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Recent Advances in Palladium-Catalyzed [4 + n] Cycloaddition of Lactones, Benzoxazinanones, Allylic Carbonates, and Vinyloxetanes 钯催化的最新进展[4] + n] 内酯、苯并恶嗪酮、烯丙基碳酸酯和乙烯氧杂环丁烷的环加成。
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-11-03 DOI: 10.1007/s41061-023-00442-9
Mengyan Guo, Panke Zhang, Er-Qing Li

Palladium-catalyzed allylation cyclization reaction has recently emerged as an efficient and powerful synthetic platform for the construction of diverse and valuable carbo- and heterocycles. Thus the development of new allylic motifs for achieving this type of transformations in high reactivity and selectivity is of great importance. Generally, these substrates have been utilized as 1,3-, 1,4-, 1,5-, 1,6-dipoles in many reactions, which are applied to prepare highly functionalized products with complete control of chemo-, regio-, diastereo-, and enantioselectivity. In this review, we focus our attention on the development of palladium-catalyzed [4 + n] cycloaddition of allylic motifs and describe a comprehensive and impressive advances in this area. Meanwhile, the related mechanism and the application of these annulation strategies in natural product total synthesis will be highlighted in detail.

Graphical Abstract

钯催化的烯丙基化环化反应最近成为一种高效而强大的合成平台,用于构建各种有价值的碳环和杂环。因此,开发新的烯丙基基序以实现高反应性和选择性的这种类型的转化是非常重要的。通常,这些底物在许多反应中被用作1,3-、1,4-、1,5-、1,6-极,用于制备高度官能化的产物,并完全控制化学、区域、非对映体和对映选择性。在这篇综述中,我们将注意力集中在钯催化[4]的发展上 + n] 烯丙基基序的环加成,并描述了该领域的全面和令人印象深刻的进展。同时,将详细介绍这些环空策略的相关机理及其在天然产物全合成中的应用。
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引用次数: 0
The Renaissance of Ferrocene-Based Electrocatalysts: Properties, Synthesis Strategies, and Applications 二茂铁基电催化剂的复兴:性能、合成策略和应用。
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-11-01 DOI: 10.1007/s41061-023-00441-w
Sariga, Anitha Varghese

The fascinating electrochemical properties of the redox-active compound ferrocene have inspired researchers across the globe to develop ferrocene-based electrocatalysts for a wide variety of applications. Advantages including excellent chemical and thermal stability, solubility in organic solvents, a pair of stable redox states, rapid electron transfer, and nontoxic nature improve its utility in various electrochemical applications. The use of ferrocene-based electrocatalysts enables control over the intrinsic properties and electroactive sites at the surface of the electrode to achieve specific electrochemical activities. Ferrocene and its derivatives can function as a potential redox medium that promotes electron transfer rates, thereby enhancing the reaction kinetics and electrochemical responses of the device. The outstanding electrocatalytic activity of ferrocene-based compounds at lower operating potentials enhances the specificity and sensitivity of reactions and also amplifies the response signals. Owing to their versatile redox chemistry and catalytic activities, ferrocene-based electrocatalysts are widely employed in various energy-related systems, molecular machines, and agricultural, biological, medicinal, and sensing applications. This review highlights the importance of ferrocene-based electrocatalysts, with emphasis on their properties, synthesis strategies for obtaining different ferrocene-based compounds, and their electrochemical applications.

氧化还原活性化合物二茂铁迷人的电化学性质激发了全球研究人员开发用于各种应用的二茂铁基电催化剂。其优点包括优异的化学和热稳定性、在有机溶剂中的溶解度、一对稳定的氧化还原态、快速的电子转移和无毒性,提高了其在各种电化学应用中的实用性。基于二茂铁的电催化剂的使用能够控制电极表面的固有性质和电活性位点,以实现特定的电化学活性。二茂铁及其衍生物可以作为潜在的氧化还原介质,促进电子转移速率,从而增强器件的反应动力学和电化学响应。二茂铁基化合物在较低的操作电位下具有出色的电催化活性,增强了反应的特异性和敏感性,也放大了反应信号。由于其多功能的氧化还原化学和催化活性,二茂铁基电催化剂广泛应用于各种能源相关系统、分子机器以及农业、生物、医药和传感应用。这篇综述强调了二茂铁基电催化剂的重要性,重点介绍了它们的性质、获得不同二茂铁化合物的合成策略及其电化学应用。
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引用次数: 0
Principles of Photocatalysts and Their Different Applications: A Review 光催化剂的原理及其不同应用:综述。
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-10-31 DOI: 10.1007/s41061-023-00444-7
Mohamed A. Hassaan, Mohamed A. El-Nemr, Marwa R. Elkatory, Safaa Ragab, Violeta-Carolina Niculescu, Ahmed El Nemr

