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Woodward-Hoffmann or Hoffmann-Woodward? Cycloadditions and the Transformation of Roald Hoffmann from a “Calculator” to an “Explainer”** 伍德沃德-霍夫曼还是霍夫曼-伍德沃德?环加成反应与罗尔德-霍夫曼从 "计算者 "到 "解释者 "的转变。
IF 7 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-27 DOI: 10.1002/tcr.202300181
Jeffrey I. Seeman

On May 1, 1965, Roald Hoffmann and R. B. Woodward published their second joint communication, Selection Rules for Concerted Cycloaddition Reactions, in the Journal of the American Chemical Society. Herein is presented a historical analysis of Woodward and Hoffmann's determination of the mechanism of cycloadditions. This analysis is based on thorough analyses with Roald Hoffmann of his 1964 and 1965 laboratory notebooks and his archived documents and on numerous in-person, video, and email interviews. This historical research pinpoints several seminal moments in chemistry and in the professional career of Hoffmann. For example, now documented is the fact that Woodward and Hoffmann had no anticipation that their collaboration would continue after the publication of their first 1965 communication on electrocyclizations. Also pinpointed is the moment in Hoffmann's professional and intellectual trajectories that he became a full-fledged, equal collaborator with Woodward and Hoffmann's transition from a “calculator” to an “explainer.”

1965 年 5 月 1 日,罗尔德-霍夫曼(Roald Hoffmann)和 R. B. 伍德沃德(R. B. Woodward)在《美国化学学会杂志》(Journal of the American Chemical Society)上发表了他们的第二篇联合通讯《协同环化反应的选择规则》(Selection Rules for Concerted Cycloaded Reactions)。本文对伍德沃德和霍夫曼确定环加成反应机理的历史进行了分析。该分析基于对罗纳德-霍夫曼(Roald Hoffmann)1964 年和 1965 年的实验笔记和档案文件的深入分析,以及大量的面谈、视频和电子邮件访谈。这项历史研究指出了霍夫曼在化学和职业生涯中的几个重要时刻。例如,伍德沃德和霍夫曼并没有预料到他们的合作会在 1965 年发表第一篇关于电环化的文章后继续下去,现在这一事实已被记录在案。此外,霍夫曼在其职业和思想轨迹中成为与伍德沃德平等的正式合作者的时刻,以及霍夫曼从 "计算者 "到 "解释者 "的转变,也被准确地记录下来。
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引用次数: 0
Cover Picture: Utilization of Reactive Nitrogen Compounds for Nitrogen Circular Economy (Chem. Rec. 8/2024) 封面图片:利用反应性氮化合物实现氮循环经济(Chem. Rec. 8/2024)
IF 7 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-27 DOI: 10.1002/tcr.202480801
Dr. Tatsuo Kimura

Cover Picture: The cover image shows the recommendation of nitrogen circulating based on the development of a catalytic technology to recycle harmful nitrogen oxides (NOx), that should be purified to N2 before releasing to the atmosphere but artificially supplied through high-temperature combustion, as nitrogen compounds like valuable ammonia (NH3), possibly contributing to the sustainability with saving green land and blue sky in future. More details can be found in article number e2024000094 by Tatsuo Kimura (DOl: 10.1002/tcr.202400094.

封面图片:封面图片显示了基于催化技术开发的氮循环建议,该技术可将有害的氮氧化物(NOx)在释放到大气中之前净化为 N2,但通过高温燃烧人为地将其作为有价值的氨(NH3)等氮化合物提供给大气,从而可能在未来为保护绿地和蓝天的可持续发展做出贡献。更多详情,请参阅木村达夫(Tatsuo Kimura)撰写的编号为 e2024000094 的文章(DOl: 10.1002/tcr.202400094.X)。
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引用次数: 0
Stereoselective Synthesis of Glycosides via Tsuji–Trost Type Glycosylation Using 3,4-Carbonate Galactals 利用 3,4-碳酸半乳糖通过辻-特罗斯特型糖基化立体选择性合成糖苷。
IF 7 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-21 DOI: 10.1002/tcr.202400067
Ye Lim Kim, Prof. Ju Hyun Kim

Pd-catalyzed stereoselective glycosylations using unsaturated sugar derivatives, glycals, have been successfully achieved in recent years. This review focuses on approaches to control the stereoselectivities of glycosides via π-allyl intermediates that mimic the Tsuji–Trost asymmetric allylic alkylation reactions, enabling stereoselectivity control through rational design. In the reaction process, zwitterionic Pd-π-allyl complexes, formed after the oxidative addition and decarboxylation, play a crucial role in increasing reactivities and enhancing the stereoselectivities of α- and β-glycosides. We summarized recently developed Tsuji–Trost type glycosylations using 3,4-carbonate galactals, featuring high efficiency, exclusive stereoselectivities, and a broad reaction scope including O-, N-, S-, and C-glycosylations.

