportunity to observe such an optical reorientation of the optic axis. This paper is a brief review of the nonlinear optical properties of these unconventional chiral nematic liquid crystals and is aimed at showing that the world of liquid crystalline phases can still amaze with new material properties and new physics.

胆甾型液晶又称手性向列液晶,具有直角螺旋结构,间距在亚微米和微米范围内。虽然自从发现向列液晶的巨大光学非线性以来,人们就一直在考虑在这类材料中实现光学重新定向的可能性,但要在光的诱导下对螺旋结构进行明显的调制,已被证明是一项具有挑战性的任务。最近通过实验发现了一种具有斜螺旋结构的手性相,即 Meyer 和 DeGennes 于 1968 年预测的螺旋相,这为观察这种光轴的光学重新定向提供了机会。本文简要回顾了这些非常规手性向列液晶的非线性光学特性,旨在说明液晶相的世界仍然可以通过新的材料特性和新的物理学而令人惊叹。
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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 Epub Date: 2024-07-14 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
Dimerized small molecule donor enables efficient ternary organic solar cells 二聚化小分子供体实现高效三元有机太阳能电池
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-01 Epub Date: 2024-07-11 DOI: 10.1016/j.giant.2024.100325
Mingrui Pu , Chunxian Ke , Yongwen Lang , Heng Li , Xiangyu Shen , Leilei Tian , Feng He

Ternary organic solar cells (OSCs) are the feasible and efficient strategy to achieve the high-performance OSCs. It is of great significance to develop a superior third component candidate for constructing efficient ternary OSCs. In this work, we intelligently designed and synthesized a dimerized small molecule donor by connecting two asymmetric small molecule donors with the vinyl group, which is named DSMD-βV. This innovative oligomeric molecule DSMD-βV not only exhibits the complementary absorption and the cascade energy level arrangement with PM6 and BTP-eC9, but also regulates the phase separation micromorphology based on PM6:BTP-eC9. Consequently, PM6:DSMD-βV:BTP-eC9 based ternary device exhibits the improved exciton dissociation, charge transport and decreased recombination, thus achieving a superior power conversion efficiency (PCE) of 18.26 %, surpassing PM6:BTP-eC9 based binary (17.63 %). This work indicates that the dimerized small molecule donor is able to become a promising third component candidate, which also opens up a unique idea for the construction of efficient ternary organic solar cells.

三元有机太阳能电池(OSCs)是实现高性能 OSCs 的可行且高效的策略。为构建高效的三元有机太阳能电池,开发一种优异的候选第三组分具有重要意义。在这项工作中,我们通过将两个不对称的小分子供体用乙烯基连接起来,智能地设计并合成了一种二聚小分子供体,并将其命名为 DSMD-βV。这种创新的低聚分子 DSMD-βV 不仅与 PM6 和 BTP-eC9 具有互补吸收和级联能级排列,还能在 PM6:BTP-eC9 的基础上调节相分离微形态。因此,基于 PM6:DSMD-βV:BTP-eC9 的三元器件在激子解离、电荷传输和减少重组方面均有改善,从而实现了 18.26% 的优异功率转换效率(PCE),超过了基于 PM6:BTP-eC9 的二元器件(17.63%)。这项工作表明,二聚化小分子供体能够成为一种前景广阔的候选第三组分,这也为构建高效的三元有机太阳能电池开辟了一种独特的思路。
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引用次数: 0
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