assembly

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  • 文章类型: Journal Article
    4-硝基苯酚(4-NP)的高效催化还原是工业和实际工程研究的热点之一。因为4-NP是生态环境和人类健康最重要的污染源之一。这里,通过一步合成方法成功开发了柱[5]芳烃(P5A)和金纳米颗粒(AuNPs)的共组装混合复合材料,作为一种用于还原4-NP的水不溶性催化剂。几何和拓扑结构,以及AuNPs/P5A复合催化剂的理化性质,通过透射电子显微镜(TEM)等各种测试进行了充分的表征和分析,X射线衍射(XRD)和傅里叶变换红外光谱(FTIR),这表明AuNP很好地分散在组装的P5A的二维膜的表面上。对4-NP催化还原的影响因素进行了进一步的研究和讨论,证实了在催化过程中AuNP的含量和4-NP的浓度非常显著。在30°C下,在100mg·L-1的催化剂浓度和90mg·L-1的初始4-NP浓度下进行催化反应。计算的反应速率常数为0.3959min-1,4-NP在20min内的还原率大于95%。此外,所制备的催化剂在5次循环后仍能保持较高的催化效率。因此,易回收的复合催化剂水溶液较差,可用于水中4-NP的处理。
    Efficient catalytic reduction of 4-nitrophenol (4-NP) is one focus of industry and practical engineering, because 4-NP is one of the most important sources of pollution of the ecological environment and human health. Here, coassembled hybrid composites of pillar[5]arene (P5A) and gold nanoparticles (Au NPs) were successfully developed by a one-step synthetic method as a type of water-insoluble catalyst for the reduction of 4-NP. The geometric and topological structures, as well as physiochemical properties of Au NPs/P5A composite catalyst, were fully characterized and analyzed through various tests such as transmission electron microscopy (TEM), X-ray diffraction (XRD), and Fourier-transform infrared spectroscopy (FTIR), indicating that Au NPs were well dispersed on the surface of the two-dimensional film of assembled P5A. The influence factors of the catalytic reduction of 4-NP were further investigated and discussed, confirming that the content of Au NPs and the concentration of 4-NP were very significant during the catalysis. The catalytic reaction was carried out at the catalyst concentration of 100 mg·L-1 and an initial 4-NP concentration of 90 mg·L-1 under 30 °C. The calculated reaction rate constant was 0.3959 min-1 and the reduction rate of 4-NP was more than 95% in 20 min. In addition, the as-prepared catalyst can maintain a high catalytic efficiency after five cycles. Thus, the easily recyclable composite catalyst with poor aqueous solution can exhibit prospective application to the treatment of 4-NP in water.
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  • 文章类型: Journal Article
    协同相互作用凝胶(SIG)可以通过混合魔芋葡甘露聚糖(KGM)和κ-角叉菜胶,并已用于修饰和改善食品体系的流变学和质地特性。然而,它们之间的组装行为尚不清楚。这项工作表明,KGM的存在可能通过促进熵增加来促进附近κ-角叉菜胶分子的相变。随后,κ-角叉菜胶的其余部分转化为螺旋结构,组装成一系列横向排列的三角单元,并形成一个三维网络。在KGM/κ-角叉菜胶SIG中,随着KGM含量的增加,聚集体中高密度域(Ξ)的大小和这些高密度域(ζ)的距离先变窄,然后增大。这些纳米级结构特征导致比例为1:9(K1C9)和3:7(K3C7)的KGM/κ-角叉菜胶SIG的相对较高的凝胶强度。这项研究有助于促进具有必要性能特征的SIG的设计和生产。
    The synergistic interaction gels (SIGs) can be created by blending konjac glucomannan (KGM) and κ-carrageenan, and have been applied to modify and improve the rheological and texture properties of food system. However, the assembly behaviors between them are still unclear. This work revealed that the presence of KGM promoted phase transition of nearby κ-carrageenan molecules probably by contributing to entropy increment. Subsequently, the rest of κ-carrageenan transformed into helical structure, assembled into a series of laterally arranged trigonal units and formed a three-dimensional network. In KGM/κ-carrageenan SIGs, the size of high density domains (Ξ) in aggregates and the distance of these high density domains (ξ) were narrowed firstly and then enlarged as increasing of KGM content. These nano-scale structure features were responsible for the relative higher gel strength for KGM/κ-carrageenan SIGs with proportion ratios of 1:9 (K1C9) and 3:7 (K3C7). This study serves to facilitate the design and production of SIGs with the requisite performance characteristics.
