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Multiple Phase Structures and Enhanced Dielectric Properties of Side-Chain Liquid Crystalline Polymer Containing Unique Biaxial Mesogen with Large Dipole Moment 含有大偶极矩独特双轴中间体的侧链液晶聚合物的多相结构和增强的介电性能
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-13 DOI: 10.1016/j.giant.2024.100305
Zi-Fan Yang , Le Zhou , Wei Xia , Lan-Ying Zhang , Huai Yang , Yang Shen , Shuang Yang , Er-Qiang Chen

To achieve all-organic polymer with high dielectric performances, we have designed a novel side-chain liquid crystalline polymer (P7) with strong polar mesogen of (Z)-4-(2-cyano-2-phenylvinyl)benzonitrile (CSCN) attached to polycyclooctene backbone. The bis-cyano-substituted CSCN is board-shaped and exhibits a large dipole moment (8.54 D) which tilts ∼34.2° away from its molecular long axis. Consequently, CSCN shows unique dual molecular anisotropy: one from biaxial shape anisotropy and the other from polarization anisotropy. The complex phase behaviors of P7 were investigated employing mainly the techniques of differential scanning calorimetry and X-ray diffraction. Four liquid crystal (LC) phases are identified as K0, K1, K2 and K3, which are SmA, highly-ordered biaxial SmA, B5-like and B7-like, respectively, with the thermal stability increased in sequence. The experimental results indicate that the different LC phases are arisen from the competition and balance between π-π stacking and dipole-dipole interaction. While the face-to-face π-π stacking is dominant in K0 and K1, optimizing the dipole-dipole interaction causes the CSCN mesogens within the smectic layer to tilt and rotate, resulting in K2 and K3. We further investigated the dielectric properties of P7 films using polarization-electric field loops test. The dielectric constant (εr) of P7 is found to be LC structure dependent, which is increased when the LC phase is varied from K0 to K3. With an average εr of 9.7 achieved in K3 and the low dielectric loss (tan δ = 0.001), P7 film offers a promising material in advanced applications like energy storage and electronic devices.

为了获得具有高介电常数性能的全有机聚合物,我们设计了一种新型侧链液晶聚合物(P7),该聚合物的聚环辛烯骨架上附有强极性介质(Z)-4-(2-氰基-2-苯基乙烯基)苯腈(CSCN)。双氰基取代的 CSCN 呈板状,具有较大的偶极矩(8.54 D),与分子长轴成 34.2° 的倾斜角。因此,CSCN 表现出独特的双分子各向异性:一种来自双轴形状各向异性,另一种来自极化各向异性。研究人员主要采用差示扫描量热法和 X 射线衍射技术对 P7 的复杂相行为进行了研究。确定了四种液晶(LC)相,分别为 K0、K1、K2 和 K3,它们分别是 SmA、高阶双轴 SmA、类 B5 和类 B7,其热稳定性依次增强。实验结果表明,不同的低浓相是由π-π堆叠和偶极-偶极相互作用之间的竞争和平衡引起的。在 K0 和 K1 中,面对面的 π-π 堆叠起主导作用,而优化偶极-偶极相互作用则会导致密相层中的 CSCN 介质倾斜和旋转,从而产生 K2 和 K3。我们利用极化-电场环测试进一步研究了 P7 薄膜的介电性能。我们发现 P7 的介电常数(εr)与 LC 结构有关,当 LC 相从 K0 变为 K3 时,介电常数增大。P7 薄膜在 K3 中的平均εr 值为 9.7,介电损耗较低(tan δ = 0.001),是一种很有前途的材料,可用于储能和电子设备等先进应用领域。
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引用次数: 0
Molecular packing regulation of dopant-free hole transport polymers for efficient perovskite solar cells 用于高效过氧化物太阳能电池的无掺杂空穴传输聚合物的分子填料调节技术
IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-12 DOI: 10.1016/j.giant.2024.100302
Hang Liu , Yuping Gao , Yufei Xin , Hao Zhang , Yu Zou , Xiyue Dong , Yanhong Lu , Qiang Fu , Yongsheng Liu

