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An electrochemical biosensor platform for kanamycin detection based on the target-induced spatial configuration of aptamer-complementary strand hybridization 基于目标诱导的适配体-互补链杂交空间构型的卡那霉素检测电化学生物传感器平台
Pub Date : 2024-03-19 DOI: 10.1007/s00706-024-03196-2
Yunyun Qiu, Lingyu Jiang, Li Xiang, Jianshe Tang

A sensitive and selective electrochemical method for the determination of kanamycin was established first at the surface of a pencil graphite-embedded PTFE cannula electrode according to the analysis mechanism of target-induced spatial configuration of aptamer-complementary strand hybridization. The electrochemical characteristics studies of homemade electrodes were using cyclic voltammetry. The result showed that the PFTE nested pencil graphite electrode with polished and gold deposits has good electrode application potential. The electrochemical analysis method for kanamycin was performed using differential pulse voltammetric techniques. Modification of the homemade electrode surface increased its DPV response of methylene blue in the presence of kanamycin because more analytes affected the aptamer-complementary strand hybridization conformation. Thus, more G-quadruplexes formed to capture methylene blue. The developed electrochemical sensor yielded a positive correlation between the electrochemical signal and the logarithmic concentration of kanamycin with a wide linear range (15.3 nM to 0.24 mM) and a low limit of detection of 10 nM. The developed sensor was assessed by the analysis of kanamycin in wastewater treatment plant effluent samples by spiked recovery method. The analysis results (recoveries range of 97.5–105% and RSD range of 2.1–7.8%, respectively) proved that the method performance was both acceptable and admirable.

Graphical abstract

根据靶标诱导的aptamer-互补链杂交空间构型的分析机制,首先在笔形石墨嵌入聚四氟乙烯套管电极表面建立了测定卡那霉素的灵敏和选择性电化学方法。采用循环伏安法研究了自制电极的电化学特性。结果表明,抛光镀金的 PFTE 嵌套铅笔石墨电极具有良好的电极应用潜力。卡那霉素的电化学分析方法采用了差分脉冲伏安技术。自制电极表面的改性增加了其在卡那霉素存在下对亚甲蓝的 DPV 响应,因为更多的分析物影响了合体-互补链杂交构象。因此,形成了更多的 G-四联体来捕获亚甲蓝。所开发的电化学传感器的电化学信号与卡那霉素的对数浓度呈正相关,线性范围宽(15.3 nM 至 0.24 mM),检测限低至 10 nM。采用加标回收法分析了污水处理厂出水样品中的卡那霉素,对所开发的传感器进行了评估。分析结果(回收率范围为 97.5%-105%,RSD 范围为 2.1%-7.8%)证明该方法的性能是可接受的,也是令人满意的。
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引用次数: 0
A short and efficient formal synthesis of (R)-pipecolic acid from the ring expansion of chiral aziridine 通过手性氮丙啶的扩环,简短高效地正式合成(R)-联哌啶酸
Pub Date : 2024-03-15 DOI: 10.1007/s00706-024-03187-3
Archana Pareek, Sonam Tashi Khom, Pranjit Saikia, Nagendra Nath Yadav

Ring expansion of 4-[(2R)-1-[(1R)-1-phenylethyl]aziridin-2-yl]butyl tosylate obtained from tosylation of 4-[(2R)-1-[(1R)-1-phenylethyl]aziridin-2-yl]butan-1-ol via formation of 1-azabicyclo[4.1.0]heptane tosylate gives substituted piperidine. The ring openings of azabicycloheptane tosylate with acetate nucleophiles proceeded in highly regio- and stereoselective manner with release of the ring-strain of the three-membered aziridine ring through the breakage of either C-N bond. This ring expansion streategy of aziridine provides a short route for asymmetric synthesis of biologically active natural alkaloid such as (R)-pipecolic acid.

