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A supported composite metal molecular sieve catalyst for catalyzing the coupling of methyl chloride to prepare low-carbon olefins

A technology for catalyzing methyl chloride and composite metals, applied in the field of supported composite metal molecular sieve catalysts, can solve the problems of reduced selectivity of low-carbon olefins, reduced Lewis acid content, reduced methyl chloride conversion rate, etc., so as to improve selectivity and prolong stability. Sexual, low-cost effects

Active Publication Date: 2019-12-17
NANJING TECH UNIV
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Problems solved by technology

In the above studies, the inventors mostly used a single alkali metal, transition metal, rare earth element or non-metallic modified HZSM-5 molecular sieve to catalyze the MeXTO reaction. Although the selectivity of olefins was improved, the reaction stability was poor. Wang Ye et al. used F pore-enlarging modified molecular sieves to catalyze the MeXTO reaction. Although the reaction stability was long, the conversion rate of methyl chloride was low.
[0005] Catalyzed chloromethane to olefins process, due to molecular sieve surface In the presence of acid, the initial product low-carbon olefins will further undergo secondary reactions such as hydrogen transfer and aromatization to generate alkanes and aromatics, resulting in a decrease in the selectivity of low-carbon olefins
A single metal modified molecular sieve not only makes the catalyst surface The acid is greatly reduced or even disappeared, and the amount of Lewis acid is also significantly reduced, so that the conversion rate of methyl chloride in the MeXTO reaction is also reduced

Method used

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  • A supported composite metal molecular sieve catalyst for catalyzing the coupling of methyl chloride to prepare low-carbon olefins
  • A supported composite metal molecular sieve catalyst for catalyzing the coupling of methyl chloride to prepare low-carbon olefins
  • A supported composite metal molecular sieve catalyst for catalyzing the coupling of methyl chloride to prepare low-carbon olefins

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0030] Get the HZSM-5 molecular sieve (SiO 2 / Al 2 o 3 =50), by gradually adding deionized water dropwise, the saturated water absorption rate of 10gHZSM-5 molecular sieve was measured to be 7.9mL.

[0031] 3.80g Ca(NO 3 ) 2 4H 2 O and 1.14g Mg(NO 3 ) 2 ·6H 2O was dissolved in 7.9mL deionized water to make nitrate aqueous solution, placed in a 50mL beaker, and under rapid stirring, 10g HZSM-5 molecular sieve (SiO 2 / Al 2 o 3 =50) into a beaker, mixed evenly, ultrasonically dissolved at 30°C for 1h, left at room temperature for 24h, then placed in an oven at 110°C for 24h; baked in a muffle furnace at 570°C for 3h, the obtained composite metal The mass percent content of the modified molecular sieve catalyst is Ca: 0.06, Mg: 0.01, and the rest is HZSM-5, named 6Ca-1Mg / HZSM-5.

[0032] The performance test of the catalyst was carried out in a glass reaction tube with a three-stage temperature-controlled fixed bed. The 6Ca-1Mg / HZSM-5 molecular sieve prepared by the abo...

Embodiment 2

[0034] Get the HZSM-5 molecular sieve (SiO 2 / Al 2 o 3 =25), by gradually adding deionized water dropwise, the saturated water absorption rate of 10gHZSM-5 molecular sieve was measured to be 7.0mL.

[0035] 3.17g Ca(NO 3 ) 2 4H 2 O and 0.56 g KNO 3 Dissolve in 7.0mL deionized water to make nitrate aqueous solution, place in a 50mL beaker, stir rapidly, mix 10g HZSM-5 molecular sieve (SiO 2 / Al 2 o 3 =25) into a beaker, after mixing evenly, ultrasonically dissolve at 50°C for 0.5h, then let it stand at room temperature for 30h, and then put it in an oven at 100°C to dry for 30h; The mass percent content of the metal-modified molecular sieve catalyst is Ca: 0.05, K: 0.02, and the rest is HZSM-5, which is named 5Ca-2K / HZSM-5.

[0036] The performance test of the catalyst was carried out in a glass reaction tube with a three-stage temperature-controlled fixed bed. The 5Ca-2K / HZSM-5 molecular sieve prepared by the above method was used to catalyze the preparation of light ...

Embodiment 3

[0038] Get the HZSM-5 molecular sieve (SiO 2 / Al 2 o 3 =80), by gradually adding deionized water dropwise, the saturated water absorption of 10gHZSM-5 molecular sieve was measured to be 8.9mL.

[0039] 3.17g Ca(NO 3 ) 2 4H 2 O and 2.27g Mg(NO 3 ) 2 ·6H 2 O was dissolved in 8.9mL deionized water to make nitrate aqueous solution and placed in a 50mL beaker, and under rapid stirring, 10g HZSM-5 molecular sieve (SiO 2 / Al 2 o 3 =80) into a beaker, mixed evenly, ultrasonically dissolved at 40°C for 1h, left to stand at room temperature for 20h, then placed in an oven at 130°C for 20h; baked in a muffle furnace at 600°C for 3h, the obtained composite metal The mass percent content of the modified molecular sieve catalyst is Ca: 0.05, Mg: 0.02, and the rest is HZSM-5, which is named 5Ca-2Mg / HZSM-5.

[0040] The performance test of the catalyst was carried out in a glass reaction tube with a three-stage temperature-controlled fixed bed. The 5Ca-2Mg / HZSM-5 molecular sieve pr...

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Abstract

The invention discloses a supported composite metal molecular sieve catalyst. The catalyst takes an HZSM-5 molecular sieve as a carrier, a composite metal oxide is supported on the HZSM-5 molecular sieve by an incipient-wetness impregnation method, the composite metal oxide is Ca-M, and M is Mg, Zn or K. The invention further discloses an application of the supported composite metal molecular sieve catalyst to coupling preparation reaction of low-carbon olefin (MeXTO) by catalyzing chloromethane. Composite metal is modified, Bronsted acid can disappear, Lewis acid is basically unaffected, and carbon deposition is relieved by inhibiting secondary reaction such as hydrogen transfer in MeXTO catalysis reaction, so that reaction stability is prolonged. The catalyst is low in preparation cost and has good industrial application prospect, the conversion rate of the chloromethane is high, the selectivity of the low-carbon olefin is good, and the reaction stability is prolonged in the MeXTO catalysis reaction.

Description

technical field [0001] The invention belongs to the field of catalysts, and relates to a supported composite metal molecular sieve catalyst used for catalyzing the coupling of methyl chloride to prepare low-carbon olefins (namely MeXTO). Background technique [0002] Low-carbon olefins (ethylene, propylene and butene) are the basic raw materials of the chemical industry and occupy an extremely important position in chemical production. The traditional process of producing ethylene and propylene is catalytic cracking of heavy oil or steam cracking of naphtha. However, with the shortage of global oil resources and the rise of oil prices, it is of great strategic significance to seek non-petroleum routes to prepare light olefins. From the perspective of economy and raw materials, the route of preparing light olefins from natural gas (methane) via methyl chloride is an ideal choice and has good development prospects. [0003] In 1985, Olah et al. [J.Am.Chem.Soc, 1985,107:7097-7...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J29/46C07C1/26C07C11/02C07C11/06
CPCB01J29/46C07C1/26C07C2529/46C07C11/02C07C11/06Y02P20/52
Inventor 崔咪芬乔旭荆开石顾奥焦澄洋费兆阳陈献汤吉海张竹修刘清
Owner NANJING TECH UNIV
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