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Recent progress in the application of amidines for the synthesis of N-heterocyclic compounds 应用脒合成 N-杂环化合物的最新进展
Pub Date : 2024-03-06 DOI: 10.1007/s00706-024-03180-w

Abstract

Nitrogen-containing heterocycles are an inseparable part of many biologically active compounds. Therefore, the synthesis of these structures is of great importance in the field of synthetic chemistry. Due to the presence of two nitrogen atoms in the amidine structure, this molecule can be considered as a dual nucleophile in the synthesis of various heterocycles. The current review highlights recent advances in the application of amidines, in particular, N-arylamidines, as versatile precursors in transition metal-catalyzed, and metal-free reactions for the construction of N-heterocyclic compounds.

Graphical abstract

摘要 含氮杂环是许多生物活性化合物不可分割的一部分。因此,合成这些结构在合成化学领域具有重要意义。由于脒结构中存在两个氮原子,这种分子在合成各种杂环时可被视为双亲核体。本综述重点介绍了在过渡金属催化和无金属反应中应用脒,特别是 N-芳基脒作为多功能前体来构建 N-杂环化合物的最新进展。 图表摘要
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引用次数: 0
Green synthesis of MnO2 using Calendula officinalis and Tilia cordata extracts for application in supercapacitors 利用金盏花和椴树提取物绿色合成 MnO2 以应用于超级电容器
Pub Date : 2024-03-05 DOI: 10.1007/s00706-024-03179-3
Borislava Mladenova, Katya Pashova, Ivaylo Hinkov, Mariela Dimitrova, Antonia Stoyanova

Green synthesis of MnO2 was carried out using natural extracts of Tilia cordata (TC) and Calendula officinalis (CO). Utilizing the transmission electron microscopy, powder X-ray diffraction, and UV–Vis spectra techniques confirmed the successful synthesis of α-MnO2. The BET analysis showed that the CO-derived material has a larger surface area and appropriate mesoporous structure. The obtained synthesized materials were assembled in asymmetric supercapacitor test cell, with a polymer membrane serving as a separator and an electrolyte. The prepared CO-MnO2 demonstrates excellent capacitance and energy characteristics and seems to be a promising electrode material for the development of environmentally friendly solid-state supercapacitors.

Graphical abstract

利用椴树(Tilia cordata,TC)和金盏花(Calendula officinalis,CO)的天然提取物进行了二氧化锰的绿色合成。透射电子显微镜、粉末 X 射线衍射和紫外可见光谱技术证实了 α-MnO2 的成功合成。BET 分析表明,CO 衍生材料具有较大的比表面积和适当的介孔结构。将合成的材料组装到不对称超级电容器试验电池中,用聚合物膜作为隔膜和电解质。所制备的 CO-MnO2 具有优异的电容和能量特性,似乎是一种很有前途的电极材料,可用于开发环境友好型固态超级电容器。
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引用次数: 0
Enhancing of methyl orange oxidation using nanotube sensor: analytical application in water 利用纳米管传感器增强甲基橙氧化:在水中的分析应用
Pub Date : 2024-03-05 DOI: 10.1007/s00706-024-03183-7
B. R. Krithi, J. G. Manjunatha, B. Kanthappa, Mika Sillanpaa, Sameh M. Osman

The electrochemical properties of poly(l-asparagine) modified carbon nanotube paste electrode (PAMCNPE) were investigated for precise detection of methyl orange. Asparagine was electrochemical polymerized and deposited onto the carbon nanotube paste surface to develop the modified electrode, and comparing to the bare carbon nanotube paste electrode. Cyclic voltammetry measurements of the modified electrode at pH 7 in a 0.2 M phosphate buffer saline showed excellent oxidizing activity towards methyl orange. Various factors were studied, including the ionic strength of the buffer. The external morphology and conversion of the perception material were studied using field emission scanning electron microscopy and electrochemical impedance spectroscopy, respectively. High sensitivity and selectivity for detecting methyl orange were also achieved by optimizing experimental conditions such of pH, concentration variation, and scan rate. The concentration range spanned from 0.2 to 9.0 µM, with the lower limit of detection at 1.368 × 10–7 M and the quantification limit of 4.562 × 10–7 M, indicating its excellent analytical performance. Additionally, the PAMCNPE shows good stability, reproducibility, and repeatability. Its remarkable recovery in real samples underscores its potential for practical applications in environmental and clinical analysis.

