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Editorial: constructive disagreement 社论:建设性分歧
IF 3.3 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-11-05 DOI: 10.1080/10610278.2023.2270760
Nicholas G. White
Published in Supramolecular Chemistry (Ahead of Print, 2023)
发表于《超分子化学》(2023年出版前)
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引用次数: 0
Eric’s Corner stereochemical pet peeves, terminology worthy of “all creatures great and small” 埃里克角立体化学的讨厌鬼,值得“所有生物大大小小”的术语
4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-10-26 DOI: 10.1080/10610278.2023.2271617
Phuoc H. Ngo, Eric V. Anslyn
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引用次数: 0
(Self) assembled news: recent highlights from the Supramolecular Chemistry literature (Quarter 3, 2023) (自我)汇编新闻:超分子化学文献的最新亮点(2023年第3季度)
4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-10-26 DOI: 10.1080/10610278.2023.2271618
Cally J. E. Haynes, Nicholas G. White
Click to increase image sizeClick to decrease image size Disclosure statementCally Haynes is a Vice Chair of WISC. The section on their recent prize was conceived and written by Nicholas White.
点击放大图片点击缩小图片披露声明卡莉·海恩斯是WISC的副主席。关于他们最近获奖的部分是由尼古拉斯·怀特构思和撰写的。
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引用次数: 0
Two novel Al 3+ fluorescent-on probes based on thiazole substituted salicylaldehyde and its applications 两种新型噻唑取代水杨醛Al - 3+荧光探针及其应用
4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-10-23 DOI: 10.1080/10610278.2023.2270600
Xiaohua Cai, Benyue Yao, Jianhui Zhang, Le Liang, Mei Han, Xiaohong Li, Yanli Leng
ABSTRACTIn this study, two structurally similar ‘turn on’ fluorescent probes B1 and B2 with high binding energy with Al3+ were synthesised. With new thiazole substituted salicylaldehyde fluorophore, these two hosts also have good selectivity and sensitivity in the detection of Al3+ based on the chelating fluorescence-enhancing effect under test conditions. They show an extremely low detection limit, 0.478 nM and 4.04 nM, respectively, with binding constants of 2.34 × 106 M−1 and 1.36 × 106 M−1. A 1:1 binding ratio of dual probes to Al3+ was demonstrated by working curves and mass spectrometry. The mechanisms were confirmed by 1H NMR and DFT calculations, defined that both two compounds combined with Al3+ by two oxygen atoms (one in C=O and another in -OH) and one nitrogen atom in -NH group to form triple coordination structure. Further application in test strips, actual soil and traditional Chinese medicine (TCM) suggest probes B1 and B2 have well application prospects in detecting Al3+.KEYWORDS: Al3+ detectionfluorescent probeSchiff baseCHEF mechanism AcknowledgmentsThis work is supported by the National Natural Science Foundation of China (51863004) and the Natural Science Foundation of the Guizhou Science and Technology Department (JZ [2018]1077).Disclosure statementNo potential conflict of interest was reported by the author(s).Supplementary materialSupplemental data for this article can be accessed online at https://doi.org/10.1080/10610278.2023.2270600.
摘要本研究合成了两个结构相似的与Al3+具有高结合能的“开启”荧光探针B1和B2。在新噻唑取代水杨醛荧光团的情况下,基于测试条件下的螯合荧光增强作用,这两种宿主对Al3+的检测也具有良好的选择性和灵敏度。它们的检出限极低,分别为0.478 nM和4.04 nM,结合常数分别为2.34 × 106 M−1和1.36 × 106 M−1。工作曲线和质谱分析表明,双探针与Al3+的结合比为1:1。1H NMR和DFT计算证实了这两种化合物与Al3+结合的机理,确定了这两种化合物与Al3+结合的两个氧原子(一个在C=O中,一个在-OH中)和一个在- nhh中的氮原子形成三重配位结构。进一步在试纸、实际土壤和中药中的应用表明,B1和B2探针在检测Al3+方面具有良好的应用前景。本文得到国家自然科学基金项目(51863004)和贵州省科技厅自然科学基金项目(JZ[2018]1077)资助。披露声明作者未报告潜在的利益冲突。补充材料本文的补充数据可在https://doi.org/10.1080/10610278.2023.2270600上在线获取。
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引用次数: 0
Terpenoid-based supramolecular materials: fabrications, performances, applications 萜类超分子材料:制造、性能、应用
IF 3.3 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-10-15 DOI: 10.1080/10610278.2023.2260044
Hao Zhang, Junbo Guo, Jun Hu, Ming Zhou
With the increasing advancement of supramolecular chemistry, the focus is gradually shifting from the preparation of traditional polymeric materials to the development of multifunctional supramolec...
