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Highly dispersed ZnO-based catalyst as well as preparation method and propane anaerobic dehydrogenation method thereof

A catalyst and highly dispersed technology, which is applied in the direction of catalyst activation/preparation, molecular sieve catalysts, and catalysts containing molecular sieves. It can solve the problems of easy loss of active components of catalysts, expensive precious metal catalysts, and environmental pollution of Cr-based catalysts. Achieve good catalysts The effect of stability, easy operation and low cost

Active Publication Date: 2018-11-02
CHINA UNIV OF PETROLEUM (BEIJING)
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

CN101785993A discloses a kind of use ZnO as the dehydrogenation active component, the HZSM-5 molecular sieve with high silicon-aluminum ratio is used as the carrier, adopts the method of ordinary impregnation, 5wt% ZnO is loaded on the carrier, under the condition of using carbon dioxide as the weak oxidizing agent For the aerobic dehydrogenation reaction of propane, it has good propane aerobic dehydrogenation activity, but the active components of the catalyst are easy to lose, resulting in a decrease in activity
Thus ZnO can be used as an active component for the dehydrogenation of low-carbon alkanes, but its activation ability to short-chain hydrocarbons such as propane is not enough, and ZnO is easy to lose under high temperature reaction conditions. Therefore, it is necessary to improve the activation ability of ZnO to propane and Its high temperature loss resistance is a problem for the wide application of ZnO-based catalysts
[0005] In the literature disclosed above, most of the anaerobic dehydrogenation reactions of propane use the noble metal Pt or environmentally unfriendly Cr as the dehydrogenation active component. The easy sintering of components and the environmental pollution of Cr-based catalysts limit their large-scale utilization

Method used

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  • Highly dispersed ZnO-based catalyst as well as preparation method and propane anaerobic dehydrogenation method thereof
  • Highly dispersed ZnO-based catalyst as well as preparation method and propane anaerobic dehydrogenation method thereof
  • Highly dispersed ZnO-based catalyst as well as preparation method and propane anaerobic dehydrogenation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0046] This embodiment provides a preparation method of a highly dispersed ZnO-based catalyst, wherein the mass content of ZnO is 2.8wt%, which is obtained according to the following steps:

[0047] At room temperature, weigh 5g of Silicalite-1 carrier and disperse it in 100mL of methanol, stir and sonicate to obtain a homogeneous mixture I;

[0048] Weigh 1.5g of zinc nitrate hexahydrate and add it to mixture I, and continue to stir at 25°C for 30 minutes to fully dissolve it to obtain mixture II;

[0049] Add 8.75g of 2-methylimidazole to the mixture II, continue to stir at 25°C for 10 hours to obtain ZIF-8 / Silicalite-1, and dry the catalyst at 40°C overnight after centrifugation and washing;

[0050] Place the dried ZIF-8 / Silicalite-1 in a tube furnace under N 2 Under the atmosphere, the temperature was raised to 700 °C at a rate of 7 °C / min and kept for 2 hours to obtain ZnO@NC / Silicalite-1, which was marked as 1#.

[0051] The above-mentioned 1# catalyst is used in the ...

Embodiment 2

[0057] This embodiment provides a method for preparing a highly dispersed and stable ZnO catalyst, wherein, ZnO@NC / Silicalite-1 catalyst (1# catalyst) is prepared according to Example 1; the obtained ZnO@NC / Silicalite-1 catalyst Weigh 1g and stir in 20mL 0.3M nitric acid solution at 25°C for 30 minutes to obtain 2# catalyst. Compared with 1# catalyst, except that the catalyst was stirred in 0.3M nitric acid for 30 minutes, the rest of the preparation process and evaluation conditions All the same as in Example 1. The results of anaerobic dehydrogenation of propane with 2# catalyst are shown in Table 2.

[0058] Table 2 The reaction result (2#) of anaerobic dehydrogenation of propane

[0059] time / min

Embodiment 3

[0061] This example provides a method for preparing a highly dispersed and stable ZnO-based catalyst. ZnO@NC / Silicalite-1 catalyst (1# catalyst) is prepared according to Example 1; the obtained ZnO@NC / Silicalite-1 catalyst is called Take 1g and stir in 20mL 0.5M nitric acid solution at 25°C for 30 minutes to obtain 3# catalyst. Compared with 1# catalyst, except that the catalyst was stirred in 0.5M nitric acid for 30 minutes, the rest of the preparation process and evaluation conditions were the same. Same as Example 1. The results of anaerobic dehydrogenation of propane with 3# catalyst are shown in Table 3.

[0062] Table 3 The reaction result (3#) of anaerobic dehydrogenation of propane

[0063] time / min

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Abstract

The invention provides a highly dispersed ZnO-based catalyst as well as a preparation method and a propane anaerobic dehydrogenation method thereof. The preparation method of the catalyst comprises the following steps: dispersing Silicalite-1 into a solvent so as to obtain a suspension I; putting a zinc source into the suspension I, and stirring so as to obtain a suspension II; putting 2-methylimidazole into the suspension II, and stirring so as to obtain a ZIF-8 / Silicalite-1 compound; and centrifuging the ZIF-8 / Silicalite-1 compound, washing, drying, and carrying out pyrolysis in a nitrogen atmosphere, thereby obtaining a ZnO@ / NC / Silialite-1 catalyst, namely the highly dispersed ZnO-based catalyst. Due to acid pickling, the stability of the catalyst can be also improved. The invention further provides a catalyst prepared by using the method and a propane anaerobic dehydrogenation method using the catalyst. The catalyst provided by the invention has no harsh requirement on a propane anaerobic dehydrogenation process, is capable of achieving efficient conversion of propane, and meanwhile has high catalyst stability.

Description

technical field [0001] The invention relates to a highly dispersed ZnO-based catalyst, a preparation method thereof and an oxygen-free dehydrogenation method of propane, belonging to the technical field of petrochemical industry. Background technique [0002] Propylene is a basic chemical raw material, which can be used to produce industrial products such as polypropylene, acrylonitrile, and propylene oxide. At present, the main sources of propylene are naphtha steam cracking and by-products of fluid catalytic cracking. With the increasing scarcity of petroleum resources, the demand for downstream products of propylene continues to increase, and the production of propylene solely relying on petroleum resources as raw materials cannot meet the current demand for propylene. Propane is one of the components of shale gas. Due to the continuous development of shale gas mining technology in recent years, the use of propane in shale gas to convert it into propylene through anaerob...

Claims

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Application Information

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IPC IPC(8): C07C5/333C07C11/06B01J29/03B01J35/00B01J37/08B01J37/06
CPCC07C5/3332B01J29/03B01J29/0308B01J37/06B01J37/082C07C2529/03B01J2229/20B01J35/394B01J35/393C07C11/06Y02P20/52
Inventor 李宇明姜桂元赵丹王雅君赵震徐春明
Owner CHINA UNIV OF PETROLEUM (BEIJING)
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