Item

Abstract

Membrane-based gas separation processes can address key challenges in energy and environment, but for many applications the permeance and selectivity of bulk membranes is insufficient for economical use. Theory and experiment indicate that permeance and selectivity can be increased by using two-dimensional materials with subnanometer pores as membranes. Motivated by experiments showing selective permeation of H₂/CO mixtures through amorphous silica bilayers, here we perform a theoretical study of gas separation through silica bilayers. Using density functional theory calculations, we obtain geometries of crystalline free-standing silica bilayers (comprised of 6-membered rings), as well as the 7-, 8- and 9- member ring that are observed in glassy silica bilayers, that arise due to Stone-Wales defects and vacancies. We then compute the potential energy barriers for gas passage through these various pore types for He, Ne, Ar, Kr, H₂, N₂, CO, and CO₂ gases, and use the data to assess their capability for selective gas separation. Our calculations indicate that crystalline bilayer silica—which is less than a nanometer thick—can be a high-selectivity and high-permeance membrane materials for ³He/⁴He, He/natural gas, and H₂/CO separations.