☆ 4.8 Review

Transformation networks of metal-organic cages controlled by chemical stimuli

CHEMICAL SOCIETY REVIEWS (2022)

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Dawei Zhang et al.

Summary: This study reports the construction of three structurally distinct self-assembled architectures formed from a single triazatriangulenium subcomponent A under different reaction conditions. The largest structure, pseudoicosahedral capsule 1, was formed at higher concentrations, while helicate 2 exclusively formed at lower concentrations. Conversion of pseudoicosahedron 1 or helicate 2 into tetrahedron 3 occurred following the addition of a CB11H12- or B12F122- template.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Multidisciplinary

Twisted rectangular subunits self-assemble into a ferritin-like capsule

Jack A. Davies et al.

Summary: The vertices of polyhedral protein capsules can be composed of multiple capsule-forming protein subunits, enabling them to enclose more volume and larger cargoes than single proteins. Applying protein cage design principles to synthetic analogs can increase their volume of encapsulation. In this study, a tetrahedral metal-organic capsule was self-assembled from a simple tetramine subcomponent, with each face composed of three ligand panels. The self-assembly rules of this system are programmed into the tetramine, favoring the formation of a large capsule over a simpler cube-like structure. Unlike other large metal-organic capsules, this new capsule has an enclosed cavity and can bind large dianionic guests.

CHEM (2022)

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Article Chemistry, Multidisciplinary

Dynamic optimization of guest binding in a library of diastereomeric heteroleptic coordination cages

Tanya K. Ronson et al.

Summary: This study reports a new type of coordination cage that can adapt and optimize the binding of guest molecules depending on the orientation of its ligands. Structural characterization and NMR spectroscopy confirmed the existence of multiple diastereomeric forms of the cage that can selectively bind to different guests.

CHEM (2022)

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Article Chemistry, Multidisciplinary

Backbone-Bridging Promotes Diversity in Heteroleptic Cages

Kai Wu et al.

Summary: By introducing covalent backbone bridges, the assembly structure can be diversified, and with the solvent and guest effects, it can modulate nuclearity, topology, and number of cavities. The nature of the linker in ligands would affect the structure of the assembly under different solvent conditions, resulting in different structural forms.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Controlled Self-Assembly and Multistimuli-Responsive Interconversions of Three Conjoined Twin-Cages

Li-Xuan Cai et al.

Summary: Controlled self-assembly of three topologically unprecedented conjoined twin-cages was achieved in this study, with structural conversions between cages 3 and 4 enabled by changing solvents. This interconversion between topologically complex superstructures may lay a solid foundation for achieving a variety of functions within a switchable system.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Multidisciplinary

Identification of a Heteroleptic Pd6L6L′6 Coordination Cage by Screening of a Virtual Combinatorial Library

Sylvain Sudan et al.

Summary: The design of structurally defined heteroleptic coordination cages is challenging and only a few examples are known. In this study, a novel hexanuclear Pd cage containing two types of dipyridyl ligands was identified using a selection approach. The structure of the cage was elucidated by single-crystal X-ray diffraction, revealing an unprecedented trigonal-antiprismatic cage structure.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Review Chemistry, Multidisciplinary

Metal-organic cages for molecular separations

Dawei Zhang et al.

Summary: Metal-organic cages, formed via coordination-driven self-assembly, show great promise as separation agents by selectively binding and distinguishing substances in solution through precise control of their structure. The use of cages as absorbents or incorporation into polymer membranes can enhance the efficiency and selectivity of separation processes. Challenges and potential future developments in using metal-organic cages for separations are also discussed.

NATURE REVIEWS CHEMISTRY (2021)

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Review Chemistry, Multidisciplinary

Electron-rich Coordination Receptors Based on Tetrathiafulvalene Derivatives: Controlling the Host-Guest Binding

Sebastien Goeb et al.

Summary: The coordination-driven self-assembly methodology is a versatile synthetic tool for obtaining complex discrete structures such as interlocked, chiral, or heteroleptic cages. Efforts have been made to control host-guest affinity, particularly in targeting substrate transportation and releasing. Redox-stimulation offers novel possibilities for controlling the host-guest binding affinity and triggering guest release.

ACCOUNTS OF CHEMICAL RESEARCH (2021)

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Article Chemistry, Multidisciplinary

Uptake, Trapping, and Release of Organometallic Cations by Redox-Active Cationic Hosts

Iram F. Mansoor et al.

