electrostatic interaction

静电相互作用
  • 文章类型: Journal Article
    快速实时PCR(一般<1h)具有广阔的前景。在这项研究中,我们合成了一种新型的金纳米粒子包覆的核-壳纳米材料树枝状聚合物(AuCSTDs),用于该领域的研究。实验结果表明,AuCSTDs可以明显缩短不同模板的实时PCR时间(从72到28分钟),而检测极限达到10个拷贝,非特异性扩增显着降低。此外,使用有限元模拟方法进行的实验分析和理论研究证实,AuCSTDs通过协同增强静电吸附和热导率而起作用。这些特性在改进实时PCR中起着关键作用,特别是在粒子-粒子相互作用中。本研究为快速实时PCR技术提供了一种先进的方法,这有望显著提高效率,降低检测限,增强分子检测的特异性。
    Rapid real-time PCR (generally <1 h) has broad prospects. In this study, we synthesized a new type of nanomaterial core-shell tecto-dendrimer coated with Au nanoparticles (Au CSTDs) for research in this field. The experimental results showed that Au CSTDs could significantly shorten the time of real-time PCR (from 72 to 28 min) with different templates, while the detection limit reached 10 copies and the nonspecific amplification was significantly reduced. Furthermore, experimental analyses and theoretical studies using the finite element simulation method confirmed that Au CSTDs function by synergistically enhancing electrostatic adsorption and thermal conductivity. These properties play a key role in improving real-time PCR, especially in particle-particle interactions. This study contributes an advanced method to rapid real-time PCR, which is expected to remarkably improve the efficiency, lower the detection limit, and enhance the specificity of molecular detection.
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  • 文章类型: Journal Article
    具有高沸点(BP)和低蒸气压(VP)的溶剂添加剂已成为提高有机太阳能电池(OSC)性能的关键手段。然而,并不总是清楚它们是否在沉积后保留在活性层膜中,这会对OSC的重现性和稳定性产生负面影响。在这项研究中,介绍了一种易于去除的溶剂添加剂(4-氯-2-氟碘苯(CFIB)),具有低BP和高VP,表现得像挥发性固体添加剂,可以在器件制造过程中完全去除。将CFIB添加到D18-Cl供体和N3受体中的深入研究验证了其通过有效的静电相互作用与N3的主要非共价分子间相互作用。这种现象通过优化形态来改善电荷动力学和动力学,导致基于D18-Cl:N3的器件的性能增强,功率转换效率为18.54%。与无CFIB器件相比,经CFIB处理的器件在85°C时表现出优异的热稳定性(T80寿命=120小时)。由于其通过在膜中没有残余CFIB进化的形态稳健性。CFIB具有溶剂(易于应用)和固体(高挥发性)添加剂的优点的组合,证明了其在商业大规模生产OSC中的巨大潜力。
    Solvent additives with a high boiling point (BP) and low vapor pressure (VP) have formed a key handle for improving the performance of organic solar cells (OSCs). However, it is not always clear whether they remain in the active-layer film after deposition, which can negatively affect the reproducibility and stability of OSCs. In this study, an easily removable solvent additive (4-chloro-2-fluoroiodobenzene (CFIB)) with a low BP and high VP is introduced, behaving like volatile solid additives that can be completely removed during the device fabrication process. In-depth studies of CFIB addition into the D18-Cl donor and N3 acceptor validate its dominant non-covalent intermolecular interactions with N3 through effective electrostatic interactions. Such phenomena improve charge dynamics and kinetics by optimizing the morphology, leading to enhanced performance of D18-Cl:N3-based devices with a power conversion efficiency of 18.54%. The CFIB-treated device exhibits exceptional thermal stability (T80 lifetime = 120 h) at 85 °C compared with the CFIB-free device, because of its morphological robustness by evolving no residual CFIB in the film. The CFIB features a combination of advantages of solvent (easy application) and solid (high volatility) additives, demonstrating its great potential use in the commercial mass production of OSCs.
