P HC3. P EtOH R HC N structures R EtOH
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1 P EtOH w = 0.12% w = 0.43% w = 1.4% w = 4.5% w = 15% w = 41% R EtOH P HC N structures R HC3-4 P HC3 Supplementary Figure 1: Distribution of performance scores. (Left) P EtOH as function of R EtOH at w = 0.12 wt% for all IZA-SC structures with the inset showing the values for the 10 structures with the highest P EtOH for all six raffinate concentrations. (Right) P HC3 as function of R HC3 for the 2835 PCOD structures retained for the high-pressure simulations with the inset showing the corresponding data for the 103 IZA-SC structures retained for the high-pressure simulations. 1
2 10 4 S EtOH 10 2 w = 0.12% w = 1.4% w = 15% Q EtOH [mol per kg] 10-4 P EtOH d free [nm] d incl [nm] ρ T [nm -3 ] Supplementary Figure 2: Scatter plots for ethanol-water adsorption. Ethanol selectivity (S EtOH, top), loading (Q EtOH, middle), and performance score (P EtOH, bottom) as a function of the diameter of the largest free-roaming sphere (d free, left), the diameter of the largest included sphere along the free sphere path (d incl, middle), and the density of framework T atoms (ρ T, right). 2
3 PCOD IZA-SC Q C18 [mmol kg -1 ] k H, C18 [mol kg -1 Pa -1 ] Supplementary Figure 3: Scatter plot for hydrocarbon adsorption. Loading (Q C18 ) at p = 3 MPa versus k H,C18 at the infinite-dilution limit. 3
4 Supplementary Figure 4: Scatter plots for hydrocarbon adsorption. Henry s constant (k H,C18 in mol kg 1 Pa 1 ), row 1) and linear-versus-branched selectivity at the infinite-dilution limit (S B0, row 2), loading (Q C18 in mmol kg 1, row 3), linear-versus-branched selectivity (S B3, row 4), long-versus-short selectivity (S L3, row 5), and performance score (P HC3, row 6) at p = 3 MPa as a function of the diameter of the largest free-roaming sphere (d free, left), the diameter of the largest included sphere along the free sphere path (d incl, middle), and the density of framework T atoms (ρ T, right). 4
5 10 5 k H, C18, long [mol kg -1 Pa -1 ] PCOD IZA-SC k H, C18, short [mol kg -1 Pa -1 ] S B0, long S L0, long S B0, short S L0, short 10-3 Supplementary Figure 5: Influence of simulation length on performance indicators. (Top) Henry s law constant for C18 (k H,C18 in mol kg 1 Pa 1 ), (left bottom) linear-versus-branched selectivity (S B0 ) and (right bottom) long-versus-short selectivity (S L0 ) for 103 IZA-SC and 2835 PCOD structures obtained from long and short GCMC simulations. 5
6 16 16 N [molecules per unit cell] Oumi, 300 K Dubinin, 303 K Sano, 303 K Zhang, 308 K Dose, 308 K TraPPE-zeo, 303 K Milestone, 293 K Cekova, 298 K Lin, 303 K TraPPE-zeo, 298 K N [molecules per unit cell] p / p c [mol L -1 ] 0 Supplementary Figure 6: Adsorption isotherms in MFI. (Left) Unary ethanol adsorption from the gas phase. The red squares, blue diamonds, magenta up triangles, cyan left triangles, purple down triangles, and black circles show the experimental measurements by Oumi et al. 1, Dubinin et al. 2, Sano et al. 3, Zhang et al. 4, and Dose et al. 5, and the predictions using the TraPPE zeo/trappe UA force fields, respectively. (Right) Ethanol adsorption from aqueous solution. The red squares, blue diamonds, green up triangles, and black circles show the experimental measurements of Milestone and Bibby 6, Cekova et al. 7, and Lin and Ma 8, and the predictions using the TraPPE zeo/trappe UA/TIP4P force fields, respectively. Pressures are converted to activities using experimentally measured and model-predicted saturation vapor pressures for experiments and simulations, respectively. 6