Graphical abstract

研究了聚天冬酰胺修饰碳纳米管浆料电极(PAMCNPE)的电化学特性,以精确检测甲基橙。天冬酰胺经电化学聚合后沉积在碳纳米管浆料表面,形成改性电极,并与裸碳纳米管浆料电极进行比较。在 pH 值为 7 的 0.2 M 磷酸盐缓冲盐溶液中对修饰电极进行的循环伏安测量显示,该电极对甲基橙具有极佳的氧化活性。研究了各种因素,包括缓冲液的离子强度。利用场发射扫描电子显微镜和电化学阻抗光谱分别研究了感知材料的外部形态和转化。通过优化 pH 值、浓度变化和扫描速率等实验条件,还实现了检测甲基橙的高灵敏度和高选择性。甲基橙的浓度范围为 0.2 至 9.0 µM,检测下限为 1.368 × 10-7 M,定量限为 4.562 × 10-7 M,显示了其卓越的分析性能。此外,PAMCNPE 还具有良好的稳定性、再现性和重复性。它在实际样品中的出色回收率突显了其在环境和临床分析中的实际应用潜力。
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引用次数: 0
Lithium-ion (LCO/NMC, NMC, LFP) battery recycling: partial LCA study 锂离子(LCO/NMC、NMC、LFP)电池回收:部分生命周期评估研究
Pub Date : 2024-03-05 DOI: 10.1007/s00706-024-03184-6
Michael Fridrich, Anna Pražanová, Jan Weinzettel, Vaclav Knap

Recycling lithium-ion batteries (LIBs) have become increasingly important in response to expanding electromobility. This paper is focused on evaluating the environmental impacts (EIs) of recycling pre-treatment of three types of LIBs with black mass as its product. A detailed gate-to-gate Life Cycle Assessment study was conducted to obtain EIs of the recycling process. The benefits of LIBs recycling pre-treatment and significant recovery of secondary aluminum for compared battery types are highlighted in the analysis. This paper points out that the varying chemistry of the compared LIBs does not affect the resulting EIs of the recycling pre-treatment procedures.

Graphical abstract

随着电动交通的不断发展,锂离子电池(LIB)的回收利用变得越来越重要。本文重点评估了以黑块为产品的三种锂离子电池回收预处理对环境的影响(EIs)。为了获得回收过程的环境影响指数,进行了详细的门到门生命周期评估研究。分析结果强调了锂电子电池回收预处理的益处,以及对比电池类型回收二次铝的显著效果。本文指出,所比较的锂离子电池的不同化学性质并不会影响回收预处理程序所产生的环境影响指数。
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引用次数: 0
Detection of ammonia mercerization in cotton textiles 棉纺织品中氨丝光的检测
Pub Date : 2024-03-05 DOI: 10.1007/s00706-024-03181-9

Abstract

Cotton textiles are mercerized with anhydrous ammonia liquefied at ca. − 33 °C to improve their mechanical performance, appearance, and handle. Similar effects may also be achieved with NaOH mercerization, but goods mercerized with liquid ammonia (L-NH3) are judged qualitatively better (e.g., softer hand) and thus command a greater price. Therefore, it is of interest to be able to test and confirm whether cotton textiles labeled as L-NH3 treated are indeed so. Building on previous work, we report on tests in collaboration with a process house on identifying ammonia-mercerized fabrics from a pool of cotton textiles treated with L-NH3, NaOH, neither, or both––using FTIR-ATR spectroscopy. It is based on detecting the change in crystal lattice structure from type I (native cellulose) to type II (after NaOH mercerization) or type III (after ammonia mercerization). We could consistently differentiate the ammonia-mercerized fabrics from the untreated and those mercerized with NaOH, but the latter could not be differentiated from fabrics mercerized with both. It was also possible to detect evidence of ammonia mercerization in 4- and 14-year-old samples.

Graphical abstract

摘要 棉纺织品用液化温度约为 33 °C 的无水氨进行丝光处理。- 33 °C 下进行丝光处理,以改善其机械性能、外观和手感。用 NaOH 丝光处理也可达到类似效果,但用液氨(L-NH3)丝光处理的产品被认为质量更好(如手感更柔软),因此价格更高。因此,我们有兴趣测试并确认标注为 L-NH3 处理过的棉纺织品是否确实如此。在以往工作的基础上,我们与一家加工厂合作,利用傅立叶变换红外-ATR 光谱法,从经过 L-NH3、NaOH 或两者处理的棉纺织品中识别氨铈化织物。其原理是检测晶格结构从 I 型(原生纤维素)到 II 型(NaOH 丝光处理后)或 III 型(氨丝光处理后)的变化。我们可以将氨丝光处理过的织物与未处理过的织物和用 NaOH 丝光处理过的织物区分开来,但无法将后者与用这两种方法丝光处理过的织物区分开来。在 4 岁和 14 岁的样品中也能检测到氨丝光的证据。 图表摘要
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引用次数: 0
Impedance changes of the Li-ion cell in the course of discharge 锂离子电池在放电过程中的阻抗变化
Pub Date : 2024-03-05 DOI: 10.1007/s00706-024-03175-7
Petr Křivík

The paper deals with the measurement of the cell impedance parameters during discharging of the Li-ion NCR18650B cell. Re (Z) and Im (Z) of the battery were measured by PEIS method. The results of the impedance changes during discharging and charging were plot to Nyquist diagrams. The important values namely Rs, Rsei, Rct, Csei, Qsei, Cdl, α, and σ were found during discharging of the Li-ion cell with and without using CPE element.

