CERAMIC MEMBRANES FOR HYDROGEN PRODUCTION FROM COAL

[摘要] The present project is devoted to developing hydrogen permselective silica membranes supported on composite supports to achieve high flux and selectivity. The supports consist of a thin zeolite silicalite layer coated on {alpha}-Al{sub 2}O{sub 3} tubes of mean pore size 1 {micro}m. The zeolite layer is grown by reaction in a suitable silicate solution at 95 C. After two or three reaction periods a layer of silicalite crystals about 20 {micro}m thick grows inside the pores of alumina. In addition to the zeolitic pores, this layer contains voids of a few nanometer diameter that remain between the crystals or between the crystals and the pore walls. The quality of the silicalite/alumina composites was evaluated by gas permeation measurements and by nitrogen adsorption and it was found that the residual voids were below 5 nm in diameter. Three techniques were investigated for chemical vapor deposition (CVD) of the silica layer on the silicalite/alumina composite support. The first was TEOS pyrolysis at approximately one millibar partial pressure and 650 C. After 8 h reaction the fluxes of hydrogen and nitrogen at ambient temperature had declined by a factor of approximately 100 indicating sealing of defects and zeolitic pores alike. The second CVD technique investigated was SiCl{sub 4} hydrolysis at 90 C. Deposition in this case was conducted in a series of cycles, each cycle comprising two half reactions, i.e. exposure to SiCl{sub 4} followed by exposure to water vapor. The deposition was interrupted every five cycles to measure the permeation properties of the nascent membrane at 120 C. After a few cycles the membrane pores were sealed, but the silica layer was not thermally stable when the temperature was raised to 400 C. In the third technique investigated, silica deposition was carried out by SiCl{sub 4} hydrolysis at 400 C, again in a sequence of half reaction cycles. After 15 cycles the membrane pores were well sealed by a layer stable to at least 400 C.

[发布日期] 2001-11-27 [发布机构] California Institute of Technology (United States)

[关键词] Coal;Water Vapor;Membranes;08 Hydrogen;01 Coal, Lignite, And Peat