Microstructural control of a SSZ-13 zeolite film via rapid thermal processing

초록

A SSZ-13 zeolite (CHA type zeolite having a pore size of 0.37 x 0.42 nm(2)) can separate CO2(0.33 nm) from larger molecules (N-2(0.364 nm) or CH4(0.38 nm)) because of the molecular size differences. However, methods to control the non-zeolitic defects of SSZ-13 membranes are lacking. Here, we demonstrate that rapid thermal processing (RTP) of as-synthesized SSZ-13 films tunes their microstructural defect properties and increases their CO2 separation ability. The maximum CO2/N-2 separation factor (SF) at 30 degrees C increased from similar to 2.9 to similar to 4.8 due to RTP because the defective region was reduced. Furthermore, the addition of water vapor (the third main component of coal-fired power plant flue gas) to the feed markedly improved the CO2/N-2 SF of the RTP-treated SSZ-13 membrane; from similar to 4.3 at 50 degrees C (a representative flue gas stream temperature) under dry conditions to -10.1 under wet conditions (vs. -1.6 across the conventionally calcined counterpart). Furthermore, the less-defective RTP-treated SSZ-13 membranes achieved a CO2/CH4SF as high as similar to 43.7 under wet conditions at 50 degrees C. Fluorescence confocal optical microscopy analyses complemented with the permeation modeling revealed that the reduced defect size after RTP (similar to 2.2 nm against similar to 3.9 nm for the conventionally calcined counterpart) improved the CO2 permselectivity, even though the defect porosities were low (similar to 0.1%).

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