CN107497480B - A kind of synthetic method of Jie's mesoporous-microporous composite molecular sieve catalyst - Google Patents
A kind of synthetic method of Jie's mesoporous-microporous composite molecular sieve catalyst Download PDFInfo
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- CN107497480B CN107497480B CN201710763658.1A CN201710763658A CN107497480B CN 107497480 B CN107497480 B CN 107497480B CN 201710763658 A CN201710763658 A CN 201710763658A CN 107497480 B CN107497480 B CN 107497480B
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- molecular sieve
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- 239000002808 molecular sieve Substances 0.000 title claims abstract description 32
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 title claims abstract description 32
- 239000002131 composite material Substances 0.000 title claims abstract description 24
- 239000003054 catalyst Substances 0.000 title claims abstract description 23
- 238000010189 synthetic method Methods 0.000 title claims abstract description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 22
- 238000000034 method Methods 0.000 claims abstract description 21
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims abstract description 13
- 229910052710 silicon Inorganic materials 0.000 claims abstract description 13
- 239000010703 silicon Substances 0.000 claims abstract description 13
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 8
- 239000003513 alkali Substances 0.000 claims abstract description 7
- 238000002425 crystallisation Methods 0.000 claims abstract description 7
- 230000008025 crystallization Effects 0.000 claims abstract description 7
- 238000003786 synthesis reaction Methods 0.000 claims abstract description 7
- 230000032683 aging Effects 0.000 claims abstract description 6
- 238000005119 centrifugation Methods 0.000 claims abstract description 6
- 239000000701 coagulant Substances 0.000 claims abstract description 6
- 238000004090 dissolution Methods 0.000 claims abstract description 6
- 239000007788 liquid Substances 0.000 claims abstract description 6
- 229910001220 stainless steel Inorganic materials 0.000 claims abstract description 6
- 239000010935 stainless steel Substances 0.000 claims abstract description 6
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 12
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 12
- 229910052782 aluminium Inorganic materials 0.000 claims description 9
- 239000004411 aluminium Substances 0.000 claims description 9
- NTHWMYGWWRZVTN-UHFFFAOYSA-N sodium silicate Chemical compound [Na+].[Na+].[O-][Si]([O-])=O NTHWMYGWWRZVTN-UHFFFAOYSA-N 0.000 claims description 8
- 239000003795 chemical substances by application Substances 0.000 claims description 6
- -1 tert-butyl aluminium Chemical compound 0.000 claims description 6
- 239000007787 solid Substances 0.000 claims description 5
- 238000010792 warming Methods 0.000 claims description 5
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 4
- 239000004115 Sodium Silicate Substances 0.000 claims description 4
- BOTDANWDWHJENH-UHFFFAOYSA-N Tetraethyl orthosilicate Chemical compound CCO[Si](OCC)(OCC)OCC BOTDANWDWHJENH-UHFFFAOYSA-N 0.000 claims description 4
- ANBBXQWFNXMHLD-UHFFFAOYSA-N aluminum;sodium;oxygen(2-) Chemical group [O-2].[O-2].[Na+].[Al+3] ANBBXQWFNXMHLD-UHFFFAOYSA-N 0.000 claims description 4
- 239000000908 ammonium hydroxide Substances 0.000 claims description 4
- 229910001388 sodium aluminate Inorganic materials 0.000 claims description 4
- 235000019795 sodium metasilicate Nutrition 0.000 claims description 4
- 229910052911 sodium silicate Inorganic materials 0.000 claims description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 3
- 239000000017 hydrogel Substances 0.000 claims description 3
- 239000000377 silicon dioxide Substances 0.000 claims description 3
- XXZNHVPIQYYRCG-UHFFFAOYSA-N trihydroxy(propoxy)silane Chemical compound CCCO[Si](O)(O)O XXZNHVPIQYYRCG-UHFFFAOYSA-N 0.000 claims description 3
- DIZPMCHEQGEION-UHFFFAOYSA-H aluminium sulfate (anhydrous) Chemical compound [Al+3].[Al+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O DIZPMCHEQGEION-UHFFFAOYSA-H 0.000 claims description 2
- 239000000463 material Substances 0.000 abstract description 10
- 239000011148 porous material Substances 0.000 abstract description 6
- 238000003756 stirring Methods 0.000 abstract description 4
- 239000002253 acid Substances 0.000 abstract description 3
- 230000003197 catalytic effect Effects 0.000 abstract description 3
- 238000004519 manufacturing process Methods 0.000 abstract description 3
- 238000000926 separation method Methods 0.000 abstract description 3