Summary: The host-guest chemistry of metal-organic nanocages is driven by thermodynamically favorable interactions, allowing control of guest uptake and release by switching affinity on or off. By reducing the host, rapid uptake of organometallic cations can be achieved, forming metastable cation-in-cation complexes with unprecedented stability. Subsequent reoxidation of the hosts traps the guests, demonstrating a way to confine guests in unfavorable environments.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Review Chemistry, Inorganic & Nuclear

Catalysis within coordination cages

Yadan Xue et al.

Summary: Coordination cages with well-defined cavities have attracted attention for their structural aesthetics and unique properties in various fields. This review summarizes the achievements of these materials in catalytic applications, including their use as catalysts and their ability to encapsulate catalytic cofactors. Furthermore, the current challenges and great potential of coordination cages in catalysis are discussed.

COORDINATION CHEMISTRY REVIEWS (2021)

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Fracture, fatigue, and friction of polymers in which entanglements greatly outnumber cross-links

Junsoo Kim et al.

Summary: By synthesizing polymers with a large number of entanglements and sparse cross-links, high toughness, strength, and fatigue resistance can be achieved, resulting in hydrogels with low hysteresis, low friction, and high wear resistance after swelling in water.

SCIENCE (2021)

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Stimuli-Responsive Topological Transformation of a Molecular Borromean Ring via Controlled Oxidation of Thioether Moieties

Hai-Ning Zhang et al.

Summary: A Cp*-Rh based D-shaped binuclear metallacycle and a template-free molecular Borromean ring were synthesized successfully using the semi-rigid thioether dipyridyl ligand Bptmb. The controlled oxidation of thioethers led to the topological transformation from binuclear metallacycles and a Borromean ring to tetranuclear metallacycles. The strategy employed in this study can be considered a new form of stimuli-responsive post-synthesis modification.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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An interlocked coordination cage based on aromatic amide ligands

Dan Luo et al.

Summary: An interlocked M4L8 coordination cage was synthesized by coordination-driven self-assembly, with the structure and formation mechanism clearly revealed through various spectroscopic techniques.

CHINESE CHEMICAL LETTERS (2021)

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Hexameric Lanthanide-Organic Capsules with Tertiary Structure and Emergent Functions

Xiao-Qing Guo et al.

Summary: Utilizing metal-directed and anion-directed assembly processes, researchers constructed a 4 nm diameter lanthanide metal self-assembled hexameric capsule, demonstrating aggregation-induced stability and emission enhancement, as well as achieving guest-encapsulation function and enantioselectivity towards terpene drugs in late-formed central cavity of the hexamers.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Multidisciplinary

Integrative Assembly of Heteroleptic Tetrahedra Controlled by Backbone Steric Bulk

Jacopo Tessarolo et al.

Summary: In this study, by designing ligands and controlling assembly conditions, the synthesis of different [PdnL2n] assemblies, including [Pd3L6A] ring, [Pd4L8A] tetrahedron, and [Pd6L12A] octahedron, was successfully achieved. Furthermore, by introducing backbone steric hindrance, specific formation of [Pd6L12B] octahedron can be realized, and integrative self-sorting of heteroleptic [(Pd4L4L4B)-L-A] tetrahedron was achieved by mixing two ligands.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Wenqi Liu et al.

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Reversible pH-Controlled Catenation of a Benzobisimidazole-Based Tetranuclear Rectangle

Maksym Dekhtiarenko et al.

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CHEMISTRY-A EUROPEAN JOURNAL (2021)

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A Highly Entangled (M3L2)8 Truncated Cube from the Anion-Controlled Oligomerization of a π-Coordinated M3L2 Subunit

Yuya Domoto et al.

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Photooxidase Mimicking with Adaptive Coordination Molecular Capsules

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Review Chemistry, Multidisciplinary

Structural Flexibility in Metal-Organic Cages

Andres E. Martin Diaz et al.

Summary: Metal-organic cages (MOCs) are a diverse class of molecular hosts with potential utility across a vast spectrum of applications. Advances in single-crystal X-ray diffraction and computational structure optimization methods have allowed for the determination of cavity sizes and educated guesses about the likelihood of particular guests being bound within these porous structures. Structural flexibility inherent to MOCs can enable large structural changes and lead to highly sophisticated and functional synthetic hosts.

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Interconversion between a Pd3L2 trigonal prism and a Pd6L8 cube via anion exchange: binding affinity of monoatomic vs. polyatomic anions

Haeri Lee et al.

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DALTON TRANSACTIONS (2021)

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