Graphical abstract

由 4-[(2R)-1-[(1R)-1-苯基乙基]氮丙啶-2-基]丁-1-醇通过形成 1-氮杂双环[4.1.0]庚烷对甲苯磺酸盐对甲苯磺酸盐进行对甲苯磺酸盐化反应得到的 4-[(2R)-1-[(1R)-1-苯基乙基]氮丙啶-2-基]丁基对甲苯磺酸盐的扩环反应生成了取代的哌啶。1- 氮杂双环[4.1.0]庚烷对甲苯磺酸酯与乙酸酯亲核物的开环反应以高度区域和立体选择性的方式进行,通过断裂任一 C-N 键释放三元氮丙啶环的环张力。氮丙啶的这种扩环链式反应为不对称合成具有生物活性的天然生物碱(如(R)-哌啶醇酸)提供了一条捷径。
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引用次数: 0
Capillary zone electrophoresis method for quantification of therapeutic peptide glatiramer acetate 毛细管区带电泳法定量检测治疗肽醋酸格拉替雷
Pub Date : 2024-03-14 DOI: 10.1007/s00706-024-03190-8

Abstract

This study presents the development and validation of a novel capillary zone electrophoresis method for the precise determination of glatiramer acetate and its amino acid constituents. A 120 mmol dm−3 phosphoric acid solution adjusted to pH 1.9 with Tris, supplemented with 20 mmol dm−3 triethylamine to achieve a final of pH 2.1, resulted in a repeatable analysis of glatiramer acetate. The method demonstrated a limit of detection and quantification of 39.2 µg cm−3 and 130.7 µg cm−3, respectively. This method allows for the rapid control of glatiramer acetate-based pharmaceuticals and distinguishes glatiramer acetate from the amino acids used in its synthesis.

Graphical abstract

摘要 本研究开发并验证了一种新型毛细管区带电泳方法,用于精确测定醋酸格拉替雷及其氨基酸成分。用三羟甲基氨基甲烷将 120 mmol dm-3 磷酸溶液调节至 pH 1.9,再加入 20 mmol dm-3 三乙胺使最终 pH 值达到 2.1,从而实现了对醋酸格拉替雷的重复性分析。该方法的检出限和定量限分别为 39.2 µg cm-3 和 130.7 µg cm-3。该方法可快速控制醋酸格拉替雷药物,并将醋酸格拉替雷与其合成过程中使用的氨基酸区分开来。 图表摘要
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引用次数: 0
Electrochemical and density functional theory studies of some newly synthesized azo-stilbene chromogenic structures 一些新合成的偶氮苯乙烯致色结构的电化学和密度泛函理论研究
Pub Date : 2024-03-13 DOI: 10.1007/s00706-024-03189-1

Abstract

The electrochemical behavior in nonaqueous media of a series of five newly synthesized azo-stilbene dyes is investigated with the aim of elucidating the anodic oxidation mechanism of the latter to gain a better understanding of potential oxidative degradation phenomena to find new and environmentally sustainable electrochemical methods for the abatement of dyes from industrial wastewater. In addition, the frontier orbital energies of optimized conformers have been computed using quantum chemical calculations at the B3LYP-D3 (dispersion corrected Becke, 3-parameter, Lee Yang Parr) level of theory. Cyclic voltammetry experiments show that anodic oxidation of the studied chromophore structures follows an irreversible pathway and most probably occurs at the amide nitrogen. Validation of experimental results has been conducted by computation of various global reactivity descriptors, confirming that substituents grafted on the benzene ring actively influence the oxidation/reduction potentials.

Graphical abstract

摘要 研究了一系列新合成的五种偶氮二苯乙烯染料在非水介质中的电化学行为,旨在阐明后者的阳极氧化机理,从而更好地了解潜在的氧化降解现象,为消除工业废水中的染料找到新的、环境可持续的电化学方法。此外,还利用 B3LYP-D3(弥散校正贝克、3 参数、李杨帕尔)理论水平的量子化学计算,计算了优化构象的前沿轨道能。循环伏安实验表明,所研究的发色团结构的阳极氧化遵循不可逆的途径,很可能发生在酰胺氮上。通过计算各种全局反应性描述符对实验结果进行了验证,证实苯环上接枝的取代基会对氧化/还原电位产生积极影响。 图表摘要
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引用次数: 0
Quantitative applications of the electronegativity scale 电负性标度的定量应用
Pub Date : 2024-03-12 DOI: 10.1007/s00706-024-03191-7
Peter F. Lang

This paper briefly discusses electronegativity and uses of the electronegativity scale. It demonstrates that values of electronegativity can be used quantitatively in simple equations. Formulas containing derived values of elemental electronegativities are shown to calculate dipole moments, bond lengths, and bond energies reliably. Comparison between calculated and experimental values shows very good agreement in the vast majority of cases.