- 229910021536 Zeolite Inorganic materials 0.000 abstract description 2
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 abstract description 2
- 239000012847 fine chemical Substances 0.000 abstract description 2
- 239000010457 zeolite Substances 0.000 abstract description 2
- 238000005406 washing Methods 0.000 abstract 1
- HUMNYLRZRPPJDN-UHFFFAOYSA-N benzaldehyde Chemical compound O=CC1=CC=CC=C1 HUMNYLRZRPPJDN-UHFFFAOYSA-N 0.000 description 6
- 238000006243 chemical reaction Methods 0.000 description 6
- 238000002360 preparation method Methods 0.000 description 6
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 4
- 235000019353 potassium silicate Nutrition 0.000 description 4
- ZWVHTXAYIKBMEE-UHFFFAOYSA-N 2-hydroxyacetophenone Chemical compound OCC(=O)C1=CC=CC=C1 ZWVHTXAYIKBMEE-UHFFFAOYSA-N 0.000 description 3
- 238000005882 aldol condensation reaction Methods 0.000 description 3
- 238000006555 catalytic reaction Methods 0.000 description 3
- 229930003949 flavanone Natural products 0.000 description 3
- 235000011981 flavanones Nutrition 0.000 description 3
- 150000002208 flavanones Chemical class 0.000 description 3
- QNGNSVIICDLXHT-UHFFFAOYSA-N para-ethylbenzaldehyde Natural products CCC1=CC=C(C=O)C=C1 QNGNSVIICDLXHT-UHFFFAOYSA-N 0.000 description 3
- SMZOGRDCAXLAAR-UHFFFAOYSA-N aluminium isopropoxide Chemical compound [Al+3].CC(C)[O-].CC(C)[O-].CC(C)[O-] SMZOGRDCAXLAAR-UHFFFAOYSA-N 0.000 description 2
- 210000003850 cellular structure Anatomy 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 239000000376 reactant Substances 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 229920002521 macromolecule Polymers 0.000 description 1
- 239000013335 mesoporous material Substances 0.000 description 1
- 238000002336 sorption--desorption measurement Methods 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/60—Catalysts, in general, characterised by their form or physical properties characterised by their surface properties or porosity
- B01J35/64—Pore diameter
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C45/00—Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds
- C07C45/45—Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by condensation
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07D—HETEROCYCLIC COMPOUNDS
- C07D311/00—Heterocyclic compounds containing six-membered rings having one oxygen atom as the only hetero atom, condensed with other rings
- C07D311/02—Heterocyclic compounds containing six-membered rings having one oxygen atom as the only hetero atom, condensed with other rings ortho- or peri-condensed with carbocyclic rings or ring systems
- C07D311/04—Benzo[b]pyrans, not hydrogenated in the carbocyclic ring
- C07D311/22—Benzo[b]pyrans, not hydrogenated in the carbocyclic ring with oxygen or sulfur atoms directly attached in position 4
- C07D311/26—Benzo[b]pyrans, not hydrogenated in the carbocyclic ring with oxygen or sulfur atoms directly attached in position 4 with aromatic rings attached in position 2 or 3
- C07D311/28—Benzo[b]pyrans, not hydrogenated in the carbocyclic ring with oxygen or sulfur atoms directly attached in position 4 with aromatic rings attached in position 2 or 3 with aromatic rings attached in position 2 only
- C07D311/32—2,3-Dihydro derivatives, e.g. flavanones
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- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Crystallography & Structural Chemistry (AREA)
- Silicates, Zeolites, And Molecular Sieves (AREA)
- Catalysts (AREA)
Abstract
The invention discloses a kind of synthetic method of Jie's mesoporous-microporous composite molecular sieve catalyst, steps are as follows: by template [C22H45‑N+(CH3)2‑C6H12‑N(CH3)2]Br‑, into the water, heat up, dissolution is added silicon source, alkali and silicon source, is down to room temperature, stirs, and the coagulant liquid after obtaining aging is transferred in stainless steel water thermal synthesis reaction kettle and seals, crystallization, centrifugation, washing, it is dry, calcine to get；The present invention is at low cost, and technical process is simple, is suitble to industrialized production.Prepared catalyst has the mesoporous order of height, sufficiently combines the high degree of hydrothermal stability of micro porous molecular sieve, improves mechanical stability, it simultaneously can be in conjunction with the acid advantage of micro-pore zeolite molecular sieve, with good catalytic activity, it is suitable for petrochemical industry, Field of Fine Chemicals.This material is hierarchical porous structure, while having MFI micropore and MCM-41 meso-hole structure, can be used for the fields such as adsorbing separation.