Spiro-OMeTAD is a primary hole transport material (HTM) employed in most state-of-the-art regular perovskite solar cells (PSCs). The essential reliance on hygroscopic ionic dopants to enhance the conductivity and mobility of Spiro-OMeTAD has dramatically compromised the stability of PSCs. Here, we demonstrated excellent photovoltaic performance of PSCs by developing two dopant-free polymers, namely L1 and L2, using thieno[3,2-b]thiophene as a building block. It is found that the n-hexyl-modified thiophene side chains endow the polymer L2 with favorable crystallinity, unique self-assembly behavior, and a preferable face-on stacking orientation. After the addition of a small amount (10 %) of PM6 to create a polymer alloy named LPA, the above properties were further improved, and the resulting film exhibited a distinct fibrous morphology, resulting in increased hole mobility and effective defect passivation. Consequently, PSCs employing LPA as a dopant-free HTM afforded a high efficiency of 23.81 %. Importantly, LPA-based PSCs exhibit significantly enhanced operational stability with a T80 lifetime of 1572 h at 55 °C. This work provides a crucial guideline for the design of dopant-free polymers, thereby advancing the practical application of PSCs.

大多数最先进的普通过氧化物太阳能电池(PSCs)都采用了螺-OMeTAD 作为主要的空穴传输材料(HTM)。由于必须依赖吸湿性离子掺杂剂来提高斯派罗-OMeTAD 的导电性和迁移率,PSCs 的稳定性大打折扣。在此,我们以噻吩并[3,2-b]噻吩为结构单元,开发了两种不含掺杂剂的聚合物(即 L1 和 L2),从而证明了 PSCs 卓越的光伏性能。研究发现,正己基改性噻吩侧链赋予了聚合物 L2 良好的结晶性、独特的自组装行为和更佳的面对堆积取向。在加入少量(10%)PM6 生成名为 LPA 的聚合物合金后,上述特性得到了进一步改善,生成的薄膜呈现出明显的纤维状形态,从而提高了空穴迁移率并有效地钝化了缺陷。因此,采用 LPA 作为无掺杂 HTM 的 PSC 的效率高达 23.81%。重要的是,基于 LPA 的 PSCs 的工作稳定性显著增强,在 55 °C 下的 T80 寿命达 1572 h。这项研究为无掺杂聚合物的设计提供了重要指导,从而推动了 PSC 的实际应用。
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引用次数: 0
Vacuum-driven orientation of Nanostructured polystyrene-block-Poly(L-lactide) block copolymer thin films for Nanopatterning 真空驱动纳米结构聚苯乙烯-嵌段-聚(L-乳酸)嵌段共聚物薄膜的定向,以实现纳米图案化
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-06 DOI: 10.1016/j.giant.2024.100303
Kang-Ping Liu, Aum Sagar Panda, Wen-Chi Huang, Rong-Ming Ho

Herein, we demonstrate a simple approach to control the orientation of cylinder-forming nanostructures in polystyrene-block-poly(L-lactide) (PS-b-PLLA) BCP thin films through thermal annealing under a high-vacuum environment. Surface tension discrepancy between the constituent blocks is critical in controlling the aimed orientation of self-assembled nanostructures in block copolymer (BCP) thin films. For BCP self-assembly, temperature has been widely utilized as a thermodynamic state variable under ambient pressure conditions, whereas the use of high vacuum (low pressure) for thermal annealing is limited. It has been observed that temperature can alter the surface tension only marginally with increasing temperature for polymeric materials; as a result, the pressure dependence of surface tension for PS and PLLA was investigated. By increasing the vacuum degree during thermal annealing, the surface tension discrepancy between the PS and PLLA blocks can be reduced significantly. Accordingly, during thermal annealing under high vacuum degree, a neutral air polymer interface can be generated for the BCP thin films, resulting in the formation of perpendicular cylinders from the neutral surface of the thin film through BCP microphase separation.