Human existence and societal growth are both dependent on the availability of clean and fresh water. Photocatalysis is a type of artificial photosynthesis that uses environmentally friendly, long-lasting materials to address energy and environmental issues. There is currently a considerable demand for low-cost, high-performance wastewater treatment equipment. By changing the structure, size, and characteristics of nanomaterials, the use of nanotechnology in the field of water filtration has evolved dramatically. Semiconductor-assisted photocatalysis has recently advanced to become among the most promising techniques in the fields of sustainable energy generation and ecological cleanup. It is environmentally beneficial, cost-effective, and strictly linked to the zero waste discharge principle used in industrial effluent treatment. Owing to the reduction or removal of created unwanted byproducts, the green synthesis of photoactive nanomaterial is more beneficial than chemical synthesis approaches. Furthermore, unlike chemical synthesis methods, the green synthesis method does not require the use of expensive, dangerous, or poisonous ingredients, making it a less costly, easy, and environmental method for photocatalyst synthesis. This work focuses on distinct greener synthesis techniques utilized for the production of new photocatalysts, including metals, metal doped-metal oxides, metal oxides, and plasmonic nanostructures, including the application of artificial intelligence and machine learning to the design and selection of an innovative photocatalyst in the context of energy and environmental challenges. A brief overview of the industrial and environmental applications of photocatalysts is also presented. Finally, an overview and recommendations for future research are given to create photocatalytic systems with greatly improved stability and efficiency.

人类生存和社会发展都依赖于清洁和淡水的供应。光催化是一种人工光合作用,使用环保、持久的材料来解决能源和环境问题。目前对低成本、高性能的废水处理设备有相当大的需求。通过改变纳米材料的结构、尺寸和特性,纳米技术在水过滤领域的应用发生了巨大变化。半导体辅助光催化最近已发展成为可持续能源生产和生态清洁领域最有前途的技术之一。它对环境有益,具有成本效益,并与工业废水处理中使用的零废物排放原则严格相关。由于减少或去除了产生的不需要的副产物,光活性纳米材料的绿色合成比化学合成方法更有益。此外,与化学合成方法不同,绿色合成方法不需要使用昂贵、危险或有毒的成分,使其成为一种成本较低、简单且环保的光催化剂合成方法。这项工作的重点是用于生产新型光催化剂的独特的绿色合成技术,包括金属、金属掺杂的金属氧化物、金属氧化物和等离子体纳米结构,包括在能源和环境挑战的背景下,将人工智能和机器学习应用于创新光催化剂的设计和选择。还简要介绍了光催化剂的工业和环境应用。最后,概述了未来的研究并提出了建议,以创建具有极大提高的稳定性和效率的光催化系统。
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引用次数: 0
Construction of 1,4-Dihydropyridines: The Evolution of C4 Source 1,4-二氢吡啶的构建:C4来源的演化。
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-09-25 DOI: 10.1007/s41061-023-00440-x
Siyu Song, Yongchao Wang, Fuchao Yu

The field of cascade cyclization for the construction of 1,4-dihydropyridines (1,4-DHPs) has been continuously expanding during the last decades because of their broad-spectrum biological and synthetic importance. To date, many methods have been developed, mainly including the Hantzsch reaction, Hantzsch-like reaction and newly developed cascade cyclization, in which various synthons have been successively developed as C4 sources of 1,4-DHPs. This review presents the cascade cyclization synthesis strategy for the construction of 1,4-DHPs according to various C4 sources from carbonyl compounds, alkenyl fragments, alcohols, aliphatic amines, glycines and other C4 sources.

