Chinese Journal of Catalysis ›› 2021, Vol. 42 ›› Issue (9): 1468-1477.DOI: 10.1016/S1872-2067(20)63777-9
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Kaipeng Caoa,b, Dong Fana, Shu Zenga,b, Benhan Fana,b, Nan Chena,b, Mingbin Gaoa,b, Dali Zhua,b, Linying Wanga, Peng Tiana,*(), Zhongmin Liua,b,#()
Received:
2020-11-19
Accepted:
2021-02-02
Online:
2021-09-18
Published:
2021-05-16
Contact:
Peng Tian,Zhongmin Liu
About author:
# E-mail: liuzm@dicp.ac.cnSupported by:
Kaipeng Cao, Dong Fan, Shu Zeng, Benhan Fan, Nan Chen, Mingbin Gao, Dali Zhu, Linying Wang, Peng Tian, Zhongmin Liu. Organic-free synthesis of MOR nanoassemblies with excellent DME carbonylation performance[J]. Chinese Journal of Catalysis, 2021, 42(9): 1468-1477.
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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63777-9
Sample | Gel molar composition a | Time (h) | Product | Solid yield c (%) | ||||
---|---|---|---|---|---|---|---|---|
SiO2 | Al2O3 | Na2O | H2O | Phase | SAR b | |||
I-5.3 | 1.0 | 0.08 | 0.13 | 15 | 30 | MOR | 5.3 (5.2) | 88 |
I-7.0 | 1.0 | 0.06 | 0.13 | 15 | 30 | MOR | 7.0 (7.3) | 84 |
I-9.4 | 1.0 | 0.05 | 0.08 | 15 | 30 | MOR | 9.4 (9.8) | 94 |
I-11.9 | 1.0 | 0.04 | 0.08 | 15 | 30 | MOR+U e | 11.9 | — |
I-9.4-N d | 1.0 | 0.05 | 0.08 | 15 | 110 | MOR+MFI | — | — |
I-9.4-H | 1.0 | 0.05 | 0.13 | 15 | 13 | MOR | 8.1 | 81 |
I-9.4-L | 1.0 | 0.05 | 0.067 | 15 | 110 | MOR+Amorphous | — | — |
Table 1 Synthesis conditions, product SAR and solid yields of MOR zeolites.
Sample | Gel molar composition a | Time (h) | Product | Solid yield c (%) | ||||
---|---|---|---|---|---|---|---|---|
SiO2 | Al2O3 | Na2O | H2O | Phase | SAR b | |||
I-5.3 | 1.0 | 0.08 | 0.13 | 15 | 30 | MOR | 5.3 (5.2) | 88 |
I-7.0 | 1.0 | 0.06 | 0.13 | 15 | 30 | MOR | 7.0 (7.3) | 84 |
I-9.4 | 1.0 | 0.05 | 0.08 | 15 | 30 | MOR | 9.4 (9.8) | 94 |
I-11.9 | 1.0 | 0.04 | 0.08 | 15 | 30 | MOR+U e | 11.9 | — |
I-9.4-N d | 1.0 | 0.05 | 0.08 | 15 | 110 | MOR+MFI | — | — |
I-9.4-H | 1.0 | 0.05 | 0.13 | 15 | 13 | MOR | 8.1 | 81 |
I-9.4-L | 1.0 | 0.05 | 0.067 | 15 | 110 | MOR+Amorphous | — | — |
Fig. 1. (a) XRD patterns of the as-synthesized MOR samples; (b) N2 adsorption-desorption isotherms of the H-MOR samples (the isotherms of I-7.0 and I-9.4 are offset by 50 and 100 cm3/g, respectively); (c-e) SEM images of the as-synthesized samples. The insets in (e) show the HRTEM image of sample I-9.4. (f) TEM image of sample I-9.4, corresponding SAED pattern viewed along the [001] direction and a schematic to illustrate the 12-MR channel system.