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  • 文章类型: Journal Article
    具有周期性排列的原子的晶体物质在现代科学技术中得到了广泛的应用。为了促进新材料的设计和现有材料的进步,准确和有效的模型,而不依赖过多的已知输入来预测功能是至关重要的。这里,我们为此提出了一种分析方法,只有晶体的结构化学知识。基于周期性排列的原子之间的静电相互作用,第一,原子间势的第二和第三衍生物,分别,能够预测总共十种机械,声学和热性能。从500篇文献中收集了1000多项测量,这导致对称平均百分比误差(SMPE)在±25%以内,对称平均绝对百分比误差(SMAPE)在预测的所有属性中介于22%〜74%之间,这进一步实现了键特征作为功能的最重要但隐含的起源的启示。
    Crystalline matters with periodically arranged atoms found wide applications in modern science and technology. To facilitate the design of new materials and the advancement of existing ones, accurate and efficient models without relying too much on known inputs for predicting the functionalities are essential. Here, we propose an analytical approach for such a purpose, with only the knowledge of the structural chemistry of crystals. Based on the electrostatic interaction between periodically arranged atoms, the 1st, 2nd and 3rd derivatives of interatomic potential, respectively, enable a prediction of ten kinds in total of mechanical, acoustical and thermal properties. Over a thousand measurements are collected from ∼500 literatures, this results in the symmetric mean percentage error (SMPE) within ±25% and the symmetric mean absolute percentage error (SMAPE) ranging from 22%∼74% across all properties predicted, which further enables a revelation of bond characteristics as the most important but implicit origin for functionalities.
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  • 文章类型: Journal Article
    在这项工作中,将铜纳米簇(CuNCs)限制在3D层状双氢氧化物(3D-LDH)上,形成具有出色电化学发光(ECL)的CuNCs@3D-LDH,用于构建超灵敏的生物传感器,以检测与阿尔茨海默病(AD)有关的胶质纤维酸性蛋白(GFAP)。更重要的是,与单个CuNCs相比,CuNCs@3D-LDH表现出强烈而稳定的ECL响应,因为3D-LDH不仅可以收集更多的CuNCs,而且可以限制分子内自由运动以减少非辐射跃迁,从而获得高ECL强度。此外,改进的级联扩增法将邻近连接法(PLA)与DNA酶结合,可以将微量的靶蛋白转化为大量的输出DNA,从而提高生物传感器的灵敏度。ECL生物传感器实现了GFAP的超灵敏检测,检出限为2ag/mL,已成功应用于神经系统疾病患者血清中GFAP的评估。这项研究提供了一种通用而简便的方法来提高CuNCs的ECL性能,以对疾病诊断的生物标志物进行灵敏检测。
    In this work, the copper nanoclusters (Cu NCs) were confined on 3D layered double hydroxide (3D-LDH) to form Cu NCs@3D-LDH with outstanding electrochemiluminescence (ECL) for constructing ultrasensitive biosensor to detect of glial fibrillary acidic protein (GFAP) implicated in Alzheimer\'s Disease (AD). More importantly, compared to the individual Cu NCs, Cu NCs@3D-LDH presented strong and stable ECL response, since 3D-LDH could not only gather more Cu NCs but also limit the intramolecular free motion to reduce nonradiative transition for obtaining high ECL intensity. In addition, the improved cascade amplification method combining proximity ligation assay (PLA) with DNAzyme could transform tiny amount of target protein into a large amount of output DNA to improve sensitivity of biosensor. The ECL biosensor realized ultrasensitive detection of GFAP with the detection limit of 2 ag/mL and it had been successfully applied to the evaluation of GFAP in the serum of patients with neurological diseases. This research offered a general and facile method to improve ECL performance of Cu NCs for sensitive detection of biomarkers for disease diagnosis.
