Journal of Inorganic Materials ›› 2016, Vol. 31 ›› Issue (12): 1355-1362.DOI: 10.15541/jim20160151
• Orginal Article • Previous Articles Next Articles
LI Yu-Ping1, SUN Cui-Juan1, JIA Kun1, ZHANG Yi1, LI Xiao-Feng2, DOU Tao2, 3
Received:
2016-03-15
Revised:
2016-04-22
Published:
2016-12-16
Online:
2016-11-23
Supported by:
CLC Number:
LI Yu-Ping, SUN Cui-Juan, JIA Kun, ZHANG Yi, LI Xiao-Feng, DOU Tao. Soft Template-directed Hierarchical Mordenites and Their Performance in Benzylation of Benzene with Benzyl Alcohol[J]. Journal of Inorganic Materials, 2016, 31(12): 1355-1362.
Samples | a Si/Al | b SBET / (m2·g-1) | Smicro / (m2·g-1) | c Sext / (m2·g-1) | d Vtotal / (cm3·g-1) | Vmicro / (cm3·g-1) | eVmeso/ (cm3·g-1) |
---|---|---|---|---|---|---|---|
CM | 6.0 | 318 | 303 | 15 | 0.14 | 0.12 | 0.02 |
HM-0.025 | 6.2 | 333 | 286 | 47 | 0.21 | 0.13 | 0.09 |
HM-0.05 | 6.9 | 366 | 291 | 75 | 0.26 | 0.11 | 0.14 |
HM-0.075 | 7.5 | 362 | 252 | 110 | 0.27 | 0.09 | 0.18 |
Table 1 Pore structure parameters of mordenite samples
Samples | a Si/Al | b SBET / (m2·g-1) | Smicro / (m2·g-1) | c Sext / (m2·g-1) | d Vtotal / (cm3·g-1) | Vmicro / (cm3·g-1) | eVmeso/ (cm3·g-1) |
---|---|---|---|---|---|---|---|
CM | 6.0 | 318 | 303 | 15 | 0.14 | 0.12 | 0.02 |
HM-0.025 | 6.2 | 333 | 286 | 47 | 0.21 | 0.13 | 0.09 |
HM-0.05 | 6.9 | 366 | 291 | 75 | 0.26 | 0.11 | 0.14 |
HM-0.075 | 7.5 | 362 | 252 | 110 | 0.27 | 0.09 | 0.18 |
Fig. 6 Thermogravimetric (TG, a) and derivative thermogravimetric (DTG, b) curves of mordenite samples synthesized with different amounts of C18-6-6Br2
Sample | Acid amount/(mmol·g-1) | Peak temperature/℃ | |||
---|---|---|---|---|---|
Total | Weak | Strong | Weak | Strong | |
CM | 0.855 | 0.463 | 0.392 | 224 | 528 |
HM-0.025 | 1.026 | 0.499 | 0.527 | 219 | 513 |
HM-0.05 | 1.094 | 0.391 | 0.703 | 220 | 525 |
HM-0.075 | 0.952 | 0.320 | 0.632 | 218 | 519 |
Table 2 Acidity data of all mordenite samples
Sample | Acid amount/(mmol·g-1) | Peak temperature/℃ | |||
---|---|---|---|---|---|
Total | Weak | Strong | Weak | Strong | |
CM | 0.855 | 0.463 | 0.392 | 224 | 528 |
HM-0.025 | 1.026 | 0.499 | 0.527 | 219 | 513 |
HM-0.05 | 1.094 | 0.391 | 0.703 | 220 | 525 |
HM-0.075 | 0.952 | 0.320 | 0.632 | 218 | 519 |
Catalysts | Conversion of BA/ % | Selectivity/ % | Yield / % | Ka × 103/ min-1 | ||
---|---|---|---|---|---|---|
DPM | DBE | DPM | DBE | |||
CMOR | 39.06 | 89.25 | 10.75 | 34.86 | 4.20 | 3.32 |
HMOR-0.025 | 76.84 | 93.63 | 6.37 | 71.95 | 4.89 | 8.50 |
HMOR-0.05 | 95.08 | 95.74 | 4.26 | 91.03 | 4.05 | 19.02 |
HMOR-0.075 | 97.33 | 97.15 | 2.85 | 94.56 | 2.77 | 22.48 |
Table 3 Benzylation of benzene with benzyl alcohol over mordenite samples a
Catalysts | Conversion of BA/ % | Selectivity/ % | Yield / % | Ka × 103/ min-1 | ||
---|---|---|---|---|---|---|
DPM | DBE | DPM | DBE | |||
CMOR | 39.06 | 89.25 | 10.75 | 34.86 | 4.20 | 3.32 |
HMOR-0.025 | 76.84 | 93.63 | 6.37 | 71.95 | 4.89 | 8.50 |
HMOR-0.05 | 95.08 | 95.74 | 4.26 | 91.03 | 4.05 | 19.02 |
