Nondissociative adsorption of H2 molecules in light-element-doped fullerenes.

First-principles density functional and quantum Monte Carlo calculations of light-element doped fullerenes reveal significantly enhanced molecular H2 binding for substitutional B and Be. A nonclassical three-center binding mechanism between the dopant and H2 is identified, which is maximized when the empty p(z) orbital of the dopant is highly localized. The calculated binding energies of 0.2-0.6 eV/H2 is suited for reversible hydrogen storage at near standard conditions. The calculated H2 sorption process is barrier-less, which could also significantly simplify the kinetics for the storage.

[1]  A. Zettl,et al.  C36, a new carbon solid , 1998, Nature.

[2]  R. Kötz,et al.  The boron heterofullerenes C59B and C69B: generation, extraction, mass spectrometric and XPS characterization , 1996 .

[3]  J. Grossman,et al.  Linear-scaling quantum Monte Carlo calculations. , 2001, Physical review letters.

[4]  H. Jónsson,et al.  Theoretical studies of atomic-scale processes relevant to crystal growth. , 2000, Annual review of physical chemistry.

[5]  J. S. Arellano,et al.  Density functional study of adsorption of molecular hydrogen on graphene layers , 2000 .

[6]  Jackson,et al.  Atoms, molecules, solids, and surfaces: Applications of the generalized gradient approximation for exchange and correlation. , 1992, Physical review. B, Condensed matter.

[7]  Baoyi Wang,et al.  Bonding character of the boron-doped C60 films prepared by radio frequency plasma assisted vapor deposition , 2002 .

[8]  P. Downes,et al.  Hydrogen storage in sonicated carbon materials , 2001 .

[9]  Richard E. Smalley,et al.  Doping bucky: formation and properties of boron-doped buckminsterfullerene , 1991 .

[10]  Young Hee Lee,et al.  Hydrogen storage in single-walled carbon nanotubes , 2000 .

[11]  Ju Li,et al.  Theoretical evaluation of hydrogen storage capacity in pure carbon nanostructures , 2003 .

[12]  K. Ishikawa,et al.  Synthesis of heterofullerenes by laser ablation , 1999 .

[13]  Hansong Cheng,et al.  Mechanism of hydrogen sorption in single-walled carbon nanotubes. , 2001, Journal of the American Chemical Society.

[14]  D. Bethune,et al.  Storage of hydrogen in single-walled carbon nanotubes , 1997, Nature.

[15]  Y. Miyamoto,et al.  Ab Initio Investigation of Physisorption of Molecular Hydrogen on Planar and Curved Graphenes , 2001 .

[16]  X. Gong,et al.  Chemisorption of hydrogen molecules on carbon nanotubes under high pressure. , 2001, Physical review letters.

[17]  G. Kubas.  Metal–dihydrogen and σ-bond coordination: the consummate extension of the Dewar–Chatt–Duncanson model for metal–olefin π bonding , 2001 .

[18]  Jena,et al.  Binding of hydrogen molecules by a transition-metal ion. , 1992, Physical review letters.

[19]  Kenneth A. Smith,et al.  Hydrogen adsorption and cohesive energy of single-walled carbon nanotubes , 1999 .

[20]  S. Zhang,et al.  Nanotube wires on commensurate InAs surfaces: binding energies, band alignments, and bipolar doping by the surfaces. , 2004, Physical review letters.

[21]  Pekka Pyykkö,et al.  How many hydrogen atoms can be bound to a metal? Predicted MH12 species. , 2004, Journal of the American Chemical Society.

[22]  George Crabtree,et al.  The hydrogen economy , 2006, IEEE Engineering Management Review.

[23]  C. Colliex,et al.  Cross-linked nano-onions of carbon nitride in the solid phase: existence of a novel C(48)N(12) aza-fullerene. , 2001, Physical review letters.

[24]  Z. Gu,et al.  Synthesis of C60-NBN and C70-NBN(N=L, 2) by DC arc Burning Method , 1998 .

[25]  B. Alder,et al.  THE GROUND STATE OF THE ELECTRON GAS BY A STOCHASTIC METHOD , 2010 .

[26]  S. Louie,et al.  Electronic and structural properties of molecular C36 , 1998 .