随着超分子化学的不断发展,其研究重点逐渐从传统高分子材料的制备转向多功能超分子材料的开发。
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引用次数: 0
A metal-organic capsule self-assembled by hydrogen bonds for adsorption of methylene blue 一种由氢键自组装的金属有机胶囊,用于吸附亚甲基蓝
4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-10-02 DOI: 10.1080/10610278.2023.2260042
Nana Chen, Xiuting Gao, Mengying Liu, Chuansheng Cui, Qingfu Zhang
ABSTRACTDyes are a class of hazardous chemicals that can cause harm to the environment and life on earth. However, it remains a huge challenge for the effective removal of the dyes. Herein, a new metal-organic capsule {[Cu(L)(bpy)(H2O)]·H2O}n (1) was synthesised by (4,4’-(((1,3,4-thiadiazole-2,5-diyl)bis(sulfanediyl))bis (methylene)) dibenzoic acid, 2,2’-bipyridine and CuCl2∙2 H2O under solvothermal condition. Interestingly, two inversion asymmetric units are connected by O-H···O and O-H···N to form a centrosymmetric capsule with cavity. The intermolecular interactions were further quantitatively analysed and visualised by the CrystalExplorer 17.5. Notably, complex 1 can effectively adsorb methylene blue (MB), and the adsorption performance is linearly correlated with MB concentration. When the concentration of MB was increased from 10 to 50 mg∙L−1, the adsorption performance of 1 was increased from 17.68 to 66.79 mg∙g−1, while reduced the MB removal efficiency from 88.4% to 66.4%. The adsorption process is suitable for the pseudo-second-order and the Langmuir model. Furthermore, complex 1 showed the good recyclability and stability for at least five runs.KEYWORDS: Metal-organic capsulehydrogen bondingπ-π stackingHirshfeld surface analysisdyes adsorptionmethylene blue Disclosure statementNo potential conflict of interest was reported by the author(s).Supplementary materialSupplemental data for this article can be accessed online at https://doi.org/10.1080/10610278.2023.2260042.Additional informationFundingThis work was supported by the [National Natural Science Foundation of China] under Grant [number 21771096].
