Preparation method and application of catalyst for preparing 2-methylnaphthalene/2, 6-dimethylnaphthalene from synthesis gas and naphthalene through one-step method

A technology of dimethylnaphthalene and catalyst, which is applied in the field of preparation and application of a catalyst for the one-step synthesis of 2-methylnaphthalene/2,6-dimethylnaphthalene from synthesis gas and naphthalene, and can solve the problem of low equilibrium conversion rate of methanol , Catalyst deactivation due to carbon deposits, low conversion rate per pass, etc., to achieve significant economic advantages, low production cost, and high product selectivity

Active Publication Date: 2021-04-16
NORTHWEST UNIV(CN)
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Although the above-mentioned two-step technical route is relatively mature, there are the following problems: first, due to thermodynamic constraints, the equilibrium conversion rate of synthesis gas to methanol is low, and a large amount of raw material gas needs to be recycled, which increases the operating cost; second, methanol itself reacts (such as methanol to olefins) is easier to carry out than the methylation of methanol and naphthalene, so that a large amount of methanol fails to participate in the methylation reaction, resulting in a low single-pass conversion rate of benzene, and methanol is easy to generate a large amount of low Carbon deposition precursors such as carbon olefins make the catalyst easy to deactivate by carbon deposition

Method used

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  • Preparation method and application of catalyst for preparing 2-methylnaphthalene/2, 6-dimethylnaphthalene from synthesis gas and naphthalene through one-step method
  • Preparation method and application of catalyst for preparing 2-methylnaphthalene/2, 6-dimethylnaphthalene from synthesis gas and naphthalene through one-step method
  • Preparation method and application of catalyst for preparing 2-methylnaphthalene/2, 6-dimethylnaphthalene from synthesis gas and naphthalene through one-step method

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preparation example Construction

[0035] The present invention is used for the preparation method of the catalyst of syngas and naphthalene one-step method system 2-methylnaphthalene / 2,6-dimethylnaphthalene, comprises the following steps:

[0036] Metal oxide part:

[0037] 1) Co-precipitation method to prepare ZnAlCrOx metal oxide

[0038] Step 1: Dissolve 0.01-0.04mol of zinc nitrate, 0.01-0.04mol of aluminum nitrate and 0.01-0.04mol of chromium nitrate in 120-140mL of deionized water;

[0039] Step 2: add 18g urea to the solution of above-mentioned step 1;

[0040] Step 3: Under continuous stirring, heat up to 90-110°C and keep for 8-12h;

[0041] Step 4: Cool down, leave to age overnight (ie 12h), then centrifuge and wash several times, dry overnight at 100°C, and finally roast at 400-600°C for 4-6h to obtain ZnAlCrOx metal oxide.

[0042] ZnZrO was simultaneously prepared by the above method x , InZrO x , ZnAlO x , ZnGaO x and other metal oxides.

[0043] Zinc nitrate in the above steps is replaced ...

Embodiment 1

[0056] Example 1ZnAlCrO x &HZSM-5 is specifically prepared through the following process:

[0057] ZnAlCrOx metal oxide is prepared by co-precipitation method, the zinc nitrate of 0.024mol, the aluminum nitrate of 0.008mol and the chromium nitrate of 0.008mol are dissolved in 140mL deionized water; Add 18g urea in the above-mentioned solution; Under continuous stirring, Raise the temperature to 110°C and keep it for 10h; cool down, let stand for aging overnight (ie 12h), then centrifuge and wash several times, dry at 100°C overnight, and finally bake at 500°C for 4h to obtain ZnAlCrOx metal oxide.

[0058] HZSM-5 is a commercial molecular sieve.

[0059] Weigh the above 0.6g of ZnAlCrOx metal oxide and 0.6g of HZSM-5 molecular sieve, and grind them in an agate mortar for 30 minutes to make them evenly mixed. Then put the above-mentioned mixed powder into a tablet machine, and sieve through the tablet to obtain 20-40 mesh ZnAlCrO x &HZSM-5 particles.

Embodiment 2Z

[0060] Example 2ZnZrO x & Preparation of HZSM-5

[0061] ZnZrO x The metal oxide is prepared by co-precipitation method. Dissolve 0.004mol of zinc nitrate and 0.036mol of zirconium nitrate in 140mL of deionized water; add 18g of urea to the above solution; heat up to 110°C under continuous stirring, and keep 10h; cool down, let it stand for aging overnight (ie 12h), then centrifuge and wash several times, dry at 100°C overnight, and finally roast at 500°C for 4h to obtain ZnZrO x Metal oxide.

[0062] HZSM-5 is the same as embodiment 1.

[0063] Weigh the above 0.6g of ZnZrO x The metal oxide and 0.6g of HZSM-5 molecular sieve were ground in an agate mortar for 30 minutes to make them evenly mixed. Then put the above mixed powder into the tablet machine, and sieve it through the tablet to obtain 20-40 mesh ZnZrO x &HZSM-5 particles.

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Abstract

The invention relates to a preparation method and application of a catalyst for preparing 2-methylnaphthalene / 2, 6-dimethylnaphthalene from synthesis gas and naphthalene through one-step method, which comprises the following steps: mixing one of ZnAlCrOx, ZnZrOx, InZrOx, ZnAlOx and ZnGaOx with a molecular sieve in equal mass, and tabletting to obtain the catalyst, being 20 ~ 40 meshes, for preparing 2-methylnaphthalene / 2, 6-dimethylnaphthalene from synthesis gas and naphthalene through one-step method. According to the invention, synthesis gas is converted into active intermediates such as methanol on a metal catalyst, and then the active intermediates and naphthalene are subjected to a methylation reaction at the acid site of a zeolite molecular sieve. Therefore, the invention for producing high-added-value chemicals through the methylation reaction of the synthesis gas and naphthalene has the advantages of short process route, high naphthalene conversion rate, high catalyst stability, high target product selectivity and the like, and is more economical and efficient.

Description

technical field [0001] The invention relates to the technical field of polycyclic aromatic hydrocarbons alkylation conversion into high value-added chemicals, in particular to the preparation of a catalyst for the one-step preparation of 2-methylnaphthalene / 2,6-dimethylnaphthalene from synthesis gas and naphthalene method and application. Background technique [0002] At present, the research on the alkylation of methanol and aromatic hydrocarbons has entered a relatively mature stage from the development of catalysts to the discussion of the reaction mechanism. Research further matures. However, there are still relatively few studies on the alkylation of PAHs. Because polycyclic aromatic hydrocarbons have more reactive sites, catalyst deactivation is more serious than monocyclic aromatic hydrocarbons. In recent years, due to the rapid development of new polymer materials, the demand for polycyclic aromatic hydrocarbons has gradually increased, making the research on poly...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/40B01J29/48B01J29/78B01J29/85C07C15/24C07C2/86
CPCY02P20/584
Inventor 代成义赵潇唐忠强金润泽任高升
Owner NORTHWEST UNIV(CN)
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