在此,我们展示了一种在高真空环境下通过热退火控制聚苯乙烯-嵌段-聚(L-内酰胺)(PS-b-PLLA)BCP 薄膜中圆柱形纳米结构取向的简单方法。组成嵌段之间的表面张力差异是控制嵌段共聚物(BCP)薄膜中自组装纳米结构定向的关键。在 BCP 自组装过程中,温度已被广泛用作常压条件下的热力学状态变量,而利用高真空(低压)进行热退火则受到限制。据观察,随着温度的升高,温度对高分子材料表面张力的改变微乎其微;因此,我们对 PS 和 PLLA 表面张力的压力依赖性进行了研究。通过在热退火过程中提高真空度,可以显著减少 PS 和 PLLA 块体之间的表面张力差异。因此,在高真空度下进行热退火时,BCP 薄膜可产生中性空气聚合物界面,从而通过 BCP 微相分离从薄膜的中性表面形成垂直的圆柱体。
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引用次数: 0
Polysaccharide-based materials as an eco-friendly alternative in biomedical, environmental, and food packaging 多糖基材料作为生物医学、环境和食品包装的生态友好型替代品
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-06 DOI: 10.1016/j.giant.2024.100301
Zahra Behrooznia, Jhamak Nourmohammadi

The global community has encountered numerous challenges concerning environmental sustainability, encompassing issues like waste generation, depletion of natural resources, air pollution, and other threats to human well-being. Consequently, the pursuit of an eco-friendly environment has emerged as a critical concern in recent years. Polysaccharides, being natural biopolymers, have garnered significant attention owing to their distinctive properties that make them versatile for various applications. Numerous sustainable and environmentally friendly polysaccharides, such as chitosan, cellulose, starch, hyaluronic acid, alginate, and inulin, have been identified. This article highlights the characteristics of renewable polysaccharides, their categorization, and their potential to contribute to environmental sustainability. It introduces environmentally friendly extraction methods aimed at minimizing chemical pollution. Through the careful selection of diverse polysaccharides and the application of functionalization techniques, the article suggests the possibility of obtaining suitable superabsorbent hydrogels, appropriate nanocomposites, and effective scaffolds. The significance of utilizing polysaccharide-based materials is explored in detail, emphasizing their exceptional properties. Additionally, the article discusses the various applications of eco-friendly polysaccharides as sustainable polymers, including in agriculture, biomedicine, and food packaging.

全球社会在环境可持续性方面遇到了诸多挑战,包括废物产生、自然资源枯竭、空气污染等问题,以及对人类福祉的其他威胁。因此,追求生态友好型环境已成为近年来人们关注的一个重要问题。作为天然生物聚合物,多糖因其独特的特性而备受关注,这些特性使其具有多种用途。目前已发现许多可持续的环保型多糖,如壳聚糖、纤维素、淀粉、透明质酸、海藻酸和菊粉。本文重点介绍了可再生多糖的特点、分类及其促进环境可持续发展的潜力。文章介绍了旨在尽量减少化学污染的环境友好型提取方法。通过精心挑选各种多糖并应用功能化技术,文章提出了获得合适的超吸水性水凝胶、适当的纳米复合材料和有效支架的可能性。文章详细探讨了利用多糖类材料的意义,强调了它们的特殊性能。此外,文章还讨论了生态友好型多糖作为可持续聚合物在农业、生物医学和食品包装等领域的各种应用。
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引用次数: 0
Shape-memory and self-healing properties of sustainable cellulosic nanofibers-based hybrid materials for novel applications 用于新型应用的可持续纤维素纳米纤维基混合材料的形状记忆和自愈合特性
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-05 DOI: 10.1016/j.giant.2024.100299
Muhammad Yasir Khalid , Zia Ullah Arif , Ans Al Rashid , Syed Muhammad Zubair Shah Bukhari , Mokarram Hossain , Muammer Koç

