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On the aromaticity of actinide compounds 关于锕系元素化合物的芳香性
IF 38.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-21 DOI: 10.1038/s41570-024-00617-y
Zahra Badri, Cina Foroutan-Nejad
The chemistry of actinides has flourished since the late 2010s with the synthesis of new actinide complexes and clusters. On the theoretical side, a range of tools is available for the characterization of these heavy element-containing compounds, but discrepancies in the assessment of aromaticity using different tools have led to controversies. In this Perspective, we examine the origin of controversies relating to the aromaticity of metallic compounds, with a focus on actinides. The aromaticity of actinides is important, not because these molecules are numerous or have a special role in catalysis or reactivity, but because this topic pushes theories of aromaticity to their limits. Owing to its reference independence, the magnetic criterion of aromaticity has been the most popular choice for the characterization of the aromaticity of metallic compounds, including actinide compounds. Through examination of several case studies, we show why this criterion might be misleading for metallic species and explain how findings relating to actinide compounds could reshape theories of aromaticity, not just for actinides but perhaps also for well-known hydrocarbons. The assessment of the aromaticity of actinide compounds has proven a controversial task. This Perspective highlights the application of state-of-the-art computational tools in assessing the aromaticity of actinide complexes and clusters and explains why commonly used magnetic probes, not just the nucleus-independent chemical shift but also the magnetically induced ring current, might be insufficient for assessing the aromaticity of these species.
自 2010 年代末以来,随着新型锕系元素络合物和簇的合成,锕系元素化学得到了蓬勃发展。在理论方面,有一系列工具可用于表征这些含重元素的化合物,但在使用不同工具评估芳香性方面的差异导致了争议。在本《视角》中,我们将以锕系元素为重点,探讨有关金属化合物芳香性争议的起源。锕系元素的芳香性之所以重要,并不是因为这些分子数量众多或在催化或反应性方面具有特殊作用,而是因为这一课题将芳香性理论推向了极限。由于其参考独立性,芳香性的磁性标准一直是表征金属化合物(包括锕系元素化合物)芳香性的最普遍选择。通过对几个案例的研究,我们说明了为什么这一标准可能会误导金属物种,并解释了与锕系元素化合物有关的发现如何重塑芳香性理论,不仅是锕系元素,也许还有众所周知的碳氢化合物。
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引用次数: 0
Hot electrodes, cool reduction 热电极,冷还原。
IF 38.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-20 DOI: 10.1038/s41570-024-00628-9
Sergio Fernández, Alexandria R. C. Bredar
Increasing the temperature of chemical systems often speeds up reactions, however, it can be expensive and inefficient to heat an entire reaction system. Here, researchers study the impact on electrochemical reactions by only heating the surfaces of electrodes.
提高化学系统的温度通常会加快反应速度,然而,加热整个反应系统的成本可能很高,而且效率低下。在这里,研究人员研究了仅加热电极表面对电化学反应的影响。
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引用次数: 0
Mind your electrolytes 注意电解质
IF 38.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-18 DOI: 10.1038/s41570-024-00625-y
Sa Suo, Colton Jacob Sheehan, Langqiu Xiao
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引用次数: 0
Atroposelective catalysis 反选择催化
IF 38.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-18 DOI: 10.1038/s41570-024-00618-x
Tanno A. Schmidt, Valeriia Hutskalova, Christof Sparr
Atropisomeric compounds—stereoisomers that arise from the restricted rotation about a single bond—have attracted widespread attention in recent years due to their immense potential for applications in a variety of fields, including medicinal chemistry, catalysis and molecular nanoscience. This increased interest led to the invention of new molecular motors, the incorporation of atropisomers into drug discovery programmes and a wide range of novel atroposelective reactions, including those that simultaneously control multiple stereogenic axes. A diverse set of synthetic methodologies, which can be grouped into desymmetrizations, (dynamic) kinetic resolutions, cross-coupling reactions and de novo ring formations, is available for the catalyst-controlled stereoselective synthesis of various atropisomer classes. In this Review, we generalize the concepts for the catalyst-controlled stereoselective synthesis of atropisomers within these categories with an emphasis on recent advancements and underdeveloped atropisomeric scaffolds beyond stereogenic C(sp2)–C(sp2) axes. We also discuss more complex systems with multiple stereogenic axes or higher-order stereogenicity. The catalyst-controlled stereoselective synthesis of atropisomers is feasible by four main concepts: desymmetrization, (dynamic) kinetic resolution, direct formation of the stereogenic axis and de novo ring construction. In this Review, pioneering work in atroposelective catalysis is discussed alongside recent advances.
异构体化合物--因围绕单键的旋转受限而产生的立体异构体--近年来引起了广泛关注,因为它们在药物化学、催化和分子纳米科学等多个领域具有巨大的应用潜力。这种日益增长的兴趣促使人们发明了新的分子马达,将阿托异构体纳入了药物发现计划,并产生了一系列新型的阿托选择性反应,包括同时控制多个立体轴的反应。在催化剂控制下立体选择性合成各类对位异构体的方法多种多样,可分为非对称反应、(动态)动力学解析、交叉偶联反应和全新成环反应。在本综述中,我们概括了催化剂控制立体选择性合成这些类别中的异构体的概念,重点是立体生成的 C(sp2)-C(sp2) 轴以外的最新进展和未充分开发的异构体支架。我们还讨论了具有多个立体构象轴或高阶立体构象的更复杂系统。
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引用次数: 0
A speedy but thorough interrogation 迅速而彻底的审讯
IF 38.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-17 DOI: 10.1038/s41570-024-00630-1
Chenyu Wang
A system enabling the rapid multiparameter optimization of conditions for electrocatalytic conversion of biomass into essential chemical feedstocks has been described.