7 Supplementary Table 1: Adsorption properties for ethanol-water separation. Ethanol loading (Q EtOH in mol kg 1 ), water loading (Q Wat in mol kg 1 ), retentate composition (r in wt%), ethanol selectivity (S EtOH ), performance score (P EtOH ), and performance rank (R EtOH ) at six different raffinate concentrations (w) for each of the five highest ranked zeolites at any w. Data for MFI and VFI are provided for comparison. The target selectivity (S target = 0.956(1 w)/0.044w) is the value required to exceed the azeotropic concentration. w = 0.12 % S target = w = 0.43 % S target = 5100 Q EtOH Q Wat r S EtOH P EtOH R Q EtOH Q Wat r S EtOH P EtOH R FER OWE ESV UFI MRE ZON ATN MAZ ZON MTT CGF CDO MFI VFI, w = 1.4 % S target = 1500 w = 4.5 % S target = 460 Q EtOH Q Wat r S EtOH P EtOH R Q EtOH Q Wat r S EtOH P EtOH R FER OWE ESV UFI MRE ZON ATN MAZ ZON MTT CGF CDO MFI Idealized siliceous structure. Zinc-containing aluminophosphate. Zeolite with Q Wat > Q EtOH at w = 0.12 %. 7
8 Supplementary Table 1 (continued): Adsorption properties for ethanol-water separation. Ethanol loading (Q EtOH in mol kg 1 ), water loading (Q Wat in mol kg 1 ), retentate composition (r in wt%), ethanol selectivity (S EtOH ), performance score (P EtOH ), and performance rank (R EtOH ) at six different raffinate concentrations (w) for each of the five highest ranked zeolites at any w. Data for MFI and VFI are provided for comparison. The target selectivity (S target = 0.956(1 w)/0.044w) is the value required to exceed the azeotropic concentration. w = 15 % S target = 120 w = 41 % S target = 31 Q EtOH Q Wat r S EtOH P EtOH R Q EtOH Q Wat r S EtOH P EtOH R FER OWE ESV UFI MRE ZON ATN MAZ ZON MTT CGF CDO MFI Idealized siliceous structure. Zinc-containing aluminophosphate. Zeolite with Q Wat > Q EtOH at w = 0.12 %. 8
9 Supplementary Table 2: Adsorption properties for hydrocarbon separation. Henry s law constant for C18 (k H,C18 in mol kg 1 Pa 1 ), high-pressure loading for C18 (Q C18 in mmol kg 1 ), linear-versus-branched selectivity (S Bp ) and long-versus-short selectivity (S Lp ), performance score (P HCp ), and performance rank (R HCp ) for the top-10 IZA-SC and PCOD structures based on simulations in the infinite-dilution limit and at p = 3 MPa. The last 5 rows show the PCOD structures with the highest R HC3 that have similar selectivities to those of the top-10 IZA-SC zeolites (S B3 < 100 and S L3 > 0.9). infinite-dilution limit p = 3 MPa name k H,C18 S B0 S L0 P HC0 R HC0 Q C18 S B3 S L3 P HC3 R HC3 ATO MRE AFO CAN AEL MTT WEN FER TON EUO MTW GON VET ITH Idealized siliceous structure. Aluminophosphate. 9
10 Supplementary References [1] Oumi, Y., Miyajima, A., Miyamoto, J. & Sano, T. Binary mixture adsorption of water and ethanol on silicalite. In Aiello, R., Giordano, G. & Testa, F. (eds.) Stud. Surf. Sci. Catal., vol. 142, (Elsevier, 2002). [2] Dubinin, M. M., Rakhmatkariev, G. U. & Isirikyan, A. A. Differential heats of adsorption and adsorption isotherms of alcohols on silicalite. B Acad Sci USSR Ch+ 38, (1989). [3] Sano, T., Yanagishita, H., Kiyozumi, Y., Mizukami, F. & Haraya, K. Separation of ethanol/water mixture by silicalite membrane on pervaporation. J. Membr. Sci. 95, (1994). [4] Zhang, K. et al. Adsorption of water and ethanol in MFI-type zeolites. Langmuir 28, (2012). [5] Dose, M. E. et al. Effect of crystal size on framework defects and water uptake in fluoride mediated silicalite-1. Chem. Mater. 26, (2014). [6] Milestone, N. B. & Bibby, D. M. Concentration of alcohols by adsorption on silicalite. J. Chem. Technol. Biotechnol. 31, (1981). [7] Cekova, B., Kocev, D., Kolcakovska, E. & Stojanova, D. Zeolites as alcohol adsorbents from aqueous solutions. Acta Periodica Technologica 37, (2006). [8] Lin, Y. S. & Ma, Y. H. Liquid diffusion and adsorption of aqueous ethanol, propanols, and butanols in silicalite by HPLC. ACS Symp. Ser. 368, (1988). 10
Correction Table for an Alcoholometer Calibrated at 20 o C
An alcoholometer is a device that measures the concentration of ethanol in a water-ethanol mixture (often in units of %abv percent alcohol by volume). The depth to which an alcoholometer sinks in a water-ethanol
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