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n-Type polythiophene as a hole-blocking layer in inverted organic photodetectors 在倒置有机光电探测器中用作空穴阻挡层的 n 型聚噻吩
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-28 DOI: 10.1016/j.giant.2024.100291
Jiahui Wang , Sihui Deng , Jun Ma , Junli Hu , Jun Liu

Organic photodetectors (OPDs) own unique advantages such as light weight, flexibility, low production cost, tunable detection wavelength, and thus are promising for a variety of applications. The lack of hole-blocking layer (HBL) materials impedes the reduction of dark current density and the enhancement of the performance of OPDs. Herein, we employed an n-type polythiophene n-PT1 as a HBL material for inverted OPDs. The specific solubility of n-PT1 in o-dichlorobenzene facilitates solution processing and enables multilayer device fabrication. The ultradeep-lying highest occupied molecular orbital energy level ensures a large hole injection barrier between cathode and active layer that suppresses dark current. As a result, compared to the control devices without n-PT1, the inverted OPD devices with n-PT1 as HBL demonstrate a two-order-of-magnitude reduction in dark current density and a one-order-of-magnitude increase in specific detectivity. To the best of our knowledge, this is the first solution processable HBL material for inverted OPDs.

有机光电探测器(OPD)具有重量轻、灵活性强、生产成本低、探测波长可调等独特优势,因此在各种应用中大有可为。由于缺乏阻孔层(HBL)材料,阻碍了 OPD 暗电流密度的降低和性能的提高。在此,我们采用 n 型聚噻吩 n-PT1 作为反相 OPD 的 HBL 材料。n-PT1 在邻二氯苯中的特异溶解性有利于溶液加工,并可实现多层器件制造。超深层的最高占据分子轨道能级确保了阴极和活性层之间的大空穴注入势垒,从而抑制了暗电流。因此,与不使用 n-PT1 的对照器件相比,使用 n-PT1 作为 HBL 的反相 OPD 器件的暗电流密度降低了两个数量级,而特定检测率则提高了一个数量级。据我们所知,这是第一种用于倒置 OPD 的可溶液加工 HBL 材料。
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引用次数: 0
Synergistically manipulating the shape of alkyl-chain and asymmetric side groups of non-fullerene acceptors enables organic solar cells to reach 18.5% efficiency 协同操纵非富勒烯受体的烷基链和不对称侧基的形状,使有机太阳能电池的效率达到 18.5%
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-23 DOI: 10.1016/j.giant.2024.100294
Xinyu Tong , Zhenyu Chen , Jingyu Shi , Jinfeng Ge , Wei Song , Yuanyuan Meng , Ziyi Ge

Side-chain modification and asymmetric design for non-fullerene acceptors (NFAs) have been proven to be effective methods for harvesting high-performance organic solar cells (OSCs). Combining the two molecular design strategies, we adopted phenyl chain and alkyl chains with different shapes to develop two novel asymmetric NFAs, named BTP-P2EHC11 and BTP-P2EHC2C4. Compared with BTP-P2EHC2C4 attached 2-ethylhexyl side chain, BTP-P2EHC11 with linear alkyl side chain have slightly red-shifted absorption and intensive absorption strength. Moreover, the PM6:BTP-P2EHC11 blend film presents higher and more balanced charge mobilities, reducing charge recombination, tighter intermolecular packing and more favorable fibrous network morphology with appropriate phase separation than PM6:BTP-P2EHC2C4, which lead to significantly enhanced short-circuit current density (JSC) of PM6:BTP-P2EHC11-based devices. Thus, the OSCs based on PM6:BTP-P2EHC11 achieve a superior power conversion efficiency (PCE) of 18.50% with a good trade-off among open-circuit voltage (VOC) of 0.876 V, JSC of 26.85 mA cm−2 and fill factor (FF) of 78.65%, while PM6:BTP-P2EHC2C4-based device exhibits a lower PCE of 17.49%. Our investigation elucidates that the combination of finely optimizing the shape of alkyl-chain and asymmetric side groups of NFAs could pave a promising avenue toward morphology optimization and performance promotion of OSCs.

