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Lee, Chang Young
Carbon Nanomaterials Lab
Research Interests
  • Carbon nanomaterials, gas sensors, neuroanalytical chemistry, biomimetic nanosystems

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Amine basicity (pK(b)) controls the analyte blinding energy on single walled carbon nanotube electronic sensor Arrays

Cited 36 times inthomson ciCited 18 times inthomson ci
Title
Amine basicity (pK(b)) controls the analyte blinding energy on single walled carbon nanotube electronic sensor Arrays
Other Titles
Amine basicity (pKb) controls the analyte binding energy on single walled carbon nanotube electronic sensor arrays
Author
Lee, Chang YoungStrano, Michael S.
Keywords
CHEMICAL SENSORS; GAS SENSOR; NO2; TRANSPARENT; ADSORPTION; NETWORKS; DYNAMICS; CHLORIDE; VAPORS; FILMS
Issue Date
2008-02
Publisher
AMER CHEMICAL SOC
Citation
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.130, no.5, pp.1766 - 1773
Abstract
A wide range of analytes adsorb irreversibly to the surfaces of single walled carbon nanotube electronic networks typically used as sensors or thin-film transistors, although to date, the mechanism is not understood. Using thionyl chloride as a model electron-withdrawing adsorbate, we show that reversible adsorption sites can be created on the nanotube array via noncovalent functionalization with amine-terminated molecules of pK(a) < 8.8. A nanotube network comprising single, largely unbundled nanotubes, near the electronic percolation threshold is required for the effective conversion to a reversibly binding array. By examining 11 types of amine-containing molecules, we show that analyte adsorption is largely affected by the basicity (pK(b)) of surface groups. The binding energy of the analyte is apparently reduced by its adsorption on the surface chemical groups instead of directly on the SWNT array itself. This mediated adsorption mechanism is supported by X-ray photoelectron spectroscopy (XPS) and molecular potential calculations. Reversible detection with no active regeneration at the parts-per-trillion level is demonstrated for the first time by creating a higher adsorption site density with a polymer amine, such as polyethyleneimine (PEI). Last, we demonstrate that this transition to reversibility upon surface functionalization is a general phenomenon
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DOI
10.1021/ja0776069
ISSN
0002-7863
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