Graphical abstract

本文涉及锂离子 NCR18650B 电池放电过程中电池阻抗参数的测量。采用 PEIS 方法测量了电池的 Re (Z) 和 Im (Z)。放电和充电过程中的阻抗变化结果绘制成奈奎斯特图。在使用和未使用 CPE 元件的锂离子电池放电过程中,发现了一些重要值,即 Rs、Rsei、Rct、Csei、Qsei、Cdl、α 和 σ。
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引用次数: 0
Comparative photoelectrochemical characteristics of heterostructure and composite based on BiVO4 and WO3 基于 BiVO4 和 WO3 的异质结构和复合材料的光电化学特性比较
Pub Date : 2024-02-27 DOI: 10.1007/s00706-023-03167-z
V. O. Smilyk, S. S. Fomanyuk, I. A. Rusetskyi, M. O. Danilov, G. Ya. Kolbasov

Films of heterostructure BiVO4/WO3, composite BiVO4 with WO3 and pure BiVO4 were obtained by electrochemical deposition. Analysis of photoelectrochemical characteristics of such films showed that observed increase in photocurrent quantum yield and decrease in overvoltage of oxygen evolution on the photoanode in row from pure BiVO4 films, than in heterostructure BiVO4/WO3, after that—composite BiVO4–WO3. The reason of such positive effect of reducing the energy losses associated with the surface recombination of electrons and holes and reduction of losses at the stage of interfacial charge transfer in the BiVO4–WO3 composite compared with the heterostructure BiVO4/WO3 and pure BiVO4.

Graphical abstract

通过电化学沉积法获得了异质结构 BiVO4/WO3、BiVO4 与 WO3 的复合薄膜以及纯 BiVO4 薄膜。对这些薄膜的光电化学特性进行的分析表明,与异质结构 BiVO4/WO3 相比,纯 BiVO4 薄膜的光电量子产率有所提高,光阳极上氧演化的过电压有所降低,而异质结构 BiVO4/WO3 和复合 BiVO4-WO3 的光电量子产率则低于纯 BiVO4 薄膜。与异质结构 BiVO4/WO3 和纯 BiVO4 相比,BiVO4-WO3 复合材料在减少与电子和空穴表面重组相关的能量损失以及减少界面电荷转移阶段的损失方面具有积极作用,其原因就在于此。
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引用次数: 0
Hydrogen production with reduced energy consumption for use in fuel cells and energy sector 生产氢气,降低能耗,用于燃料电池和能源领域
Pub Date : 2024-02-26 DOI: 10.1007/s00706-023-03159-z

Abstract

The possibility of increasing the hydrogen release rate and reducing energy consumption was analyzed using a system in which the anodic process of metal (aluminum) dissolution occurred on one electrode and the process of H2 release on the other (nickel) electrode. The possibility of generating hydrogen with a current density of ~ 400 mA cm–2 in NaOH solutions with a concentration of 6–8 mol dm–3 at a cell voltage of ~ 0.5 V was confirmed. When the electrodes were short-circuited, hydrogen was generated on nickel when aluminum was dissolved at a rate corresponding to current density ~ 100 mA cm–2. The possibility of simultaneous hydrogen production and electricity generation in the system under consideration was shown. It was found that the maximum net power was generated in 6 mol dm–3 NaOH. The specific power in such a solution can reach a value of 8 mW cm–2 at a cell voltage of about 0.15 V. In this case, the hydrogen release rate corresponded to a current density of 60 mA cm–2.

Graphical abstract

摘要 利用一个系统分析了提高氢气释放率和降低能耗的可能性,在该系统中,金属(铝)的阳极溶解过程发生在一个电极上,而氢气释放过程发生在另一个电极(镍)上。实验证实,在浓度为 6-8 mol dm-3 的 NaOH 溶液中,电池电压约为 0.5 V,电流密度约为 400 mA cm-2,即可产生氢气。当电极短路时,当铝溶解时,镍上产生氢气的速率相当于电流密度 ~ 100 mA cm-2。研究表明,在所考虑的系统中,可以同时制氢和发电。研究发现,在 6 mol dm-3 NaOH 溶液中产生的净功率最大。在这种情况下,氢气释放率相当于 60 mA cm-2 的电流密度。 图表摘要
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引用次数: 0
Synthesis of novel GABA-Triazole tethered derivatives of Noscapine and their anticancer activities 合成新型 GABA-三唑拴系的莨菪碱衍生物及其抗癌活性
Pub Date : 2024-02-24 DOI: 10.1007/s00706-024-03170-y
Farzaneh Karimi, Peyman Salehi, Morteza Bararjanian

