CN104445252B - Utilize the Kenyaite method synthesizing MFI type zeolite - Google Patents
Utilize the Kenyaite method synthesizing MFI type zeolite Download PDFInfo
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Abstract
The present invention relates to and a kind of utilize the Kenyaite method synthesizing MFI type zeolite, what mainly solve is that in existing MFI type zeolite technology of preparing, template consumption is big and the problem that could prepare corresponding hydrogen type molecular sieve after needing ammonium ion exchange. The present invention is included Kenyaite, quaternary ammonium salt Q by employing, and water is according to following mixed in molar ratio: Q/SiO2=0.015 ~ 0.20, H2O/SiO2=2 ~ 50, form mixture, by said mixture crystallization 10 ~ 120 hours at 150 ~ 190 DEG C, crystallization product is scrubbed, dry, obtains MFI type zeolite; Wherein, quaternary ammonium salt Q is the compound with following chemical formula: R4N+X-, wherein: R is at least one in the alkyl of 1 ~ 20 selected from carbon number, X-For Cl-,Br-And I-In at least one technical scheme, solve this technical problem preferably, can be used for preparing in the commercial production of MFI type zeolite.
Description
Technical field
The present invention relates to a kind of method synthesizing MFI type zeolite, in particular with the Kenyaite method synthesizing MFI type zeolite as silicon source and aluminum source.
Background technology
Zeolite molecular sieve is owing to having unique duct shape selectivity, unique solid acid character and excellent ion exchangeable matter, thus application is widely, has all shown, at aspects such as absorption, separation and catalysis, the commercial application value that they are huge. Such as at petroleum refining and chemical field, the application of Y zeolite brings the revolution of a hop to petroleum catalytic cracking technology, and other molecular sieve catalyst, such as ZSM-5 zeolite, modenite, �� zeolite, MCM-22 zeolite, the application of SAPO-34 molecular sieve etc. brings substantial breakthrough also to cracking, reformation, isomerization, aromatic disproportion and the important petroleum refining of alkylation, methanol conversion etc. and Chemical Engineering Technology. Therefore in view of molecular sieve important function in many industrial circles, document and always all very abundant for the research of recruit's sieve and the research of novel synthesis in patent.
Mainly there are two aspects in the source of molecular sieve, and one is obtain from nature mineral, and two is obtained by the way of synthetic, and some molecular sieve can be obtained by both approach, but some molecular sieve obtains only by one of both. But at petroleum refining and chemical field, the way that most of molecular sieve catalyst is all by synthetic obtains. Conventional molecular sieve artificial synthesis is hydrothermal synthesis method, such as ZSM-5 (US3702886), ZSM-11 (US3709979), ZSM-23 (US4076842), ZSM-35 (US4016245), Zeolitebeta (US3308069), SAPO-34 (US4440871), MCM-22 (US4954325). Using water heat transfer zeolite molecular sieve to be usually to first pass through silicon source compound, aluminum source compound, alkali, template, and water etc. and be obtained by reacting starting sol, then this colloidal sol hydro-thermal reaction under enclosed system obtains the molecular sieve product of crystallization. Ludox, silica gel, sodium silicate, White Carbon black and organosilicon etc. generally can be used in silicon source, and aluminum source generally uses aluminum sulfate, aluminum nitrate, sodium metaaluminate, alumina sol, organo-aluminium and boehmite etc., and alkali can be organic base, ammonia, NaOH, KOH etc.Alkali is the key factor affecting Zeolite synthesis, but excessive alkali can make molecular sieve dissolve, product yield is made to reduce, simultaneously, the introducing of inorganic base will make to prepare acidic molecular sieve increases a step, the i.e. exchange process to metal cation, this process makes process costs increase, and wastewater treatment capacity increases.
Having document and patent report, some lamellar compounds can also be taken as silicon source and use and synthesize zeolite molecular sieve, and the advantage being carried out synthesis of molecular sieve by this path is that template consumption is few, and crystallization condition is relatively mild, and gained crystal is more regular. US4676958 adopts Magadiite to synthesize multiple zeolite molecular sieve as silicon source, including ZSM-5, ZSM-12, ZSM-39, ZSM-48, SSZ-15 etc., the Magadiite itself adopted due to this invention, without aluminum, therefore needs to add aluminum source and alkali in reaction system.