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  • 文章类型: Journal Article
    微/纳米马达代表一类有前途的药物递送载体,能够将周围的化学能或外部能转化为机械动力,实现自主运动。它们独特的自主推进力使它们区别于其他航母,为增强药物在细胞和组织屏障中的渗透提供了巨大的潜力。全面了解具有各种电源的微/纳米运动动力学对于促进其从概念验证到临床应用的过渡至关重要。在这次审查中,微型/纳米马达根据其能量来源分为三类:内源性刺激,外生刺激,活细胞驱动。该综述总结了在这些能源下控制微/纳米运动的机制,并探讨了影响自主运动的因素。此外,它讨论了控制微/纳米运动的方法,涵盖与它们的结构相关的方面,composition,和环境因素。微/纳米马达所表现出的显着推进力使它们对重要的生物医学应用有价值,包括肿瘤治疗,生物检测,细菌感染治疗,炎症治疗,胃肠疾病治疗,和环境修复。最后,该综述讨论了微/纳米马达应用的挑战和前景。总的来说,这篇综述强调了微/纳米马达在克服生物障碍和增强治疗功效方面的转化潜力,突出了它们在各个生物医学领域的有前途的临床应用。
    Micro/nanomotors represent a promising class of drug delivery carriers capable of converting surrounding chemical or external energy into mechanical power, enabling autonomous movement. Their distinct autonomous propulsive force distinguishes them from other carriers, offering significant potential for enhancing drug penetration across cellular and tissue barriers. A comprehensive understanding of micro/nanomotor dynamics with various power sources is crucial to facilitate their transition from proof-of-concept to clinical application. In this review, micro/nanomotors are categorized into three classes based on their energy sources: endogenously stimulated, exogenously stimulated, and live cell-driven. The review summarizes the mechanisms governing micro/nanomotor movements under these energy sources and explores factors influencing autonomous motion. Furthermore, it discusses methods for controlling micro/nanomotor movement, encompassing aspects related to their structure, composition, and environmental factors. The remarkable propulsive force exhibited by micro/nanomotors makes them valuable for significant biomedical applications, including tumor therapy, bio-detection, bacterial infection therapy, inflammation therapy, gastrointestinal disease therapy, and environmental remediation. Finally, the review addresses the challenges and prospects for the application of micro/nanomotors. Overall, this review emphasizes the transformative potential of micro/nanomotors in overcoming biological barriers and enhancing therapeutic efficacy, highlighting their promising clinical applications across various biomedical fields.
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  • 文章类型: Journal Article
    精确控制金属纳米粒子(NP)在嵌段共聚物中的空间分布和排列对于制造具有所需光学和电子性能的新型纳米材料非常重要。在这里,我们开发了一种简单而通用的策略来制备由乳液液滴中的聚苯乙烯-嵌段-聚(4-乙烯基吡啶)(PS-b-P4VP)和PS系金纳米颗粒(AuNPs@PS)共组装形成的有机/无机纳米片。嵌段共聚物(BCP)/AuNP纳米片内的AuNP@PS结构单元的排列可以通过调节有效尺寸比(λeff)来调节,这可以通过AuNP的核心直径和PS的分子量来控制。此外,AuNP的含量也是操纵具有特定λeff的纳米片结构的另一个基本参数。因此,通过调整λeff和AuNP的含量,成功制备了具有可控分布和AuNP排列的BCP/AuNP杂化纳米片。这项研究提供了一种简单的方法来制造有序的混合纳米片。
    Precisely controlling the spatial distributions and arrangements of metal nanoparticles (NPs) into block copolymers is of great importance for fabricating novel nanomaterials with the desired optical and electronic properties. Herein, we develop a simple yet versatile strategy to prepare organic/inorganic nanosheets formed by the coassembly of polystyrene-block-poly(4-vinylpyridine) (PS-b-P4VP) and PS tethered gold nanoparticles (AuNPs@PS) within emulsion droplets. The arrangement of the AuNPs@PS building blocks within the block copolymers (BCP)/AuNPs nanosheets can be adjusted by tuning the effective size ratio (λeff), which can be controlled by the core diameter of the AuNPs and the molecular weight of the PS. Furthermore, the content of the AuNPs is also another essential parameter to manipulate the structures of the nanosheets with the specific λeff. Thus, the BCP/AuNPs hybrid nanosheets with controllable distributions and arrangements of the AuNPs were successfully prepared via tuning of λeff and the content of AuNPs. This study provides a facile way to fabricate well-ordered hybrid nanosheets.