该系统可对生物质转化为基本化学原料的电催化条件进行快速多参数优化。
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引用次数: 0
From lab coats to winning votes 从白大褂到赢得选票
IF 38.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-17 DOI: 10.1038/s41570-024-00626-x
Najat Aoun Saliba, Stephanie Greed
As an atmospheric chemist in Lebanon, Najat Aoun Saliba was propelled towards activism to combat rising pollution levels and inequality. This culminated in her election to become a member of the Lebanese parliament.
纳贾特-奥恩-萨利巴(Najat Aoun Saliba)是黎巴嫩的一名大气化学家,在她的推动下,黎巴嫩积极行动起来,应对日益严重的污染和不平等现象。最终,她当选为黎巴嫩议会议员。
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引用次数: 0
Physicochemical reactions in e-waste recycling 电子废物回收中的物理化学反应。
IF 38.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-11 DOI: 10.1038/s41570-024-00616-z
Bo Niu, Shanshan E, Qingming Song, Zhenming Xu, Bing Han, Yufei Qin
Electronic waste (e-waste) recycling is becoming a global concern owing to its immense quantity, hazardous character and the potential loss of valuable metals. The many processes involved in e-waste recycling stem from a mixture of physicochemical reactions, and understanding the principles of these reactions can lead to more efficient recycling methods. In this Review, we discuss the principles behind photochemistry, thermochemistry, mechanochemistry, electrochemistry and sonochemistry for metal recovery, polymer decomposition and pollutant elimination from e-waste. We also discuss how these processes induce or improve reaction rates, selectivity and controllability of e-waste recycling based on thermodynamics and kinetics, free radicals, chemical bond energy, electrical potential regulation and more. Lastly, key factors, limitations and suggestions for improvements of these physicochemical reactions for e-waste recycling are highlighted, wherein we also indicate possible research directions for the future. Electronic waste (e-waste) can be recycled by physicochemical reactions. This Review discusses the principles, limitations and improvement strategies from a photo-induced, thermal-induced, force-induced, electro-induced and sonication-induced chemical reaction perspective, aiming to guide future e-waste recycling efforts towards more efficient, sustainable and economical procedures.
电子废弃物(e-waste)的回收利用正成为全球关注的问题,这是因为电子废弃物数量巨大、具有危险性并可能造成贵重金属的损失。电子废弃物回收所涉及的许多过程都源于物理化学反应的混合物,了解这些反应的原理可以开发出更有效的回收方法。在本综述中,我们将讨论光化学、热化学、机械化学、电化学和声化学背后的原理,以便从电子垃圾中回收金属、分解聚合物和消除污染物。我们还讨论了这些过程如何根据热力学和动力学、自由基、化学键能、电势调节等诱导或改善电子废物回收的反应速率、选择性和可控性。最后,我们强调了这些物理化学反应在电子垃圾回收利用方面的关键因素、局限性和改进建议,并指出了未来可能的研究方向。
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引用次数: 0
Defects orchestrate concerted CO2 catalysis 缺陷协调了二氧化碳的协同催化。
IF 38.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-07 DOI: 10.1038/s41570-024-00621-2
Scott McGuigan, Emmanuel Adu Fosu
By combining defect-chemistry with metal organic frameworks, researchers have produced a photocatalyst capable of effectively and selectively producing specific products, such as acetone, from carbon dioxide and water.
通过将缺陷化学与金属有机框架相结合,研究人员制造出了一种光催化剂,能够有效地、有选择性地从二氧化碳和水中生产出丙酮等特定产品。
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引用次数: 0
Finding great beauty in cosmetic chemistry 从化妆品化学中发现美
IF 38.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-06 DOI: 10.1038/s41570-024-00620-3
Kelly A. Dobos
Cosmetic science has driven innovations that have substantially improved the quality of life for people around the world. While the field is often first associated with makeup products, research and advances in cosmetic science have had a broader impact on human health, societal progress, and the pursuit of scientific knowledge.
化妆品科学推动的创新极大地提高了全世界人民的生活质量。虽然这一领域通常首先与化妆产品联系在一起,但化妆品科学的研究和进步对人类健康、社会进步和科学知识的追求产生了更广泛的影响。
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引用次数: 0
Chiral and magnetic butterflies 手性和磁性蝴蝶
IF 36.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-03 DOI: 10.1038/s41570-024-00624-z
Alexander Rosu-Finsen
The fundamental knowledge of molecules with magneto-optical properties is still being built as researchers fine-tune their synthesis to optimize their properties. Researchers now add chiral ligands to magnetic heterometallic lanthanide compounds to study their impact on electronic transitions.
随着研究人员对分子合成进行微调以优化其特性,有关具有磁光特性的分子的基础知识仍在不断积累。现在,研究人员将手性配体添加到磁性杂金属镧系化合物中,研究它们对电子跃迁的影响。
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引用次数: 0
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