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Mechanism of Hydrogen Storage on Reduced Carbon Single-Walled Nanotubes

Published online by Cambridge University Press:  01 February 2011

Calvin J Curtis
Affiliation:
calvin_curtis@nrel.gov, National Renewable Energy Laboratory, Computational and Materials Science, 1617 Cole Blvd., MS 3313, Golden, CO, 80401, United States, 303-384-6270, 303-384-6150
Thomas Gennett
Affiliation:
thomas_gennett@nrel.gov, National Renewable Energy Laboratory, Computational and Materials Science Center, Golden, CO, 80401, United States
Chaiwat Engtrakul
Affiliation:
chaiwat_engtrakul@nrel.gov, National Renewable Energy Laboratory, Computational and Materials Science Center, Golden, CO, 80401, United States
Kevin O'Neill
Affiliation:
kevin_oneill@nrel.gov, National Renewable Energy Laboratory, Computational and Materials Science Center, Golden, CO, 80401, United States
Jamie E. Ellis
Affiliation:
jamie.ellis@rit.edu, Rochester Institute of Technology, Department of Chemistry, Rochester, NY, 14623, United States
Michael J. Heben
Affiliation:
michael_heben@nrel.gov, National Renewable Energy Laboratory, Computational and Materials Science Center, Golden, CO, 80401, United States
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Abstract

Carbon single-walled nanotubes (SWNTs) have been studied extensively as hydrogen storage materials. Herein, a novel hydrogen sorbtion behavior was observed for alkali metal reduced SWNTs and the mechanism of hydrogen binding in these materials has now been elucidated. SWNTs prepared by laser vaporization and purified by oxidation were reduced with Na in combination with naphthalene in tetrahydrofuran (THF) solution. The product, initially formulated as (Na+)xSWNTx-, was dark colored and insoluble in all common solvents examined. Temperature programmed desorption studies showed that hydrogen amounting to 3.5-4.2% w/w was released between 200 and 500°C from the Na-reduced material. This is consistent with hydrogenation of the reduced nanotubes to form C-H bonds with a C2H empirical formula. It appears that SWNT radical anions produced by reaction with sodium deprotonate THF to form hydrogenated nanotubes and the THF cleavage products ethylene and sodium enolate, as confirmed by isotope labeling. A structure consisting of pairs of lines of C-H units that spiral about the long tube axis with a coverage of 50% of the tube carbons is proposed.

Type
Research Article
Copyright
Copyright © Materials Research Society 2008

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