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Regeneration method of methane oxygen-free dehydrogenation aromatization catalyst

A dehydrogenation aromatization and catalyst technology, which is applied in physical/chemical process catalysts, molecular sieve catalysts, chemical instruments and methods, etc., can solve the problems of low efficiency, complicated operation of carbon elimination and regeneration methods, etc., and achieves elimination of carbon deposits and easy operation. Process and technology, the effect of reducing unnecessary energy consumption

Active Publication Date: 2016-08-24
CHINA PETROLEUM & CHEM CORP +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0007] The technical problem to be solved by the present invention is that in the prior art, the carbon deposition and deactivation behavior of the methane anaerobic dehydrogenation aromatization catalyst is very easy to exist in the anaerobic reaction process, and the various carbon removal and regeneration methods are complicated to operate and low in efficiency. , providing a regeneration method for methane oxygen-free dehydrogenation aromatization catalyst

Method used

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  • Regeneration method of methane oxygen-free dehydrogenation aromatization catalyst
  • Regeneration method of methane oxygen-free dehydrogenation aromatization catalyst
  • Regeneration method of methane oxygen-free dehydrogenation aromatization catalyst

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0032] Ammonium heptamolybdate and HZSM-5 molecular sieve (SiO 2 / Al 2 o 3The molar ratio is 25) as the Mo species precursor and carrier of the Mo / zeolite-supported catalyst to prepare the catalyst Mo / HZSM-5 for the oxygen-free dehydrogenation of methane, where the weight percentage of Mo is 6%. The specific preparation method of the catalyst is as follows: Weigh 3 g of HZSM-5 and immerse in 2.8 ml of 0.122 g / ml ammonium heptamolybdate aqueous solution, ultrasonically disperse for 0.5 h, let it stand for 12 h, and place o Drying at C, 530 o Calcined at C for 10 h, the obtained powdery Mo / HZSM-5 catalyst was pressed into tablets, crushed, and sieved into 20-60 meshes for later use.

[0033] According to the catalyst evaluation method of Comparative Example 1, the methane raw material gas was contacted with the fresh Mo / HZSM-5 catalyst obtained by the above method to carry out the oxygen-free dehydrogenation aromatization reaction of methane. After 2 hours of reaction, witho...

Embodiment 2

[0039] Ammonium heptamolybdate and HZSM-5 molecular sieve (SiO 2 / Al 2 o 3 The molar ratio is 25) as the Mo species precursor and carrier of the Mo / zeolite-supported catalyst to prepare the catalyst Mo / HZSM-5 for the oxygen-free dehydrogenation of methane, where the weight percentage of Mo is 6%. The specific preparation method of the catalyst is as follows: Weigh 3 g of HZSM-5 and immerse in 2.8 ml of 0.122 g / ml ammonium heptamolybdate aqueous solution, ultrasonically disperse for 0.5 h, let it stand for 12 h, and place o Drying at C, 530 o Calcined at C for 10 h, the obtained powdery Mo / HZSM-5 catalyst was pressed into tablets, crushed, and sieved into 20-60 meshes for later use.

[0040] According to the catalyst evaluation method of Comparative Example 1, the methane raw material gas was contacted with the fresh Mo / HZSM-5 catalyst prepared by the above method to carry out the oxygen-free dehydrogenation aromatization reaction of methane. After 2 hours of reaction, with...

Embodiment 3

[0043] Ammonium heptamolybdate and HZSM-5 molecular sieve (SiO 2 / Al 2 o 3 The molar ratio is 25) as the Mo species precursor and carrier of the Mo / zeolite-supported catalyst to prepare the catalyst Mo / HZSM-5 for the oxygen-free dehydrogenation of methane, where the weight percentage of Mo is 6%. The specific preparation method of the catalyst is as follows: Weigh 3 g of HZSM-5 and immerse in 2.8 ml of 0.122 g / ml ammonium heptamolybdate aqueous solution, ultrasonically disperse for 0.5 h, let it stand for 12 h, and place o Drying at C, 530 o Calcined at C for 10 h, the obtained powdery Mo / HZSM-5 catalyst was pressed into tablets, crushed, and sieved into 20-60 meshes for later use.

[0044] According to the catalyst evaluation method of Comparative Example 1, the methane raw material gas was contacted with the fresh Mo / HZSM-5 catalyst prepared by the above method to carry out the oxygen-free dehydrogenation aromatization reaction of methane. After 2 hours of reaction, with...

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Abstract

The invention relates to a method for regeneration of a methane oxygen-free dehydrogenation aromatization catalyst, which mainly solves the problems in the prior art that it is difficult to regenerate in situ after the catalyst is deactivated by carbon deposits, and the regeneration process is complex in operation, long in cycle and low in production efficiency. . According to the structural characteristics and deactivation mechanism of the methane oxygen-free dehydrogenation aromatization catalyst, the present invention adopts the technical scheme of periodic continuous switching and in-situ regeneration of the regeneration gas composed of methane raw material gas, carbon dioxide and hydrogen, and solves the above problems Problems, can effectively restore the activity of the catalyst and maintain its high catalytic activity for a long time, and can be used in the industrial production of methane anaerobic dehydrogenation aromatization reaction.

Description

technical field [0001] The invention relates to a regeneration method of a methane oxygen-free dehydrogenation aromatization catalyst, which is particularly suitable for the regeneration of a carbon-deactivated Mo / molecular sieve supported catalyst. Background technique [0002] Methane anaerobic dehydroaromatization reaction is a reaction that directly converts methane with considerable reserves and high hydrogen-to-carbon ratio into benzene and hydrogen under anaerobic conditions. It is considered to be a process route for efficient utilization of natural gas resources. Effectively alleviate the current shortage of oil resources (Xu et al., J. Catal. ,2003, 216: 386; Ismagilov et al., Energy Environ. Sci. , 2008, 1: 526). [0003] Since Xu et al. (Xu et al., Catal. Lett. ,1995, 30: 135) proposed that the catalyst for anaerobic dehydroaromatization of methane has dual-functional catalytic properties of dehydrogenation activation and shape-selective cyclization, that is...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C07C15/02C07C15/04C07C15/24C07C5/393B01J29/90
CPCY02P20/52Y02P20/584
Inventor 金中豪秦磊刘苏王仰东
Owner CHINA PETROLEUM & CHEM CORP