Document (MicroporousandMesoporousMaterials69 (2004) 85-96) uses the Kenyaite of total silicon to synthesize the MFI zeolite molecular sieve of total silicon as silicon source, but also adds inorganic base or organic base in reaction system.
Summary of the invention
To be solved by this invention is that in existing MFI type zeolite technology of preparing, template consumption is big and the problem that could prepare corresponding hydrogen type molecular sieve after needing ammonium ion exchange. Thering is provided a kind of and new utilize the Kenyaite method synthesizing MFI type zeolite, the method has that quaternary ammonium salt. template dosage amounts is few, advantage without adding hydroxide, obtained MFI zeolite product purity is high in reaction system.
For solving above-mentioned technical problem, the technical solution used in the present invention is as follows: a kind of utilize the Kenyaite method synthesizing MFI type zeolite, and including by Kenyaite, quaternary ammonium salt Q, and water is according to following mixed in molar ratio: Q/SiO2=0.015 ~ 0.20, H2O/SiO2=2 ~ 50, form mixture, by said mixture crystallization 10 ~ 120 hours at 150 ~ 190 DEG C, crystallization product is scrubbed, dry, obtains MFI type zeolite;
Wherein, quaternary ammonium salt Q is the compound with following chemical formula:
R4N+X-
Wherein: R is at least one in the alkyl of 1 ~ 20 selected from carbon number, X-For Cl-,Br-And I-In at least one.
In technique scheme, the method for described synthesis MFI type zeolite, it is characterised in that in mixture, each component has following molar ratio: Q/SiO2=0.02 ~ 0.15, H2O/SiO2=8 ~ 40, mixture is crystallization 20 ~ 120 hours at 160 ~ 190 DEG C.
The method of the synthesis MFI type zeolite described in technique scheme, it is characterised in that quaternary ammonium salt is the compound with following chemical formula: R4N+X-
Wherein: R is at least one in the alkyl of 2 ~ 15 selected from carbon number, X-For Cl-,Br-In at least one.
The method of the synthesis MFI type zeolite described in technique scheme, it is characterized in that quaternary ammonium salt is 4-propyl bromide, 4-propyl ammonium chloride, tetraethylammonium bromide, tetraethylammonium chloride, tetrabutyl ammonium bromide, tetrabutylammonium chloride, at least one in dimethyl diethyl ammonium bromide and dimethyl diethylammonium chloride.
The method of the synthesis MFI type zeolite described in technique scheme, it is characterised in that Kenyaite used is synthetically derived through the following steps:
A) according to 10SiO2:(0~2.0)Y2O3: (0.4 ~ 2.4) alkaline matter A:(0.05 ~ 5) Organic substance R:(0.05 ~ 5) alkali metal salt S:(85 ~ 500) H2The mol ratio of O, by silicon source, hetero atom source Y2O3, alkaline matter A, Organic substance R, alkali metal salt S and water Homogeneous phase mixing prepare mixture;Wherein silicon source is selected from Ludox, solid silicone, gas-phase silica, amorphous silica or at least one in organic silicone grease; Alkaline matter A is selected from lithium oxide, sodium oxide, potassium oxide, Cs2O, Lithium hydrate, sodium hydroxide, potassium hydroxide, rubidium hydroxide and at least one in Cesium hydrate.; Alkali metal salt S is selected from the oxalates of alkali metal, sulfate, acetate, nitrate, carbonate, phosphate and at least one in halogenide;
B) by said mixture hydrothermal crystallizing 12 ~ 160 hours at 150 ~ 210 DEG C, Kenyaite is obtained.
The method of the synthesis MFI type zeolite described in technique scheme, it is characterised in that in the method for synthesis Kenyaite, the mol ratio of mixture is 10SiO2:(0~2.0)Y2O3: (0.5 ~ 2.0) alkaline matter A:(1.0 ~ 5.0) Organic substance R:(1.0 ~ 5.0) alkali metal salt S:(100 ~ 400) H2O��
The method of the synthesis MFI type zeolite described in technique scheme, it is characterised in that synthesis Kenyaite method in, mixture at 155 ~ 195 DEG C, hydrothermal crystallizing 16 ~ 120 hours.
The method of the synthesis MFI type zeolite described in technique scheme, it is characterised in that in the method for synthesis Kenyaite, element Y at least one in Al, B and Ga.
The method of the synthesis MFI type zeolite described in technique scheme, it is characterised in that in the method for synthesis Kenyaite, Organic substance R is crown ether, Polyethylene Glycol and at least one in tetraethylene glycol dimethyl ether.