In the era of smart and sustainable technology driven by naturally occurring materials, various nanocellulose-based materials play a crucial role. Shape memory behaviour and self-healing capabilities of nanocelluloses are emerging as focal points in numerous research domains. Nanocellulose and its derivatives such as cellulose nanocrystals (CNC) and cellulose nanofibers (CNF), are currently in the limelight due to their excellent shape-memory and self-healing properties, making them suitable for multifunctional devices. In this regard, CNF, as a cutting-edge material, has spurred researchers to explore its potential in developing contemporary multifunctional and personalized health devices. Therefore, a timely and comprehensive review is essential to gain deep insights into the effectiveness of shape-memory and self-healing capabilities of CNF for multifunctional devices. Herein, we first provide a brief introduction to all nanocellulose materials. This review also depicts recent advancements and breakthroughs in the large and effective synthesis of CNF-based hybrid materials. Next, focusing on their self-healing and shape-memory performance, this review sheds new light on the advanced applications of CNF materials. Finally, perspectives on the current challenges and opportunities in this field are summarized for future researchers to gain an in-depth understanding of CNF-based smart and sustainable materials.

在由天然材料驱动的智能和可持续技术时代,各种以纳米纤维素为基础的材料发挥着至关重要的作用。纳米纤维素的形状记忆行为和自愈能力正成为众多研究领域的焦点。纳米纤维素及其衍生物,如纤维素纳米晶体(CNC)和纤维素纳米纤维(CNF),因其优异的形状记忆和自愈性能,使其成为多功能设备的理想材料,目前正备受瞩目。在这方面,CNF 作为一种前沿材料,促使研究人员探索其在开发当代多功能和个性化健康设备方面的潜力。因此,为了深入了解 CNF 在多功能设备中的形状记忆和自修复功能的有效性,及时进行全面综述至关重要。在此,我们首先简要介绍了所有纳米纤维素材料。这篇综述还描述了最近在大规模有效合成 CNF 基混合材料方面取得的进展和突破。接下来,本综述将重点关注 CNF 材料的自愈合和形状记忆性能,为 CNF 材料的先进应用提供新的启示。最后,本综述总结了该领域当前面临的挑战和机遇,供未来研究人员深入了解基于 CNF 的智能和可持续材料。
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引用次数: 0
Biopolymer networks packed with microgels combine strain stiffening and shape programmability 含有微凝胶的生物聚合物网络兼具应变刚性和形状可编程性
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-03 DOI: 10.1016/j.giant.2024.100297
Vignesh Subramaniam , Abhishek M. Shetty , Steven J. Chisolm , Taylor R. Lansberry , Anjana Balachandar , Cameron D. Morley , Thomas E. Angelini

Biomaterials that can be reversibly stiffened and shaped could be useful in broad biomedical applications where form-fitting scaffolds are needed. Here we investigate the combination of strong non-linear elasticity in biopolymer networks with the reconfigurability of packed hydrogel particles within a composite biomaterial. By packing microgels into collagen-1 networks and characterizing their linear and non-linear material properties, we empirically determine a scaling relationship that describes the synergistic dependence of the material's linear elastic shear modulus on the concentration of both components. We perform high-strain rheological tests and find that the materials strain stiffen and also exhibit a form of programmability, where no applied stress is required to maintain stiffened states of deformation after large strains are applied. We demonstrate that this non-linear rheological behavior can be used to shape samples that do not spontaneously relax large-scale bends, holding their deformed shapes for days. Detailed analysis of the frequency-dependent rheology reveals an unexpected connection to the rheology of living cells, where models of soft glasses capture their low-frequency behaviors and polymer elasticity models capture their high-frequency behaviors.