在过去的几十年里,用于构建1,4-二氢吡啶(1,4-DHP)的级联环化领域由于其广谱的生物和合成重要性而不断扩大。到目前为止,已经开发了许多方法,主要包括Hantzsch反应、Hantzsch-like反应和新开发的级联环化,其中各种合成子相继被开发为1,4-DHP的C4来源。本文介绍了从羰基化合物、烯基片段、醇、脂族胺、甘氨酸和其他C4来源构建1,4-DHP的级联环化合成策略。
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引用次数: 0
C–H Bond Functionalization of N-Heteroarenes Mediated by Selectfluor 选择性荧光介导N-杂芳烃的C-H键功能化。
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-09-22 DOI: 10.1007/s41061-023-00437-6
Angel H. Romero

Herein, recent developments for Selectfluor-mediated C–H functionalization of N-heteroarenes are described. This type of C–H bond activation is an attractive and competitive alternative to traditional methodologies, allowing the functionalization of a variety of chemical functions. In addition, Selectfluor is a more sustainable and economically accessible oxidant compared with expensive/toxic metals or hazardous peroxides. For a practical understanding, the current review classified systematically the reported strategies in four subsections as follows: (1) carbon–carbon formation, (2) carbon–nitrogen bond formation, (3) carbon–chalcogen bond, and (4) carbon–halogen bond formation. Mechanistic aspects and reaction conditions are fully discussed to provide an understanding of the aspects that govern C–H functionalization in N-heteroarenes mediated by Selectfluor.

Graphical Abstract

本文介绍了选择性荧光介导的N-杂芳烃的C-H功能化的最新进展。这种类型的C-H键活化是传统方法的一种有吸引力和竞争力的替代方法,允许各种化学功能的功能化。此外,与昂贵/有毒的金属或危险的过氧化物相比,Selectfluor是一种更可持续、更经济的氧化剂。为了便于实际理解,本综述将所报道的策略系统地分为四个子部分,如下:(1)碳-碳形成,(2)碳-氮键形成,(3)碳-硫族键和(4)碳-卤键形成。充分讨论了机理方面和反应条件,以提供对由Selectfluor介导的N-杂芳烃中C-H官能化的控制方面的理解。
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引用次数: 1
Functionalization of BODIPY Dyes with Additional C–N Double Bonds and Their Applications 附加C-N双键的BODIPY染料的功能化及其应用。
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-09-07 DOI: 10.1007/s41061-023-00438-5
Huriye Ilhan, Yusuf Cakmak

BODIPY (4-bora-3a,4a-diaza-s-indacene) dyes are regarded as highly useful compounds due to their rich photophysical properties, stability, and ease of functionalization. In recent years, hot topics studied with this class of compounds are targeted photodynamic therapy, photothermal therapy, fluorescent bioimaging agents, structural modification of the BODIPY core, synthesis of BODIPY analogs, and BODIPY-based supramolecular constructs. This review covers the advances in BODIPY structures substituted with additional carbon–nitrogen double bonds, namely imines, hydrazones, oximes, and related derivatives for various applications. Works based on fluorescent indicators of anions, cations, and neutral molecules are included in this review. In addition, the use of such structures for pharmaceutical applications, photodynamic therapy, fluorescent switches, and fluorescent building blocks are also investigated. In addition to covering the major literature within the mentioned subclass, design principles, working mechanisms, and outlooks are also provided to enlighten forthcoming promising efforts. With this work, we aim to provide insights about the synthesis, photophysical properties, contribution of C=N bonds to a class of dye, and possible areas of use and stimulate researchers to present new ideas and overcome the current problems using these derivatives.

Graphical Abstract

BODIPY(4-硼-3a,4-二氮杂-s-茚)染料由于其丰富的光物理性质、稳定性和易于官能化而被认为是非常有用的化合物。近年来,这类化合物的研究热点是靶向光动力疗法、光热疗法、荧光生物成像剂、BODIPY核心的结构修饰、BODIPY类似物的合成以及基于BODIPY的超分子构建。本文综述了用额外的碳氮双键取代的BODIPY结构的进展,即亚胺、腙、肟和用于各种应用的相关衍生物。基于阴离子、阳离子和中性分子的荧光指示剂的工作包括在这篇综述中。此外,还研究了这种结构在药物应用、光动力治疗、荧光开关和荧光构建块中的应用。除了涵盖上述子类中的主要文献外,还提供了设计原则、工作机制和展望,以启发即将进行的有希望的工作。通过这项工作,我们旨在提供关于合成、光物理性质、C=N键对一类染料的贡献以及可能的使用领域的见解,并激励研究人员提出新的想法,使用这些衍生物克服当前的问题。
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引用次数: 0
Recent Advances in MXene Quantum Dots: A Platform with Unique Properties for General-Purpose Functional Materials with Novel Biomedical Applications MXene量子点的最新进展:一种具有独特性能的平台,用于具有新型生物医学应用的通用功能材料。
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-09-05 DOI: 10.1007/s41061-023-00439-4
Elham Einafshar, Nafiseh Einafshar, Majid Khazaei