非富勒烯受体(NFAs)的侧链修饰和不对称设计已被证明是获得高性能有机太阳能电池(OSCs)的有效方法。结合这两种分子设计策略,我们采用不同形状的苯基链和烷基链开发了两种新型不对称非富勒烯受体,分别命名为 BTP-P2EHC11 和 BTP-P2EHC2C4。与带有 2-乙基己基侧链的 BTP-P2EHC2C4 相比,带有线性烷基侧链的 BTP-P2EHC11 的吸收率略有红移,吸收强度较大。此外,与 PM6:BTP-P2EHC2C4 相比,PM6:BTP-P2EHC11 混合薄膜具有更高更均衡的电荷迁移率、更低的电荷重组、更紧密的分子间堆积和更有利的纤维状网络形态以及适当的相分离,从而显著提高了基于 PM6:BTP-P2EHC11 器件的短路电流密度(JSC)。因此,基于 PM6:BTP-P2EHC11 的 OSC 在开路电压 (VOC) 0.876 V、短路电流密度 (JSC) 26.85 mA cm-2 和填充因子 (FF) 78.65% 之间实现了 18.50% 的出色功率转换效率 (PCE),而基于 PM6:BTP-P2EHC2C4 的器件则表现出 17.49% 的较低 PCE。我们的研究阐明,将烷基链的形状和 NFA 的不对称侧基进行精细优化相结合,可以为 OSC 的形态优化和性能提升铺平道路。
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引用次数: 0
Fatigue failure of soft adhesive systems: A state-of-the-art review 软粘合剂系统的疲劳失效:最新技术综述
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-23 DOI: 10.1016/j.giant.2024.100292
Chengbin Yao , Yan Xia , Zhuoran Yang , Zhongmeng Zhu , Zheyu Li , Han Jiang

Soft adhesive systems (SASs), which consist of a soft adhesive layer and/or soft adherends, have been extensively applied in advanced fields such as biomedicine, flexible electronics, and soft robotics. Understanding the fatigue failure of SASs is crucial for ensuring their structural safety and functional stability, as they are often subjected to fatigue loading. This paper systematically reviews the fatigue failure of SASs, aiming to provide a comprehensive understanding and contribute to the study of fatigue failure mechanisms and lifetime prediction of SASs. The review starts by introducing classical research methods for fatigue failure of adhesive systems, with a focus on total fatigue lifetime and fatigue crack growth (FCG). After summarizing the complexity of fatigue failure in SASs, it provides an overview of fatigue research for the three types of SASs: “soft interface”, “soft adherend”, and “soft-soft” adhesive systems. Then, the relations between the fatigue failure and energy dissipation of various SASs are specifically discussed noting that significant energy dissipation accompanying the cyclic deformation of SASs during fatigue loading can substantially affect the final fatigue failure of SASs. Finally, the current unresolved issues and challenges in this field are presented.

软粘合系统(SAS)由软粘合层和/或软粘合剂组成,已广泛应用于生物医学、柔性电子和软机器人等先进领域。由于 SAS 经常承受疲劳载荷,因此了解 SAS 的疲劳失效对于确保其结构安全和功能稳定性至关重要。本文对 SAS 的疲劳失效进行了系统综述,旨在提供一个全面的理解,为 SAS 的疲劳失效机制研究和寿命预测做出贡献。综述首先介绍了粘合剂系统疲劳失效的经典研究方法,重点是总疲劳寿命和疲劳裂纹增长(FCG)。在总结了 SAS 疲劳破坏的复杂性后,综述了三种类型 SAS 的疲劳研究:"软界面"、"软粘合剂 "和 "软-软 "粘合剂系统。然后,具体讨论了各种 SAS 的疲劳失效与能量耗散之间的关系,指出在疲劳加载过程中伴随 SAS 循环变形的大量能量耗散会对 SAS 的最终疲劳失效产生重大影响。最后,介绍了该领域目前尚未解决的问题和面临的挑战。
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引用次数: 0
Raining-inspired method for construction of porous film material 受雨水启发的多孔薄膜材料构建方法
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-23 DOI: 10.1016/j.giant.2024.100293
Xiaomin Wang , Heyi Pan , Lin Lian , Xiangjun Gong , Yang Wang , Chaoqun Zhang