可以可逆地硬化和塑形的生物材料可广泛应用于需要塑形支架的生物医学领域。在这里,我们研究了生物聚合物网络中的强非线性弹性与复合生物材料中包装水凝胶颗粒的可重构性的结合。通过将微凝胶填充到胶原蛋白-1 网络中并表征其线性和非线性材料特性,我们根据经验确定了一种比例关系,该关系描述了材料的线性弹性剪切模量对两种成分浓度的协同依赖性。我们进行了高应变流变测试,发现材料在应变变硬的同时,还表现出一种可编程性,即在施加大应变后,无需施加应力即可维持变硬的变形状态。我们证明,这种非线性流变行为可用于塑造不会自发松弛大规模弯曲的样品,使其变形形状保持数天之久。对频率相关流变学的详细分析揭示了与活细胞流变学之间意想不到的联系,其中软玻璃模型捕捉了它们的低频行为,而聚合物弹性模型则捕捉了它们的高频行为。
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引用次数: 0
Marine biomaterials for sustainable bone regeneration 用于可持续骨再生的海洋生物材料
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-03 DOI: 10.1016/j.giant.2024.100298
Haowei Wang , Xinyu Li , Mingcheng Xuan , Ren Yang , Jianhui Zhang , Jinke Chang

The field of bone regeneration has witnessed significant advancements with the exploration and incorporation of marine biomaterials, offering promising avenues for orthopaedic and dental applications. Marine environments are a rich source of biological materials with unique properties conducive to bone healing and regeneration. Repurposing and reusing some waste by-products of marine products for bone regeneration not only contribute to environmental protection but also drives the development of the marine economy, thereby achieving sustainable development. Moreover, the lower production costs associated with the abundant availability and easy processing of marine biomaterials make bone regeneration therapies more accessible to a broader population, enhancing global health equity. By exploring the current research progressions on marine biomaterials and recounting their sources, properties, mechanisms of action, and applications in bone regeneration research, this review provides a comprehensive overview of the potential and challenges of marine biomaterials for future bone healing and regeneration applications.

随着海洋生物材料的探索和应用,骨再生领域取得了重大进展,为整形外科和牙科应用提供了前景广阔的途径。海洋环境中蕴藏着丰富的生物材料,其独特的特性有利于骨骼的愈合和再生。将海洋产品的一些废弃副产品再利用和再循环用于骨再生,不仅有助于环境保护,还能推动海洋经济的发展,从而实现可持续发展。此外,由于海洋生物材料丰富且易于加工,生产成本较低,因此骨再生疗法更容易被更多人接受,从而提高了全球健康公平性。本综述通过探讨当前海洋生物材料的研究进展,阐述其来源、特性、作用机制以及在骨再生研究中的应用,全面概述了海洋生物材料在未来骨愈合和再生应用中的潜力和挑战。
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引用次数: 0
Skin-like breathable wound dressings with antimicrobial and hemostatic properties 具有抗菌和止血功能的类肤透气伤口敷料
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-03 DOI: 10.1016/j.giant.2024.100300
Hanbai Wu , Chuanwei Zhi , Yuhan Chen , Xiong Zhou , Cong Wang , Raymond H.W. Lam , Tingwu Qin , Guibing Fu , Zhu Xiong , Kaisong Huang , Jia-Horng Lin , Shuo Shi , Jinlian Hu

Wound healing requires a contamination-free, sterile, and breathable environment. However, to develop an ideal wound dressing with all these functionalities simultaneously poses significant challenges. In this study, we designed a wound dressing that mimics the structure of skin with good breathability and protective functions. The wound dressing consists of a hydrophilic Poly(3-hydroxybutyrate-co-4-hydroxybutyrate) (P34HB) membrane coated with zinc oxide nanoparticles and a hydrophobic polyvinylidene fluoride (PVDF) membrane. Meanwhile, plasma treatment was also utilized to bond the two layers, resulting in an enhancement of 60 % in mechanical properties. The crosslinked fibrous membranes exhibited uniform stress distribution when stretching. Due to the unique structures of the wound dressing, it demonstrates wound exudate management, antibacterial functions, and hemostatic properties. The hydrophobic layer guided wound exudate towards the hydrophilic layer and the zinc oxide nanoparticles acted as a barrier against external bacteria and released zinc ions to inhibit bacterial growth in the exudate. Moreover, the water vapor transmission rate (WVTR) was measured to be over 86.55 kg/m2/day, the hemolysis rate was 2.38 %, and an impressive 81.98 % healing rate was recorded during in vitro wound healing. This skin-mimicking wound dressing shows great potential as a promising solution for the therapy of chronic wounds and infections.