摘要染料是一类对地球环境和生命造成危害的危险化学物质。然而,如何有效去除染料仍然是一个巨大的挑战。在溶剂热条件下,以(4,4′-((1,3,4-噻二唑-2,5-二基)双(磺胺二基)双(亚甲基))二苯甲酸、2,2′-联吡啶和CuCl2∙2h2o为原料合成了新型金属有机胶囊{[Cu(L)(bpy)(H2O)]·H2O}n(1)。有趣的是,两个反转不对称单元由O- h··O和O- h··N连接,形成一个带腔的中心对称胶囊。通过CrystalExplorer 17.5进一步定量分析和可视化分子间相互作用。值得注意的是,配合物1能有效吸附亚甲基蓝(MB),且吸附性能与MB浓度呈线性相关。当MB的浓度从10 mg∙L−1增加到50 mg∙L−1时,1的吸附性能从17.68 mg∙g−1增加到66.79 mg∙g−1,而MB的去除率从88.4%降低到66.4%。吸附过程适用于拟二阶和Langmuir模型。此外,配合物1在至少5次运行中表现出良好的可回收性和稳定性。关键词:金属有机胶囊,氢键,π-π堆积,hirshfeld表面分析,染料吸附,亚甲基蓝。补充资料本文的补充资料可通过https://doi.org/10.1080/10610278.2023.2260042.Additional info在线获取。本研究由[中国国家自然科学基金基金委]资助,基金号[21771096]。
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引用次数: 0
(Self) assembled news: recent highlights from the supramolecular chemistry literature (Quarter 2, 2023) (自我)汇编新闻:超分子化学文献的最新亮点(2023年第2季度)
IF 3.3 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-02-01 DOI: 10.1080/10610278.2023.2230659
Hiral A. Kotak, Nicholas G. White, Cally J. E. Haynes
Allostery – the control of macromolecule conformation and function by the remote binding to an effector molecule – allows numerous biological machines to carry out their roles in the body. Writing in Chem, Cheng-Yong Su and colleagues have described a metallo-amine cage (MOC-68, Figure 1) that exhibits intricate, proton-driven allostery underpinned by water binding and release [1], with implications in controlled guest binding, transport and release. MOC-68 (Figure 1) comprises flexible, amine corners and face-capping metalloligands containing imidazole linkers; thus, numerous acid/base sites are accessible. When protonated, these sites bind water molecules which rigidify the cage; when deprotonated, water is released and the conformational flexibility of the cage increases. The initial state can only bind guests on the exterior of the cage (exo-binding); however, pH-driven allosteric switching provides a larger cavity, allowing endobinding. Interestingly, the corners of the cage can be capped with CB[10], yielding a rare ‘ring-on-cage’ system. This locks the conformation of the cage, can trigger the release of endo-bound guests, and prevents allosteric switching and endo-guest binding. Another consequence of the changes in protonation state is that the charge of the cage can be drastically altered by changing the pH. This affects the polarity of the system and means that the cage can reversibly phase transfer from polar to non-polar solvent mixtures.
变构-通过远程结合效应分子来控制大分子的构象和功能-允许许多生物机器在体内发挥它们的作用。在Chem上,Cheng-Yong Su及其同事描述了一种金属胺笼(MOC-68,图1),它表现出复杂的质子驱动变构,以水的结合和释放为基础[1],这意味着受控的客体结合、运输和释放。MOC-68(图1)包括柔性、胺角和含有咪唑连接剂的面盖金属配体;因此,可以访问许多酸/碱位点。当质子化时,这些位点与水分子结合,使笼变硬;当去质子化时,水被释放,笼的构象柔韧性增加。初始状态下只能将来宾绑定在笼的外部(外绑定);然而,ph驱动的变构开关提供了更大的空腔,允许内结合。有趣的是,笼子的角落可以用CB[10]封顶,从而产生罕见的“笼上环”系统。这锁定了笼的构象,可以触发释放内结合客体,并防止变构转换和内结合客体。质子化状态变化的另一个结果是,笼的电荷可以通过改变ph值而急剧改变。这影响了系统的极性,意味着笼可以从极性溶剂混合物可逆地相转移到非极性溶剂混合物。
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引用次数: 0
Eric’s Corner – My Sabbatical Tour - “Tik-Tok of Oz”a Labs 埃里克的角落-我的休假之旅-“绿野仙踪”实验室
IF 3.3 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-02-01 DOI: 10.1080/10610278.2023.2226479
E. Anslyn, James R. Howard
a
一个
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引用次数: 0
Salt effects on the rates of a thiol cyclisation reaction within a yocto-litre inner-space 盐对微升内空间内硫醇环化反应速率的影响
IF 3.3 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-02-01 DOI: 10.1080/10610278.2023.2231120
Kaiyu Wang, Wei Yao, Xiaoyang Cai, B. Gibb