Fig. 2. (a) 27Al, (b) 29Si and (c) 23Na MAS NMR spectra of the as-synthesized samples. The samples were dehydrated at 400 °C for 12 h in vacuum before 23Na MAS NMR measurement.
Sample | Surface area a (m2/g) | Pore volume b (cm3/g) | |||||
---|---|---|---|---|---|---|---|
SBET | Smicro | Sext | Vtotal | Vmicro | Vmeso | ||
I-5.3 | 418 | 374 | 44 | 0.24 | 0.18 | 0.06 | |
I-7.0 | 438 | 392 | 47 | 0.24 | 0.19 | 0.05 | |
I-9.4 | 428 | 375 | 53 | 0.24 | 0.18 | 0.06 |
Table 2 Textural properties of the samples.
Sample | Surface area a (m2/g) | Pore volume b (cm3/g) | |||||
---|---|---|---|---|---|---|---|
SBET | Smicro | Sext | Vtotal | Vmicro | Vmeso | ||
I-5.3 | 418 | 374 | 44 | 0.24 | 0.18 | 0.06 | |
I-7.0 | 438 | 392 | 47 | 0.24 | 0.19 | 0.05 | |
I-9.4 | 428 | 375 | 53 | 0.24 | 0.18 | 0.06 |
Fig. 3. Acidity of the H-MOR samples. (a) NH3-TPD profiles; (b) NH3-adsorption FTIR spectra; (c) FTIR spectra of H-MOR; (d) Deconvoluted bands corresponding to the acid hydroxyls in the 12-MR channels (HF) and the side pockets (LF). The numbers in (d) refer to the percentage of Br?nsted acids in the side pockets.
Sample | NH3-TPD (mmol/g) | NH3-FTIR b (mmol/g) | ||||||||
---|---|---|---|---|---|---|---|---|---|---|
Weak | Moderate | Strong | M+S a | BAS | LAS | B+L c | BAS/LAS | |||
I-5.3 | 1.03 | 0.4 | 0.79 | 1.19 | 1.01 | 0.17 | 1.18 | 5.82 | ||
I-7.0 | 0.97 | 0.32 | 0.82 | 1.14 | 0.83 | 0.15 | 0.98 | 5.53 | ||
I-9.4 | 0.77 | 0.26 | 0.89 | 1.15 | 0.91 | 0.08 | 0.99 | 10.87 |
Table 3 Acid amounts of the H-MOR samples based on NH3-TPD and NH3-FTIR.
Sample | NH3-TPD (mmol/g) | NH3-FTIR b (mmol/g) | ||||||||
---|---|---|---|---|---|---|---|---|---|---|
Weak | Moderate | Strong | M+S a | BAS | LAS | B+L c | BAS/LAS | |||
I-5.3 | 1.03 | 0.4 | 0.79 | 1.19 | 1.01 | 0.17 | 1.18 | 5.82 | ||
I-7.0 | 0.97 | 0.32 | 0.82 | 1.14 | 0.83 | 0.15 | 0.98 | 5.53 | ||
I-9.4 | 0.77 | 0.26 | 0.89 | 1.15 | 0.91 | 0.08 | 0.99 | 10.87 |
Fig. 4. ν(OH) vibration region of the H-MOR samples (a) before and after pyridine adsorption at 150 °C, (b) after pyridine adsorption and desorption at 300 °C.
Fig. 5. (a) Uptake rate of MAc in pyridine-modified H-MOR measured by IGA (50 °C, 1 mbar). (b) Initial uptake rate. The scatters represent the experimental data while dash lines are fitting results by Eq. (2).
Fig. 6. (a) DME conversion during DME carbonylation over pyridine-modified H-MOR catalysts. (b) Hydrocarbon by-products (HCx) selectivity. Reaction conditions: 200 °C, 2 MPa, GHSV = 3600 mL/g/h. DME/CO/N2 = 5/35/60.
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