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Illuminating spin-crossover octanuclear metal-organic cages

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Science China Chemistry 2024年第4期67卷 1208-1215页

作者： Zhi-Kun Liu Alyona A.Starikova Yu-Xia Li Ke Sun Meng Yu Zi-Shuo Yao Jun Tao Key Laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringLiangxiang CampusBeijing Institute of TechnologyBeijing 102488China Institute of Physical and organic Chemistry Southern Federal UniversityRostov-on-Don 344090Russia

Spin-crossover(SCO)materials that reversibly switch between high-and low-spin states have potential for the storage of spin state-relative information,and have gained much attention incorporating secondary physical properties,such as fluorescence and magneto-optical *** this study,we synthesized three octanuclear metal-organic cages(MOCs)using tetraphenylethylene-based luminophores,aldehydes,and Fe^(Ⅱ)salts,by subcomponent self-assembly approach,namely[Fe1]-[Fe3].By controlling the ligand-field strength and guest encapsulation,we finely tuned their SCO *** them,MOC[Fe2]displayed nearly complete SCO behavior in the solid state,which is rare for high-nuclearity *** also demonstrated the coupling of SCO with fluorescence emission in these MOCs by using isostructural Zn^(Ⅱ)complexes([Zn1]-[Zn3])as control experiments,for the first *** calculations revealed the energy-transfer mechanism between fluorophores and SCOactive centers,which emphasizes the significant contribution of d-d transitions in the interplay between the occurrence of SCO and fluorescence emission.

关键词： metal-organic cages spin crossover fluorescence switching materials DFT calculation

Stabilizing the Extrinsic Porosity in metal-organic cages-Based Supramolecular Framework by In Situ Catalytic Polymerization

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CCS Chemistry 2021年第5期3卷 1382-1390页

作者： Guoliang Liu Mi Zhou Kongzhao Su Ravichandar Babarao Daqiang Yuan Maochun Hong State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002 University of the Chinese Academy of Sciences Beijing 100049 Commonwealth Scientific and Industrial Research Organization(CSIRO)Manufacturing MelbourneVIC 3169 School of Science RMIT UniversityMelbourneVIC 3001

Porous supramolecular frameworks based on metal-organic cages(MOCs)usually have poor structural stability after *** issue narrows the scope of their potential applications,particularly for the inclusion of guest molecules that demand high ***,the authors have reported the stabilization of a mesoporous zirconium MOC-based supramolecular framework with an in situ catalytic polymerization *** to the passivation effect imparted by this strategy,the introduced polymer is primarily distributed on the surface of the crystals,which results in the hybrid material retaining its crystallinity and permanent porosity.A preliminary application of this type of stabilized mesoporous supramolecular framework shows that among MOC-based supramolecular frameworks,it has the highest high-pressure methane *** a facile strategy may provide a general way to stabilize fragile porous materials and facilitate exploration of their potential applications.

关键词： in situ catalytic polymerization metal-organic cages supramolecular frameworks framework stabilization methane uptake

Selective photosynthesis of Z-olefins through crystalline metal-organic cage-initiated expeditious cascade reactions

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Carbon Energy 2024年第3期6卷 118-131页

作者： Jia-Ni Lu Yunze Huang Yuan-Sheng Xia Long-Zhang Dong Lei Zhang Jing-Jing Liu Lan-Gui Xie Jiang Liu Ya-Qian Lan Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceJiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNanjingChina School of Chemistry South China Normal UniversityGuangzhouChina

