Insights into Adsorption of Chlorobenzene in High Silica MFI and FAU Zeolites Gained from Chromatographic and Diffractometric Techniques
Abstract
:1. Introduction
2. Experimental Methods
2.1. Materials and Methods
2.2. Batch Adsorption
2.3. Thermal Analyses
2.4. X-ray Powder Diffraction Data Collection and Refinement Strategy
3. Results and Discussion
3.1. Adsorption Isotherms from Aqueous Solutions
3.2. Structural Modifications upon Chlorobenzene Adsorption on High Silica Zeolites
3.2.1. Y–CB
3.2.2. ZSM-5–CB
4. Conclusions
Supplementary Materials
Acknowledgments
Author Contributions
Conflicts of Interest
References
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Parameter | ZSM-5 | ZSM-5–CB | Y | Y–CB |
---|---|---|---|---|
[Si96O192] | [Si96O192]·6(C6H5Cl)·8(H2O) | [Si192O384] | [Si192O384]·32(C6H5Cl)·70(H2O) | |
Space group | P21/n | P21/n | Fd-3m | Fd-3 |
a (Å) | 19.899(5) | 19.919(1) | 24.259(1) | 24.263(1) |
b (Å) | 20.117(6) | 20.107(1) | 24.259(1) | 24.263(1) |
c (Å) | 13.389(4) | 13.3967(1) | 24.259(1) | 24.263(1) |
α (°) | 90 | 90 | 90 | 90 |
β (°) | 90.546(3) | 90.528(3) | 90 | 90 |
γ (°) | 90 | 90 | 90 | 90 |
V (Å3) | 5359.9(3) | 5365.7(5) | 14,277.1(1) | 14,284.4(6) |
Wavelength (Å): Cu Kα1 | 1.540593 | 1.540593 | 1.540593 | 1.540593 |
Cu Kα2 | 1.544427 | 1.544427 | 1.544427 | 1.544427 |
Refined 2θ (°) range | 3°–110° | 3°–110° | 3°–100° | 3°–100° |
Contributing reflections | 5861 | 6362 | 620 | 620 |
Nobs | 5350 | 5350 | 4850 | 4850 |
Nvar | 289 | 301 | 40 | 40 |
Rwp (%) | 10.3 | 13.3 | 12.8 | 12.9 |
Rp (%) | 9.4 | 10.4 | 12.5 | 12.6 |
RF2 (%) | 7.00 | 7.25 | 9.95 | 10.0 |
Rp = Σ[Yio − Yic]/ΣYio; Rwp = [Σwi(Yio − Yic)2/ΣwiYio2]0.5; RF2 = Σ|Fo2 − Fc2|/|Fo2| |
C0 (mg·L−1) | qt (mg·g−1) | k2 (g·L−1·mg−1) | R2 | |
---|---|---|---|---|
ZSM-5 | 15 | 23.4 (23.3, 23.5) | 0.44 (0.41, 0.47) | 0.9845 |
25 | 44.3 (44.2, 44.3) | 0.37 (0.33, 0.41) | 0.9803 | |
35 | 67.6 (67.5, 67.6) | 0.21 (0.19, 0.23) | 0.9985 | |
Y | 25 | 39.3 (39.2, 39.4) | 0.14 (0.11, 0.17) | 0.9822 |
35 | 70.3 (70.2, 70.3) | 0.13 (0.11, 0.15) | 0.9969 | |
45 | 82.3 (82.4, 82.5) | 0.10 (0.085, 0.12) | 0.9935 |
R2 | SSE | |||
---|---|---|---|---|
CB–ZSM-5 | Langmuir | |||
qs | 76.6 (74.8, 79.5) | 0.9874 | 198 | |
b | 5.0 (3.7, 6.6) | |||
CB–Y | Hill | |||
qs | 227 (218, 245) | 0.9654 | 2135 | |
KH | 9.2 (6.6, 12.1) | |||
n | 5.5 (4.3, 6.7) |
Parameter | Y–CB | Y [11] |
---|---|---|
O4–O4 distance (Å) | 11.16 | 9.81 |
O1–O1 distance (Å) | 9.68 | 9.70 |
Free diameter O4–O4 (Å) | 8.46 | 7.11 |
Free diameter O1–O1 (Å) | 6.98 | 7.00 |
Mean diameter (Å) | 7.72 | 7.06 |
Mean radius (Å) | 3.86 | 3.53 |
C.F.A. (Å2) | 46.81 | 39.07 |
ε | 1.21 | 1.01 |
Straight Channel | ||||||
O–O distance (Å) | O7–O1 | O8–O2 | O31–O37 | O44–O46 | O47–O48 | ε |