近年来,利用不饱和糖衍生物(糖醛)进行钯催化的立体选择性糖基化反应已经成功实现。本综述重点介绍通过π-烯丙基中间体来控制糖苷的立体选择性的方法,这些中间体模仿了 Tsuji-Trost 不对称烯丙基烷基化反应,通过合理设计实现了立体选择性控制。在反应过程中,氧化加成和脱羧反应后形成的 Zwitterionic Pd-π-allyl 复合物在提高α-和β-糖苷的反应活性和立体选择性方面起着至关重要的作用。我们总结了最近开发的使用 3,4-碳酸半乳糖的辻-特罗斯特型糖基化反应,该反应具有高效率、独特的立体选择性以及广泛的反应范围,包括 O-、N-、S-和 C-糖基化反应。
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引用次数: 0
Ubiquitous Role of Phosphine-Based Water-Soluble Ligand in Promoting Catalytic Reactions in Water 磷基水溶性配体在促进水中催化反应中的普遍作用
IF 7 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-20 DOI: 10.1002/tcr.202400057
Manisha A. Patel, Dr. Anant R. Kapdi

Catalysis has been at the forefront of the developments that has revolutionised synthesis and provided the impetus in the discovery of platform technologies for efficient C−C or C−X bond formation. Current environmental situation however, demands a change in strategy with catalysis being promoted more in solvents that are benign (Water) and for that the development of hydrophilic ligands (especially phosphines) is a necessity which could promote catalytic reactions in water, allow recyclability of the catalytic solutions and make it possible to isolate products using column-free techniques that involve lesser usage of hazardous organic solvents. In this review, we therefore critically analyse such catalytic processes providing examples that do follow the above-mentioned parameter.

催化技术一直处于发展的前沿,它彻底改变了合成技术,并推动了高效 C-C 或 C-X 键形成平台技术的发现。然而,当前的环境形势要求我们改变策略,更多地在良性溶剂(水)中促进催化反应,因此亲水性配体(尤其是膦类配体)的开发势在必行,这种配体可以促进水中的催化反应,使催化溶液可以循环使用,并可以使用无柱技术分离产品,从而减少有害有机溶剂的使用。因此,在本综述中,我们将对此类催化过程进行批判性分析,并提供确实符合上述参数的实例。
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引用次数: 0
Biomimetic Nanoparticles for the Diagnosis and Therapy of Atherosclerosis 用于诊断和治疗动脉粥样硬化的仿生纳米粒子。
IF 7 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-15 DOI: 10.1002/tcr.202400087
Yan Wang, Yize Li, Yuqing Lu, Jingjing Li

Atherosclerosis (AS) is a chronic inflammation of blood vessels, which often has no obvious symptoms in the early stage of the disease, but when atherosclerotic plaques are formed, they often cause lumen blockage, and even plaque rupture leads to thrombosis, that is the essential factor of cardiovascular events, for example myocardial infarction, cerebral infarction, and renal atrophy. Therefore, it is considerably significant for the early recognition and precise therapy of plaque. Biomimetic nanoparticles (BNPs), especially those coated with cell membranes, can retain the biological function of cell membranes or cells, which has led to extensive research and application in the diagnosis and treatment of AS in recent years. In this review, we summarized the roles of various key cells in AS progression, the construction of biomimetic nanoparticles based on these key cells as well as their applications in AS diagnosis and therapy. Furthermore, we give a challenge and prospect of biomimetic nanoparticles in AS, hoping to elevate their application quality and the possibility of clinical translation.

