Improving hydrogen permeation and interface property of ceramic-supported graphene oxide membrane via embedding of silicalite-1 zeolite into Al2O3 hollow fiber

Abstract

Graphene oxide (GO)-based membranes have previously demonstrated great gaseous molecular separation potential. However, defect-free GO-based laminar membrane presents major challenge given the difficulty to deposit configured GO film onto the porous ceramic support. This work reports single-step synthesis of a molecular sieving GO membrane film on top of silicalite-1 (Sil-1)-modified alumina (Al2O3) (Sil-1-Al2O3) hollow fiber. The critical Sil-1 content in the support is 2 wt%, above which there is marginal improvement of the interfacial adhesion, d-spacing, and hydrogen permeance. Binary gas permeation experiments on GO/2 wt% Sil-1-Al2O3 membrane revealed parallel increase of H2 and N2 permeance with temperature rise and decrease in H2 selectivity at higher temperatures. The operational stability of the composite membrane was demonstrated by stable H2 permeance (1.22 · 10−7 mol m−2 s−1 Pa−1) and selectivity (40.7) over 240-h operation at 20 °C, and maintained consistently following 210-h operation at 100 °C. Modeling study revealed major driving force contribution near the fiber inlet to increase the overall membrane H2 permeance.