伤口愈合需要一个无污染、无菌和透气的环境。然而,要开发一种同时具备所有这些功能的理想伤口敷料却面临着巨大的挑战。在这项研究中,我们设计了一种模仿皮肤结构、具有良好透气性和保护功能的伤口敷料。该伤口敷料由亲水性聚(3-羟基丁酸-4-羟基丁酸)(P34HB)膜和疏水性聚偏二氟乙烯(PVDF)膜组成,前者涂有纳米氧化锌颗粒。同时,还利用等离子处理将两层膜粘合在一起,从而使机械性能提高了 60%。交联纤维膜在拉伸时表现出均匀的应力分布。由于伤口敷料的独特结构,它具有伤口渗液管理、抗菌和止血功能。疏水层能引导伤口渗出物流向亲水层,而纳米氧化锌颗粒则能阻挡外部细菌,并释放锌离子抑制渗出物中的细菌生长。此外,经测量,水蒸气透过率(WVTR)超过 86.55 千克/平方米/天,溶血率为 2.38%,体外伤口愈合率高达 81.98%。这种仿皮伤口敷料显示出巨大的潜力,是治疗慢性伤口和感染的理想解决方案。
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引用次数: 0
Sustainable foams from hemp, lignin, xylan, pectin, and glycerol: tunable via reversible citric acid crosslinking for absorption and insulation applications 由大麻、木质素、木聚糖、果胶和甘油制成的可持续泡沫:可通过可逆柠檬酸交联进行调节,用于吸收和隔热应用
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-30 DOI: 10.1016/j.giant.2024.100295
Sergejs Beluns , Oskars Platnieks , Maksims Jurinovs , Rinalds Buss , Sergejs Gaidukovs , Liga Orlova , Olesja Starkova , Vijay Kumar Thakur

This study investigates the development of sustainable multifunctional foams utilizing hemp stalk waste, lignin, xylan, pectin, glycerol, and citric acid. Using the freeze-drying method for foam formation in combination with industrial waste products and renewable resources, we emphasize a green, scalable material development approach. In total, 25 distinct formulations were prepared and methodically examined, mainly focusing on the roles of citric acid, pectin, and glycerol. Thermal crosslinking, conducted at 140°C, was analyzed using FTIR, confirming the formation of ester bonds. The microstructural characterization of the foams revealed distinct variations from nanofibrillar to microfibrillar structures based on composition. The bulk density of the foams ranged from 13 to 152 mg/cm3, and porosity values varied from 97 % to 99 % for most of the compositions. Foams showed up to 50 g/g water, 51 g/g rapeseed oil, and 46 g/g kerosine absorption. Foam absorption capacity changes were examined through 10 iterative cycles in water, demonstrating that most compositions retained near-original absorption capacities. Adding glycerol conferred exceptional hydrophobic properties to the foam surfaces, as evidenced by water contact angles ranging between 140° and 150°. The thermal conductivity of foams ranged from 0.040 to 0.046 W/mK. The mechanical properties of foams were assessed using compression testing, which showed highly tunable structures ranging from soft to rigid. This study illustrates the broad applicability of these foams, emphasizing their utility in thermal insulation, filtration systems, and environmental cleanup, among other potential uses.

