Graphene is impermeable to gases, but introducing subnanometer pores can allow for selective gas separation. Because graphene is only one atom thick, tunneling can play an important role, especially for low-mass gases such as helium, and this has been proposed as a means of separating (3)He from (4)He. In this paper, we consider the possibility of utilizing resonant tunneling of helium isotopes through nanoporous graphene bilayers. Using a model potential fit to previously reported DFT potential energy surfaces, we calculate the thermal rate constant as a function of interlayer separation using a recently described time-independent method for arbitrary multibarrier potentials. Resonant transmission allows for the total flux rate of (3)He to remain the same as the best-known single-barrier pores but doubles the selectivity with respect to (4)He when the optimal interlayer spacing of 4.6 Å is used. The high flux rate and selectivity are robust against variations of the interlayer spacing and asymmetries in the potential that may occur in experiment.

Helium Isotope Enrichment by Resonant Tunneling through Nanoporous Graphene Bilayers / S. Mandrà, J. Schrier, M. Ceotto. - In: JOURNAL OF PHYSICAL CHEMISTRY. A, MOLECULES, SPECTROSCOPY, KINETICS, ENVIRONMENT, & GENERAL THEORY. - ISSN 1089-5639. - 118:33(2014), pp. 6457-6465. [10.1021/jp502548r]

Helium Isotope Enrichment by Resonant Tunneling through Nanoporous Graphene Bilayers

M. Ceotto
Ultimo
2014

Abstract

Graphene is impermeable to gases, but introducing subnanometer pores can allow for selective gas separation. Because graphene is only one atom thick, tunneling can play an important role, especially for low-mass gases such as helium, and this has been proposed as a means of separating (3)He from (4)He. In this paper, we consider the possibility of utilizing resonant tunneling of helium isotopes through nanoporous graphene bilayers. Using a model potential fit to previously reported DFT potential energy surfaces, we calculate the thermal rate constant as a function of interlayer separation using a recently described time-independent method for arbitrary multibarrier potentials. Resonant transmission allows for the total flux rate of (3)He to remain the same as the best-known single-barrier pores but doubles the selectivity with respect to (4)He when the optimal interlayer spacing of 4.6 Å is used. The high flux rate and selectivity are robust against variations of the interlayer spacing and asymmetries in the potential that may occur in experiment.
graphene; resonant tunneling; rate constant; time-independent method
Settore CHIM/02 - Chimica Fisica
2014
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/2434/238227
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