Preparation and Gas Permeation Properties of Fluorine-Silica Membranes with Controlled Amorphous Silica Structures: Effect of Fluorine Source and Calcination Temperature on Network Size

摘要

Triethoxyfluorosilane (TEFS), which is a pendant-type alkoxysilane with a Si-F bond, was utilized for the development of a molecular sieving membrane. The effect that a source of fluorine and calcination temperature exerted on gas permeation properties and network pore size was evaluated via single-gas permeation properties across a wide range of temperatures. A TEFS membrane calcined at 350 degrees C showed high H-2 permeance (2.0 X 10(-6) mol m(-2) s(-1) Pa-1) and high selectivity for H-2 over larger molecules (H-2/CF4:300; H-2/SF6: >18 000), indicating that this network pore size would be suitable for a H-2 permselective membrane that could promOte the process of methylcyclohexane (MCH) dehydrogenation to produce toluene (TOL). Based on the gas permeation properties and the results of XPS,and FTIR, networlcpore Size depended on the fluorine concentration incorporated in SiO2 that existed as Si F bonds, irrespective of the fluorine source. A TEFS membrane showed approximately the same pore size distribution and level of gas,permeance, irrespettive of calcination temperature (350 and 550 degrees C), due to the low Si OH density in the networks as sugpsted by the result of FTIR, which (an prevent the densification caused by the condensation of Si OH groups. The pair distribution function also suggested that densification of the network structure for TEFS was, apparently suppressed compared with that of a tetraethoxysilane,(TEOS)derived structure.