Description
Technical field
The invention belongs to porous material and catalytic fields, more particularly to a kind of conjunction of Jie's mesoporous-microporous composite molecular sieve catalyst
At method.
Background technique
Porous material is since it is with specific cellular structure, biggish specific surface area, preferable hydrothermal stability by
Extensive concern.Currently, porous molecular screen catalysis material is divided into two classes according to its duct size, mesoporous (2-50nm) molecular sieve is urged
Change material and micropore (< 2nm).Microporous molecular sieve catalyst has specific sour site, has stronger Acidity, crystallization
Skeleton there is stronger hydrothermal stability, while it can be provided with unique pore structure and basket structure for reactant molecule
The duct of specific dispersion, absorption, catalysis.However, the aperture of micro porous molecular sieve is smaller, macromolecular is limited in expansion wherein
It dissipates, duct is relatively narrow, makes macromolecule reactant that can not make full use of the internal surface area of poromerics, limits micro porous molecular sieve
Application of the catalyst in bulky molecular catalysis field.Meso-porous molecular sieve material has more uniform aperture and in a certain range may be used
It adjusts, higher specific surface area, makes macromolecular that there is good diffusion.However, mesoporous material due to its skeleton have nothing
Stereotyped structure, hydrothermal stability is poor, acid weaker disadvantage.
Mesopore and micropore composite material be there is mesoporous and micropore porous composite molecular screen material simultaneously, while have it is mesoporous and
The advantages of micro porous molecular sieve, has received widespread attention.There are many methods to synthesize Jie's mesoporous-microporous composite molecular sieve at present, including
Skeleton removing and single template agent method.Due to there is preparation in preparation Jie's mesoporous-microporous composite molecular sieve materials process middle skeleton removal method
Complex process hardly results in the shortcomings that molecular screen material of uniform pore-size distribution and is restricted its application.Single template
Method mainly includes soft template method and hard mould agent method, and wherein hard mould agent method preparation process is complicated, and obtained material is de-
Except that can damage to structure during hard mould agent, application is restricted.Therefore, at present soft template method due to its preparation
Simple process, variable is easily controllable and is favored extensively.But presently, there are soft template method, it is expensive.
Summary of the invention
The purpose of the present invention is overcoming synthesis cost of the existing technology expensive, the deficiency of process complexity is provided
A kind of preparation process is simple, the synthetic method of cheap Jie's mesoporous-microporous composite molecular sieve catalyst.
A kind of synthetic method of Jie's mesoporous-microporous composite molecular sieve catalyst, includes the following steps: template [C22H45-N+
(CH3)2-C6H12-N(CH3)2]Br-, into the water, it is warming up to 50-70 DEG C, dissolution is added silicon source, alkali and silicon source, is cooled to room
Temperature stirs 1-3 hours, and the coagulant liquid after obtaining aging is transferred in stainless steel water thermal synthesis reaction kettle and seals, in 100-160
Crystallization 8-14 days under the conditions of DEG C, centrifugation, solid are washed with water, dry, calcine, and obtain Jie's mesoporous-microporous composite molecular sieve catalyst；
Template [the C22H45-N+(CH3)2-C6H12-N(CH3)2]Br-, silicon source, the molar ratio of alkali and silicon source be 6:50-
70:10-40:0.1-3 template [the C22H45-N+(CH3)2-C6H12-N(CH3)2]Br-Mass ratio with water is 1:160-
230。
Preferably, silicon source is tetraethyl orthosilicate, waterglass, Silica hydrogel, sodium metasilicate or positive silicic acid propyl ester.
Preferably, alkali is sodium hydroxide, potassium hydroxide or ammonium hydroxide.
