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The Intramolecular Povarov Tool in the Construction of Fused Nitrogen-Containing Heterocycles 构建含氮杂环的分子内Povarov工具
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-05-30 DOI: 10.1007/s41061-023-00428-7
Carme Masdeu, Jesús M. de los Santos, Francisco Palacios, Concepción Alonso

Nitrogen heterocycles are part of the structure of natural products and agents with important biological activity, such as antiviral, antibiotic, and antitumor drugs. For this reason, heterocyclic compounds are one of today’s most desirable synthetic targets and the Povarov reaction is a powerful synthetic tool for the construction of highly functionalized heterocyclic systems. This process involves an aromatic amine, a carbonyl compound, and an olefin or acetylene to give rise to the formation of a nitrogen-containing heterocycle. This review illustrates advances in the synthetic aspects of the intramolecular Povarov reaction for the construction of intricate nitrogen-containing polyheterocyclic compounds. This original review presents research done in this field, with references to important works by internationally relevant research groups on this current topic, covering the literature from 1992 to 2022. The intramolecular Povarov reactions are described here according to the key processes involved, using different combinations of aromatic or heteroaromatic amines, and aliphatic, aromatic, or heteroaromatic aldehydes. Some catalytic reactions promoted by transition metals are detailed, as well as the oxidative Povarov reaction and some asymmetric intramolecular Povarov processes.

氮杂环是抗病毒、抗生素、抗肿瘤药物等具有重要生物活性的天然产物和制剂结构的一部分。因此,杂环化合物是当今最理想的合成靶点之一,而Povarov反应是构建高功能化杂环体系的有力合成工具。这一过程涉及芳香胺、羰基化合物和烯烃或乙炔,以形成含氮杂环。本文综述了分子内Povarov反应合成复杂含氮多杂环化合物的研究进展。这篇原创综述介绍了在这一领域所做的研究,并参考了国际相关研究小组在这一当前主题上的重要工作,涵盖了从1992年到2022年的文献。分子内Povarov反应在这里根据所涉及的关键过程进行描述,使用芳香或杂芳香胺以及脂肪、芳香或杂芳香醛的不同组合。详细介绍了过渡金属催化的一些反应,以及氧化波瓦洛夫反应和一些不对称分子内波瓦洛夫过程。
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引用次数: 1
Photothermal Catalytic CO2 Conversion: Beyond Catalysis and Photocatalysis 光热催化CO2转化:超越催化与光催化
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-05-30 DOI: 10.1007/s41061-023-00430-z
Fernando Fresno, Ana Iglesias-Juez, Juan M. Coronado

In recent years, the combination of both thermal and photochemical contributions has provided interesting opportunities for solar upgrading of catalytic processes. Photothermal catalysis works at the interface between purely photochemical processes, which involve the direct conversion of photon energy into chemical energy, and classical thermal catalysis, in which the catalyst is activated by temperature. Thus, photothermal catalysis acts in two different ways on the energy path of the reaction. This combined catalysis, of which the fundamental principles will be reviewed here, is particularly promising for the activation of small reactive molecules at moderate temperatures compared to thermal catalysis and with higher reaction rates than those attained in photocatalysis, and it has gained a great deal of attention in the last years. Among the different applications of photothermal catalysis, CO2 conversion is probably the most studied, although reaction mechanisms and photonic-thermal synergy pathways are still quite unclear and, from the reaction route point of view, it can be said that photothermal-catalytic CO2 reduction processes are still in their infancy. This article intends to provide an overview of the principles underpinning photothermal catalysis and its application to the conversion of CO2 into useful molecules, with application essentially as fuels but also as chemical building blocks. The most relevant specific cases published to date will be also reviewed from the viewpoint of selectivity towards the most frequent target products.