Developing new, high-performance materials is a prerequisite for technological advancement. In comparison to bulk materials, quantum dots have a number of good advantages due to their small size, high surface area, and quantum dimensions. Quantum dots, two-dimensional materials with lateral dimensions less than 100 nm, can be generated by the quantum confinement effect. Mxene quantum dots (MQDs) retain some of their two-dimensional characteristics. They also exhibit novel physicochemical properties, including enhanced dispersibility in aqueous and nonaqueous phases, modification or doping capabilities, and photoluminescence. MQDs, due to their unique and diverse properties, have been receiving a great deal of attention as new members of the Mxene group and wide use for biotechnology, bioimaging, optoelectronics, catalysis, cancer therapy, etc. This review aims to provide an overview of the synthesis of MQDs, their optical properties, and their cancer therapy applications. MQDs exhibit remarkable photothermal and photodynamic features and can be suitable for bioimaging. In addition to obtaining bioimaging, photothermal therapy (PTT) and photodynamic therapy (PDT) effects simultaneously, MQDs have high biocompatibility in vitro and in vivo, providing evidence of their potential clinical utility. Herein, recent developments and future prospects concerning MQDs biomedical applications are discussed.

Graphical Abstract

开发新的高性能材料是技术进步的先决条件。与大块材料相比,量子点由于其小尺寸、高表面积和量子尺寸而具有许多良好的优势。量子点是横向尺寸小于100nm的二维材料,可以通过量子约束效应产生。Mxene量子点(MQD)保留了它们的一些二维特性。它们还表现出新的物理化学性质,包括在水相和非水相中增强的分散性、改性或掺杂能力以及光致发光。MQD由于其独特和多样的性质,作为Mxene组的新成员,以及在生物技术、生物成像、光电子、催化、癌症治疗等方面的广泛应用,受到了广泛的关注。本综述旨在概述MQD的合成、其光学性质及其癌症治疗应用。MQD表现出显著的光热和光动力特性,可适用于生物成像。除了同时获得生物成像、光热治疗(PTT)和光动力治疗(PDT)效果外,MQD在体外和体内都具有高度的生物相容性,为其潜在的临床应用提供了证据。本文讨论了MQDs生物医学应用的最新进展和未来前景。
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引用次数: 2
The Novel Organic Emitters for High-Performance Narrow-Band Deep Blue OLEDs 用于高性能窄带深蓝OLED的新型有机发光体。
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-08-26 DOI: 10.1007/s41061-023-00436-7
Jialu Gu, Wei Shi, Haixia Zheng, Guo Chen, Bin Wei, Wai-Yeung Wong

Narrow-band deep-blue organic light-emitting diodes (OLEDs) have played a key role in the field of high-quality full-color displays. However, because of the considerable challenges of inherent band gaps, unbalanced carrier injection and the lack of molecular structures, narrow-band deep-blue emitters develop slowly compared with red- and green-emitting materials. Encouragingly, with the continuous efforts of scientists in recent years, great progress has been made in the molecule design and material synthesis of highly efficient narrow-band deep-blue emitters. The typical deep-blue emitters which exhibit narrow emission with a full width at half maximum of < 50 nm are summarized in this article. They are divided into the three categories: fluorescence, phosphorescence and thermally activated delayed fluorescence. The methods of molecular design for realizing narrow-band deep-blue emission are described in detail and future research directions are also discussed in this article.

窄带深蓝色有机发光二极管(OLED)在高质量全色显示器领域发挥了关键作用。然而,由于固有带隙、不平衡载流子注入和分子结构的缺乏等诸多挑战,与红色和绿色发射材料相比,窄带深蓝色发射体发展缓慢。令人鼓舞的是,近年来,在科学家的不断努力下,高效窄带深蓝发射体的分子设计和材料合成取得了巨大进展。本文总结了典型的深蓝色发射体,它们表现出窄发射,半峰全宽<50nm。它们分为三类:荧光、磷光和热激活延迟荧光。本文详细介绍了实现窄带深蓝色发射的分子设计方法,并对未来的研究方向进行了讨论。
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引用次数: 0
Recent Progress on Nitrogen-Rich Energetic Materials Based on Tetrazole Skeleton 基于四唑骨架的富氮含能材料研究进展。
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-08-23 DOI: 10.1007/s41061-023-00435-8
Bihai Chen, Han Lu, Jiayi Chen, Zhaoxu Chen, Shuang-Feng Yin, Lifen Peng, Renhua Qiu

