Catalyst for producing aromatics from synthesis gas and method of use thereof

Abstract

The invention relates to a catalyst for preparing arene from synthesis gas and a use method of the catalyst, and mainly solves the technical problems of long technological process, high production cost and low arene yield which exist during a process of preparing the arene from the synthesis gas in the prior art. According to the use method, under the condition of the temperature of 250-450 DEG C, pressure of 0.01-8.0 MPa and synthesis gas volume space velocity of 400-10000h<-1>, an oxygenated compound is taken as raw material, the raw material is in contact with and is reacted with the catalyst in an reactor, so that a material flow containing the arene is obtained; by utilizing the technical scheme of a Fe-containing composite oxide and a molecular sieve composite catalyst, the above problems are well solved; and the catalyst can be applied to industrial production of preparing the arene from the synthesis gas.

Description

technical field

[0001] The invention relates to a catalyst for producing aromatics from synthesis gas and its application method. Background technique

[0002] Aromatics (in which benzene, toluene and xylene are called B, T and X respectively, and the three are collectively called BTX) are important basic organic chemical raw materials. Aromatics mainly come from catalytic reforming and steam cracking by-product pyrolysis gasoline (nearly 90%)-petroleum route, and only about 10% from coal route. From the perspective of energy distribution, my country lacks oil and gas but is rich in coal, and its dependence on foreign crude oil has exceeded 50%, which has threatened national energy security. Moreover, the depletion of petroleum resources and the long-term high volatility of petroleum prices have brought unprecedented severe challenges to energy and chemical industries based on petroleum routes. Therefore, it is imperative to develop new technologies to replace petroleum rou...

Examples

Embodiment 1

[0035] After weighing 539 grams of ferric nitrate, 182.5 grams of manganese nitrate (50%), 11.7 grams of lanthanum nitrate and 500 grams of water, mix them uniformly, precipitate with 500 grams of concentrated ammonia water (25%), and after aging for 12 hours at room temperature, wash , centrifuged, dried at 120°C for 8 hours, and calcined at 550°C for 6 hours to obtain Fe-Mn oxide solid. Weigh 72.1 g Fe-Mn oxide solid, impregnate 42 g containing 0.53 g K 2 CO 3 Aqueous solution, dried at 120°C for 6 hours, calcined at 500°C for 4 hours to obtain Fe composite component F-1.

[0036] Weigh 60 grams of ZSM-5 molecular sieves (the molar ratio of silicon oxide to aluminum oxide is 400), impregnate with 116 grams of aqueous solution containing 36.7 grams of zinc nitrate and 16.2 grams of phosphoric acid (85%), and after aging for 4 hours at room temperature MZ1 was obtained by drying at 120°C for 8 hours and calcining at 600°C for 6 hours.

[0037] Weigh 40 grams of F-1, 40 gram...

Embodiment 2-7

[0040] F2-F9 were prepared by the same method as in Example 1, and their compositions are listed in Table 1.

[0041] Catalysts b to i were prepared by the same method as in Embodiment 1, and the evaluation method was the same as in Embodiment 1.

[0042] Catalyst components and evaluation results are listed in Table 2 and Table 3, respectively.

Embodiment 8-11

[0050] Using catalyst e, the evaluation conditions and evaluation results are shown in Table 4.

[0051] Table 1

[0052] Fe composite oxide

Weight composition (wt%)

F-1

74.7Fe: 20Mn: 0.3K: 5.0La

F-2

50Fe: 25Mn: 5Na: 10La

F-3

39.9Fe: 50Mn: 10Mg: 0.1La

F-4

58.5Fe: 35Mn: 4.0K: 2.5.0Ce

[0053] F-5

55.3Fe: 35.2Mn: 5.2Ca: 4.3Zn

F-6

50.4Fe: 38.7Mn: 6.0K: 2.0Ce: 2.9Si

F-7

65Fe: 25Mn: 4.8K: 2.0La: 2.2Ce: 1.0Ga

F11

50.4Fe: 38.7Mn: 6.0K: 2.9Si (weight ratio)