动脉粥样硬化(AS)是一种慢性血管炎症,在发病早期往往没有明显症状,但当动脉粥样硬化斑块形成后,往往会造成管腔堵塞,甚至斑块破裂导致血栓形成,是心肌梗死、脑梗死、肾萎缩等心血管事件的重要诱因。因此,早期识别和精确治疗斑块意义重大。仿生纳米粒子(BNPs),尤其是包覆细胞膜的纳米粒子,可以保留细胞膜或细胞的生物功能,近年来在强直性脊柱炎的诊断和治疗中得到了广泛的研究和应用。在这篇综述中,我们总结了各种关键细胞在强直性脊柱炎进展中的作用、基于这些关键细胞的仿生纳米颗粒的构建及其在强直性脊柱炎诊断和治疗中的应用。此外,我们还对生物仿生纳米颗粒在强直性脊柱炎中的应用提出了挑战和展望,希望能提高其应用质量和临床转化的可能性。
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引用次数: 0
Research Advances of Cathode Materials for Rechargeable Aluminum Batteries 可充电铝电池阴极材料的研究进展。
IF 7 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-15 DOI: 10.1002/tcr.202400085
Yanhong Gao, Dan Zhang, Shengrui Zhang, Le Li

Rechargeable aluminum ion batteries (AIBs) have recently gained widespread research concern as energy storage technologies because of their advantages of being safe, economical, environmentally friendly, sustainable, and displaying high performance. Nevertheless, the intense Coulombic interactions between the Al3+ ions with high charge density and the lattice of the electrode body lead to poor cathode kinetics and limited cycle life in AIBs. This paper reviews the recent advances in the cathode design of AIBs to gain a comprehensive understanding of the opportunities and challenges presented by current AIBs. In addition, the advantages, limitations, and possible solutions of each cathode material are discussed. Finally, the future development prospect of the cathode materials is presented.

可充电铝离子电池(AIBs)具有安全、经济、环保、可持续发展和高性能等优点,作为一种储能技术,近年来受到了广泛的研究关注。然而,高电荷密度的 Al3+ 离子与电极体晶格之间强烈的库仑相互作用导致 AIBs 阴极动力学性能不佳,循环寿命有限。本文回顾了 AIB 阴极设计的最新进展,以全面了解当前 AIB 带来的机遇和挑战。此外,还讨论了每种阴极材料的优势、局限性和可能的解决方案。最后,介绍了阴极材料的未来发展前景。
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引用次数: 0
Advancement in Synthetic Strategies of Phosphorus Heterocycles: Recent Progress from Synthesis to Emerging Class of Optoelectronic Materials 磷杂环合成策略的进展:从合成到新兴光电材料的最新进展。
IF 7 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-13 DOI: 10.1002/tcr.202400058
Deepika Thakur, Dr. Sushmita, Shivam A. Meena, Prof. Akhilesh K. Verma

Organophosphorus heterocycles have long been acknowledged for their significant potential across diverse fields, including catalysis, material science, and drug development. Incorporating phosphorus functionalities into organic compounds offers a means to effectively tailor their medicinal properties, augment biological responses, and enhance selectivity and bioavailability. The distinctive physical and photoelectric characteristics of phosphorus-containing conjugated compounds have garnered considerable interest as promising materials for organic optoelectronics. These compounds find extensive utility in various applications such as light-emitting diodes, photovoltaic cells, phosphole-based fluorophores, and semiconductors.

长期以来,有机磷杂环因其在催化、材料科学和药物开发等多个领域的巨大潜力而备受认可。在有机化合物中加入磷官能团可以有效地调整其药用特性、增强生物反应、提高选择性和生物利用度。含磷共轭化合物具有独特的物理和光电特性,作为有机光电材料前景广阔,已引起人们的极大兴趣。这些化合物在发光二极管、光伏电池、磷基荧光体和半导体等各种应用中都有广泛的用途。
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引用次数: 0
Utilization of Reactive Nitrogen Compounds for Nitrogen Circular Economy 利用活性氮化合物实现氮循环经济。
IF 7 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-02 DOI: 10.1002/tcr.202400094
Dr. Tatsuo Kimura

Nitrogen oxides (NOx) should be purified according to environmental regulations, being restricted increasingly year by year. A wide variety of denitration technologies, such as selective catalytic reduction (SCR) of NOx to nitrogen (N2) and NOx storage reduction (NSR) to N2 by injecting reducing agents like ammonia (NH3), has so far been developed practically. Sophisticated catalytic approaches are perhaps mandatory for the sustainability in energy including complete purification of NOx. As one of the solutions to overcome problems for environment and resource simultaneously, this concept article focuses on the utilization of reactive nitrogen (Nr) compounds, mainly NOx, for encouraging an opening to consider nitrogen circular economy. For the recycling of NOx via NH3, a challenging but rational catalytic technology can be proposed by an alternate switching the inlet gas between NOx containing oxidative gas and H2 containing reductive one without an operation to change the reaction temperature. Considering the reactivity of NOx higher than that of N2, this kind of NOx to NH3 (NTA) process is promising for synthesizing NH3, being valuable not only as fertilizer but also as fuel in near future.