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  • 文章类型: Journal Article
    已经开发了体内自组装策略以改善抗癌药物在肿瘤组织中的富集和长期保留。然而,大多数具有非共价键相互作用的自组装体对复杂的生理环境敏感,导致弱的稳定性和生物功能的丧失。这里,我们开发了一种耦合诱导组装(CIA)策略来产生共价交联的纳米纤维,用于在线粒体上原位构建人工外壳。合成了氧化响应肽-卟啉缀合物P1,自组装成纳米粒子。在线粒体的氧化微环境下,P1中硫醇的偶联导致二聚体的形成,其进一步有序并堆叠成交联的纳米纤维。因此,由于结合位点的增加,人工壳通过多价协同相互作用有效地构建在线粒体上。在超声(US)照射下,壳中的卟啉分子产生大量的活性氧(ROS),作用于相邻的线粒体膜,在体外和体内表现出比纳米颗粒高~2倍的抗肿瘤活性。因此,线粒体靶向CIA策略为改进的声动力疗法(SDT)提供了新的视角,并显示了在抗肿瘤治疗中的潜在应用.
    The strategy of in vivo self-assembly has been developed for improved enrichment and long-term retention of anticancer drug in tumor tissues. However, most self-assemblies with non-covalent bonding interactions are susceptible to complex physiological environments, leading to weak stability and loss of biological function. Here, we develop a coupling-induced assembly (CIA) strategy to generate covalently crosslinked nanofibers, which is applied for in situ constructing artificial shell on mitochondria. The oxidation-responsive peptide-porphyrin conjugate P1 is synthesized, which self-assemble into nanoparticles. Under the oxidative microenvironment of mitochondria, the coupling of thiols in P1 causes the formation of dimers, which is further ordered and stacked into crosslinked nanofibers. As a result, the artificial shell is constructed on the mitochondria efficiently through multivalent cooperative interactions due to the increased binding sites. Under ultrasound (US) irradiation, the porphyrin molecules in the shell produce a large amount of reactive oxygen species (ROS) that act on the adjacent mitochondrial membrane, exhibiting ~2-fold higher antitumor activity than nanoparticles in vitro and in vivo. Therefore, the mitochondria-targeted CIA strategy provides a novel perspective on improved sonodynamic therapy (SDT) and shows potential applications in antitumor therapies.
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  • 文章类型: Journal Article
    在这里,氧化的3,3\',开发了5,5'-四甲基联苯胺(oxTMB)纳米带,以增强H2O2的比色和纸基传感。研究发现,Na2SO4试剂中的少量Fe2成分可以催化H2O2将TMB氧化为带正电荷的oxTMB,通过与SO42-的静电相互作用进一步组装成深蓝色的oxTMB纳米带。源自oxTMB纳米带的吸收和散射的消光被用于定量检测H2O2,具有宽的线性检测范围(1.0-300μM)和低的检测限(0.48μM)。此外,在纸基比色阵列的测试区中没有观察到咖啡环效应,有利于肉眼判断颜色。最后,采用比色法检测隐形眼镜护理液中的H2O2。这项工作不仅提出了一种新的H2O2比色传感平台,而且还强调了试剂中的次要成分可能会影响实验结果。
    Herein, oxidized 3,3\',5,5\'-tetramethylbenzidine (oxTMB) nanobelts were developed to enhance the colorimetric and paper-based sensing of H2O2. It was found that the minor component of Fe2+ in Na2SO4 reagent could catalyze the oxidization of TMB by H2O2 into positively charged oxTMB, which was further assembled into dark blue oxTMB nanobelts via electrostatic interaction with SO42-. The extinction originating from the absorption and scattering of oxTMB nanobelts was utilized to quantitatively detect H2O2 with a wide linear detection range (1.0-300 μM) and a low limit of detection (0.48 μM). In addition, no coffee-ring effect was observed in the test zone of the paper-based colorimetric array, which was beneficial to judge the color by naked eye. Finally, the colorimetric method was applied to detect H2O2 in contact lens care solution. This work not only proposed a new colorimetric sensing platform for H2O2, but also highlighted the minor component in the reagent might influence the experimental result.
