Controlled hierarchical self-assembly of networked coordination nanocapsules<i>via</i>the use of molecular chaperones

Hu, Xiangquan; Feng, Sisi; Du, Jialei; Shao, Li; Lang, Jinxin; Zhang, Chen; Kelley, Steven P.; Lin, Jian; Dalgarno, Scott J.; Atwood, David A.; Atwood, Jerry L.

doi:10.1039/d0sc05002d

Cited by 11 publications

(13 citation statements)

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“…Inspired by living organisms, where hierarchical proteins with metal ions like Fe, Mn, or Cu can be efficiently formed with the aid of supramolecular chaperones, 63,64 herein we introduce proline as the molecular chaperone, which can capture, protect, and insert Mn II ions into the framework. 51 The synthesis of CP-MONCs has been accomplished by employing PgC 3 OH, Mn II ions, and proline using a solvothermal method. Moreover, upon increase of the water content in the reaction mixture, the resulting assemblies transform from 2D (11) to 3D (12) CP-MONCs (Figure 7).…”

Section: Coordination Polymers Based On Hexameric Moncsmentioning

confidence: 99%

Coordination Polymers Constructed from Pyrogallol[4]arene-Assembled Metal–Organic Nanocapsules

Shao

Sikligar

et al. 2021

Acc. Chem. Res.

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Conspectus Coordination polymers, commonly known as infinite crystalline lattices, are versatile networks and have diverse potential applications in the fields of gas storage, molecular separation, catalysis, optics, and drug delivery, among other areas. Secondary building blocks, mainly incorporating rigid polydentate organic linkers and metal ions or clusters, are commonly employed to construct coordination polymers. Recently, novel building blocks such as coordination polyhedra have been utilized as metal nodes to fabricate coordination polymers. Benefiting from the rigid porous structure of the coordination polyhedron, prefabricated designer “pores” can be incorporated in this type of coordinate polymer. In this Account, coordination polymers built by pyrogallol[4]arene-assembled metal–organic nanocapsules are summarized. This class of metal–organic nanocapsule possesses the following advantages that make them excellent candidates in the construction of coordination polymers: (i) Various geometrical shapes with different volumes of the inner cavities can be obtained from these capsules. Among them, the two main categories illustrated are dimeric and hexameric capsules, which comprise two and six pyrogallol[4]arenes units, respectively. (ii) A wide range of possible metal ions ranging from main group metals to transition metals and even lanthanides have been demonstrated to seam the capsules. Therefore, these coordination polymers can be endowed with fascinating functionalities such as magnetism, semiconductivity, luminescence, and radioactivity. (iii) Up to 24 metal ions have been successfully embedded on the surface of the nanocapsule, each a potential reaction site in the construction of coordination polymers, opening up pathways for the formation of multidimensional frameworks. In this Account, we focus primarily on the synthesis and the structural information on pyrogallol[4]arene-derived coordination polymers. Coordination polymers can be formed by introducing linkers with two coordination sites, using pyrogallol[4]arenes with coordination sites on the tail, or even via metal ions cross-linking with each other. Machine learning was recently developed to help us predict and screen the structures of the coordination polymers. With single crystal analysis in hand, detailed structural information provides a molecular-level perspective. Significantly, following the formation of coordination polymers, the overall shape and structure of the discrete metal–organic nanocapsules remains essentially unchanged, with full retention of the prefabricated pores. If a rigid linker is used to connect capsules, more than one lattice void with different volumes can be found within the framework. Thus, molecules with different sizes could potentially be encapsulated within these coordination polymers. In addition, flexible ligands can also be employed as linkers. For example, polymers have been employed as large linkers that transform the crystalline coordination polymers into polymer matrices, paving the way toward the ...

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Section: Coordination Polymers Based On Hexameric Moncsmentioning

confidence: 99%

Coordination Polymers Constructed from Pyrogallol[4]arene-Assembled Metal–Organic Nanocapsules

Shao

Sikligar

et al. 2021

Acc. Chem. Res.

