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The sol–gel method was employed for the synthesis of binary X–Co (X: Mn, Cr) oxide-doped silicamembranes with different X/Co molar ratios (X/Co: 0.1, 0.3, 0.9). Single-gas permeation tests wereperformed at 200 C to determine the effect of the binary oxide composition on the amorphous silicanetwork. The X-ray diffraction (XRD), X-ray Photoelectron Spectroscopy (XPS) and Transmission ElectronMicroscopy (TEM) indicated the presence of smaller MnxCo3xO4 and CrxCo3xO4 oxide nanocrystals inthe silica matrix in addition to amorphous Co, Mn and Cr species. The H2/N2 permeance ratio decreasedfrom (126.3  9) to (10.7  2) with an increase in X/Co molar ratio from 0.1 to 0.9 due to the formationof larger pores. However, the binary Co–X oxide-doped silica membrane with the lowest X contentshowed a H2/N2 permeance ratio, (126.3  9), higher than that, (63.6  6), of the single cobalt oxidesilica membrane. Based on FTIR analysis, it was found that the densification of the membrane at low Xcontent resulted from the formation of silica structures with narrowed siloxane rings. In contrast, theenlargement of siloxane rings due to favorable condensation reactions occurred at high X content

Tailoring the structure and gas permeation properties of silica membranes via binary metal oxides doping