近年来,热化学和光化学的结合为太阳能催化过程的升级提供了有趣的机会。光热催化作用于纯光化学过程和经典热催化之间的界面,前者将光子能量直接转化为化学能,后者由温度激活催化剂。因此,光热催化在反应的能量路径上以两种不同的方式起作用。与热催化相比,这种组合催化尤其有希望在中等温度下激活小活性分子,并具有比光催化更高的反应速率,近年来得到了广泛的关注。在光热催化的不同应用中,CO2转化可能是研究最多的,尽管反应机理和光热协同途径还很不清楚,从反应途径来看,可以说光热催化CO2还原过程还处于起步阶段。本文旨在概述光热催化的基本原理及其在将二氧化碳转化为有用分子方面的应用,其应用主要是作为燃料,但也作为化学基石。还将从对最常见的目标产品的选择性角度审查迄今发表的最相关的具体案例。
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引用次数: 0
Multicomponent Reactions Using C,N-Binucleophilic Nature of Aminopyrazoles: Construction of Pyrazole-Fused Heterocycles 利用氨基吡唑的C, n -双亲核性质的多组分反应:吡唑融合杂环的构建
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-05-26 DOI: 10.1007/s41061-023-00427-8
Tasneem Parvin

Synthesis of pyrazole-fused heterocycles has gained considerable attention in recent years due to their wide applications in medicinal chemistry. Aminopyrazoles are versatile building blocks for the synthesis of pyrazole-fused heterocycles by multicomponent reactions. Due to the presence of multiple reaction sites, they have fascinating chemical reactivity. Thus, they have been extensively used in multicomponent reactions for the construction of pyrazole-fused heterocycles. Although few review articles on the preparation and applications of aminopyrazoles are known in the literature, to date there is no dedicated review article on the construction of pyrazole-fused heterocycles exploring the reactivity of amino pyrazoles as C,N-binucleophiles in multicomponent reactions. Considering this, herein the multicomponent reactions for the construction of pyrazole-fused heterocycles exploring C,N-binucleophilic nature of amino pyrazoles have been reported.

Graphical Abstract

近年来,吡唑类杂环化合物的合成因其在药物化学中的广泛应用而备受关注。氨基吡唑是通过多组分反应合成吡唑-杂环化合物的通用构件。由于存在多个反应位点,它们具有迷人的化学反应活性。因此,它们在多组分反应中被广泛用于构建吡唑-杂环。虽然文献中很少有关于氨基吡唑的制备和应用的综述文章,但迄今为止还没有专门的关于构建吡唑-融合杂环的综述文章,探讨氨基吡唑作为C, n -双亲核试剂在多组分反应中的反应性。考虑到这一点,本文报道了构建吡唑-融合杂环的多组分反应,以探索氨基吡唑的C, n -二亲核性质。图形抽象
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引用次数: 0
Laser-Induced Transfer of Functional Materials 功能材料的激光诱导转移
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-05-22 DOI: 10.1007/s41061-023-00429-6
Connie Kong Wai Lee, Yexin Pan, Rongliang Yang, Minseong Kim, Mitch Guijun Li

Patterning is crucial for the large-scale application of functional materials. Laser-induced transfer is an emerging patterning method for additively depositing functional materials to the target acceptor. With the rapid development of laser technologies, this laser printing method emerges as a versatile method to deposit functional materials in either liquid or solid format. The emerging applications such as solar interfacial evaporation, solar cells, light-emitting diodes, sensors, high-output synthesis, and other fields are rising fields benefiting from laser-induced transfer. Following a brief introduction to the principles of laser-induced transfer, this review will comprehensively deliberate this novel additive manufacturing method, including preparing the donor layer and the applications, advantages, and limitations of this technique. Finally, perspectives for handling current and future functional materials using laser-induced transfer will also be discussed. Non-experts in laser technologies can also gain insights into this prevailing laser-induced transfer process, which may inspire their future research.

图案化对于功能材料的大规模应用至关重要。激光诱导转移是一种新兴的将功能材料增材沉积到目标受体上的图案化方法。随着激光技术的快速发展,激光打印技术作为一种多用途的液体或固体形式沉积功能材料的方法而出现。新兴的应用如太阳界面蒸发、太阳能电池、发光二极管、传感器、高输出合成等领域都是受益于激光诱导转移的新兴领域。在简要介绍了激光诱导转移的原理之后,本文将全面讨论这种新型的增材制造方法,包括供体层的制备以及该技术的应用、优点和局限性。最后,还将讨论利用激光诱导转移处理当前和未来功能材料的前景。非激光技术专家也可以深入了解这种流行的激光诱导转移过程,这可能会启发他们未来的研究。
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引用次数: 1
Oxime Esters: Flexible Building Blocks for Heterocycle Formation 肟酯:杂环形成的柔性构建块
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-05-18 DOI: 10.1007/s41061-023-00431-y
Faeze Yousefnejad, Fatemeh Gholami, Bagher Larijani, Mohammad Mahdavi

Oxime esters as the applicable building blocks, internal oxidizing agents, and directing groups in the synthesis of –, S-, and O-containing heterocycle scaffolds have gained great attention in the last decade. This review provides an overview of recent advances in the cyclization of oxime esters with various functional group reagents under transition metal and transition metal-free catalyzed conditions. Moreover, the mechanistic aspects of these protocols are explained in detail.