Graphical abstract

本文简要讨论了电负性和电负性标度的用途。它证明了电负性值可以在简单的方程式中定量使用。包含元素电负性推导值的公式可以可靠地计算偶极矩、键长和键能。计算值与实验值的比较表明,在绝大多数情况下,两者的一致性非常好。
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引用次数: 0
Spray drying synthesis of perspective materials for cathodes of Li-ion batteries 喷雾干燥法合成锂离子电池阴极透视材料
Pub Date : 2024-03-12 DOI: 10.1007/s00706-024-03186-4
Hana Hálová, Ladislav Chladil, Antonín Šimek, Marek Kunz

Our contribution discusses the possibility of using spray drying synthesis for the preparation of active cathode material for Li-ion batteries. The particles were synthesized using a two-stage spray drying synthesis of NMC material (Li1.2Ni0.13Mn0.54Co0.13O2), when we separated the processes of synthesizing the nanoparticles (step 1) themselves and the subsequent calcination were separated from each other. Synthesis was based on spraying of precursor solution via ultrasonic atomizer and dried particles were captured using an electrostatic separator. During the following calcination step, the effect of temperature on the crystallization of the sample was investigated in the temperature range of 400–900 ℃. The temperature of 750 ℃ proved to be ideal for sufficient formation of a crystalline structure while maintaining a sufficiently fine-grained structure. At this temperature, the influence of the length of calcination was also investigated for the following times: 2.5, 5, 10, and 20 h. The structural and morphologic characterization of synthesized material was examined with X-ray diffraction and scanning electron microscopy with energy dispersive spectroscopy.

Graphical abstract

我们的论文讨论了利用喷雾干燥合成法制备锂离子电池活性正极材料的可能性。我们采用两阶段喷雾干燥法合成了 NMC 材料(Li1.2Ni0.13Mn0.54Co0.13O2),将合成纳米粒子(第 1 步)和随后的煅烧过程分开。合成是通过超声波雾化器喷洒前驱体溶液,然后使用静电分离器捕获干燥的颗粒。在接下来的煅烧步骤中,研究了温度在 400-900 ℃ 范围内对样品结晶的影响。750 ℃ 的温度被证明是理想的温度,既能充分形成结晶结构,又能保持足够的细粒结构。用 X 射线衍射和扫描电子显微镜以及能量色散光谱分析了合成材料的结构和形态特征。
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引用次数: 0
Electrochemical sensing of brucine using polymer modified nanotube sensor 利用聚合物修饰的纳米管传感器对布鲁碱进行电化学检测
Pub Date : 2024-03-12 DOI: 10.1007/s00706-024-03192-6
D. Sumanth, J. G. Manjunatha, B. Kanthappa, S. A. Aldossari, M. S. Mushab, Mika Sillanpää

In this innovative approach, a methodology was formulated to simplify the electrochemical analysis of the specified anti-inflammatory and analgesic drug, brucine (BCN), in 0.2 M phosphate buffer solution (PBS) by preparing an affordable, easy to use, and eco-friendly carbon nanotube paste electrode (CNTPE). This method was created using an electrode treated with glutamic acid (GL) through electrochemical polymerization along with a bare carbon nanotube paste electrode (BCNTPE) using pH 7 for different cycles (5, 10, 15, 20), with ten cycles revealing the optimum peak. This study presents an innovative electrochemical sensor employing a polymerized glutamic acid (GL) modified carbon nanotube paste electrode (P-GL(MCNTPE)). The sensor is specifically designed to detect BCN with high sensitivity and selectivity. The prepared electrodes, namely P-GL(MCNTPE) and BCNTPE, are utilized for comprehensive material and system characterization using various electrochemical techniques, including cyclic voltammetry (CV), differential pulse voltammetry (DPV), scanning electron microscopy (SEM), and electrochemical impedance spectroscopy (EIS). The developed sensor noticeably enhanced the electrochemical activity of BCN when placed in a pH of 4.0 PBS (0.2 M). BCN undergoes a distinctive two-proton and two-electron transfer process. Scan rate studies reveal that the electrode surface behaviour is largely governed by diffusion control. By varying the BCN concentration at pH of 4.0 in a scan rate of 0.1 V/s using DPV technique, the lower limit of detection was found to be 1.5 × 10–8 M, and the lower limit of quantification was determined to be 5 × 10–8 M. These measurements were obtained as the BCN concentration varied from 0.2 to 1.2 µM. The developed electrode maintains good sensitivity for detecting BCN, despite the presence of potential interferents like organic compounds and metal ions. This sensor is stable, repeatable, and reproducible in oxidizing BCN. Real sample (tablets) analysis was done using DPV method demonstrates a favorable recovery rate.