The method of the synthesis MFI type zeolite described in technique scheme, it is characterised in that in the method for synthesis Kenyaite, the molecular weight of Organic substance R is between 200 to 1000. Quaternary ammonium salt is 4-propyl bromide, 4-propyl ammonium chloride, tetraethylammonium bromide, tetraethylammonium chloride, tetrabutyl ammonium bromide, tetrabutylammonium chloride, at least one in dimethyl diethyl ammonium bromide and dimethyl diethylammonium chloride.
MFI type zeolite synthetic method provided by the present invention has the advantage that 1) quaternary ammonium salt. template dosage amounts is few; 2) without adding hydroxide in reaction system; 3) obtained MFI zeolite product purity is high; 4) corresponding hydrogen type molecular sieve just can directly be prepared without ammonium ion exchange.
The invention will be further elaborated by the examples below, but does not therefore limit the scope of the invention.
Detailed description of the invention
[embodiment 1]
By the NaCl of 0.41 gram, the sodium hydrate aqueous solution of 1.1175 gram 30%, the PEG300 of 10 gram 50% Polyethylene Glycol of 300 (mean molecule quantity be about) solution, the silicon sol solution mix homogeneously of the 40% of the water of 11 grams and 8.1 milliliters, the mol ratio of gained mixture is:
10SiO2: 1.0NaCl:0.6Na2O:2.5PEG300:175H2O
Said mixture is moved in reactor in 180oC crystallization 40 hours, reaction terminate after through washing, dried, be accredited as Kenyaite through XRD.
2.0 grams of above-mentioned Kenyaite and 0.8 gram TPABr and 10 ml deionized water being mixed, the mol ratio of mixed serum is:
TPABr/SiO2=0.09; H2O/SiO2=16.67
Then above-mentioned serosity is placed in closed reactor, in 170oCrystallization 80 hours under C, solid product scrubbed dry after be accredited as MFI zeolite through XRD.
[embodiment 2]
By the NaCl of 0.41 gram, the sodium hydrate aqueous solution of 1.1175 gram 30%, the PEG300 of 10 gram 50% Polyethylene Glycol of 300 (mean molecule quantity be about) solution, the silicon sol solution mix homogeneously of the 40% of the water of 11 grams and 8.1 milliliters, the mol ratio of gained mixture is:
10SiO2: 1.0NaCl:0.6Na2O:2.5PEG300:175H2O
Said mixture is moved in reactor in 180oC crystallization 40 hours, reaction terminate after through washing, dried, be accredited as Kenyaite through XRD.
2.0 grams of above-mentioned Kenyaite and 0.2 gram TPABr and 10 ml deionized water being mixed, the mol ratio of mixed serum is:
TPABr/SiO2=0.02; H2O/SiO2=16.67
Then above-mentioned serosity is placed in closed reactor, in 170oCrystallization 80 hours under C, solid product scrubbed dry after be accredited as MFI zeolite through XRD.
[embodiment 3]
By the NaCl of 0.41 gram, the sodium hydrate aqueous solution of 1.1175 gram 30%, the PEG300 of 10 gram 50% Polyethylene Glycol of 300 (mean molecule quantity be about) solution, the silicon sol solution mix homogeneously of the 40% of the water of 11 grams and 8.1 milliliters, the mol ratio of gained mixture is:
10SiO2: 1.0NaCl:0.6Na2O:2.5PEG300:175H2O
Said mixture is moved in reactor in 180oC crystallization 40 hours, reaction terminate after through washing, dried, be accredited as Kenyaite through XRD.
2.0 grams of above-mentioned Kenyaite and 0.2 gram TPABr and 10 ml deionized water being mixed, the mol ratio of mixed serum is:
TPABr/SiO2=0.02; H2O/SiO2=16.67
Then above-mentioned serosity is placed in closed reactor, in 190oCrystallization 24 hours under C, solid product scrubbed dry after be accredited as MFI zeolite through XRD.
[embodiment 4]
By the NaF of 0.2932 gram, 0.9692 gram of 30(weight) sodium hydrate aqueous solution of %, the sodium metaaluminate of 0.0572 gram, 10 grams of 50(weight) the PEG300 Polyethylene Glycol of 300 (mean molecule quantity be about) solution of %, 10.3 gram water and the 40(weight of 8.1 milliliters) the silicon sol solution mix homogeneously of %, the mol ratio of gained mixture is:
10SiO2:0.05Al2O3:1.0NaF:0.6Na2O:2.5PEG300:175H2O
Said mixture is moved in reactor in 170oC crystallization 60 hours, reacts through washing, drying after terminating, and XRD is accredited as Kenyaite.