Graphical Abstract

近十年来,肟酯作为一种适用于含-、S-和o型杂环支架合成的构建基、内氧化剂和导向基团受到了广泛的关注。本文综述了近年来在过渡金属和无过渡金属催化条件下肟酯与各种官能团试剂的环化反应的研究进展。此外,还详细解释了这些协议的机制方面。图形抽象
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引用次数: 0
Spectroscopic Determination of Acetylcholine (ACh): A Representative Review 光谱法测定乙酰胆碱(ACh)的研究进展
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-05-11 DOI: 10.1007/s41061-023-00426-9
Paweł Świt, Aleksandra Pollap, Joanna Orzeł

Acetylcholine (ACh) is one of the most crucial neurotransmitters of the cholinergic system found in vertebrates and invertebrates and is responsible for many processes in living organisms. Disturbances in ACh transmission are closely related to dementia in Alzheimer’s and Parkinson’s disease. ACh in biological samples is most often determined using chromatographic techniques, radioenzymatic assays, enzyme-linked immunosorbent assay (ELISA), or potentiometric methods. An alternative way to detect and determine acetylcholine is applying spectroscopic techniques, due to low limits of detection and quantification, which is not possible with the methods mentioned above. In this review article, we described a detailed overview of different spectroscopic methods used to determine ACh with a collection of validation parameters as a perspective tool for routine analysis, especially in basic research on animal models on central nervous system. In addition, there is a discussion of examples of other biological materials from clinical and preclinical studies to give the whole spectrum of spectroscopic methods application. Descriptions of the developed chemical sensors, as well as the use of flow technology, were also presented. It is worth emphasizing the inclusion in the article of multi-component analysis referring to other neurotransmitters, as well as the description of the tested biological samples and extraction procedures. The motivation to use spectroscopic techniques to conduct this type of analysis and future perspectives in this field are briefly discussed.

Graphical Abstract

乙酰胆碱(ACh)是在脊椎动物和无脊椎动物中发现的胆碱能系统中最重要的神经递质之一,负责生物体的许多过程。乙酰胆碱传递障碍与阿尔茨海默病和帕金森病的痴呆密切相关。生物样品中的乙酰胆碱通常使用色谱技术、放射酶测定、酶联免疫吸附测定(ELISA)或电位测定法测定。另一种检测和测定乙酰胆碱的方法是应用光谱技术,由于检测和定量限低,这是不可能用上述方法。在这篇综述文章中,我们详细概述了不同的光谱方法,通过一系列验证参数来确定乙酰胆碱,作为常规分析的透视工具,特别是在中枢神经系统动物模型的基础研究中。此外,还讨论了其他生物材料的临床和临床前研究实例,给出了全光谱光谱方法的应用。介绍了化学传感器的发展情况,以及流动技术的应用。值得强调的是,文章中包含了涉及其他神经递质的多组分分析,以及对测试生物样品和提取程序的描述。本文简要讨论了利用光谱技术进行这类分析的动机和该领域的未来前景。图形抽象
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引用次数: 1
Photocatalytic Synthesis of Hydrogen Peroxide from Molecular Oxygen and Water 分子氧与水光催化合成过氧化氢的研究
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-05-09 DOI: 10.1007/s41061-023-00423-y
Patricia Garcia-Munoz, Laura Valenzuela, Deborah Wegstein, Tobias Schanz, Girlie Eunice Lopez, Agnieszka M. Ruppert, Hynd Remita, Jonathan Z. Bloh, Nicolas Keller