The low-temperature environment caused by solvent evaporation leads to the condensation of water vapor into water droplets that remain on the surface of the film to form breath figure patterns. The conventional approach to regulate the pore morphology in the breath figure process is to optimize the ambient temperature, humidity, and solution concentration. However, realizing a wide adjustable window of pore size and uniform distribution of the pore are still challenges. Here, inspired by the rainfall phenomenon, we proposed a simple and efficient method called the “raining boxing method” (RBM) for preparing porous films based on exogenously given water droplets as templates. The RBM broadened the adjustable window of pore size (0.6–225 µm in this work) and solved the inherent problem of radial reduction of pore size from the film center to the edge caused by the significant difference in low-temperature duration at different locations accompanying the solvent evaporation process. Furthermore, this method could realize multi-types porous films, including surface porous films, spongy porous films, and honeycomb porous films, and could be universally applied in the casting process of various polymer solutions.

溶剂蒸发造成的低温环境会导致水蒸气凝结成水滴,这些水滴留在薄膜表面,形成呼吸图纹。调节透气图形过程中孔隙形态的传统方法是优化环境温度、湿度和溶液浓度。然而,实现孔隙大小的宽可调窗口和孔隙的均匀分布仍然是一个挑战。在此,我们受降雨现象的启发,提出了一种简单而高效的方法,即 "降雨拳法"(RBM),用于以外加水滴为模板制备多孔薄膜。RBM 拓宽了孔径的可调窗口(本研究中为 0.6-225 µm),解决了溶剂蒸发过程中不同位置低温持续时间的显著差异导致孔径从薄膜中心向边缘径向减小的固有问题。此外,该方法可实现多类型多孔薄膜,包括表面多孔薄膜、海绵状多孔薄膜和蜂窝状多孔薄膜,可普遍应用于各种聚合物溶液的浇铸过程。
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引用次数: 0
Room temperature stable twist-bend nematic materials without crystallization over 1 year 室温下稳定扭弯向列材料 1 年不结晶
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-22 DOI: 10.1016/j.giant.2024.100290
Conglong Yuan , Yuxing Zhan , Huixian Liu , Zhaoyi Wang , Ning Shen , Binghui Liu , Honglong Hu , Zhigang Zheng

The twist-bend nematic (NTB) phase of achiral liquid crystals (LCs) manifests a unique self-assembled heliconical structure with nanometer-scale pitch length, mirroring the chiral symmetry-breaking phenomena in nature, thus sparking widespread research interest. However, the ingenious NTB phase is only stable at high temperatures within a very limited temperature interval, often undergoing inevitable crystallization at low temperatures. Herein, room temperature supercooled NTB material systems composed of meticulously designed LC dimer mixtures with varying molecular curvatures and central flexibility were developed, resulting in complete resistance to crystallization even after 1 year of storage. Furthermore, the proposed NTB material systems demonstrated exceptional compatibility with common nematic LCs, facilitating the tailoring of overall physical parameters, particularly to achieve a sufficiently low bend elastic constant with excellent stability. This work represents a paradigmatic advancement forward in realizing stable NTB phase materials with a broad temperature range and resistance to crystallization, thereby tackling the enduring and seemingly insurmountable challenge while providing impetus for further exploration of their applications in soft matter, crystallography, and advanced photonics.