本研究调查了利用麻杆废料、木质素、木聚糖、果胶、甘油和柠檬酸开发可持续多功能泡沫的情况。我们采用冷冻干燥法形成泡沫,并结合工业废品和可再生资源,强调一种绿色、可扩展的材料开发方法。我们总共制备了 25 种不同的配方并进行了方法学研究,主要侧重于柠檬酸、果胶和甘油的作用。利用傅立叶变换红外光谱分析了在 140°C 温度下进行的热交联,确认了酯键的形成。泡沫的微观结构特征显示,根据成分的不同,从纳米纤丝结构到微纤丝结构存在明显的差异。泡沫的体积密度从 13 到 152 mg/cm3 不等,大多数成分的孔隙率从 97% 到 99% 不等。泡沫对水、菜籽油和煤油的吸收率分别高达 50 克/克、51 克/克和 46 克/克。通过在水中反复循环 10 次,对泡沫吸收能力的变化进行了检测,结果表明大多数成分都保持了接近原始的吸收能力。添加甘油可使泡沫表面具有特殊的疏水特性,水接触角在 140° 和 150° 之间就是证明。泡沫的导热系数在 0.040 到 0.046 W/mK 之间。通过压缩测试评估了泡沫的机械性能,结果表明泡沫结构从柔软到坚硬,具有很强的可调性。这项研究说明了这些泡沫的广泛适用性,强调了它们在隔热、过滤系统和环境清洁等方面的用途。
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引用次数: 0
Converting “sliding” to “rolling” design for high-performance lubricating hydrogel 将高性能润滑水凝胶的 "滑动 "设计转变为 "滚动 "设计
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-29 DOI: 10.1016/j.giant.2024.100296
Fangbin Fan , Jinrui Han , Li Zhao , Bo Yu , Meirong Cai , Xiaowei Pei , Zhizhi Zhang , Shuanhong Ma , Yanfei Ma , Feng Zhou

Despite the excellent lubricity of conventional hydrogel materials due to their wet-soft properties, they produce severe mechanical elastic deformation at higher interfacial contact stresses. Balancing the load-bearing capacity and lubricating properties of hydrogel material is the difficulty of the current research work for articular cartilage substitutes. Great progress has been made in developing bionic joint materials with high load-bearing and low-friction hydrogels based on gradient designs. However, most bionic materials are based on sliding friction greatly limiting the improvement of lubrication performance. Herein, we designed and prepared a new hydrogel material with high load-bearing capacity and stable lubrication performance, breaking through the traditional friction method and turning to “sliding” for “rolling”. The network on the hydrogel surface was dissociated by UV irradiation and the pores on the surface were filled with SiO2 nanoparticles. The dense network structure of the underlying layer endows the hydrogel material with good load-bearing properties, while the high degree of hydration of the surface layer and the rolling friction effect of SiO2 nanoparticles greatly enhance the lubrication property. With the synergistic effect of these designs, the multi-layered hydrogel with nanoparticles on the surface achieved an ultra-low average coefficient of friction (COF) of ∼0.00809 at a high load of 50 N during 30,000 cycles. This idea of hydrogel material design provides a new strategy for the replacement of biomimetic articular cartilage materials.

尽管传统的水凝胶材料因其湿软特性而具有极佳的润滑性,但在较高的界面接触应力下会产生严重的机械弹性变形。如何平衡水凝胶材料的承重能力和润滑特性,是目前关节软骨替代品研究工作的难点。基于梯度设计的高承重、低摩擦水凝胶仿生关节材料的开发取得了很大进展。然而,大多数仿生材料都是基于滑动摩擦,大大限制了润滑性能的提高。在此,我们设计制备了一种具有高承载能力和稳定润滑性能的新型水凝胶材料,突破了传统的摩擦方式,变 "滑动 "为 "滚动"。通过紫外线照射,水凝胶表面的网络被解离,表面的孔隙被二氧化硅纳米颗粒填充。底层致密的网络结构赋予了水凝胶材料良好的承重性能,而表层的高水合度和 SiO2 纳米粒子的滚动摩擦效应则大大增强了其润滑性能。在这些设计的协同作用下,表面含有纳米颗粒的多层水凝胶在 30,000 次循环中承受 50 N 的高负载时,实现了 0.00809 ∼ 0.00809 的超低平均摩擦系数(COF)。这种水凝胶材料设计理念为替代仿生物关节软骨材料提供了一种新策略。
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