2.0 grams of above-mentioned Kenyaite and 0.4 containing aluminum gram TPABr and 10 ml deionized water being mixed, the mol ratio of mixed serum is:
TPABr/SiO2=0.045; H2O/SiO2=16.67
Then above-mentioned serosity is placed in closed reactor, in 170oCrystallization 60 hours under C, solid product scrubbed dry after be accredited as MFI zeolite through XRD.
[embodiment 5]
By the NaF of 0.2932 gram, 0.9692 gram of 30(weight) sodium hydrate aqueous solution of %, the sodium metaaluminate of 0.0572 gram, 10 grams of 50(weight) the PEG300 Polyethylene Glycol of 300 (mean molecule quantity be about) solution of %, 10.3 gram water and the 40(weight of 8.1 milliliters) the silicon sol solution mix homogeneously of %, the mol ratio of gained mixture is:
10SiO2:0.05Al2O3:1.0NaF:0.6Na2O:2.5PEG300:175H2O
Said mixture is moved in reactor in 170oC crystallization 60 hours, reacts through washing, drying after terminating, and XRD is accredited as Kenyaite.
2.0 grams of above-mentioned Kenyaite and 0.8 containing aluminum gram TEABr and 10 ml deionized water being mixed, the mol ratio of mixed serum is:
TPABr/SiO2=0.10; H2O/SiO2=16.67
Then above-mentioned serosity is placed in closed reactor, in 180oCrystallization 90 hours under C, solid product scrubbed dry after be accredited as MFI zeolite through XRD.
[embodiment 6]
By the NaF of 0.2932 gram, 0.9692 gram of 30(weight) sodium hydrate aqueous solution of %, the sodium metaaluminate of 0.0572 gram, 10 grams of 50(weight) the PEG300 Polyethylene Glycol of 300 (mean molecule quantity be about) solution of %, 10.3 gram water and the 40(weight of 8.1 milliliters) the silicon sol solution mix homogeneously of %, the mol ratio of gained mixture is:
10SiO2:0.05Al2O3:1.0NaF:0.6Na2O:2.5PEG300:175H2O
Said mixture is moved in reactor in 170oC crystallization 60 hours, reacts through washing, drying after terminating, and XRD is accredited as Kenyaite.
2.0 grams of above-mentioned Kenyaite and 0.8 containing aluminum gram TBABr and 10 ml deionized water being mixed, the mol ratio of mixed serum is:
TBABr/SiO2=0.085; H2O/SiO2=16.67
Then above-mentioned serosity is placed in closed reactor, in 180oCrystallization 90 hours under C, solid product scrubbed dry after be accredited as MFI zeolite through XRD.
[embodiment 7]
By the NaF of 0.2932 gram, 0.9692 gram of 30(weight) sodium hydrate aqueous solution of %, the sodium metaaluminate of 0.0572 gram, 10 grams of 50(weight) the PEG300 Polyethylene Glycol of 300 (mean molecule quantity be about) solution of %, 10.3 gram water and the 40(weight of 8.1 milliliters) the silicon sol solution mix homogeneously of %, the mol ratio of gained mixture is:
10SiO2:0.05Al2O3:1.0NaF:0.6Na2O:2.5PEG300:175H2O
Said mixture is moved in reactor in 170oC crystallization 60 hours, reacts through washing, drying after terminating, and XRD is accredited as Kenyaite.
2.0 grams of above-mentioned Kenyaite and 0.2 containing aluminum gram TPABr and 10 ml deionized water being mixed, the mol ratio of mixed serum is:
TPABr/SiO2=0.023; H2O/SiO2=16.67
Then above-mentioned serosity is placed in closed reactor, in 170oCrystallization 60 hours under C, solid product scrubbed dry after be accredited as MFI zeolite through XRD.