非手性液晶(LCs)的扭转弯曲向列(NTB)相表现出独特的自组装螺旋结构,其间距长度达到纳米级,反映了自然界中的手性对称破缺现象,因此引发了广泛的研究兴趣。然而,巧妙的 NTB 相只能在非常有限的温度区间内的高温下保持稳定,在低温下往往会发生不可避免的结晶。在此,我们开发了由精心设计的具有不同分子曲率和中心柔性的低聚物二聚体混合物组成的室温过冷 NTB 材料体系,即使在储存一年后也能完全防止结晶。此外,所提出的 NTB 材料体系与普通向列低聚物具有出色的兼容性,有助于定制整体物理参数,特别是实现足够低的弯曲弹性常数和出色的稳定性。这项工作代表了在实现具有宽温度范围和抗结晶性的稳定 NTB 相材料方面取得的典范性进展,从而解决了看似难以克服的持久挑战,同时为进一步探索其在软物质、晶体学和先进光子学中的应用提供了动力。
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引用次数: 0
Anti-impact composite based on shear stiffening gel: Structural design and multifunctional applications 基于剪切加固凝胶的抗冲击复合材料:结构设计与多功能应用
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-17 DOI: 10.1016/j.giant.2024.100285
Yue Yao , Ziyang Fan , Min Sang , Xinglong Gong , Shouhu Xuan

With the development of intelligent protective wearable equipment, flexible materials with impact resistance have become a focus of attention. Shear stiffening gel (SSG) is a flexible smart material that can perceive external force loads and generate mechanical responses, boasting exceptional properties like fast response, adaptability, and self-healing. Since the SSG can absorb a large amount of energy during dynamic impact, it shows remarkable advantages for safety protection applications. During the past decade, there has been strong interests in the research community on the SSG composites and their various applications in cutting-edge fields. In this review, we summarize the recent research achievements of SSG composite, by focusing on the improved properties, enhanced functions, and manifold structures. Meanwhile, we also discuss the practical applications of SSG composite in battery protection, vibration control, intelligent sensing, wearable safety protection, and triboelectric nanogenerator (TENG). Finally, we propose the prospects and challenges for the further development and application of SSG composite in the future.

随着智能防护可穿戴设备的发展,具有抗冲击性能的柔性材料成为人们关注的焦点。剪切增韧凝胶(SSG)是一种柔性智能材料,能够感知外力负载并产生机械响应,具有快速响应、适应性强和自我修复等优异特性。由于 SSG 可以在动态冲击中吸收大量能量,因此在安全保护应用方面具有显著优势。过去十年间,研究界对 SSG 复合材料及其在尖端领域的各种应用产生了浓厚的兴趣。在这篇综述中,我们总结了 SSG 复合材料的最新研究成果,重点关注其性能的改善、功能的增强以及流形结构。同时,我们还讨论了 SSG 复合材料在电池保护、振动控制、智能传感、可穿戴安全保护和三电纳米发电机(TENG)中的实际应用。最后,我们提出了 SSG 复合材料未来进一步发展和应用的前景与挑战。
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引用次数: 0
Biodegradation of microbial plastic poly(3-hydroxybutyrate) in soil ecosystems at different latitudes 不同纬度土壤生态系统中微生物塑料聚(3-羟基丁酸)的生物降解
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-16 DOI: 10.1016/j.giant.2024.100288
Svetlana V. Prudnikova , Evgeniy G. Kiselev , Aleksey V. Demidenko , Ivan V. Nemtsev , Ekaterina I. Shishatskaya , Sabu Thomas , Tatiana G. Volova

The features of the degradation of the "green" plastic poly(3-hydroxybutyrate) [P(3HB)] in the soil of various geographical regions were studied: in red ferralitic soil under tropical conditions (Kerala, India) and in chernozem soil under conditions of a sharply continental climate (Eastern Siberia, Russia). Significant differences in the chemical composition, temperature, and humidity of the studied soils were revealed. The number of bacteria and mycelial fungi in the Siberian chernozem was higher than in the red soil of India, from 2-3 to 10 or more times. The degradation of P(3HB) films in the chernozem occurred faster than in the red soil, which was drier, with a low content of humus and minerals, and fewer microorganisms than the chernozem. The half-life of polymer samples in Siberia and India was 64.8 and 126.4 days, respectively. During degradation, a decrease in the molecular weight and an increase in the degree of crystallinity of polymer samples were revealed, which indicates a more active biodegradation of the amorphous phase of the polymer by soil microorganisms. The primary degraders of the polymer have been isolated and identified, and it has been shown that the complexes of degrading bacteria and fungi in different types of soils did not have common species. Despite the presence of species with pronounced depolymerase activity, the rate of film degradation in red ferralitic soils was slowed down by unfavorable environmental conditions. The obtained results confirm the importance of studying the process of PHA degradation in natural conditions.