Graphical abstract

在这一创新方法中,通过制备一种经济实惠、易于使用且环保的碳纳米管浆糊电极(CNTPE),制定了一种简化 0.2 M 磷酸盐缓冲溶液(PBS)中特定消炎镇痛药物布鲁氨酸(BCN)电化学分析的方法。这种方法是使用通过电化学聚合法用谷氨酸(GL)处理过的电极和裸碳纳米管浆糊电极(BCNTPE),在 pH 值为 7 的条件下进行不同的循环(5、10、15、20),其中 10 个循环可达到最佳峰值。本研究利用聚合谷氨酸(GL)修饰的碳纳米管浆状电极(P-GL(MCNTPE))提出了一种创新的电化学传感器。该传感器专为检测 BCN 而设计,具有高灵敏度和高选择性。利用各种电化学技术,包括循环伏安法(CV)、差分脉冲伏安法(DPV)、扫描电子显微镜(SEM)和电化学阻抗谱(EIS),对制备的电极(即 P-GL(MCNTPE)和 BCNTPE)进行了全面的材料和系统表征。当 BCN 被置于 pH 值为 4.0 的 PBS(0.2 M)中时,所开发的传感器明显增强了 BCN 的电化学活性。BCN 经历了一个独特的双质子和双电子转移过程。扫描速率研究表明,电极表面行为主要受扩散控制。在 pH 值为 4.0 的条件下,使用 DPV 技术以 0.1 V/s 的扫描速率改变 BCN 的浓度,发现检测下限为 1.5 × 10-8 M,定量下限为 5 × 10-8 M。尽管存在有机化合物和金属离子等潜在干扰物,所开发的电极仍能保持良好的 BCN 检测灵敏度。该传感器在氧化 BCN 方面具有稳定性、可重复性和再现性。使用 DPV 方法对实际样品(药片)进行分析,显示出良好的回收率。
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引用次数: 0
Chemistry and uses of 1-(2-benzothiazolyl)pyrazolines: a mini-review 1-(2-苯并噻唑基)吡唑啉的化学性质和用途:小型综述
Pub Date : 2024-03-07 DOI: 10.1007/s00706-024-03182-8
Gheorghe Roman

The current report provides an overview of the rapidly developing class of pyrazolines having a benzothiazole moiety at N1. The synthetic approaches (mainly through the [3 + 2] cyclo-condensation of chalcone analogs with 2-hydrazinobenzothiazole) toward these particular pyrazolines, along with their chemical transformation to pyrazoles through oxidation are outlined. The photophysical properties (absorption and emission spectra) along with their applications as fluorescent chemosensors have been summarized. 1-(2-Benzothiazolyl)pyrazolines exhibit significant fluorescence quenching mostly in the presence of transition metal ions, such as Fe3+, Cu2+, Hg2+, Zn2+, or Ni2+, but also toward Al3+, thus enabling the selective detection of these analytes. In addition, examples of 1-(2-benzothiazolyl)pyrazolines acting as chemosensors for anions such as S2− or F are also available. Comprehensive examination of the biological properties of 1-(2-benzothiazolyl)pyrazolines shows that members of this class possess either broad or selective significant antimicrobial activity, along with tuberculostatic activity and cytotoxicity that is sometimes better than that of positive controls. The antidiabetic, anti-inflammatory, anthelmintic, and antimalarial activity of these compounds, along with their potential for inhibition of enzymes such as carbonic anhydrase or acetylcholinesterase have been briefly explored.