Hydrogen peroxide is a powerful and green oxidant that allows for the oxidation of a wide span of organic and inorganic substrates in liquid media under mild reaction conditions, and forms only molecular water and oxygen as end products. Hydrogen peroxide is therefore used in a wide range of applications, for which the well-documented and established anthraquinone autoxidation process is by far the dominating production method at the industrial scale. As this method is highly energy consuming and environmentally costly, the search for more sustainable synthesis methods is of high interest. To this end, the article reviews the basis and the recent development of the photocatalytic synthesis of hydrogen peroxide. Different oxygen reduction and water oxidation mechanisms are discussed, as well as several kinetic models, and the influence of the main key reaction parameters is itemized. A large range of photocatalytic materials is reviewed, with emphasis on titania-based photocatalysts and on high-prospect graphitic carbon nitride-based systems that take advantage of advanced bulk and surface synthetic approaches. Strategies for enhancing the performances of solar-driven photocatalysts are reported, and the search for new, alternative, photocatalytic materials is detailed. Finally, the promise of in situ photocatalytic synthesis of hydrogen peroxide for water treatment and organic synthesis is described, as well as its coupling with enzymes and the direct in situ synthesis of other technical peroxides.

过氧化氢是一种强大的绿色氧化剂,它允许在温和的反应条件下氧化液体介质中广泛的有机和无机底物,并且只形成分子水和氧作为最终产物。因此,过氧化氢在广泛的应用中得到了广泛的应用,其中有充分记录和建立的蒽醌自氧化工艺是迄今为止工业规模上的主要生产方法。由于这种方法耗能大,环境成本高,因此寻找更可持续的合成方法是人们高度关注的问题。为此,本文综述了光催化合成过氧化氢的基础和最新进展。讨论了不同的氧还原和水氧化机理,以及几种动力学模型,并列举了主要关键反应参数的影响。综述了大量的光催化材料,重点介绍了钛基光催化剂和具有高前景的石墨氮化碳基系统,它们利用了先进的体和表面合成方法。报告了提高太阳能驱动光催化剂性能的策略,并详细介绍了寻找新的替代光催化材料的情况。最后,介绍了原位光催化合成过氧化氢用于水处理和有机合成的前景,以及它与酶的偶联和其他技术过氧化物的直接原位合成。
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引用次数: 0
Strategies Toward the Catalyst-Free α-C–H Functionalizations of Tertiary Amines 叔胺无催化剂α-C-H官能化的研究策略
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-05-03 DOI: 10.1007/s41061-023-00424-x
Mohit L. Deb, Pranjal K. Baruah

α-C–H functionalization of tertiary amines has been a highly studied field for the past two decades because several important nitrogen containing heterocycles or compounds can be synthesized through this strategy. Though transition metal catalysts and some metal-free catalysts are mainly used for these reactions, a few catalyst-free reactions have recently been efficiently performed. Catalyst-free reactions are cost-effective, less sensitive to air/moisture, easier to operate, have a simple purification process, and are relatively environment-friendly. In this article, we have summarized all the α-C–H functionalization reactions of tertiary amines performed without using any external catalysts. The content of this article will undoubtedly encourage readers to do more work in this area.

Graphical Abstract

叔胺的α-C-H功能化在过去的二十年里一直是一个高度研究的领域,因为通过这种策略可以合成几种重要的含氮杂环或化合物。虽然过渡金属催化剂和一些无金属催化剂主要用于这些反应,但近年来一些无催化剂的反应也得到了有效的实现。无催化剂反应具有成本效益高、对空气/水分不敏感、操作简单、净化过程简单、相对环保等优点。本文综述了在不使用任何外部催化剂的情况下叔胺的α-C-H功能化反应。这篇文章的内容无疑会鼓励读者在这方面做更多的工作。图形抽象
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引用次数: 0
Solid-State Nanopore/Nanochannel Sensing of Single Entities 单一实体的固态纳米孔/纳米通道传感
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-04-27 DOI: 10.1007/s41061-023-00425-w
Wei Yi, Chuanping Zhang, Qianchun Zhang, Changbo Zhang, Yebo Lu, Lanhua Yi, Xingzhu Wang

