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Microstructural control of a SSZ-13 zeolite film via rapid thermal processing
Kim, Jinseong,Jang, Eunhee,Hong, Sungwon,Kim, Dongjae,Kim, Eunjoo,Ricther, Hannes,Simon, Adrian,Choi, Nakwon,Korelskiy, Danil,Fouladvand, Shahpar,Nam, Jaewook,Choi, Jungkyu Elsevier 2019 Journal of membrane science Vol.591 No.-
<P><B>Abstract</B></P> <P>A SSZ-13 zeolite (CHA type zeolite having a pore size of 0.37 × 0.42 nm<SUP>2</SUP>) can separate CO<SUB>2</SUB> (0.33 nm) from larger molecules (N<SUB>2</SUB> (0.364 nm) or CH<SUB>4</SUB> (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 CO<SUB>2</SUB> separation ability. The maximum CO<SUB>2</SUB>/N<SUB>2</SUB> separation factor (SF) at 30 °C increased from ~2.9 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 CO<SUB>2</SUB>/N<SUB>2</SUB> SF of the RTP-treated SSZ-13 membrane; from ~4.3 at 50 °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 CO<SUB>2</SUB>/CH<SUB>4</SUB> SF as high as ~43.7 under wet conditions at 50 °C. Fluorescence confocal optical microscopy analyses complemented with the permeation modeling revealed that the reduced defect size after RTP (~2.2 nm against ~3.9 nm for the conventionally calcined counterpart) improved the CO<SUB>2</SUB> permselectivity, even though the defect porosities were low (~0.1%).</P> <P><B>Highlights</B></P> <P> <UL> <LI> Rapid thermal processing (RTP) of SSZ-13 films improved the CO<SUB>2</SUB> permselectivities. </LI> <LI> The improved separation performance was attributed to the reduced defect size. </LI> <LI> Despite the comparable degree of defects, their size determined the performance. </LI> <LI> Such improvement was pronounced with respect to water vapor-containing feeds. </LI> <LI> Robust CO<SUB>2</SUB> permselectivities were achieved using the RTP-treated SSZ-13 membranes. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>