Preferably, silicon source is sodium aluminate, aluminum sulfate, tert-butyl aluminium or aluminium isopropoxide.
Advantages of the present invention:
Method of the invention reduces production cost, and technical process is simple and effective, is suitble to industrialized production.Prepared Jie
Mesoporous-microporous composite molecular sieve catalyst has the mesoporous order of height, sufficiently combines the height hydrothermally stable of micro porous molecular sieve
Property, the hydrothermal stability and mechanical stability of the material are improved, while the acid advantage of micro-pore zeolite molecular sieve can be combined,
Good catalytic activity is made it have, petrochemical industry, the fields such as preparation of fine chemicals can be suitable for.This material is multistage
Pore structure, while there is MFI micropore and MCM-41 meso-hole structure, special cellular structure allows to be applied to adsorbing separation
Equal separation fields.
Detailed description of the invention
Fig. 1 is the XRD diagram of Jie's mesoporous-microporous composite molecular sieve catalyst.
Fig. 2 is the N of Jie's mesoporous-microporous composite molecular sieve catalyst2Adsorption/desorption curve figure.
Fig. 3 is that the SEM of Jie's mesoporous-microporous composite molecular sieve catalyst schemes.
Fig. 4 is that the TEM of Jie's mesoporous-microporous composite molecular sieve catalyst schemes.
Specific embodiment
Below by specific embodiment, the present invention is further illustrated.
Embodiment 1
A kind of synthetic method of Jie's mesoporous-microporous composite molecular sieve catalyst, includes the following steps: template [C22H45-N+
(CH3)2-C6H12-N(CH3)2]Br-Into the water, 60 DEG C are warming up to, tetraethyl orthosilicate, sodium hydroxide and sulfuric acid is added in dissolution
Aluminium is cooled to room temperature, stirs 2 hours, and the coagulant liquid after obtaining aging is transferred in stainless steel water thermal synthesis reaction kettle and seals,
The crystallization 11 days under the conditions of 130 DEG C, centrifugation, solid is washed with water, dries, 550 DEG C calcine 6 hours, obtain compound point of Jie's micropore
Sub- sieve catalyst；
Template [the C22H45-N+(CH3)2-C6H12-N(CH3)2]Br-, tetraethyl orthosilicate, sodium hydroxide and sulfuric acid
The molar ratio of aluminium is 6:60:25:2, the template [C22H45-N+(CH3)2-C6H12-N(CH3)2]Br-Mass ratio with water is
1:200；See Fig. 1, Fig. 2, Fig. 3, Fig. 4.
The Aldol condensation reaction of flavanones and 2- hydroxylated chalcone is generated for benzaldehyde and the reaction of 2- hydroxy acetophenone, instead
Answering conversion ratio is 85.2%.
Embodiment 2
A kind of synthetic method of Jie's mesoporous-microporous composite molecular sieve catalyst, includes the following steps: template [C22H45-N+
(CH3)2-C6H12-N(CH3)2]Br-Into the water, 50 DEG C are warming up to, sodium metasilicate, potassium hydroxide and sodium aluminate, drop is added in dissolution
It warms to room temperature, stirs 3 hours, the coagulant liquid after obtaining aging is transferred in stainless steel water thermal synthesis reaction kettle and seals, 100
Crystallization 14 days under the conditions of DEG C, centrifugation, solid is washed with water, dries, 550 DEG C calcine 6 hours, obtain Jie's mesoporous-microporous composite molecular sieve and urge
Agent；
Template [the C22H45-N+(CH3)2-C6H12-N(CH3)2]Br-, sodium metasilicate, potassium hydroxide and sodium aluminate rub
You are than being the 6:50:10:0.1, [C22H45-N+(CH3)2-C6H12-N(CH3)2]Br-Mass ratio with water is 1:160.
The Aldol condensation reaction of flavanones and 2- hydroxylated chalcone is generated for benzaldehyde and the reaction of 2- hydroxy acetophenone, instead
Answering conversion ratio is 86.5%.