Solid-state nanopores/nanochannels, with their high stability, tunable geometry, and controllable surface chemistry, have recently become an important tool for constructing biosensors. Compared with traditional biosensors, biosensors constructed with solid-state nanopores/nanochannels exhibit significant advantages of high sensitivity, high specificity, and high spatiotemporal resolution in the detection single entities (such as single molecules, single particles, and single cells) due to their unique nanoconfined space-induced target enrichment effect. Generally, the solid-state nanopore/nanochannel modification method is the inner wall modification, and the detection principles are the resistive pulse method and the steady-state ion current method. During the detection process, solid-state nanopore/nanochannel is easily blocked by single entities, and interfering substances easily enter the solid-state nanopore/nanochannel to generate interference signals, resulting in inaccurate measurement results. In addition, the problem of low flux in the detection process of solid-state nanopore/nanochannel, these defects limit the application of solid-state nanopore/nanochannel. In this review, we introduce the preparation and functionalization of solid-state nanopore/nanochannel, the research progress in the field of single entities sensing, and the novel sensing strategies on solving the above problems in solid-state nanopore/nanochannel single-entity sensing. At the same time, the challenges and prospects of solid-state nanopore/nanochannel for single-entity electrochemical sensing are also discussed.

Graphical Abstract

固体纳米孔/纳米通道以其高稳定性、可调节的几何结构和可控制的表面化学性质,近年来成为构建生物传感器的重要工具。与传统的生物传感器相比,固体纳米孔/纳米通道构建的生物传感器由于其独特的纳米受限空间诱导靶富集效应,在检测单个实体(如单分子、单颗粒和单细胞)方面具有高灵敏度、高特异性和高时空分辨率的显著优势。一般固态纳米孔/纳米通道修饰方法为内壁修饰,检测原理为电阻脉冲法和稳态离子电流法。在检测过程中,固态纳米孔/纳米通道容易被单一实体堵塞,干扰物质容易进入固态纳米孔/纳米通道产生干扰信号,导致测量结果不准确。此外,固态纳米孔/纳米通道在检测过程中存在低通量问题,这些缺陷限制了固态纳米孔/纳米通道的应用。本文介绍了固态纳米孔/纳米通道的制备、功能化、单实体传感领域的研究进展,以及在固态纳米孔/纳米通道单实体传感中解决上述问题的新型传感策略。同时,讨论了固态纳米孔/纳米通道用于单实体电化学传感的挑战和前景。图形抽象
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引用次数: 0
The Rise of MXene: A Wonder 2D Material, from Its Synthesis and Properties to Its Versatile Applications—A Comprehensive Review MXene的崛起:一种神奇的2D材料,从它的合成和性能到它的多功能应用-全面回顾
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-03-13 DOI: 10.1007/s41061-023-00420-1
Kamna Chaturvedi, Vaishnavi Hada, Sriparna Paul, Bibek Sarma, Deeksha Malvi, Manish Dhangar, Harsh Bajpai, Anju Singhwane, Avanish Kumar Srivastava, Sarika Verma

MXene, a new member of 2D material, unites the eminence of hydrophilicity, large surface groups, superb flexibility and excellent conductivity. Because of its prodigious characteristics, MXene has gained much approbation among researchers worldwide. MXene’s noteworthy features, such as its electrical conductivity, structural property, magnetic behaviour, etc., manifest a broad spectrum of applications, including environment, catalytic, wireless communications, electromagnetic interference (EMI) shielding, drug delivery, wound dressing, bio-imaging, antimicrobial and biosensor. In this review article, an overview of the latest advancements in the applications of MXene has been reported. First, various synthesis strategies of MXene will be summarized, followed by the different structural, physical and chemical properties. The current advances in versatile applications have been discussed. The article aims to incorporate all the possible applications of MXene, making it a versatile material that juxtaposes it with other 2D materials. A separate section is dedicated to the bottlenecks for future developments and recommendations.

Graphical Abstract

MXene是一种新型的二维材料,具有优异的亲水性、大的表面基团、极好的柔韧性和优异的导电性。由于其惊人的特性,MXene得到了全世界研究人员的广泛认可。MXene的显著特性,如导电性、结构特性、磁性行为等,体现了广泛的应用,包括环境、催化、无线通信、电磁干扰(EMI)屏蔽、药物输送、伤口敷料、生物成像、抗菌和生物传感器。在这篇综述文章中,综述了MXene应用的最新进展。首先,综述了MXene的各种合成策略,然后介绍了MXene的不同结构、物理和化学性质。讨论了多功能应用的最新进展。本文旨在结合MXene的所有可能的应用,使其成为与其他2D材料并列的通用材料。有一个单独的部分专门讨论未来开发的瓶颈和建议。图形抽象
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引用次数: 4
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Topics in Current Chemistry
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