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  • 文章类型: Journal Article
    具有可编码特性的光子异质结构作为微型和纳米级的通用信息载体已显示出巨大的价值。这些异质结构通常通过逐步生长或后官能化方法来制备,以实现不同结构单元之间的不同发射颜色。为了实现高通量、多变量信息加载,我们在这里报告了一种将极化信号集成到光子异质结中的策略。通过强的分子间Pt····Pt相互作用,将U形di-Pt(II)配合物组装成高度极化的黄色磷光晶体微棒(Y棒)。在最终引发引入的CH2Cl2溶剂的解吸后,Y棒以多米诺方式转化为具有交替的红-黄-红发射或红色磷光微棒(R棒)的三块极化光子异质结(PPH)。这些结构的红色发射也是高度极化的;然而,它们的偏振方向与Y棒的黄色磷光方向正交。借助图案化的掩模,通过侧向允许的CH2Cl2蒸气吸附,将R-rod进一步编程为具有精确控制的嵌段尺寸的多嵌段PPH。X射线衍射分析和理论计算表明,分子内和分子间激发态的溶剂调节调制对于这些PPH的构建至关重要。
    Photonic heterostructures with codable properties have shown great values as versatile information carriers at the micro and nanoscale. These heterostructures are typically prepared by a step-by-step growth or post-functionalization method to achieve varied emission colors among different building blocks. In order to realize high-throughput and multivariate information loading, we report here a strategy to integrate polarization signals into photonic heterojunctions. A U-shaped di-Pt(II) complex is assembled into highly-polarized yellow-phosphorescent crystalline microrods (Y-rod) by strong intermolecular Pt···Pt interaction. Upon end-initiated desorption of the incorporated CH2Cl2 solvents, Y-rod is transformed in a domino fashion into tri-block polarized photonic heterojunctions (PPHs) with alternate red-yellow-red emissions or red-phosphorescent microrods (R-rod). The red emissions of these structures are also highly polarized; however, their polarization directions are just orthogonal to those of the yellow phosphorescence of Y-rod. With the aid of a patterned mask, R-rod is further programmed into multi-block PPHs with precisely-controlled block sizes by side-allowed adsorption of CH2Cl2 vapor. X-ray diffraction analysis and theoretical calculations suggest that the solvent-regulated modulation of intramolecular and intermolecular excited states is critical for the construction of these PPHs.
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  • 文章类型: Journal Article
    未经结构修饰的治疗剂的自组装超分子水凝胶在生物医学应用中具有重要意义。然而,治疗分子的复杂构象和难以捉摸的相互作用限制了水凝胶的受控组装。与散装水溶液中的分子相比,界面处的分子可能具有不同的排列和组装。这可能会改变超分子多晶型物的选择性。然而,这种影响仍然没有得到很好的理解。这里,我们展示了用于水凝胶的界面诱导的纤维自组装,这与本体水溶液中的球形聚集体不同,使用头孢拉定(CEP)作为模型化合物。这种现象是由各向异性分子在界面处堆积引起的,它可用于控制超分子多态性,以直接自组装治疗剂的水凝胶。界面诱导的水凝胶表现出高度的可调节释放和长效杀菌效果。
    Self-assembled supermolecular hydrogels of therapeutic agents without structural modification are of great significance in biomedical applications. Nevertheless, the complex conformations and elusive interactions of therapeutic molecules limit the controlled assembly of hydrogels. Molecules at the interface might have different arrangements and assemblies compared to those in bulk aqueous solution, which could potentially alter the selectivity of supramolecular polymorphs. However, this effect is still not well understood. Here, we demonstrate the interface-induced self-assembly of fibers for hydrogels, which is distinct from the spherical aggregates in the bulk aqueous solution, using cephradine (CEP) as a model compound. This phenomenon is caused by the packing of anisotropic molecules at the interface, and it can be applied to control the supramolecular polymorphism for the direct self-assembly of hydrogels of therapeutic agents. The interface-induced hydrogel exhibits a high degree of adjustable release and a long-acting bactericidal effect.