Synthesis of novel noscapine triazole tethered derivatives with γ-aminobutyric acid (GABA) linker is reported. Attachment of the linker was done by N-demethylation of noscapine followed by coupling with N-Boc protected GABA. The straightforward synthesis of the target molecules was made by a three-component reaction between GABA-noscapine, p-nitrophenyl azide, and commercially available ketones under metal-free conditions to produce a library with diverse functional groups. Anticancer activity of the synthesized derivatives was evaluated on MCF-7 cancer cell line. The best anticancer activity was demonstrated by a compound with an IC50 value of 57.2 µM, close to that of noscapine (IC50 = 55.2 µM).

Graphical abstract

报告了带有γ-氨基丁酸(GABA)连接物的新型莨菪三唑系链衍生物的合成。通过对莨菪碱进行 N-去甲基化,然后与 N-Boc 保护的 GABA 偶联,实现了连接体的连接。在无金属条件下,通过 GABA-noscapine、对硝基苯叠氮化物和市售酮类之间的三组份反应,直接合成了目标分子,从而产生了具有不同官能团的化合物库。在 MCF-7 癌细胞系上评估了合成衍生物的抗癌活性。其中一个化合物的抗癌活性最佳,其 IC50 值为 57.2 µM,接近莨菪碱(IC50 = 55.2 µM)。
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引用次数: 0
Redox cationic frontal polymerization: a rapid curing approach for carbon fiber-reinforced composites with high fiber content 氧化还原阳离子正面聚合:高纤维含量碳纤维增强复合材料的快速固化方法
Pub Date : 2024-02-22 DOI: 10.1007/s00706-023-03168-y

Abstract

Conventional frontal polymerization processes for epoxy-based composites rely on cations and radicals generated by a short (and local) light or heat stimulus in the presence of an iodonium salt and a radical thermal initiator. However, due to heat losses, the propagation of the exothermic curing front is often limited by sample geometry and filler concentration. Redox cationic frontal polymerization (RCFP) is a promising approach to radically expand the composition and design options of frontally cured epoxy-based composites. By adding stannous octoate as reducing agent, a higher number of radicals and cations are generated at lower temperature, which yields highly cured composite even at elevated filler content. In the current study, RCFP was used to cure standard unidirectional carbon fiber-reinforced composites based on a commercially available epoxy resin and the properties were compared with its anhydride hardener-cured counterpart. Cure degree and thermal properties of the resins were determined by ATR FT-IR spectroscopy and DMA analysis. Subsequently, unidirectional composites with a fiber volume content of ~ 60% were produced via vacuum infusion and subjected to DMA, tensile, compression, and inter-laminar shear tests. The results showed a remarkable similarity between mechanical properties of RCFP and anhydride hardener-cured composites. The RCFP-cured composites exhibited even a higher damping resistance and compression strength than anhydride hardener-cured composites. The results show that RCFP allows for a significant reduction in the curing time (from several hours to 60 min), while it yields composites with properties comparable to classic anhydride-cured systems.

Graphical abstract

摘要 环氧基复合材料的传统前沿聚合工艺依赖于在碘盐和自由基热引发剂存在下,通过短时间(和局部)光或热刺激产生的阳离子和自由基。然而,由于热损失,放热固化前沿的传播往往受到样品几何形状和填料浓度的限制。氧化还原阳离子正面聚合(RCFP)是一种很有前途的方法,可从根本上扩展正面固化环氧基复合材料的组成和设计选择。通过添加辛酸亚锡作为还原剂,可在较低温度下生成更多的自由基和阳离子,即使在填料含量较高的情况下也能得到高度固化的复合材料。在目前的研究中,RCFP 被用于固化基于市售环氧树脂的标准单向碳纤维增强复合材料,并与酸酐固化剂固化的复合材料进行了性能比较。通过 ATR 傅立叶变换红外光谱和 DMA 分析确定了树脂的固化度和热性能。随后,通过真空灌注生产了纤维体积含量约为 60% 的单向复合材料,并对其进行了 DMA、拉伸、压缩和层间剪切试验。结果表明,RCFP 和酸酐固化剂固化复合材料的机械性能非常相似。与酸酐固化剂固化复合材料相比,RCFP 固化复合材料甚至表现出更高的抗阻尼性和压缩强度。研究结果表明,RCFP 可大大缩短固化时间(从数小时缩短至 60 分钟),同时可获得与传统酸酐固化体系性能相当的复合材料。 图表摘要
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引用次数: 0
期刊
Monatshefte für Chemie / Chemical Monthly
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