F12

65Fe: 25Mn: 4.8K: 1.0Ga (weight ratio)

[0054] Table 2

[0055]

[0056] table 3

[0057] Example

catalyst

Aromatics yield / %

1

a

69.7

2

b

72.3

3

c

71.0

4

d

70.2

5

e

79.2

6

f

59.7

7

g

56.8

8

h

63.2

9

i

57.6

comparative example

1

x

54.2

2

y

...

technical field

[0001] The invention relates to a catalyst for producing aromatics from synthesis gas and its application method. Background technique

[0002] Aromatics (in which benzene, toluene and xylene are called B, T and X respectively, and the three are collectively called BTX) are important basic organic chemical raw materials. Aromatics mainly come from catalytic reforming and steam cracking by-product pyrolysis gasoline (nearly 90%)-petroleum route, and only about 10% from coal route. From the perspective of energy distribution, my country lacks oil and gas but is rich in coal, and its dependence on foreign crude oil has exceeded 50%, which has threatened national energy security. Moreover, the depletion of petroleum resources and the long-term high volatility of petroleum prices have brought unprecedented severe challenges to energy and chemical industries based on petroleum routes. Therefore, it is imperative to develop new technologies to replace petroleum rou...

Examples

Embodiment 1

[0035] After weighing 539 grams of ferric nitrate, 182.5 grams of manganese nitrate (50%), 11.7 grams of lanthanum nitrate and 500 grams of water, mix them uniformly, precipitate with 500 grams of concentrated ammonia water (25%), and after aging for 12 hours at room temperature, wash , centrifuged, dried at 120°C for 8 hours, and calcined at 550°C for 6 hours to obtain Fe-Mn oxide solid. Weigh 72.1 g Fe-Mn oxide solid, impregnate 42 g containing 0.53 g K 2 CO 3 Aqueous solution, dried at 120°C for 6 hours, calcined at 500°C for 4 hours to obtain Fe composite component F-1.

[0036] Weigh 60 grams of ZSM-5 molecular sieves (the molar ratio of silicon oxide to aluminum oxide is 400), impregnate with 116 grams of aqueous solution containing 36.7 grams of zinc nitrate and 16.2 grams of phosphoric acid (85%), and after aging for 4 hours at room temperature MZ1 was obtained by drying at 120°C for 8 hours and calcining at 600°C for 6 hours.

[0037] Weigh 40 grams of F-1, 40 gram...

Embodiment 2-7

[0040] F2-F9 were prepared by the same method as in Example 1, and their compositions are listed in Table 1.

[0041] Catalysts b to i were prepared by the same method as in Embodiment 1, and the evaluation method was the same as in Embodiment 1.

[0042] Catalyst components and evaluation results are listed in Table 2 and Table 3, respectively.

Embodiment 8-11

[0050] Using catalyst e, the evaluation conditions and evaluation results are shown in Table 4.

[0051] Table 1

[0052] Fe composite oxide

Weight composition (wt%)

F-1

74.7Fe: 20Mn: 0.3K: 5.0La

F-2

50Fe: 25Mn: 5Na: 10La

F-3

39.9Fe: 50Mn: 10Mg: 0.1La

F-4

58.5Fe: 35Mn: 4.0K: 2.5.0Ce

[0053] F-5

55.3Fe: 35.2Mn: 5.2Ca: 4.3Zn

F-6

50.4Fe: 38.7Mn: 6.0K: 2.0Ce: 2.9Si

F-7

65Fe: 25Mn: 4.8K: 2.0La: 2.2Ce: 1.0Ga

F11

50.4Fe: 38.7Mn: 6.0K: 2.9Si (weight ratio)

F12

65Fe: 25Mn: 4.8K: 1.0Ga (weight ratio)

[0054] Table 2

[0055]

[0056] table 3

[0057] Example

catalyst

Aromatics yield / %

1

a

69.7

2

b

72.3

3

c

71.0

4

d

70.2

5

e

79.2

6

f

59.7

7

g

56.8

8

h

63.2

9

i

57.6

comparative example

1

x

54.2

2

y

...

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