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An Organic Zeolite With 10?A Diameter Pores Assembles From a Soluble and Flexible Building Block by Non-Covalent Interactions.

ABSTRACT: Two similar molecular building blocks, which both contain a hydrogen-bonded nitro group, have been prepared and crystallised. One structure has more flexibility with a butyl side chain which allows an open framework organic zeolite to form with large 10?Å diameter pores, whereas the other structure has less flexibility with an aryl side chain and is close packed. The pore size is comparable with those of the aluminophosphate VPI-5 (12?Å). It is concluded that some flexibility in the design of the building block for porous organic molecular materials was beneficial.

SUBMITTER: Plater MJ

PROVIDER: S-EPMC6454218 | biostudies-literature | 2019 Apr

REPOSITORIES: biostudies-literature

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An Organic Zeolite With 10 Å Diameter Pores Assembles From a Soluble and Flexible Building Block by Non-Covalent Interactions.

Plater M John MJ Harrison William T A WTA

ChemistryOpen 20190408 4

Two similar molecular building blocks, which both contain a hydrogen-bonded nitro group, have been prepared and crystallised. One structure has more flexibility with a butyl side chain which allows an open framework organic zeolite to form with large 10 Å diameter pores, whereas the other structure has less flexibility with an aryl side chain and is close packed. The pore size is comparable with those of the aluminophosphate VPI-5 (12 Å). It is concluded that some flexibility in the design of th ...[more]

PMID: 31008010

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Project description:Nanoparticle-based devices, materials and technologies will demand a new era of synthetic chemistry where predictive principles familiar in the molecular regime are extended to nanoscale building blocks. Typical covalent strategies for modifying nanoparticle-bound species rely on kinetically controlled reactions optimised for efficiency but with limited capacity for selective and divergent access to a range of product constitutions. In this work, monolayer-stabilized nanoparticles displaying complementary dynamic covalent hydrazone exchange reactivity undergo distinct chemospecific transformations by selecting appropriate combinations of 'nucleophilic' or 'electrophilic' nanoparticle-bound monolayers with nucleophilic or electrophilic molecular modifiers. Thermodynamically governed reactions allow modulation of product compositions, spanning mixed-ligand monolayers to exhaustive exchange. High-density nanoparticle-stabilizing monolayers facilitate in situ reaction monitoring by quantitative 19F NMR spectroscopy. Kinetic analysis reveals that hydrazone exchange rates are moderately diminished by surface confinement, and that the magnitude of this effect is dependent on mechanistic details: surface-bound electrophiles react intrinsically faster, but are more significantly affected by surface immobilization than nucleophiles. Complementary nanoparticles react with each other to form robust covalently connected binary aggregates. Endowed with the adaptive characteristics of the dynamic covalent linking process, the nanoscale assemblies can be tuned from extended aggregates to colloidally stable clusters of equilibrium sizes that depend on the concentration of a monofunctional capping agent. Just two 'dynamic covalent nanoparticles' with complementary thermodynamically governed reactivities therefore institute a programmable toolkit offering flexible control over nanoparticle surface functionalization, and construction of adaptive assemblies that selectively combine several nanoscale building blocks.

Dataset Information

An Organic Zeolite With 10?A Diameter Pores Assembles From a Soluble and Flexible Building Block by Non-Covalent Interactions.

Publications

An Organic Zeolite With 10 Å Diameter Pores Assembles From a Soluble and Flexible Building Block by Non-Covalent Interactions.

Similar Datasets

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