The semi-hydrogenation of alkyne to form Z-olefins with high conversion and high selectivity is still a huge challenge in the chemical ***,flammable and explosive hydrogen as the common hydrogen source of this reaction increases the cost and danger of industrial ***,we connect the photocatalytic hydrogen evolution reaction and the semihydrogenation reaction of alkynes in series and successfully realize the high selective production of Z-alkenes using low-cost,safe,and green water as the proton *** the cascade reaction,a series of isomorphic metal–organic cage catalysts(Co_(x)Zn_(8−x)L_(6),x=0,3,4,5,and 8)are designed and synthesized to improve the yield of the photocatalytic hydrogen *** them,Co_(5)Zn_(3)L_(6) shows the highest photocatalytic activity,with a H_(2) generation rate of 8.81 mmol g^(−1) h^(−1).Then,Co_(5)Zn_(3)L_(6) is further applied in the above tandem reaction to efficiently reduce alkynes to Z-alkenes under ambient conditions,which can reach high conversion of>98%and high selectivity of>99%,and maintain original catalytic activity after multiple ***“one-pot”tandem reaction can achieve a highly selective and safe stepwise conversion from water into hydrogen into Z-olefins under mild reaction conditions.

关键词： alkyne semi-hydrogenation hydrogen evolution reaction metal-organic cages photocatalysis Z-olefins

Coordination Assembly of Tetrahedral Ti_(4)(embonate)_(6) cages with Alkaline-Earth metal Ions

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Chinese Journal of Structural Chemistry 2022年第1期41卷 1-6页

作者： Ruiyan Chen Guanghui Chen Yanping He Jian Zhang College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Recently,the tetrahedral Ti_(4)L_(6) cage(L=embonate)has been applied as the starting material to realize coordination assembly with transition and rare-earth ornoble metal ions through a two-step *** this work,by employing the Ti_(4)L_(6) cages to assemble with alkaline-earth metal ions(such as Mg^(2+),Ca^(2+)and Ba^(2+))under different solvothermal conditions,a series of Ti_(4)L_(6)-based structures from simple cages to 1D chain,2D layer and 3D framework have been synthesized and structurally *** addition,thermal stability,phase purity,UV-vis absorption spectrum,the fluorescent and third-order nonlinear-optical properties are also investigated.

关键词： metal-organic cages stepwise-assembly alkaline-earth structures nonlinear optics

Steric Control over Interligand Dihedrals and Splay Leads to the Formation of Fe^(II)_(6)L_(6)and Fe^(II)_(8)L_(8)Antiprisms

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CCS Chemistry 2024年第10期6卷 2411-2419页

作者： Yuchong Yang Yuyin Du Tanya K.Ronson Jonathan R.Nitschke Yusuf Hamied Department of Chemistry University of CambridgeCambridge CB21EW

Macrocycles have found uses in guest capture,sensing,and porous materials,motivating the development of new methods for their *** we report the construction of two types of barrelshaped macrocyclic assemblies,with trigonal antiprismatic Fe^(II)_(6)L_(6)and square antiprismatic Fe^(II)_(8)L_(8)architectures,from FeII and boron-containing tritopic *** factors,the steric hindrance of ligands and the preferred coordination angles at different vertices,were observed to regulate the dihedral angles between adjacent ligands,leading to the formation of the structures *** effects of ligand steric hindrance led to the formation of a Fe^(II)_(6)L_(6)trigonal antiprism,which efficiently encapsulated persistent environmental pollutant perfluorosulfonate *** contrast with the iminopyridine chelating groups of the Fe^(II)_(6)L_(6)structure,the incorporation of azopyridine moieties coordinated with the FeII centers not only increased the vertex opening angle,resulting in the construction of a Fe^(II)_(8)L_(8)square antiprism,but also enabled the redox-driven reversible disassembly of this *** design strategies that have enabled the construction of these antiprismatic macrocycles may provide insight into the design principles governing the formation of more complex functional assemblies.

