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Catalyst for preparing ethylene through ethane dehydrogenation under carbon dioxide atmosphere, and preparation method thereof

A carbon dioxide and catalyst technology, which is applied in the field of catalysts for ethylene production by dehydrogenation of ethane in a carbon dioxide atmosphere and its preparation field, can solve the problems of lack of price catalysts, improved ethylene selectivity and the like, and achieves simple preparation method, ethylene selectivity and high yield. High rate, slow inactivation effect

Active Publication Date: 2017-04-19
FUDAN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Our research group has also reported a catalyst with submicron NaZSM-5 zeolite as the carrier and chromium oxide as the active component (Y. Cheng et al. Chin J Catal, 2015, 36, 1242). The reaction of ethane dehydrogenation to ethylene has good activity and stability, but the selectivity of ethylene still needs to be further improved
All in all, the lack of low-cost and high-performance catalysts is the main problem in the field of oxidative dehydrogenation of ethane carbon dioxide to ethylene.

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0023] Using silicalite-1 with a grain size of about 300 nm as the carrier, Cr(NO 3 ) 3 9H 2 O as a precursor, impregnated with 0.5wt% Cr at a liquid-solid ratio of 2mL / g 2 o 3 , the slurry was heated, stirred and dried under an infrared lamp, dried at 110° C. for 4 hours, and calcined at 600° C. for 4 hours in an air atmosphere to obtain Catalyst-1.

[0024] The above catalysts were measured in a continuous microreactor 2 Ethane dehydrogenation activity under atmosphere. The specific reaction conditions are as follows: the amount of catalyst is 0.2 g, the catalyst is activated at 650 °C under nitrogen atmosphere for 1 hour before the reaction, and then the reaction gas is introduced at 650 °C, the reaction pressure is 1 atm, and the total flow rate of the reaction gas is 30 mL / min. The gas composition is 3 vol% ethane, 15 vol% CO 2 , and the rest is nitrogen. The initial ethylene yield of catalyst-1 was 36.2%, and the ethylene selectivity was 93.0%; after 6 hours of re...

Embodiment 2

[0026] Using silicalite-1 with a grain size of about 80 nm as the carrier, Cr(NO 3 ) 3 9H 2 O was used as a precursor, and 0.5wt% Cr was impregnated at a liquid-solid ratio of 3 mL / g 2 o 3 , the slurry was heated, stirred and dried under an infrared lamp, dried at 110°C for 8 hours, and calcined at 550°C in an air atmosphere for 8 hours to obtain Catalyst-2. Utilize the method for example 1 to measure catalyst-2 in CO 2 Ethane dehydrogenation activity under atmosphere. The initial ethylene yield of catalyst-2 was 33.8%, and the ethylene selectivity was 93.4%; after 6 hours of reaction, the ethylene yield was 31.3%, and the ethylene selectivity was 93.3%.

Embodiment 3

[0028] Using silicalite-1 with a grain size of about 400 nm as the carrier, Cr(NO 3 ) 3 9H 2 O as a precursor, impregnated with 3.0wt% Cr at a liquid-solid ratio of 4 mL / g 2 o 3 , the slurry was heated, stirred and dried under an infrared lamp, dried at 110°C for 8 hours, and calcined at 750°C for 10 hours in an air atmosphere to obtain Catalyst-3. Utilize the method for example 1 to measure catalyst-3 in CO 2 Ethane dehydrogenation activity under atmosphere. The initial ethylene yield of catalyst-3 was 49.7%, and the ethylene selectivity was 77.0%; after 6 hours of reaction, the ethylene yield was 48.5%, and the ethylene selectivity was 78.0%.

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Abstract

The invention belongs to the technical field of chemical catalysts, and specifically discloses a catalyst for preparing ethylene through ethane dehydrogenation under a carbon dioxide atmosphere, and a preparation method thereof. The existing catalyst has the shortages of high dosage of chromium, low selectivity of ethylene, low stability, and the like. According to the catalyst disclosed by the invention, small-crystal-grain all-silicon silicalite-1 with an MFI structure is taken as a support, chromium oxide is taken as an active component with a content of 0.3%-5.0%. A soluble chromium salt is taken as a precursor and introduced into the silicalite-1 zeolite by virtue of an impregnation method, and then is prepared into a supported catalyst through roasting during preparation. According to the preparation method disclosed by the invention, the impregnation method is adopted, and the preparation process is simple and convenient. The catalyst is used for a reaction of preparing ethylene through ethane dehydrogenation under a carbon dioxide atmosphere, and has the advantages of being simple in process, high in activity, high in selectivity and stability, and the like.

Description

technical field [0001] The invention belongs to the technical field of chemical catalysts, and in particular relates to a catalyst used for dehydrogenating ethane to produce ethylene under a carbon dioxide atmosphere and a preparation method thereof. Background technique [0002] Ethylene is a very important intermediate in petrochemical industry, and its production mainly comes from the cracking process of naphtha or light oil. As oil resources become increasingly tight, the use of abundant and cheap sources of ethane dehydrogenation to produce ethylene can avoid the oil route, thus attracting more and more attention. [0003] Although the dehydrogenation of ethane to ethylene has been industrialized, due to the limitation of thermodynamic equilibrium conversion rate, the process requires a relatively high temperature to obtain the ideal ethylene yield. The high reaction temperature leads to the decline of ethylene selectivity, severe catalyst deactivation, frequent regene...

Claims

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Application Information

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IPC IPC(8): B01J29/035C07C5/333C07C11/04
CPCB01J29/0358B01J2229/18C07C5/3332C07C2523/26C07C2529/035C07C11/04Y02P20/52
Inventor 程彦虎乐英红雷天起华伟明高滋
Owner FUDAN UNIV
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