氮氧化物(NOx)应根据逐年增加的环境法规进行净化。迄今为止,已开发出多种脱硝技术,如通过注入氨(NH3)等还原剂将氮氧化物选择性催化还原(SCR)为氮气(N2)和将氮氧化物储存还原(NSR)为氮气。要实现能源的可持续性,包括氮氧化物的完全净化,也许必须采用先进的催化方法。作为同时解决环境和资源问题的解决方案之一,这篇概念文章重点关注活性氮(Nr)化合物(主要是氮氧化物)的利用,以鼓励考虑氮循环经济。为了通过 NH3 循环利用氮氧化物,我们提出了一种具有挑战性但合理的催化技术,即在不改变反应温度的情况下,在含氧化性氮氧化物的气体和含还原性 H2 的气体之间交替切换入口气体。考虑到 NOx 的反应活性高于 N2,这种 NOx 到 NH3(NTA)工艺在合成 NH3 方面前景广阔,在不久的将来不仅可用作肥料,还可用作燃料。
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引用次数: 0
Valorization of Agriculture Residues into Value-Added Products: A Comprehensive Review of Recent Studies 将农业残余物转化为增值产品:近期研究综述》。
IF 7 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-25 DOI: 10.1002/tcr.202300333
Tuan-Dung Hoang, Dr. Nguyen Van Anh, Dr. Mohammad Yusuf, Dr. Muhammed Ali S. A, Yathavan Subramanian, Dr. Nguyen Hoang Nam, Dr. Nguyen Minh Ky, Dr. Van-Giang Le, Dr. Nguyen Thi Thanh Huyen, Alien Abi Bianasari, Dr. Abul K Azad

Global agricultural by-products usually go to waste, especially in developing countries where agricultural products are usually exported as raw products. Such waste streams, once converted to “value-added” products could be an additional source of revenue while simultaneously having positive impacts on the socio-economic well-being of local people. We highlight the utilization of thermochemical techniques to activate and convert agricultural waste streams such as rice and straw husk, coconut fiber, coffee wastes, and okara power wastes commonly found in the world into porous activated carbons and biofuels. Such activated carbons are suitable for various applications in environmental remediation, climate mitigation, energy storage, and conversions such as batteries and supercapacitors, in improving crop productivity and producing useful biofuels.

全球农业副产品通常会被浪费掉,特别是在发展中国家,那里的农产品通常作为原材料出口。这些废物流一旦转化为 "增值 "产品,就可以成为额外的收入来源,同时对当地人民的社会经济福祉产生积极影响。我们重点介绍利用热化学技术活化和转化农业废弃物流,如世界上常见的稻米和稻草壳、椰子纤维、咖啡废料和秋葵发电废料,将其转化为多孔活性炭和生物燃料。这种活性炭适用于环境修复、气候减缓、能源储存和转换(如电池和超级电容器)、提高作物产量和生产有用的生物燃料等各种应用。
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引用次数: 0
Gold-Catalyzed Lactone Synthesis: Advancements and Insights 金催化内酯合成:进展与启示。
IF 7 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-25 DOI: 10.1002/tcr.202400071
D. Ravi Sankar, Mohan Neetha, Prof. Dr. Gopinathan Anilkumar

Lactones represent a class of fundamental structural motifs ubiquitous in nature, holding significance across diverse scientific domains such as pharmaceuticals, natural products, drug discovery, and industry. Despite their simplicity, the synthesis of lactones has garnered considerable interest due to their pivotal roles. Gold, traditionally regarded as a noble metal, has emerged as an efficient catalyst, challenging conventional perceptions. The utilization of gold in lactone synthesis has captivated researchers, leading to the development of numerous effective methodologies. Motivated by this, we present a comprehensive compilation of reports on the gold-catalyzed synthesis of lactones, encompassing literature till date.

内酯是自然界中无处不在的一类基本结构基团,在制药、天然产品、药物发现和工业等不同科学领域都具有重要意义。尽管内酯非常简单,但由于其举足轻重的作用,合成内酯已引起了人们的极大兴趣。传统上被视为贵金属的金已成为一种高效催化剂,对传统观念提出了挑战。金在内酯合成中的应用令研究人员着迷,并开发出了许多有效的方法。为此,我们对迄今为止有关金催化合成内酯的文献进行了全面汇编。
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引用次数: 0
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