研究了 "绿色 "塑料聚(3-羟基丁酸)[P(3HB)]在不同地理区域土壤中的降解特征:热带条件下的红铁质土壤(印度喀拉拉邦)和大陆性气候条件下的切尔诺泽姆土壤(俄罗斯东西伯利亚)。研究发现,所研究土壤的化学成分、温度和湿度存在显著差异。西伯利亚chernozem土壤中的细菌和菌丝真菌数量高于印度红壤,从2-3倍到10倍甚至更多。P(3HB)薄膜在chernozem中的降解速度快于红壤,因为红壤更干燥,腐殖质和矿物质含量低,微生物数量也少于chernozem。西伯利亚和印度聚合物样本的半衰期分别为 64.8 天和 126.4 天。在降解过程中,聚合物样本的分子量下降,结晶度增加,这表明土壤微生物对聚合物无定形相的生物降解更为活跃。聚合物的主要降解者已被分离和鉴定出来,并表明不同类型土壤中降解细菌和真菌的复合体没有共同的物种。尽管存在具有明显解聚酶活性的菌种,但在不利的环境条件下,红铁矿土壤中的薄膜降解速度减慢。研究结果证实了在自然条件下研究 PHA 降解过程的重要性。
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引用次数: 0
Mechanics of single-network hydrogels with network imperfection 具有网络缺陷的单网络水凝胶的力学特性
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-14 DOI: 10.1016/j.giant.2024.100287
Zhi Sheng, Siqi Yan, Jie Ma, Jiabao Bai, Zihang Shen, Zheng Jia

Polymer network is a crucial component of hydrogels, and network imperfection is a prominent feature of polymer networks, significantly influencing the performance of hydrogels. Two essential features of network imperfection are unequal chain lengths and dangling chains, both of which have a significant impact on the mechanical properties of single-network (SN) hydrogels. However, a theoretical framework considering network imperfection in SN hydrogels is still lacking. Here, we propose a theoretical model for SN hydrogels with network imperfection to study the damage behavior during deformation, in which we adopt different chain length distributions to accurately depict the real physical characteristics of the polymer network and incorporate the normalized critical chain force for a more precise measurement of network damage. To verify our theory, we discuss the effects of model parameters on the stress-stretch responses of SN hydrogels and predict the results of uniaxial loading-unloading tests of SN hydrogels, which agree well with experimentally measured stress-stretch behaviors. Finally, we implement the constitutive model into ABAQUS as a user subroutine to study the inhomogeneous deformation of hydrogels.

聚合物网络是水凝胶的重要组成部分,而网络不完善是聚合物网络的一个突出特征,对水凝胶的性能有重大影响。网络不完善的两个基本特征是链长不等和悬链,两者都对单网络(SN)水凝胶的机械性能有重大影响。然而,目前仍缺乏考虑单网络水凝胶中网络不完善的理论框架。我们采用不同的链长分布来准确描述聚合物网络的真实物理特性,并结合归一化临界链力来更精确地测量网络损伤。为了验证我们的理论,我们讨论了模型参数对 SN 水凝胶应力拉伸响应的影响,并预测了 SN 水凝胶单轴加载-卸载试验的结果,结果与实验测量的应力拉伸行为非常吻合。最后,我们将构成模型作为用户子程序应用到 ABAQUS 中,以研究水凝胶的不均匀变形。
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引用次数: 0
Development of a Facile, Versatile and Scalable Fabrication Approach of Solid, Coated, and Dissolving Microneedle Devices for Transdermal Drug Delivery Applications 开发用于透皮给药的固体、涂层和溶解微针设备的简便、多功能和可扩展的制造方法
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-11 DOI: 10.1016/j.giant.2024.100284
Mohammad Hassan Shahriari , Hossein Salmani , Mohammad Akrami , Zeinab Salehi