Graphical abstract

本报告概述了发展迅速的 N1 位具有苯并噻唑分子的吡唑啉类化合物。报告概述了这些特殊吡唑啉类化合物的合成方法(主要是通过查尔酮类似物与 2-肼基苯并噻唑的[3 + 2]环缩合),以及它们通过氧化作用转化为吡唑的化学过程。总结了它们的光物理特性(吸收和发射光谱)以及作为荧光化学传感器的应用。1-(2-苯并噻唑基)吡唑在过渡金属离子(如 Fe3+、Cu2+、Hg2+、Zn2+ 或 Ni2+)以及 Al3+ 的作用下会出现明显的荧光淬灭,从而实现了对这些分析物的选择性检测。此外,还有 1-(2-苯并噻唑基)吡唑作为 S2- 或 F- 等阴离子化学传感器的实例。对 1-(2-苯并噻唑基)吡唑啉类化合物生物特性的全面研究表明,该类化合物具有广泛的或选择性的显著抗菌活性,以及抗结核活性和细胞毒性,有时甚至优于阳性对照组。此外,还简要探讨了这些化合物的抗糖尿病、抗炎、驱虫和抗疟活性,以及它们抑制碳酸酐酶或乙酰胆碱酯酶等酶的潜力。
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引用次数: 0
Hybrid organic–inorganic fibers for solid-state batteries 用于固态电池的有机-无机混合纤维
Pub Date : 2024-03-06 DOI: 10.1007/s00706-024-03185-5

Abstract

This study is dedicated to the acquisition and quantification of processing parameters essential for the fabrication of customizable organic–inorganic hybrid nano/microfibers through electrospinning. These fibers are generated from suspensions comprising active electrode materials utilized in the construction of all solid-state batteries. Owing to the catalytic properties exhibited by certain electroactive materials and the coagulation tendencies stemming from the presence of various particles, there exists a limited operational interval within which stable fibers can be produced while maintaining the suspension at a suitable viscosity. Our second goal was to ascertain the relationship between the quality of the resulting fibers and the spinnability of the suspension, particularly regarding its electrical conductivity. Solutions and suspensions were studied with help of 29Si NMR spectroscopy, EIS, and conductometry, fiber morphology with confocal and electron microscopy.

Graphical abstract

摘要 本研究致力于获取和量化通过电纺丝制造可定制的有机-无机混合纳米/微纤维所必需的加工参数。这些纤维是从悬浮液中生成的,悬浮液中含有用于制造所有固态电池的活性电极材料。由于某些电活性材料表现出的催化特性以及各种颗粒存在的凝结倾向,在将悬浮液保持在适当粘度的情况下生产出稳定纤维的操作区间是有限的。我们的第二个目标是确定所制备纤维的质量与悬浮液可纺性之间的关系,特别是在导电性方面。我们利用 29Si NMR 光谱、EIS 和电导率测定法对溶液和悬浮液进行了研究,并利用共聚焦显微镜和电子显微镜对纤维形态进行了研究。 图表摘要
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引用次数: 0
Ionic liquids in green energy storage devices: lithium-ion batteries, supercapacitors, and solar cells 绿色能源存储设备中的离子液体:锂离子电池、超级电容器和太阳能电池
Pub Date : 2024-03-06 DOI: 10.1007/s00706-024-03178-4
Setareh Sheikh, Alireza Haghpanah Jahromi

Due to characteristic properties of ionic liquids such as non-volatility, high thermal stability, negligible vapor pressure, and high ionic conductivity, ionic liquids-based electrolytes have been widely used as a potential candidate for renewable energy storage devices, like lithium-ion batteries and supercapacitors and they can improve the green credentials and performance of energy storage devices. Furthermore, ionic liquids have found extensive use in solar cells as electrolytes, demonstrating favorable outcomes in terms of increased durability and heightened efficiency of the devices. These devices have become indispensable in human life and they are playing a vital and promising role in the worldwide endeavor to address both the challenges of renewable energy supply and air pollution simultaneously. The energy storage ability and safety of energy storage devices are in fact determined by the arrangement of ions and electrons between the electrode and the electrolyte. In this review, we provide an overview of ionic liquids as electrolytes in lithium-ion batteries, supercapacitors and, solar cells.

Graphical abstract

由于离子液体具有不挥发性、高热稳定性、可忽略的蒸汽压和高离子电导率等特性,基于离子液体的电解质已被广泛用作锂离子电池和超级电容器等可再生能源存储设备的潜在候选材料,它们可以提高能源存储设备的绿色证书和性能。此外,离子液体作为电解质已广泛应用于太阳能电池,并在提高设备的耐用性和效率方面取得了良好的效果。这些设备已成为人类生活中不可或缺的设备,在全球同时应对可再生能源供应和空气污染两大挑战的努力中,它们正发挥着至关重要且前景广阔的作用。事实上,储能设备的储能能力和安全性取决于电极和电解质之间的离子和电子排列。在本综述中,我们将概述离子液体作为电解质在锂离子电池、超级电容器和太阳能电池中的应用。
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引用次数: 0
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Monatshefte für Chemie / Chemical Monthly
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