Pd/SiO2 Inorganic–Organic Composite Membrane Calcined Under N2 Atmosphere: Thermal Stability and H2/CO2 Separation

Abstract

A novel Pd/SiO2 inorganic–organic composite material was developed for the selective separation of H2 from a mixture of H2 and CO2. Its thermal stability and microstructure calcined under N2 atmosphere were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, scanning electron microscopy, transmission electron microscopy and N2 sorption–desorption measurements. Pd element in Pd/SiO2 gel material exists in PdCl2 form, calcination at 350 °C can result in the complete transformation of Pd2+ to metallic Pd0. With the increase of calcination temperature, the hydrophobic Si–CH3 bands decreased in intensity. The residue of Pd/SiO2 material calcined at 800 °C was mainly composed of Si–O–Si, metallic Pd0, CSi4 and some elemental C0. The mean pore size, BET specific surface area and total pore volume of the as-prepared Pd/SiO2 material calcined at 350 °C was about 2.26 nm, 417.35 m2 g−1 and 0.288 m3 g−1, respectively. The mean H2 and CO2 permeances of the corresponding Pd/SiO2 membrane were 9.90×10−6 and 9.10×10−7 mol m−2 Pa−1 s−1, respectively, when operating at 200 °C and a pressure difference of 0.3 MPa. After the steam exposure at 200 °C for 168 h, the H2 permeance decreased by 3.23% while the H2/CO2 permselectivity increased by 2.50%.