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  • 文章类型: Journal Article
    单壁碳纳米管(SWCNT)具有可穿戴和柔性设备所需的优异的电子和机械性能。SWCNT膜的制备是制造各种器件的第一步。这项工作开发了一种可扩展且可行的方法,基于表面张力梯度诱导的Marangoni流,在水表面上组装SWCNT薄膜。薄膜具有40厘米×30厘米(可延伸)的大面积,可调厚度为15~150nm,高达96%的高透明度,和一个体面的导电性。它们准备直接转移到各种基材上,包括灵活的。柔性应变传感器是用柔性衬底上的膜制造的。这些传感器具有高灵敏度和可重复性。通过实现多功能人体运动传感,包括回应声音,监测动脉搏动,检测关节和肌肉动作,组装的SWCNT薄膜显示了在智能设备中应用的潜力。
    Single-walled carbon nanotubes (SWCNTs) present excellent electronic and mechanical properties desired in wearable and flexible devices. The preparation of SWCNT films is the first step for fabricating various devices. This work developed a scalable and feasible method to assemble SWCNT thin films on water surfaces based on Marangoni flow induced by surface tension gradient. The films possess a large area of 40 cm × 30 cm (extensible), a tunable thickness of 15∼150 nm, a high transparency of up to 96%, and a decent conductivity. They are ready to be directly transferred to various substrates, including flexible ones. Flexible strain sensors were fabricated with the films on flexible substrates. These sensors worked with high sensitivity and repeatability. By realizing multi-functional human motion sensing, including responding to voices, monitoring artery pulses, and detecting knuckle and muscle actions, the assembled SWCNT films demonstrated the potential for application in smart devices.
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  • 文章类型: Journal Article
    农药投放智能系统的开发在提高农药利用效率和减轻环境风险方面取得了重大进展。在此,提出了一种酸响应性农药递送系统,该系统使用由埃洛石粘土纳米管(HNT)的自组装形成的微球。杀虫剂阿维菌素(AVM)和除草剂prometryn(PMT)被用作疏水性农药的两种模型,并被封装在多孔微球中,然后是单宁酸/铁(TA/FeIII)复合膜的涂层,以产生两种控释农药,被命名为HCEAT和HCEPT,导致AVM和PMT的负载能力分别为113.3和120.3mgg-1。HCEAT和HCEPT都表现出对弱酸的响应性,在pH值为5.5时,24h释放率分别为85.8%和80.5%。实验和仿真结果表明,EDTA2-与Ca2+之间的配位相互作用促进了HNTs的球形聚集。此外,这些新型农药制剂表现出更好的抗紫外线(UV)辐射,较高的叶面亲和力,浸出效果较小,载体材料对植物和陆地生物的影响可以忽略不计。这项工作提出了一种有希望的方法来开发高效和生态友好的农药制剂,为农业的可持续发展做出了巨大贡献。
    The development of smart systems for pesticidal delivery presents a significant advancement in enhancing the utilization efficiency of pesticides and mitigating environmental risks. Here an acid-responsive pesticidal delivery system using microspheres formed by the self-assembly of halloysite clay nanotubes (HNTs) is proposed. Insecticide avermectin (AVM) and herbicide prometryn (PMT) are used as two models of hydrophobic pesticide and encapsulated within the porous microspheres, followed by a coating of tannic acid/iron (TA/FeIII) complex films to generate two controlled-release pesticides, named as HCEAT and HCEPT, resulting in the loading capacity of AVM and PMT being 113.3 and 120.3 mg g-1, respectively. Both HCEAT and HCEPT exhibit responsiveness to weak acid, achieving 24 h-release ratios of 85.8% and 80.5% at a pH of 5.5. The experiment and simulation results indicate that the coordination interaction between EDTA2- and Ca2+ facilitates the spherical aggregation of HNTs. Furthermore, these novel pesticide formulations demonstrate better resistance against ultraviolet (UV) irradiation, higher foliar affinity, and less leaching effect, with negligible impact of the carrier material on plants and terrestrial organisms. This work presents a promising approach toward the development of efficient and eco-friendly pesticide formulations, greatly contributing to the sustainable advancement of agriculture.
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