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  • 文章类型: Journal Article
    金纳米棒(GNR)在用近红外光照射时会产生热量,实现肿瘤靶向光热治疗。在这项研究中,我们制备了硫酸化透明质酸(sHA)包被的GNR,通过静电相互作用对CD44具有结合亲和力,以有效和稳定地将GNR递送到肿瘤,并评估了它们对光热疗法的有用性。用三甲基铵基团修饰的阳离子GNR以不同程度的硫酸化与天然HA或sHA静电相互作用以形成复合物。虽然GNR/HA在盐水中不稳定,GNR/sHA在近红外区保持吸收峰,特别是对于硫酸化程度较高的GNR/sHA。GNR/sHA在用近红外光照射时表现出强烈的光热效应。此外,体外和体内研究表明,每个HA单位含有约1.2个硫酸化基团的sHA包被的GNR可以通过HA特异性途径在CD44阳性肿瘤中积累。这些发现表明GNR/sHA作为肿瘤靶向光热治疗剂的有效性。
    Gold nanorods (GNR) produce heat upon irradiation with near-infrared light, enabling a tumor-targeted photothermal therapy. In this study, we prepared GNR coated with sulfated hyaluronic acid (sHA) with a binding affinity for CD44 via electrostatic interactions to deliver GNR to tumors efficiently and stably, and evaluated their usefulness for photothermal therapy. Cationic GNR modified with trimethylammonium groups electrostatically interacted with native HA or sHA with varying degrees of sulfation to form complexes. While GNR/HA was unstable in saline, GNR/sHA maintained the absorbance peak in the near-infrared region, particularly for GNR/sHA with higher degrees of sulfation. GNR/sHA exhibited an intense photothermal effect upon irradiation with near-infrared light. Furthermore, in vitro and in vivo studies revealed that GNR coated with sHA containing approximately 1.2 sulfated groups per HA unit could accumulate in CD44-positive tumors via an HA-specific pathway. These findings indicate the effectiveness of GNR/sHA as a tumor-targeted photothermal therapeutic agent.
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  • 文章类型: Journal Article
    热响应聚合物刷由于其独特的性能而引起了相当多的研究关注。在这里,我们开发了用聚(N-异丙基丙烯酰胺(NIPAAm)-co-3-丙烯酰胺丙基三甲基氯化铵(APTAC)-co-叔丁基丙烯酰胺(tBAAm)和P(NIPAAm-co-APTAC-co-甲基丙烯酸正丁酯(nBMA))刷接枝的二氧化硅珠。碳,氢气,共聚物磨碎的二氧化硅珠粒的氮元素分析表明,二氧化硅珠粒上存在大量接枝共聚物。通过使用共聚物刷改性的珠子作为固定相的高效液相色谱法观察生物分子与制备的共聚物刷之间的静电和疏水相互作用,分析了它们的洗脱行为。腺苷核苷酸保留在珠子填充的柱子中,这归因于共聚物和腺苷核苷酸之间的静电相互作用。胰岛素在高温下吸附在共聚物刷上,这归因于其与共聚物的静电和疏水相互作用。在白蛋白的情况下观察到类似的吸附行为。Further,在低浓度的磷酸盐缓冲溶液中,由于白蛋白与共聚物的静电相互作用增强,即使在相对较低的温度下,白蛋白也会吸附到共聚物刷上。这些结果表明,开发的热响应性强阳离子共聚物刷可以通过静电和温度调节的疏水相互作用的组合与肽和蛋白质相互作用。因此,开发的共聚物刷具有在色谱基质中用于肽和蛋白质的分析和纯化的巨大潜力。
    Thermoresponsive polymer brushes have attracted considerable research attention owing to their unique properties. Herein, we developed silica beads grafted with poly(N-isopropylacrylamide (NIPAAm)-co-3-acrylamidopropyl trimethylammonium chloride (APTAC)-co-tert-butyl acrylamide (tBAAm) and P(NIPAAm-co-APTAC-co-n-butyl methacrylate(nBMA)) brushes. The carbon, hydrogen, and nitrogen elemental analysis of the copolymer-grated silica beads revealed the presence of a large amount of the grafted copolymer on the silica beads. The electrostatic and hydrophobic interactions between biomolecules and prepared copolymer brushes were analyzed by observing their elution behaviors via high-performance liquid chromatography using the copolymer-brush-modified beads as the stationary phase. Adenosine nucleotides were retained in the bead-packed columns, which was attributed to the electrostatic interaction between the copolymers and adenosine nucleotides. Insulin was adsorbed on the copolymer brushes at high temperatures, which was attributed to its electrostatic and hydrophobic interactions with the copolymer. Similar adsorption behavior was observed in case of albumin. Further, at a low concentration of the phosphate buffer solution, albumin was adsorbed onto the copolymer brushes even at relatively low temperatures owing to its enhanced electrostatic interaction with the copolymer. These results indicated that the developed thermoresponsive strong cationic copolymer brushes can interact with peptides and proteins through a combination of electrostatic and temperature-modulated hydrophobic interactions. Thus, the developed copolymer brushes exhibits substantial potential for application in chromatographic matrices for the analysis and purification of peptides and proteins.
