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Solution-Phase Synthesis of Heteroatom-Substituted Carbon Scaffolds for Hydrogen Storage

Jin, Zhong and Sun, Zhengzong and Simpson, Lin J. and O’Neill, Kevin J. and Parilla, Philip A. and Li, Yan and Stadie, Nicholas P. and Ahn, Channing C. and Kittrell, Carter and Tour, James M. (2010) Solution-Phase Synthesis of Heteroatom-Substituted Carbon Scaffolds for Hydrogen Storage. Journal of the American Chemical Society, 132 (43). pp. 15246-15251. ISSN 0002-7863.

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This paper reports a bottom-up solution-phase process for the preparation of pristine and heteroatom (boron, phosphorus, or nitrogen)-substituted carbon scaffolds that show good surface areas and enhanced hydrogen adsorption capacities and binding energies. The synthesis method involves heating chlorine-containing small organic molecules with metallic sodium at reflux in high-boiling solvents. For heteroatom incorporation, heteroatomic electrophiles are added to the reaction mixture. Under the reaction conditions, micrometer-sized graphitic sheets assembled by 3−5 nm-sized domains of graphene nanoflakes are formed, and when they are heteroatom-substituted, the heteroatoms are uniformly distributed. The substituted carbon scaffolds enriched with heteroatoms (boron ~7.3%, phosphorus ~8.1%, and nitrogen ~28.1%) had surface areas as high as 900 m^2 g^(−1) and enhanced reversible hydrogen physisorption capacities relative to pristine carbon scaffolds or common carbonaceous materials. In addition, the binding energies of the substituted carbon scaffolds, as measured by adsorption isotherms, were 8.6, 8.3, and 5.6 kJ mol^(−1) for the boron-, phosphorus-, and nitrogen-enriched carbon scaffolds, respectively.

Item Type:Article
Related URLs:
Tour, James M.0000-0002-8479-9328
Additional Information:© 2010 American Chemical Society. Received June 21, 2010. Publication Date (Web): October 7, 2010. Financial support was provided by the U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy within the Hydrogen Sorption Center of Excellence at the National Renewable Energy Laboratory (DEFC-36-05GO15073).
Funding AgencyGrant Number
Department of Energy (DOE) Office of Energy Efficiency and Renewable EnergyDEFC-36-050015073
Issue or Number:43
Record Number:CaltechAUTHORS:20101208-090302226
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Official Citation:Solution-Phase Synthesis of Heteroatom-Substituted Carbon Scaffolds for Hydrogen Storage Zhong Jin, Zhengzong Sun, Lin J. Simpson, Kevin J. O’Neill, Philip A. Parilla, Yan Li, Nicholas P. Stadie, Channing C. Ahn, Carter Kittrell, James M. Tour Journal of the American Chemical Society 2010 132 (43), 15246-15251
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:21232
Deposited By: Tony Diaz
Deposited On:11 Dec 2010 00:44
Last Modified:09 Mar 2020 13:19

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