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Imaging carbon nanostructures' reactivity: a complementary strategy to define chemical structure.

ABSTRACT: In the search for the integration of carbon nanostructures in composite and functional materials, covalent organic reactions are successfully performed. This approach resulted in the construction of tailored chemical interfaces facilitating incorporation of nanocarbons. By a combination of different characterization techniques, such as high-resolution X-ray photo-spectroscopy, thermogravimetric analysis, Raman spectroscopy, UV-vis-nIR, and fluorescence spectroscopies, it is possible to identify and quantify the functional moieties covalently attached to the carbon frame. However, the determination of the structural conformation of functionalized nanostructures remains a difficult task. In this work, we present a straightforward methodology to visualize by transmission electron microscopy the functional moieties covalently attached to the carbon network in carbon nanotubes and graphene. The identification of the functionalities occurs in colloidal dispersions by using gold nanoparticles (AuNPs) as discriminating markers by molecular recognition or by the direct growth of AuNPs on the oxygenated moieties. This methodology, in combination with other characterization analysis, is expected to improve the design of hierarchical interfaces by the spatial localization of the functionalities responsible for colloidal stabilization in solvents with different polarities, different from their homogeneous incorporation into different matrices.

SUBMITTER: Perez-Luna V

PROVIDER: S-EPMC6124117 | biostudies-literature | 2018 Aug

REPOSITORIES: biostudies-literature

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Imaging carbon nanostructures' reactivity: a complementary strategy to define chemical structure.

Pérez-Luna Verónica V Cisneros Mario M Bittencourt Carla C Saucedo-Orozco Izcoatl I Quintana Mildred M

Royal Society open science 20180808 8

In the search for the integration of carbon nanostructures in composite and functional materials, covalent organic reactions are successfully performed. This approach resulted in the construction of tailored chemical interfaces facilitating incorporation of nanocarbons. By a combination of different characterization techniques, such as high-resolution X-ray photo-spectroscopy, thermogravimetric analysis, Raman spectroscopy, UV-vis-nIR, and fluorescence spectroscopies, it is possible to identify ...[more]

PMID: 30225055

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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

Imaging carbon nanostructures' reactivity: a complementary strategy to define chemical structure.

Publications

Imaging carbon nanostructures' reactivity: a complementary strategy to define chemical structure.

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