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  • 文章类型: Journal Article
    在水-油界面处组装的纳米颗粒表面活性剂可以显着降低界面张力并且可以用于稳定液体。了解并积极调整产生的膜的机械性能,其中包括纳米粒子表面活性剂,对纳米颗粒的界面行为和水净化具有重要的基本意义,药物封装,提高石油采收率,和创新的能量转换应用。这里,我们介绍了静电相互作用驱动的直径最大为0.10mm的独立式和紧密堆积的SiO2表面活性剂膜的制造。厚度为20-30nm的膜跨越直径为2μm的孔,表现出的杨氏模量范围从1.5到5.9GPa。发现制造的纳米颗粒表面活性剂膜的可控弹性特性由纳米颗粒和配体之间的相互作用强度决定,在配体和配体之间,和纳米颗粒表面活性剂之间。结果为制造和开发基于纳米表面活性剂的大面积纳米粒子提供了一种有效的方法,独立式,以及具有大规模精细可调机械性能的超薄膜。
    Nanoparticle surfactants assembled at water-oil interfaces can significantly lower the interfacial tension and can be used to stabilize liquids. Understanding and actively tuning the mechanical properties of the generated membranes, which comprise the nanoparticle surfactants, are of significant fundamental interest for the interfacial behavior of nanoparticles and of interest for water purification, drug encapsulation, enhanced oil recovery, and innovative energy transduction applications. Here, we present electrostatic interaction-driven fabrication of freestanding and close-packed SiO2 surfactant membranes with diameters up to 0.10 mm. The membranes of 20-30 nm in thickness were spanned over holes with a diameter of 2 μm, exhibiting a Young\'s modulus ranging from 1.5 to 5.9 GPa. The controllable elastic properties of the fabricated nanoparticle surfactant membranes are found to be dictated by the strength of interactions between nanoparticles and ligands, between ligands and ligands, and between the nanoparticle surfactants. The results present an efficient approach for fabricating and developing nanoparticle surfactant-based large-area, freestanding, and ultrathin membranes with finely tunable mechanical properties on a large scale.
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  • 文章类型: Journal Article
    从废水中回收稀土元素的研究日益受到重视。与其他方法相比,生物吸附是一个简单的,高效,和环保的稀土废水处理方法,具有更大的发展前景。本研究的目的是研究Yarrowialipolytica对五种稀土离子的生物吸附行为和机理(La3,Nd3,Er3,Y3,和Sm3by),特别关注生物吸附行为,生物吸附动力学,和生物吸附等温线。结果表明,在最佳条件下,Y的生物吸附能力为76.80mg/g。发现生物吸附过程符合伪二级动力学模型和Langmuir生物吸附等温线,表明Y.lipolytica采用单层化学生物吸附过程来生物吸附稀土离子。表征分析表明,参与稀土离子生物吸附的主要官能团为氨基,羧基,和羟基。通过表面络合促进了Y.Lipolytica对稀土离子的协同生物吸附,离子交换,和静电相互作用。这些发现表明,Y。lipolytica具有从废水中去除稀土元素的有效生物吸附剂的潜力。
    Research on the recovery of rare earth elements from wastewater has attracted increasing attention. Compared with other methods, biosorption is a simple, efficient, and environmentally friendly method for rare earth wastewater treatment, which has greater prospects for development. The objective of this study was to investigate the biosorption behavior and mechanism of Yarrowia lipolytica for five rare earth ions (La3⁺, Nd3⁺, Er3⁺, Y3⁺, and Sm3⁺) with a particular focus on biosorption behavior, biosorption kinetics, and biosorption isotherm. It was demonstrated that the biosorption capacity of Y. lipolytica at optimal conditions was 76.80 mg/g. It was discovered that the biosorption process complied with the pseudo-second-order kinetic model and the Langmuir biosorption isotherm, indicating that Y. lipolytica employed a monolayer chemical biosorption process to biosorb rare earth ions. Characterization analysis demonstrated that the primary functional groups involved in rare earth ion biosorption were amino, carboxyl, and hydroxyl groups. The cooperative biosorption of rare earth ions by Y. lipolytica was facilitated by means of surface complexation, ion exchange, and electrostatic interactions. These findings suggest that Y. lipolytica has the potential to be an effective biosorbent for the removal of rare earth elements from wastewater.