关键词： self-assembly metal-organic cages host-guest chemistry redox-responsive materials dihedral control

用于气体分离的含多孔材料的混合基质膜--从金属有机框架到离散分子笼

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Engineering 2023年第4期23卷 40-55,M0003页

作者： Ziqi Yang Zhongjie Wu Shing Bo Peh Yunpan Ying Hao Yang Dan Zhao Department of Chemical and Biomolecular Engineering National University of SingaporeSingapore 117585Singapore Joint School of the National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China

混合基质膜(MMMs)将多孔材料与聚合物基质相结合,因其互补特性和协同激活已经在气体分离领域引起了相当大的研究兴趣。多孔材料的可塑性和多样性赋予MMMs可延伸的功能和出色的分离性能。为了发挥MMMs的全部潜力,研究人员关注多孔填料与... 详细信息

混合基质膜(MMMs)将多孔材料与聚合物基质相结合,因其互补特性和协同激活已经在气体分离领域引起了相当大的研究兴趣。多孔材料的可塑性和多样性赋予MMMs可延伸的功能和出色的分离性能。为了发挥MMMs的全部潜力,研究人员关注多孔填料与聚合物基质的合理匹配,以实现这些材料之间界面的增强相容性。在本文中,我们重点介绍采用不同策略将金属-有机框架(MOFs)和金属-有机笼(MOCs)与聚合物基质相结合制备MMMs的最新进展。文中进一步讨论未来MMMs发展所面临的机遇和挑战,并旨在通过合理的材料设计和选择推动MMMs的制备。

关键词： Gas separation metal-organic frameworks metal-organic cages Mixed-matrix membranes Interfacial compatibility

Selective Sensing of Nucleoside Molecules by Fluorescent Response of Cerium-based Cage

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Selective Sensing of Nucleoside Molecules by Fluorescent Res...

Photoinduced energy-and electron-transfer from a photoactive metal-organic cage to bound guests

中国化学会第八届全国配位化学会议

作者： Lu Yang Cheng He Chunying Duan State Key Laboratory of Fine Chemicals Dalian University of Technology

The selective recognition of nucleoside derivatives, which represented as an important part of biological genetic functions, is difficult to detect mainly due to the subtle variation of their structures. Generally, the main interactions between biochemical species rely on the complementary hydrogen bonding and π stacking interactions. The host-guest supramolecular interaction could be considered as an efficient candidate to achieve the selective recognition via the active sites. Various well-defined metal-organic cages(MOCs) with nanosized molecular cavity can be constructed by the pre-designed organic and inorganic building blocks incorporating multiple hydrogen bonding sites to encapsulate and stabilize specific guest molecules with suitable size and shape. Herein, we prepared a supramolecular Ce-based nanocage, containing 12-fold amide and 4-fold secondary amine groups as active sites, to selectively recognize RNA nucleosides through complementary hydrogen bonding. The opening faces and confined cavity provide adequate space for the size-suitable guests to access. Fluorescent titration revealed that the addition of guanosine in the solution of Ce-based cage caused 3.6 times emission enhancement, much larger than those of other RNA nucleosides.

关键词： supramolecular interaction metal-organic cages fluorescent response

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Photoinduced energy-and electron-transfer from a photoactive...

Construction and Regulation of Optically Active Ir(Ⅲ) Mteal–organic cages Based on DCC

中国化学会第十届全国无机化学学术会议

作者： Hechuan Li Cheng He Chunying Duan State Key Laboratory of Fine Chemicals Dalian University of Technology

In recent years, metal-organic cages(MOCs) constructed by coordination-driven self-assembly have been gradually developed, because of their well-defined hydrophobic cavities and the easy-modified organic ligands, which endows them excellent supramolecular behavior to interact with the specific guest molecules. Recently, we assembled a new photoactive MOC based on triphenylamine. In the MOC which contains an array of four triphenylamine chromophores surrounding a central cavity, photoinduced energy or electron-transfer can occur from the chromophore array to the bound guest in supramolecular host/guest complexes.

关键词： metal-organic cages Supramolecular behavior Photoinduced energy-transfer Photoinduced electron-transfer

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Construction and Regulation of Optically Active Ir(Ⅲ) Mteal...