ABSTRACT The appreciation of the central role of Coulombic interactions in enzyme catalysis has led to the development of many ‘spin-off’ strategies for controlling chemical reactions. In particular, supramolecular chemistry has become increasingly proficient in using encapsulation/compartmentalisation to control both stoichiometric and catalytic reactions within the inner-spaces of hosts. This noted, there are still many open questions around the design of electrostatic potential fields within such hosts, and how exogenous factors can be used to fine-tune these properties. Here, we report on the cyclisation of 12-bromododecane-1-thiol 2 inside supramolecular capsule 1 2 to give thiacyclotridecane 3, and how the rate of this reaction changes as a function of exogenous salts. We find that this cyclisation is slowed in the presence of exogenous anions, with attenuation being highly dependent on both their nature and concentration. Thus, this work demonstrates how anions at the more-weakly solvated end of the Hofmeister series can associate with the outer walls of the capsule and so attenuate cyclisation. This suggests new ways in which reactions in inner-spaces can be indirectly modulated by exogeneous chemical entities. GRAPHICAL ABSTRACT
对库仑相互作用在酶催化中的核心作用的认识已经导致了许多控制化学反应的“衍生”策略的发展。特别是,超分子化学已经越来越熟练地使用包封/区隔化来控制宿主内部空间内的化学计量和催化反应。值得注意的是,围绕这种宿主内静电势场的设计,以及如何使用外生因素来微调这些特性,仍然存在许多悬而未决的问题。在这里,我们报道了12-溴十二烷-1-硫醇2在超分子胶囊12内环化生成噻环三烷3,以及该反应的速率如何随外源盐的变化而变化。我们发现这种环化在外源阴离子的存在下减慢,衰减高度依赖于它们的性质和浓度。因此,这项工作证明了Hofmeister系列的弱溶剂化末端的阴离子如何与胶囊的外壁结合,从而减弱环化。这表明了内部空间的反应可以通过外源性化学实体间接调节的新方法。图形抽象
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引用次数: 0
Large Azobenzene Macrocycles: Formation and Detection by NMR and MS Methods 大偶氮苯大环:核磁共振和质谱方法的形成和检测
IF 3.3 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-02-01 DOI: 10.1080/10610278.2023.2230334
H. Roithmeyer, Merle Uudsemaa, A. Trummal, Mari-Liis Brük, Sebastian Krämer, I. Reile, Vitālijs Rjabovs, Kirsti Palmi, M. Rammo, R. Aav, Elina Kalenius, J. Adamson
ABSTRACT Azobenzene macrocycles are widely investigated as potential drug delivery systems and as part of molecular machines due to their photo-responsive properties. Herein, we detect the formation of a series of new azobenzene macrocycles that feature up to eight switchable repeating units. High-resolution mass spectrometry and ion mobility (IM) mass spectrometry experiments and 1H and diffusion-ordered spectroscopy (DOSY) NMR are used to detect the presence of the macrocycles that contain 10 to 40 aromatic rings in the gas phase and solution, respectively. The responsiveness of the Z-to-E photo-switching of the smallest of the macrocycles, exhibiting two azobenzene units and in total 10 aromatic rings, separated with column chromatography, is studied with irradiation experiments, using both UV-Vis light and thermal excitation and relaxation, and monitoring the sample with UV-Vis absorption and 1H NMR spectroscopy. DFT calculations are used to understand the conformation of this isolated species in solution.
偶氮苯大环由于其光响应特性,作为潜在的药物传递系统和分子机器的一部分被广泛研究。在这里,我们检测到一系列新的偶氮苯大环的形成,这些大环具有多达8个可切换的重复单元。采用高分辨率质谱和离子迁移率(IM)质谱实验以及1H和扩散有序谱(DOSY) NMR分别检测气相和溶液中含有10 ~ 40个芳环的大环的存在。采用紫外-可见光、热激发和弛豫的辐照实验,利用紫外-可见吸收和1H NMR光谱监测样品,研究了最小的大环(含2个偶氮苯单元和共10个芳环)的z - e光开关的响应性。DFT计算被用来理解这个孤立的物种在溶液中的构象。
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引用次数: 0
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Supramolecular Chemistry
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