HMOR-0.075 | 97.33 | 97.15 | 2.85 | 94.56 | 2.77 | 22.48 |
[1] | 徐如人, 庞文琴, 于吉红, 等.分子筛与多孔材料化学. 北京, 科学出版社, 2004: 34-39. |
[2] | CHEN L H, LI X Y, ROOKE J C,et al.. Hierarchically structured zeolites: synthesis, mass transport properties and applications. J. Mater. Chem., 2012, 22(34): 17381-17403. |
[3] | NA K, CHOI M, RYOO R.Recent advances in the synthesis of hierarchically nanoporous zeolites.Micropor. Mesopor. Mater., 2013, 166: 3-19. |
[4] | LI K H, VALLA J, GARCIA-MARTINEZ J.Realizing the commercial potential of hierarchical zeolites: new opportunities in catalytic cracking. ChemCatChem, 2014, 6(1): 46-66. |
[5] | ZHOU J, HUA Z L, SHI J L, et al.Synthesis of a hierarchical micro/mesoporous structure by steam-assisted post-crystallization.Chem. Eur. J., 2009, 15(47): 12949-12954. |
[6] | BOVERI M, MÁRQUEZ-ÁLVAREZ C, LABORDE M Á,et al.. Steam and acid dealumination of mordenite characterization and influence on the catalytic performance in linear alkylbenzene synthesis. Catal Today., 2006, 114(2/3): 217-225. |
[7] | VERBOEKEND D, PÉREZ-RAMÍREZ J. Desilication mechanism revisited: highly mesoporous all-silica zeolites enabled through pore-directing agents.Chem. Eur. J., 2011, 17(4): 1137-1147. |
[8] | GROEN J C, EFFER L A A, MOULIJN J A,et al.. PMechanism of hierarchical porosity development in MFI zeolites by desilication: the role of aluminium as a pore-directing agent .Chem. Eur. J. 2005, 11(17): 4983-4994. |
[9] | BOISEN A, SCHMIDT I, CARLSSON A,et al.. TEM stereo imaging of mesoporous zeolite single crystals. Chem. Commun., 2003, 3(8): 958-959. |
[10] | JACOBSEN C J H, MADSEN C, HOUZVICKA J,et al.. Mesoporous zeolite single crystals. J. Am. Chem. Soc., 2000, 122(29): 7116-7117. |
[11] | CHOI M, NA K, KIM J,et al.. Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts. Nature, 2009, 461(7261): 246-249. |
[12] | LIU B Y, TAN Y Z, REN Y Q,et al.. Fabrication of a hierarchically structured beta zeolite by a dual-porogenic surfactant. J. Mater. Chem., 2012, 22(35): 18631-18638. |
[13] | LIU B Y, REN Y Q, DUAN Q Q,et al.. Facile synthesis of mesoporous aluminosilicates constructed with crystalline microporous frameworks. Appl. Surf. Sci., 2013, 279: 55-61. |
[14] | CHOI M, CHO H S, SRIVASTAVA R,et al.. Amphiphilic organosilane-directed synthesis of crystalline zeolite with tunable mesoporosity. Nat. Mater., 2006, 5(9): 718-723. |
[15] | NA K, CHOI M, PARK W,et al..Pillared MFI zeolite nanosheets of a single-unit-cell thickness. J. Am. Chem. Soc., 2010, 132(12): 4169-4177. |
[16] | WU L L, DEGIRMENCI V,MAGUSIN P C M M,et al.. Mesoporous SSZ-13 zeolite prepared by a dual-template method with improved performance in the methanol-to-olefins reaction. J. Catal., 2013, 298: 27-40. |
[17] | WU L L, DEGIRMENCI V, MAGUSIN P C M M,et al.. Dual template synthesis of a highly mesoporous SSZ-13 zeolite with improved stability in the methanol-to-olefins reaction. Chem. Commun., 2012, 48(76): 9492-9494. |
