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Figure 7. CO2 (Left) and N2 (Right) Adsorption Sites in Cu-SSZ-13 at 4 K The positions of CO2 and N2 in relation to the 8-ring pore windows are shown as a space-filling representation in the middle (yellow spheres, O atoms; black spheres, C atoms; pale blue spheres, N atoms). Note that the figure represents only the adsorption sites and does not quantify the amounts of gas at each location; the actual occupancy is much greater for CO2. Reprinted with permission from Hudson et al.36 Copyright 2012 American Chemical Society. the adsorption of CO2. Therefore, zeolites have been studied extensively for capturing CO2 from N2, CH4, or H2 in various industrial processes.35 For instance, the low-pressure adsorption of CO2 and N2 over H- and Cu-exchanged zeolites SSZ-13 (CHA type) was investigated.36 The maximum CO2 uptake for H- and Cu-SSZ-13 at 1 bar was 3.98 and 3.75 mmol g1, respectively. More importantly, un- der ideal conditions for CO2/N2 separation for industrial flue gas (a mixture of 0.15 bar CO2 and 0.75 bar N2), H- and Cu-SSZ-13 exhibited the ideal adsorbed so- lution theory selectivity of 73.6 and 72.0, respectively. Such high CO2 uptake and selectivity were attributed to the small-pore nature of SSZ-13, in which the 8-ring pore window matched the kinetic diameter of CO2 well, producing a special binding effect toward CO2 (Figure 7). Another family of small-pore aluminosilicate zeolites with extending complexity and embedded isoreticular frameworks were reported to exhibit high CO2 uptake and selectivity.37 In particular, at room temperature, Na-ZSM-25 (MTF type) in this family exhibited a CO2/CH4 selectivity of 331 at 0.1 bar and 22 at 1.0 bar. Moreover, Na-ZSM-25 could achieve CO2 adsorption equilibrium in 2 min and its CO2 uptake remained the same over 100 adsorption- desorption cycles. Such high performance for CO2 capture was attributed to the ‘‘molecular trapdoor’’ effect, by which the extra-framework cations blocked the 8-ring pore windows and only allowed the entrance of molecules strongly interacting with them, such as CO2.38 The fast diffusion of CO2 was also observed in other zeolites. Using interference microscopy, Lauerer et al.39 studied the diffusion of CO2–C2H6 mixtures in small-pore zeolite ZSM-58 (DDR type). The diffusion of CO2 was so fast in comparison with C2H6 that the CO2 uptake instantly exceeded its final equilibrium value, which was known as the ‘‘overshooting’’ behavior of the fast-diffu- sive component as a result of the ‘‘uphill diffusion’’ effect. In comparison, the local C2H6 concentration increased gradually to reach the final equilibrium value. Taking advantage of the diffusion speed difference, small-pore zeolites such as ZSM-58 could be utilized to kinetically separate CO2 from other species. Zeolites can be made into CO2-selective permeance membranes for CO2 separa- tion. For instance, a 0.5-mm-thick silica zeolite MFI membrane was reported with the straight channels along the b axis uniformly aligned.40 This membrane exhibited a separation selectivity of 109 for a 50:50 CO2/H2 mixture and a CO2 permeance of Chem 3, 928–949, December 14, 2017 939PDF Image | Applications of Zeolites in Sustainable Chemistry
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