[embodiment 8]
By the NaF of 0.2932 gram, 2.6074 grams of 30(weight) sodium hydrate aqueous solution of %, the boric acid of 0.3452 gram, 10 grams of 50(weight) the PEG300 Polyethylene Glycol of 300 (mean molecule quantity be about) solution of %, the 40(weight of the water of 9.8 grams and 8.1 milliliters) the silicon sol solution mix homogeneously of %, the mol ratio of gained mixture is:
10SiO2:0.4B2O3:1.0NaF:1.5Na2O:2.5PEG300:175H2O
Said mixture is moved in reactor in 170oC crystallization 60 hours, reacts through washing, drying after terminating, and XRD is accredited as Kenyaite.
Kenyaite and the 0.4 gram TPABr of 2.0 grams of above-mentioned boracics and 10 ml deionized water being mixed, the mol ratio of mixed serum is:
TPABr/SiO2=0.045, H2O/SiO2=16.67
Then above-mentioned serosity is placed in closed reactor, in 170oCrystallization 48 hours under C, solid product scrubbed dry after be accredited as MFI zeolite through XRD.
[embodiment 9]
By the NaF of 0.2932 gram, 2.6074 grams of 30(weight) sodium hydrate aqueous solution of %, the boric acid of 0.6904 gram, 10 grams of 50(weight) the PEG300 Polyethylene Glycol of 300 (mean molecule quantity be about) solution of %, the 40(weight of the water of 9.8 grams and 8.1 milliliters) the silicon sol solution mix homogeneously of %, the mol ratio of gained mixture is:
10SiO2:2.0B2O3:1.0NaF:1.5Na2O:2.5PEG300:175H2O
Said mixture is moved in reactor in 170oC crystallization 60 hours, reacts through washing, drying after terminating, and XRD is accredited as Kenyaite.
Kenyaite and the 0.4 gram TPABr of 2.0 grams of above-mentioned boracics and 10 ml deionized water being mixed, the mol ratio of mixed serum is:
TPABr/SiO2=0.045, H2O/SiO2=16.67
Then above-mentioned serosity is placed in closed reactor, in 170oCrystallization 48 hours under C, solid product scrubbed dry after be accredited as MFI zeolite through XRD.
[embodiment 10]
By the NaF of 0.2932 gram, 2.6074 grams of 30(weight) sodium hydrate aqueous solution of %, the boric acid of 0.3452 gram, 10 grams of 50(weight) the PEG300 Polyethylene Glycol of 300 (mean molecule quantity be about) solution of %, the 40(weight of the water of 9.8 grams and 8.1 milliliters) the silicon sol solution mix homogeneously of %, the mol ratio of gained mixture is:
10SiO2:0.4B2O3:1.0NaF:1.5Na2O:2.5PEG300:175H2O
Said mixture is moved in reactor in 170oC crystallization 60 hours, reacts through washing, drying after terminating, and XRD is accredited as Kenyaite.
Kenyaite and the 0.4 gram TPABr of 2.0 grams of above-mentioned boracics and 10 ml deionized water being mixed, the mol ratio of mixed serum is:
TPABr/SiO2=0.045, H2O/SiO2=16.67
Then above-mentioned serosity is placed in closed reactor, in 150oCrystallization 72 hours under C, solid product scrubbed dry after be accredited as MFI zeolite through XRD.
[embodiment 11]
By the NaF of 0.2932 gram, 0.9692 gram of 30(weight) sodium hydrate aqueous solution of %, the 16 water gallium sulfates of 0.155 gram, 10 grams of 50(weight) the PEG300 Polyethylene Glycol of 300 (mean molecule quantity be about) solution of %, 10.3 gram water and the 40(weight of 8.1 milliliters) the silicon sol solution mix homogeneously of %, the mol ratio of gained mixture is:
10SiO2:0.05Ga2O3:1.0NaF:0.6Na2O:2.5PEG300:175H2O
Said mixture is moved in reactor in 170oC crystallization 60 hours, reacts through washing, drying after terminating, and XRD is accredited as Kenyaite.
2.0 grams of above-mentioned Kenyaite and 0.4 containing gallium gram TPABr and 10 ml deionized water being mixed, the mol ratio of mixed serum is:
TPABr/SiO2=0.045, H2O/SiO2=16.67
Then above-mentioned serosity is placed in closed reactor, in 170oCrystallization 60 hours under C, solid product scrubbed dry after be accredited as MFI zeolite through XRD.
[embodiment 12]
Hydrogen is containing the synthesis of aluminum MFI zeolite
Hydrogen within 5 hours, is namely obtained containing aluminum MFI zeolite, wherein Na in 550 DEG C of roastings by what embodiment 4 obtained in air atmosphere containing aluminum MFI zeolite by 2.0 grams2The content of O is lower than 2.0%.