Embodiment 3
A kind of synthetic method of Jie's mesoporous-microporous composite molecular sieve catalyst, includes the following steps: template [C22H45-N+
(CH3)2-C6H12-N(CH3)2]Br-Into the water, 70 DEG C are warming up to, waterglass, ammonium hydroxide and tert-butyl aluminium is added in dissolution,
It is cooled to room temperature, is stirred 1 hour, the coagulant liquid after obtaining aging is transferred in stainless steel water thermal synthesis reaction kettle and seals,
Crystallization 8 days under the conditions of 160 DEG C, centrifugation, solid is washed with water, dries, 550 DEG C calcine 6 hours, obtain Jie's mesoporous-microporous composite molecular sieve
Catalyst；
Template [the C22H45-N+(CH3)2-C6H12-N(CH3)2]Br-, waterglass, ammonium hydroxide and tert-butyl aluminium
Molar ratio is 6:70:40:3, the template [C22H45-N+(CH3)2-C6H12-N(CH3)2]Br-Mass ratio with water is 1:
230。
The Aldol condensation reaction of flavanones and 2- hydroxylated chalcone is generated for benzaldehyde and the reaction of 2- hydroxy acetophenone, instead
Answering conversion ratio is 87.5%.
The waterglass of the present embodiment is substituted with Silica hydrogel or positive silicic acid propyl ester respectively, other same the present embodiment prepare one kind
Jie's mesoporous-microporous composite molecular sieve catalyst.
The tert-butyl aluminium of the present embodiment is substituted with aluminium isopropoxide, other same the present embodiment prepare a kind of compound point of Jie's micropore
Sub- sieve catalyst.
Claims (4)
1. a kind of synthetic method of Jie's mesoporous-microporous composite molecular sieve catalyst, it is characterized in that including the following steps: template
[C22H45-N+(CH3)2-C6H12-N(CH3)2]Br-, into the water, it being warming up to 50-70 DEG C, silicon source, alkali and silicon source is added in dissolution,
It is cooled to room temperature, is stirred 1-3 hours, the coagulant liquid after obtaining aging is transferred in stainless steel water thermal synthesis reaction kettle and seals,
Crystallization 8-14 days under the conditions of 100-160 DEG C, centrifugation, solid are washed with water, dry, calcine, obtain Jie's mesoporous-microporous composite molecular sieve and urge
Agent；
Template [the C22H45-N+(CH3)2-C6H12-N(CH3)2]Br-, silicon source, the molar ratio of alkali and silicon source be 6:50-70:
10-40:0.1-3 template [the C22H45-N+(CH3)2-C6H12-N(CH3)2]Br-Mass ratio with water is 1:160-230.
2. according to the method described in claim 1, it is characterized in that the silicon source be tetraethyl orthosilicate, Silica hydrogel, sodium metasilicate or
Positive silicic acid propyl ester.
3. according to the method described in claim 1, it is characterized in that the alkali is sodium hydroxide, potassium hydroxide or ammonium hydroxide.
4. according to the method described in claim 1, it is characterized in that source of aluminium is sodium aluminate, aluminum sulfate, tert-butyl aluminium or isopropyl
Aluminium alcoholates.
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Citations (3)
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|---|---|---|---|---|
| CN1762806A (en) * | 2004-10-21 | 2006-04-26 | 中国石油天然气股份有限公司 | Method for mesoporous molecular sieve overgrowth on microporous molecular sieve surface |
| CN101873997A (en) * | 2007-10-26 | 2010-10-27 | 埃克森美孚化学专利公司 | The manufacture method of M41S family molecular sieve |
| CN103058216A (en) * | 2012-11-05 | 2013-04-24 | 新疆大学 | Method for preparing mesoporous molecular sieve having crystal microporous wall |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1762806A (en) * | 2004-10-21 | 2006-04-26 | 中国石油天然气股份有限公司 | Method for mesoporous molecular sieve overgrowth on microporous molecular sieve surface |
| CN101873997A (en) * | 2007-10-26 | 2010-10-27 | 埃克森美孚化学专利公司 | The manufacture method of M41S family molecular sieve |
| CN103058216A (en) * | 2012-11-05 | 2013-04-24 | 新疆大学 | Method for preparing mesoporous molecular sieve having crystal microporous wall |
Non-Patent Citations (1)
| Title |
|---|
| Directing Zeolite Structures into Hierarchi-cally Nanoporous Architectures;Kyungsu Na et al.;《Science》;20110715;第333卷(第6040期);第328-332页 |
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