Nowadays, microneedles as novel transdermal delivery systems are interested in scientists for biomedical applications. This work aims to present a Cascade Microneedle Molding Technique (CMMT) for the reusable fabrication of polydimethylsiloxane (PDMS) molds to produce microneedle devices. To produce a positive master mold from epoxy resin, a negative PDMS mold was first fabricated. PDMS can be molded, and microneedles can be fabricated using this epoxy mold in a scalable and cost-effective manner. These molds were used to manufacture solid, coated, and dissolving microneedles, which were characterized comprehensively. Microneedle morphology and geometry were evaluated using Scanning Electron Microscopy (SEM). The mechanical integrity and ability to insert the microneedle device into the skin were assessed using compression strength analysis and force-displacement measurements. Drug penetration through animal skin was evaluated for Rhodamine B (RhB) loaded microneedles. The depth of needle insertion was also visualized using histological analysis while the spatial distribution of released cargo was determined by using confocal microscopy. Taken together, CMMT offers a simple, rapid, cost-effective, and scalable method for mass-producing microneedles with remarkable properties compared to direct 3D printing or laser ablation.

如今,微针作为新型透皮给药系统在生物医学应用领域受到科学家们的关注。这项研究旨在提出一种级联微针成型技术(CMMT),用于制造可重复使用的聚二甲基硅氧烷(PDMS)模具,以生产微针装置。为了用环氧树脂制作阳模,首先要制作阴模 PDMS。PDMS 可以成型,使用这种环氧树脂模具可以以可扩展和具有成本效益的方式制造微针。这些模具被用来制造固体微针、涂层微针和溶解微针,并对这些微针进行了全面的表征。使用扫描电子显微镜(SEM)对微针的形态和几何形状进行了评估。使用压缩强度分析和力-位移测量法评估了微针装置的机械完整性和插入皮肤的能力。评估了负载罗丹明 B(RhB)的微针在动物皮肤中的药物渗透性。此外,还利用组织学分析观察了微针的插入深度,并利用共聚焦显微镜确定了释放货物的空间分布。综上所述,与直接三维打印或激光烧蚀相比,CMMT 提供了一种简单、快速、经济高效且可扩展的方法,用于大规模生产具有显著特性的微针。
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引用次数: 0
Tuning conditions for the amine-functionalization of carbonyls formed in biobased polyfurfuryl alcohol 生物基聚糠醇中形成的羰基胺功能化的调整条件。
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-11 DOI: 10.1016/j.giant.2024.100283
Pierre Delliere, Nathanael Guigo

Biobased furan resins (furfuryl alcohol based) are functionalized by taking advantage of a side-reaction occurring during its polymerization. The furan ring-opening reactions yields carbonyls which can be functionalized by reaction with primary amines. Light is shed on unexplored parameters impacting the properties of PFA/Amine systems. First, PFA/Amines were prepared using PFA resins at conversion degree between 0.3 and 0.95. Overall, high conversion degrees (0.9 and above) are best suited to produce rigid materials. In addition, a precipitation process may be used to reach high Tg biobased materials (145 °C). Finally, the impact of the amines’ basicity on the properties of PFA/Amines was investigated. The results highlighted that PFAs at conversion degrees above 0.9 are little affected by the basicity. However, the properties of PFA functionalized at lower conversion degrees are strongly affected by the bases, i.e. high brittleness. This can be circumvented by limiting the functionalization degree to 0.25 and below.

生物基呋喃树脂(基于糠醇)是利用其聚合过程中发生的副反应进行功能化的。呋喃开环反应产生的羰基可通过与伯胺反应进行官能化。本研究揭示了影响 PFA/Amine 系统特性的未探索参数。首先,使用转化率在 0.3 至 0.95 之间的 PFA 树脂制备 PFA/胺。总体而言,高转化率(0.9 及以上)最适合生产刚性材料。此外,还可以使用沉淀工艺来达到生物基材料的高 Tg 值(145 °C)。最后,研究了胺的碱性对 PFA/Amines 性能的影响。结果表明,转化率高于 0.9 的 PFA 几乎不受碱性的影响。然而,转化度较低的官能化 PFA 的特性受碱的影响很大,即脆性较高。将官能化程度限制在 0.25 及以下可以避免这种情况。
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引用次数: 0
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