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  • 文章类型: Journal Article
    由聚(2-(甲基丙烯酰氧基)乙基磷酰胆碱)(PMPC,M)和聚(3-((2-(甲基丙烯酰氧基)乙基)二甲基铵)丙酸酯)(PCBMA,C)通过可逆加成-断裂链转移(RAFT)聚合合成。双亲水二嵌段共聚物(M100S100)由PMPC和阴离子聚(甲基丙烯酸3-磺丙酯钾盐)(PMPS,S)通过RAFT合成。每个嵌段的聚合度为100。PMPC的电荷被分子内中和。在中性pH下,PCBMA中的电荷也由于其羧基甜菜碱结构而被分子内中和。在酸性条件下,当侧羧基被质子化时,PCBMA表现出聚阳离子行为,形成阳离子叔胺基团。PMPS显示出与pH无关的永久阴离子性质。阳离子M100C100和阴离子M100S100在酸性水溶液中的电荷中和混合物由于静电吸引相互作用而形成水溶性聚离子复合物(PIC)胶束。核心由阳离子PCBMA和阴离子PMPS嵌段组成,PMPC块作为覆盖核心表面的外壳,形成球形核壳PIC胶束。pH高于4时,PCBMA中的侧羧基会发生去质子化,过渡到两性离子状态,从而消除PCBMA中的阳离子电荷。因此,在pH高于4时,PIC胶束由于电荷相互作用的消失而解离。
    A dual zwitterionic diblock copolymer (M100C100) consisting of poly(2-(methacryloyloxy)ethyl phosphorylcholine) (PMPC, M) and poly(3-((2-(methacryloyloxy)ethyl) dimethylammonio) propionate) (PCBMA, C) is synthesized via reversible addition-fragmentation chain transfer (RAFT) polymerization. A double hydrophilic diblock copolymer (M100S100) consist of PMPC and anionic poly(3-sulfopropyl methacrylate potassium salt) (PMPS, S) is synthesized via RAFT. The degrees of polymerization of each block are 100. The charges of PMPC are neutralized intramolecularly. At neutral pH, the charges in PCBMA are also neutralized intramolecularly due to its carboxybetaine structure. Under acidic conditions, PCBMA exhibits polycation behavior as the pendant carboxy groups become protonated, forming cationic tertiary amine groups. PMPS shows permanent anionic nature independent of pH. Charge neutralized mixture of cationic M100C100 and anionic M100S100 in acidic aqueous solution forms water-soluble polyion complex (PIC) micelle owing to electrostatic attractive interactions. The core is composed of the cationic PCBMA and anionic PMPS blocks, with the PMPC blocks serving as shells that covered the core surface, forming spherical core-shell PIC micelles. Above pH 4 the pendant carboxy groups in PCBMA undergo deprotonation, transitioning to a zwitterionic state, thereby eliminating the cationic charge in PCBMA. Therefore, above pH 4 the PIC micelles are dissociated due to the disappearance of the charge interactions.
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  • 文章类型: Journal Article
    具有受控结构的纳米粒子(NP)簇阵列在纳米激光器中显示出广泛的应用,传感器,和光催化,但是在衬底上制造这些阵列仍然是一个巨大的挑战。这篇综述提出了一种高效的基于聚合物的策略,用于通过静电相互作用将带有相反电荷的二元聚电解质接枝NP(PGNP)的过程定向自组装成稳定的胶体分子(CM)。ABxCM的配位数(X)可以通过调节溶液的pH或离子强度或通过采用具有不同电荷密度的PGNP的不同组合来调节。可以在衬底上以高产率构建具有从AB到AB7的各种结构的大面积CM。这种方法适用于具有不同NP核的PGNP。这种组装策略为在具有广泛应用的基板上制造结构精确的组件提供了有用的工具。
    Arrays of nanoparticle (NP) clusters with controlled architectures show broad applications in nanolasers, sensors, and photocatalysis, but the fabrication of these arrays on substrates remains a grand challenge. This review presents a highly effective polymer-based strategy for the process-directed self-assembly of binary polyelectrolyte-grafted NPs (PGNPs) bearing opposite charges into stable colloidal molecules (CMs) on substrates via electrostatic interactions. The coordination number (x) of ABx CMs can be tuned by adjusting the pH or ionic strength of the solution or by employing different combinations of PGNPs with varying charge densities. Large-area CMs with diverse structures ranging from AB to AB7 can be constructed on substrates in high yields. This approach is applicable to PGNPs with different cores of NPs. This assembly strategy offers a useful tool for the fabrication of structurally precise assemblies on substrates with broad applications.
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