Solution-phase synthesis of heteroatom-substituted carbon scaffolds for hydrogen storage |
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Authors: | Jin Zhong Sun Zhengzong Simpson Lin J O'Neill Kevin J Parilla Philip A Li Yan Stadie Nicholas P Ahn Channing C Kittrell Carter Tour James M |
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Affiliation: | Department of Chemistry, and The Richard E. Smalley Institute for Nanoscale Science and Technology, Rice University, MS-222, 6100 Main Street, Houston, Texas 77005, United States. |
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Abstract: | 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. |
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