Development of nitrogen-rich energetic materials has gained much attention because of their remarkable properties including large nitrogen content and energy density, good thermal stability, low sensitivity, good energetic performance, environmental friendliness and so on. Tetrazole has the highest nitrogen and highest energy contents among the stable azoles. The incorporation of diverse explosophoric groups or substituents into the tetrazole skeleton is beneficial to obtain high-nitrogen energetic materials having excellent energetic performance and suitable sensitivity. In this review, the development of high-nitrogen energetic materials based on tetrazole skeleton is highlighted. Initially, the property and utilization of nitrogen-rich energetic materials are presented. After showing the advantage of the tetrazole skeleton, the high-nitrogen energetic materials based on tetrazole are classified and introduced in detail. Based on different types of energetic materials (EMs), the synthesis and properties of nitrogen-rich energetic materials based on mono-, di-, tri- and tetra-tetrazole are summarized in detail.

Graphical Abstract

富氮含能材料因其氮含量和能量密度大、热稳定性好、灵敏度低、高能性能好、环境友好等显著性能而备受关注。在四唑骨架中掺入不同的爆炸基团或取代基有利于获得具有优异能量性能和合适灵敏度的高氮含能材料。综述了基于四唑骨架的高氮含能材料的研究进展。首先介绍了富氮含能材料的性质及其利用。在展示了四唑骨架的优点后,对基于四唑的高氮含能材料进行了详细的分类和介绍。基于不同类型的含能材料,详细总结了基于单、二、三和四唑的富氮含能材料的合成和性能。
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引用次数: 1
Performance Regulation of Single-Atom Catalyst by Modulating the Microenvironment of Metal Sites 通过调节金属位点的微环境来调节单原子催化剂的性能。
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2023-07-22 DOI: 10.1007/s41061-023-00434-9
Hanyu Hu, Yanyan Zhao, Yue Zhang, Jiangbo Xi, Jian Xiao, Sufeng Cao

Metal-based catalysts, encompassing both homogeneous and heterogeneous types, play a vital role in the modern chemical industry. Heterogeneous metal-based catalysts usually possess more varied catalytically active centers than homogeneous catalysts, making it challenging to regulate their catalytic performance. In contrast, homogeneous catalysts have defined active-site structures, and their performance can be easily adjusted by modifying the ligand. These characteristics lead to remarkable conceptual and technical differences between homogeneous and heterogeneous catalysts. As a recently emerging class of catalytic material, single-atom catalysts (SACs) have become one of the most active new frontiers in the catalysis field and show great potential to bridge homogeneous and heterogeneous catalytic processes. This review documents a brief introduction to SACs and their role in a range of reactions involving single-atom catalysis. To fully understand process-structure-property relationships of single-atom catalysis in chemical reactions, active sites or coordination structure and performance regulation strategies (e.g., tuning chemical and physical environment of single atoms) of SACs are comprehensively summarized. Furthermore, we discuss the application limitations, development trends and future challenges of single-atom catalysis and present a perspective on further constructing a highly efficient (e.g., activity, selectivity and stability), single-atom catalytic system for a broader scope of reactions.

Graphical Abstract

金属基催化剂包括均相和非均相催化剂,在现代化学工业中发挥着至关重要的作用。非均相金属基催化剂通常比均相催化剂具有更多变化的催化活性中心,这使得调节其催化性能具有挑战性。相反,均相催化剂具有明确的活性位点结构,并且可以通过修饰配体来容易地调节它们的性能。这些特征导致均相催化剂和非均相催化剂之间存在显著的概念和技术差异。单原子催化剂(SACs)作为一种新兴的催化材料,已成为催化领域最活跃的新前沿之一,在连接均相和非均相催化过程方面显示出巨大的潜力。这篇综述简要介绍了SAC及其在涉及单原子催化的一系列反应中的作用。为了充分理解化学反应中单原子催化的过程-结构-性质关系,全面总结了SAC的活性位点或配位结构和性能调节策略(如调节单原子的化学和物理环境)。此外,我们还讨论了单原子催化的应用局限性、发展趋势和未来挑战,并对进一步构建高效(如活性、选择性和稳定性)的单原子催化体系以用于更广泛的反应提出了展望。
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引用次数: 1
期刊
Topics in Current Chemistry
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