Claims (9)
1. utilizing the Kenyaite method synthesizing MFI type zeolite, including by Kenyaite, quaternary ammonium salt Q, and water is according to following mixed in molar ratio: Q/SiO2=0.015��0.20, H2O/SiO2=2��50, form mixture, by said mixture crystallization 10��120 hours at 150��190 DEG C, crystallization product is scrubbed, dry, obtains MFI type zeolite;
Wherein, quaternary ammonium salt Q is the compound with following chemical formula:
R4N+X-
Wherein: R is at least one in the alkyl of 1��20 selected from carbon number, X-For Cl-,Br-And I-In at least one;
Wherein Kenyaite is synthetically derived through the following steps:
A) according to 10SiO2: (0��2.0) Y2O3: (0.4��2.4) alkaline matter A:(0.05��5) Organic substance R:(0.05��5) alkali metal salt S:(85��500) H2The mol ratio of O, by silicon source, hetero atom source Y2O3, alkaline matter A, Organic substance R, alkali metal salt S and water Homogeneous phase mixing prepare mixture; Wherein silicon source is selected from Ludox, solid silicone, gas-phase silica, amorphous silica or at least one in organic silicone grease; Alkaline matter A is selected from lithium oxide, sodium oxide, potassium oxide, Cs2O, Lithium hydrate, sodium hydroxide, potassium hydroxide, rubidium hydroxide and at least one in Cesium hydrate.; Alkali metal salt S is selected from the oxalates of alkali metal, sulfate, acetate, nitrate, carbonate, phosphate and at least one in halogenide;
B) by said mixture hydrothermal crystallizing 12��160 hours at 150��210 DEG C, Kenyaite is obtained.
2. the method utilizing Kenyaite synthesis MFI type zeolite according to claim 1, it is characterised in that in mixture, each component has following molar ratio: Q/SiO2=0.02��0.15, H2O/SiO2=8��40.
3. the method utilizing Kenyaite synthesis MFI type zeolite according to claim 1, it is characterised in that mixture is crystallization 20��120 hours at 160��190 DEG C.
4. the method utilizing Kenyaite synthesis MFI type zeolite according to claim 1, it is characterised in that in the method for synthesis Kenyaite, the mol ratio of mixture is 10SiO2: (0��2.0) Y2O3: (0.5��2.0) alkaline matter A:(1.0��5.0) Organic substance R:(1.0��5.0) alkali metal salt S:(100��400) H2O��
5. according to claim 1 utilize Kenyaite synthesize MFI type zeolite method, it is characterised in that synthesis Kenyaite method in, mixture at 155��195 DEG C, hydrothermal crystallizing 16��120 hours.
6. the method utilizing Kenyaite synthesis MFI type zeolite according to claim 1, it is characterised in that in the method for synthesis Kenyaite, element Y at least one in Al, B and Ga.
7. the method utilizing Kenyaite synthesis MFI type zeolite according to claim 1, it is characterised in that in the method for synthesis Kenyaite, Organic substance R is crown ether, Polyethylene Glycol and at least one in tetraethylene glycol dimethyl ether.
8. the method utilizing Kenyaite synthesis MFI type zeolite according to claim 1, it is characterised in that in the method for synthesis Kenyaite, the molecular weight of Organic substance R is between 200 to 1000.
9. the method utilizing Kenyaite synthesis MFI type zeolite according to claim 1, it is characterized in that quaternary ammonium salt is 4-propyl bromide, 4-propyl ammonium chloride, tetraethylammonium bromide, tetraethylammonium chloride, tetrabutyl ammonium bromide, tetrabutylammonium chloride, at least one in dimethyl diethyl ammonium bromide and dimethyl diethylammonium chloride.
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Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB2125390B (en) * | 1982-08-16 | 1985-12-24 | Ici Plc | Preparation of zeolites |
| CN103183358A (en) * | 2013-01-21 | 2013-07-03 | 华东师范大学 | Preparation method of ZSM-5 molecular sieve |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB2125390B (en) * | 1982-08-16 | 1985-12-24 | Ici Plc | Preparation of zeolites |
| CN103183358A (en) * | 2013-01-21 | 2013-07-03 | 华东师范大学 | Preparation method of ZSM-5 molecular sieve |
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