Reticular Chemistry in All Dimensions

Yaghi, Omar M.

doi:10.1021/acscentsci.9b00750

“…Many MOFs are designed according to the “node and linker” approach and elaborated using “reticular chemistry” . The key design concept in generating protein‐encapsulating ZMOFs (for example, ZIF‐8 and ZIF‐90 ) is the tetrahedral geometry of the metal atoms (for example, Zn 2+ ) and a suitable subtended linker angle (for example, 142.4° for 2‐R‐imidazole, R=methyl or aldehyde).…”

Section: Methodsmentioning

confidence: 99%

Protein‐Structure‐Directed Metal–Organic Zeolite‐like Networks as Biomacromolecule Carriers

Wang

¹

,

Han

²

,

Zheng

³

et al. 2020

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Fabrication of zeolite‐like metal–organic frameworks (ZMOFs) for advanced applications, such as enzyme immobilization, is of great interest but is a great synthetic challenge. Herein, we have developed a new strategy using proteins as structure‐directed agents to direct the formation of new ZMOFs that can act as versatile platforms for the in situ encapsulation of proteins under ambient conditions. Notably, protein incorporation directs the formation of a ZMOF with a sodalite (sod) topology instead of a non‐porous diamondoid (dia) topology under analogous synthetic conditions. Histidines in proteins play a crucial role in the observed templating effect. Modulating histidine content thereby influenced the resultant MOF product (from dia to dia + sod mixture and, ultimately, to sod MOF). Moreover, the resulting ZMOF‐incorporated proteins preserved their activity even after exposure to high temperatures and organic solvents, demonstrating their potential for biocatalysis and biopharmaceutical applications.

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“…The directional assembly of coordination polymers and networks depends upon the compatibility of directing-nodes and linkers [1]. Directional metal nodes are key to the rational design of 2-and 3-dimensional inorganic materials and is at the heart of 'reticular chemistry' in which well-defined molecular units, so-called secondary building units (SBUs), are used to direct extended frameworks in a pre-determined and controlled fashion [2,3]. One of the simplest SBUs is the M 2 (µ-O 2 CR) 4 paddle-wheel motif in which the axial sites of the dinuclear core provide linear directionality (Scheme 1) [4,5].…”

Section: Introductionmentioning

confidence: 99%

Single and Double-Stranded 1D-Coordination Polymers with 4′-(4-Alkyloxyphenyl)-3,2′:6′,3″-terpyridines and {Cu2(μ-OAc)4} or {Cu4(μ3-OH)2(μ-OAc)2(μ3-OAc)2(AcO-κO)2} Motifs

Rocco

¹

,

Manfroni

²

,

Prescimone

³

et al. 2020

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Five coordination polymers formed from combinations of copper(II) acetate and 4′-(4-alkyloxyphenyl)-3,2′:6′,3″-terpyridines with methoxy (1), n-butoxy (2), n-pentyloxy (3) and n-heptyloxy (4) substituents are reported. Reaction of 1 with Cu(OAc)2∙H2O leads to the 1D-polymer [Cu2(μ-OAc)4(1)]n in which {Cu2(μ-OAc)4} paddle-wheel units are connected by ligands 1, or [{Cu4(μ3-OH)2(μ-OAc)2(μ3-OAc)2(AcO-κO)2(1)2}·2MeOH]n in which centrosymmetric tetranuclear clusters link pairs of ligands 1 to give a double-stranded 1D-polymer. Layering solutions of Cu(OAc)2∙H2O (in MeOH) over 2, 3 or 4 (in CHCl3) leads to the assembly of the 1D-polymers [2{Cu2(μ-OAc)4(2)}·1.25MeOH]n, [Cu2(μ-OAc)4(3)]n and [{Cu2(μ-OAc)4(4)}·0.2CHCl3]n. In all compounds, the 3,2′:6′,3″-tpy unit coordinates only through the outer pyridine rings, but the conformation of the 3,2′:6′,3″-tpy responds to changes in the length of the alkyloxy tails leading to changes in the conformation of the polymer backbone and in the packing of the chains in the crystal lattice in the chains featuring {Cu2(μ-OAc)4} paddle-wheel linkers.

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“…The discovery of the templating effect of proteins and a more developed understanding of the mechanism should provide guidance for the design and synthesis of a broad range of functional porous materials that incorporate biomacromolecules.Many MOFs are designed according to the "node and linker" approach and elaborated using "reticular chemistry". [30] The key design concept in generating protein-encapsulating ZMOFs (for example, ZIF-8 and ZIF-90) [10][11][12] is the…”

mentioning

confidence: 99%

“…Many MOFs are designed according to the "node and linker" approach and elaborated using "reticular chemistry". [30] The key design concept in generating protein-encapsulating ZMOFs (for example, ZIF-8 and ZIF-90) [10][11][12] is the…”

mentioning

confidence: 99%

“…Many MOFs are designed according to the "node and linker" approach and elaborated using "reticular chemistry". [30] The key design concept in generating protein-encapsulating ZMOFs (for example, ZIF-8 and ZIF-90) [10][11][12] is the tetrahedral geometry of the metal atoms (for example, Zn 2+ ) and a suitable subtended linker angle (for example, 142.48 for 2-R-imidazole, R = methyl or aldehyde). Pyrimidine derivatives are a basic building block of genetic material and possess structural similarity with the imidazole derivatives that generate ZIF-8 and ZIF-90.…”

mentioning

confidence: 99%

See 1 more Smart Citation

Protein‐Structure‐Directed Metal–Organic Zeolite‐like Networks as Biomacromolecule Carriers

Wang

¹

,

Han

²

,

Zheng

³

et al. 2020

View full text Add to dashboard Cite

Fabrication of zeolite‐like metal–organic frameworks (ZMOFs) for advanced applications, such as enzyme immobilization, is of great interest but is a great synthetic challenge. Herein, we have developed a new strategy using proteins as structure‐directed agents to direct the formation of new ZMOFs that can act as versatile platforms for the in situ encapsulation of proteins under ambient conditions. Notably, protein incorporation directs the formation of a ZMOF with a sodalite (sod) topology instead of a non‐porous diamondoid (dia) topology under analogous synthetic conditions. Histidines in proteins play a crucial role in the observed templating effect. Modulating histidine content thereby influenced the resultant MOF product (from dia to dia + sod mixture and, ultimately, to sod MOF). Moreover, the resulting ZMOF‐incorporated proteins preserved their activity even after exposure to high temperatures and organic solvents, demonstrating their potential for biocatalysis and biopharmaceutical applications.

show abstract

Reticular Chemistry in All Dimensions

Cited by 196 publications

References 36 publications

Protein‐Structure‐Directed Metal–Organic Zeolite‐like Networks as Biomacromolecule Carriers

Protein‐Structure‐Directed Metal–Organic Zeolite‐like Networks as Biomacromolecule Carriers

Single and Double-Stranded 1D-Coordination Polymers with 4′-(4-Alkyloxyphenyl)-3,2′:6′,3″-terpyridines and {Cu2(μ-OAc)4} or {Cu4(μ3-OH)2(μ-OAc)2(μ3-OAc)2(AcO-κO)2} Motifs

Protein‐Structure‐Directed Metal–Organic Zeolite‐like Networks as Biomacromolecule Carriers

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