[18] | NA K, JO C, KIM J,et al.. Directing zeolite structures into hierarchically nanoporous architectures . Science, 2011, 333(6040): 328-332. |
[19] | XIAO F S, WANG L F, YIN C Y,et al.. Catalytic properties of hierarchical mesoporous zeolites templated with a mixture of small organic ammonium salts and mesoscale cationic polymers . Angew. Chem., 2006, 118(19): 3162-3165. |
[20] | LI Y P, SUN C J, FAN W B,et al.. One-pot synthesis of hierarchical mordenite and its performance in the benzylation of benzene with benzyl alcohol . J. Mater. Sci., 2015, 50(14): 5059-5067. |
[21] | BAERLOCHER C, MEIER W M, OLSON D H.Atlas of Zeolite Framework Types, fifth Ed.Amsterdam, Elsevier, 2001. |
[22] | GROEN J C, SANO T, MOULIJN J A,et al.. Alkaline-mediated mesoporous mordenite zeolites for acid-catalyzed conversions . J. Catal., 2007, 251(1): 21-27. |
[23] | TAO Y S, KANOH H, ABRAMS L,et al.. Mesopore-modified zeolites: preparation, characterization, and applications . Chem. Rev., 2006, 106(3): 896-910. |
[24] | TREACY M M J, HIGGINS J B, VON B R. Collection of Simulated XRD Powder Patterns for Zeolite. 3rd Revised Ed . New York,Elsevier, 1996. |
[25] | SOHN J R, DECANIO S J, LUNSFORD J H,et al.. Determination of framework aluminium content in dealuminated Y-type zeoLites: a comparison based on unit cell size and wavenumber of i.r. bands . Zeolites, 1986, 6(3): 225-227. |
[26] | ZHANG Q, LIU S J, YU S H.Recent advances in oriented attachment growth and synthesis of functional materials: concept, evidence, mechanism, and future.J. Mater. Chem., 2009, 19: 191-207. |
[27] | CHEN J, HUA W M, XIAO Y,et al.. Tailoring the structure of hierarchically porous zeolite Beta through modified orientated attachment growth in a dry Gel system . Chem. Eur. J., 2014, 20: 14744-14755. |
[28] | OCCELLI M L, BIZ S, AUROUX A,et al.. Effects of the nature of the aluminum source on the acidic properties of some mesostructured materials . Micropor Mesopor Mater., 1998, 26(1/2/3): 193-213. |
[29] | HU S, SHAN J, ZHANG Q, et al. Selective formation of propylene from methanol over high-silica nanosheets of MFI zeolite. Appl. Catal. A, 2012,445-446: 215-220. |
[30] | LENG K Y, WANG Y, HOU C M,et al.. Enhancement of catalytic performance in the benzylation of benzene with benzyl alcohol over hierarchical mordenite . J. Catal., 2013, 306: 100-108. |
[31] | PENG P, ZHANG Z Q, WANG Y H,et al.. Hierarchical molecular sieves: synthesis and catalytic applications . Progress in Chemistry, 2013, 25(12): 2028-2037. |
[32] | SUN Y Y, PRINS R.Friedel-crafts alkylations over hierarchical zeolite catalysts.Appl. Catal. A, 2008, 336(1/2): 11-16. |
[33] | CHOUDHARY V R, JANA S K, PATIL N S,et al.. Friedel-Crafts type benzylation and benzoylation of aromatic compounds over Hβ zeolite modified by oxides or chlorides of gallium and indium. Micropor. Mesopor. Mater., 2003, 57(1): 21-35. |
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