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Catalyst for preparing paraxylene and low-carbon olefin by methyl alcohol conversion, preparation method and application thereof

A low-carbon olefin and p-xylene technology, applied in chemical instruments and methods, physical/chemical process catalysts, molecular sieve catalysts, etc., can solve the problems of low market value of mixed aromatics, difficulty in application and promotion, poor selectivity of ethylene and propylene, etc.

Active Publication Date: 2012-04-18
CHINA NAT OFFSHORE OIL CORP +2
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

The content of the main product of methanol conversion in any method is relatively low, such as the poor selectivity of ethylene and propylene in the production of low-carbon olefins from methanol conversion, and the low market value of mixed aromatics produced by direct conversion of methanol, which makes these processes difficult to industrialize. application promotion

Method used

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  • Catalyst for preparing paraxylene and low-carbon olefin by methyl alcohol conversion, preparation method and application thereof
  • Catalyst for preparing paraxylene and low-carbon olefin by methyl alcohol conversion, preparation method and application thereof
  • Catalyst for preparing paraxylene and low-carbon olefin by methyl alcohol conversion, preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0031] Embodiment 1, Zn-La-HZSM-5 zeolite molecular sieve

[0032] 1) ZSM-5 zeolite molecular sieve raw powder (SiO 2 / Al 2 o 3 =61, Fushun Catalyst Factory) was roasted at 550°C to remove template agent, exchanged 4 times with 0.5 molar equivalent ammonium nitrate solution in 80°C water bath, dried in 120°C air after exchange, and roasted at 550°C for 3 hours, Obtain HZSM-5 zeolite molecular sieve.

[0033] 2) get step 1) HZSM-5 zeolite molecular sieve 50g prepared, use 10wt% concentration Zn(NO 3 ) 2 The aqueous solution was soaked for 10 hours, dried and then calcined at 550° C. for 3 hours to obtain a Zn-HZSM-5 zeolite molecular sieve, wherein the Zn loading amount was 5 wt%.

[0034] 3) Get Zn-HZSM-5 zeolite molecular sieve 20g, use the La(NO 3 ) 3 The aqueous solution was soaked for 10 hours, dried, and then calcined at 550° C. for 3 hours to obtain a Zn-La-HZSM-5 zeolite molecular sieve, wherein the La loading amount was 3 wt%.

Embodiment 2

[0035] Embodiment 2, Fe-La-HZSM-5 zeolite molecular sieve

[0036] 1) ZSM-5 zeolite molecular sieve raw powder (SiO 2 / Al 2 o 3=61, Fushun Catalyst Factory) was roasted at 550°C to remove template agent, exchanged 4 times with 0.5 molar equivalent ammonium nitrate solution in 80°C water bath, dried in 120°C air after exchange, and roasted at 550°C for 3 hours, Obtain HZSM-5 zeolite molecular sieve.

[0037] 2) get step 1) HZSM-5 zeolite molecular sieve 50g prepared, use 12wt% concentration Fe(NO 3 ) 3 The aqueous solution was immersed for 12 hours, dried, and then calcined at 550° C. for 3 hours to obtain Fe-HZSM-5 zeolite molecular sieve, wherein the Fe loading amount was 6 wt%.

[0038] 3) Get Fe-HZSM-5 zeolite molecular sieve 20g, use 10wt% concentration La(NO 3 ) 3 The aqueous solution was immersed for 10 hours, dried, and then calcined at 550° C. for 3 hours to obtain Fe-La-HZSM-5 zeolite molecular sieve, wherein the La loading amount was 3 wt%.

Embodiment 3

[0039] Example 3, Preparation of Catalyst for Preparing p-Xylene and Light Olefins with High Selectivity in Methanol Conversion

[0040] Zn-La-HZSM-5, Fe-La-HZSM-5 zeolite molecular sieves obtained in Example 1 and Example 2 are surface-modified using siloxane reagent tetraethyl silicate:

[0041] (1) Immerse 10 grams of Zn-La-HZSM-5 in 20 grams of tetraethyl silicate for 12 hours, pour out the liquid, dry at 120°C, and bake at 550°C for 3 hours to obtain modified Zn - La-HZSM-5 zeolite molecular sieve, numbered MTAC-11; wherein, the mass content of Zn is 4.7%, the mass content of La is 2.9%, and the loading amount of silicon is 4.2% of the total mass of the catalyst.

[0042] (2) Put 10 grams of Fe-La-HZSM-5 into 20 grams of tetraethyl silicate and soak for 12 hours. After pouring out the liquid, dry it at 120°C and bake it at 550°C for 3 hours to obtain the modified Fe - La-HZSM-5 zeolite molecular sieve, numbered MTAC-12; wherein, the mass content of Fe is 5.6%, the mass c...

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Abstract

The invention discloses a catalyst for preparing paraxylene and low-carbon olefin by methyl alcohol conversion, a preparation method and application thereof. The catalyst provided by the invention is obtained by the method that a zeolite molecular sieve modified by transition metal and rare-earth metal is performed with the surface acidity and the pore structure modification by a siloxy group compound, wherein the transition metal is 0.1-10 wt% of the total weight of catalyst, the rare-earth metal is 0.1-5 wt% of total weight of the catalyst, and the modified siloxy group compound which is accounted by Si is 0.1-8 wt% of total weight of the catalyst; the catalyst can realize that methyl alcohol is used for directly preparing three basic chemicals in one reaction process, i.e. ethylene, propylene and paraxylene; the selectivity of the obtained hydrocarbon products in paraxylene is more than 80 wt%, and the selectivity of ethylene and propylene in C1-C5 is more than 80 wt%.

Description

technical field [0001] The invention relates to a technology for preparing low-carbon olefins and aromatics from methanol, in particular to a catalyst for the high-selectivity preparation of p-xylene and co-production of ethylene and propylene from methanol, its preparation method and application. Background technique [0002] Ethylene, propylene and p-xylene are the basic raw materials of modern chemical industry. At present, p-xylene production mainly uses toluene, C 9 Aromatic hydrocarbons and mixed xylenes are used as raw materials, and are produced through disproportionation, isomerization, adsorption separation or cryogenic separation. Since the p-xylene content in its products is thermodynamically controlled, p-xylene is at C 8 Mixed aromatics only account for about 20%. In the process, the amount of material circulation is large, the equipment is huge, and the operating cost is high. In particular, the difference between the boiling points of the three isomers of ...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J29/40B01J29/46C07C15/08C07C1/20C07C11/04C07C11/06
CPCY02P20/52Y02P30/20Y02P30/40
Inventor 许磊李铭芝刘中民张莹袁翠峪张今令欧书能马跃龙金阳肖钢郑长波
Owner CHINA NAT OFFSHORE OIL CORP
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