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“…Other bowl-shaped host molecules of the calixarene-family have also been shown to form MOFs/coordination polymers with embedded metallo-capsules, 6 and Atwood and co-workers have also reported much larger network nano-cages with pyrogallol [4]arene hosts. 7 Holman et al have also reported a coordination chain material with embedded cryptophanes which are organic CTV-based capsules. 36 The earliest examples with CTV-ligands were the series [Ag 3 (L10) 2 (CH 3 -CN) 3 Cl]•2X•n(CH 3 CN) where X = BF 4 , AsF 6 or ClO 4 .…”

Section: Linked Capsules and Cagesmentioning

confidence: 99%

“…This is also the case for networked coordination capsules and coordination cages with other host molecules. 6,7 As for the CTV examples, these included networks of vertex-linked capsules as well as those linked by an additional ligand. Examples of post-synthetic assembly of showing the 2D network of Ag 3 L 2 capsules linked by μ 3 -Cl − (larger olive spheres) and inset is side-view of one capsule highlighting that the μ 3 -Cl − are endo to the cage.…”

Section: Linked Capsules and Cagesmentioning

confidence: 99%

“…4 There are many different types of molecular hosts which are generally macrocyclic and feature a molecular cavity of some type as a guest-binding site, a variety of molecular host have been employed as bridging ligands for MOFs and coordination polymers. [4][5][6][7][8] The most commonly thus utilised macrocycles are calixarenes and related cone-shaped hosts. Pillararenes, crown ethers, cucurbiturils and cyclodextrins have also been employed.…”

Section: Introductionmentioning

confidence: 99%

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Coordination polymers with embedded recognition sites: lessons from cyclotriveratrylene-type ligands

Snelgrove

Hardie

2021

CrystEngComm

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“…[ 19‐26 ] Low‐symmetry architectures such as crowns and bowls are difficult to design and synthesis. [ 27‐29 ] Only a few coordination complexes could be described as molecular bowls. [ 29‐31 ]…”

Section: Background and Originality Contentmentioning

confidence: 99%

Solvent‐Controlled Construction of Molecular Chains and Bowls/Sieves from a Bent Dipyridyl Ligand^†

et al. 2021

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Main observation and conclusion Solvothermal reactions of 3,6‐di(pyridin‐4‐yl)‐9H‐carbazole (dpc) with Cu(II) yielded crystals of two new coordination complexes, namely [Cu(CH3COO)2(dpc)(H2O)2]n·xGuest (1) and [Cu13(HCOO)16(dpc)16(H2O)6](HCOO)10·Guest (2), in which CH3COO– and HCOO– were generated from the hydrolysis of the solvents N,N‐dimethylacetamide (DMA) and N,N‐dimethylformamide (DMF), respectively. Single‐crystal X‐ray diffraction showed that 1 possesses simple wavy coordination chains, while 2 possesses large molecular bowls/sieves with outer and inner effective sizes of 30.2 × 30.2 × 25.5 Å3 and 15.0 × 15.0 × 18.6 Å3, respectively, which consists of 4 linear Cu3(HCOO)4(H2O) clusters and 12 dpc ligands as the square‐shaped wall and a claw‐like Cu(dpc)4 fragment as the bottle. Guest‐free 2 can adsorb considerable amounts of CO2, H2O and CH3OH but completely exclude C2H4 and C3H6, which shows a potential application for olefin drying.

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Controlled hierarchical self-assembly of networked coordination nanocapsulesviathe use of molecular chaperones

Abstract: Molecular chaperones play a critical role in directing the assembly of nanocapsules that assemble into 2D or 3D coordination networks.

Cited by 11 publications

References 50 publications

Coordination Polymers Constructed from Pyrogallol[4]arene-Assembled Metal–Organic Nanocapsules

Coordination Polymers Constructed from Pyrogallol[4]arene-Assembled Metal–Organic Nanocapsules

Coordination polymers with embedded recognition sites: lessons from cyclotriveratrylene-type ligands

Solvent‐Controlled Construction of Molecular Chains and Bowls/Sieves from a Bent Dipyridyl Ligand^†

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Controlled hierarchical self-assembly of networked coordination nanocapsulesviathe use of molecular chaperones

Abstract: Molecular chaperones play a critical role in directing the assembly of nanocapsules that assemble into 2D or 3D coordination networks.

Cited by 11 publications

References 50 publications

Coordination Polymers Constructed from Pyrogallol[4]arene-Assembled Metal–Organic Nanocapsules

Coordination Polymers Constructed from Pyrogallol[4]arene-Assembled Metal–Organic Nanocapsules

Coordination polymers with embedded recognition sites: lessons from cyclotriveratrylene-type ligands

Solvent‐Controlled Construction of Molecular Chains and Bowls/Sieves from a Bent Dipyridyl Ligand†

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Solvent‐Controlled Construction of Molecular Chains and Bowls/Sieves from a Bent Dipyridyl Ligand^†