ZSM-5–CB | 8.22 | 8.20 | 8.02 | 8.22 | 7.97 | 1.03 |
ZSM-5 | 7.90 | 7.94 | 8.04 | 8.41 | 7.80 | 1.08 |
Free diameter (Å) | O7–O1 | O8–O2 | O31–O37 | O44–O46 | O47–O48 | |
ZSM-5–CB | 5.52 | 5.50 | 5.32 | 5.52 | 5.27 | - |
ZSM-5 | 5.20 | 5.24 | 5.34 | 5.71 | 5.10 | - |
Mean diameter (Å) | Mean radius (Å) | C.F.A. (Å2) | ||||
ZSM-5–CB | 5.43 | 2.71 | 23.12 | - | ||
ZSM-5 | 5.32 | 2.66 | 22.20 | - | ||
O–O distance (Å) | O11–O5 | O20–O18 | O21–O22 | O27–O33 | O28–O34 | ε |
ZSM-5–CB | 8.08 | 7.89 | 8.11 | 8.22 | 8.08 | 1.04 |
ZSM-5 | 8.19 | 8.35 | 7.98 | 8.13 | 7.76 | 1.08 |
Free diameter (Å) | O11–O5 | O20–O18 | O21–O22 | O27–O33 | O28–O34 | |
ZSM-5–CB | 5.38 | 5.19 | 5.41 | 5.52 | 5.38 | |
ZSM-5 | 5.49 | 5.65 | 5.28 | 5.43 | 5.06 | |
Mean diameter (Å) | Mean radius (Å) | C.F.A. (Å2) | ||||
ZSM-5–CB | 5.37 | 2.69 | 22.67 | |||
ZSM-5 | 5.38 | 2.69 | 22.74 | |||
Sinusoidal Channel | ||||||
O–O distance (Å) | O20–O15 | O24–O26 | O27–O2 | O28–O1 | O41–O46 | ε |
ZSM-5–CB | 8.08 | 7.87 | 7.76 | 8.16 | 8.69 | 1.12 |
ZSM-5 | 8.15 | 8.07 | 7.97 | 7.76 | 8.51 | 1.10 |
Free diameter (Å) | O20–O15 | O24–O26 | O27–O2 | O28–O1 | O41–O46 | |
ZSM-5–CB | 5.38 | 5.17 | 5.06 | 5.46 | 5.99 | |
ZSM-5 | 5.45 | 5.37 | 5.27 | 5.06 | 5.81 | |
Mean diameter (Å) | Mean radius (Å) | C.F.A. (Å2) | ||||
ZSM-5–CB | 5.41 | 2.71 | 23.01 | |||
ZSM-5 | 5.39 | 2.70 | 22.82 | |||
O–O distance (Å) | O17–O18 | O23–O25 | O30–O5 | O31–O4 | O44–O43 | ε |
ZSM-5–CB | 7.50 | 8.58 | 8.20 | 7.89 | 7.75 | 1.14 |
ZSM-5 | 7.30 | 8.31 | 8.32 | 8.05 | 7.95 | 1.14 |
Free diameter (Å) | O17–O18 | O23–O25 | O30–O5 | O31–O4 | O44–O43 | |
ZSM-5–CB | 4.80 | 5.88 | 5.50 | 5.19 | 5.05 | |
ZSM-5 | 4.60 | 5.61 | 5.62 | 5.35 | 5.25 | |
Mean diameter (Å) | Mean radius (Å) | C.F.A. (Å2) | ||||
ZSM-5–CB | 5.28 | 2.64 | 21.92 | |||
ZSM-5 | 5.29 | 2.64 | 21.93 |
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Pasti, L.; Rodeghero, E.; Beltrami, G.; Ardit, M.; Sarti, E.; Chenet, T.; Stevanin, C.; Martucci, A. Insights into Adsorption of Chlorobenzene in High Silica MFI and FAU Zeolites Gained from Chromatographic and Diffractometric Techniques. Minerals 2018, 8, 80. https://doi.org/10.3390/min8030080
Pasti L, Rodeghero E, Beltrami G, Ardit M, Sarti E, Chenet T, Stevanin C, Martucci A. Insights into Adsorption of Chlorobenzene in High Silica MFI and FAU Zeolites Gained from Chromatographic and Diffractometric Techniques. Minerals. 2018; 8(3):80. https://doi.org/10.3390/min8030080
Chicago/Turabian StylePasti, Luisa, Elisa Rodeghero, Giada Beltrami, Matteo Ardit, Elena Sarti, Tatiana Chenet, Claudia Stevanin, and Annalisa Martucci. 2018. "Insights into Adsorption of Chlorobenzene in High Silica MFI and FAU Zeolites Gained from Chromatographic and Diffractometric Techniques" Minerals 8, no. 3: 80. https://doi.org/10.3390/min8030080