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Composite oxide catalyst for preparing propylene by oxidative dehydrogenation of propane and preparation method thereof

A composite oxide and oxidative dehydrogenation technology, which is applied in metal/metal oxide/metal hydroxide catalysts, physical/chemical process catalysts, hydrocarbons, etc., can solve the problems of easy deactivation of catalysts and achieve easy preparation , low price, and the effect of improving selectivity

Inactive Publication Date: 2004-12-29
FUDAN UNIV
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  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Nickel molybdate is one of the more effective dehydrogenation catalysts, especially for the oxidative dehydrogenation of propane to propylene. The selectivity is only 63% [J.Catal., 1997,170:346]; phosphate catalysts can be divided into pyrophosphate, substituted vanadium aluminum phosphate and molybdenum phosphate, and there are few research reports at present; rare earth oxyfluoride It has good catalytic performance for the selective oxidation of low-carbon alkanes, especially for the oxidative dehydrogenation of propane to propylene. The best result is at 500 ° C, at 3% Cs 2 O / 2CeO 2 / CeF 3 The propane conversion rate is 53.4%, the propylene selectivity is about 67.5%, and the propylene yield reaches 36% [Catal.Today, 1999, 51:161], but this type of catalyst is very easy to deactivate

Method used

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  • Composite oxide catalyst for preparing propylene by oxidative dehydrogenation of propane and preparation method thereof

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Experimental program
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Effect test

Embodiment 1

[0014] 17.3 g Ce(NO 3 ) 3 ·6H 2 O and 1.5 g Ni(NO 3 ) 2 ·6H 2 O was dissolved in 100 mL of absolute ethanol. Dissolve 7.6 grams of oxalic acid in 100 milliliters of absolute ethanol, slowly add the ethanol solution of oxalic acid into the cerium and nickel solution under vigorous stirring at room temperature, and stir for 4 hours. Then centrifuge, wash, dry overnight at 120°C, and bake at 500°C for 2 hours in an air atmosphere. The molar ratio of cerium and nickel in the prepared nanocomposite catalyst is 8:1. The reaction condition of oxidative dehydrogenation of propane to propylene is: the ratio of reaction gas is C 3 h 8 :O 2 :N 2 =16:16:68, reaction temperature 300°C, catalyst consumption 0.15g, space velocity 6000h -1 . Analysis of the reaction tail gas shows that the conversion rate of propane is 28.2%, the selectivity to propylene is 18.9%, and the yield of propylene is 5.3%.

Embodiment 2

[0016] 17.3 g Ce(NO 3 ) 3 ·6H 2 O and 2.9 g Ni(NO 3 ) 2 ·6H 2 O was dissolved in 120 ml absolute ethanol. Dissolve 7.6 grams of oxalic acid in 100 milliliters of absolute ethanol, slowly add the ethanol solution of oxalic acid into the cerium and nickel solution under vigorous stirring at room temperature, and stir for 8 hours. Then centrifuge, wash, dry overnight at 120°C, and bake at 700°C for 2 hours in an air atmosphere. The molar ratio of cerium and nickel in the prepared nanocomposite catalyst is 4:1. The reaction condition of oxidative dehydrogenation of propane to propylene is: the ratio of reaction gas is C 3 h 8 :O 2 :N 2 =16:16:68, reaction temperature 300°C, catalyst consumption 0.15g, space velocity 6000h -1 . Analysis of the reaction tail gas shows that the conversion rate of propane is 34.3%, the selectivity to propylene is 18.9%, and the yield of propylene is 6.5%.

Embodiment 3

[0018] Put 13.0 g Ce(NO 3 ) 3 ·6H 2 O and 8.7 g Ni(NO 3 ) 2 ·6H 2 O was dissolved in 120 ml absolute ethanol. Dissolve 9.8 grams of oxalic acid in 120 milliliters of absolute ethanol, slowly add the ethanol solution of oxalic acid into the cerium and nickel solution under room temperature under vigorous stirring, and stir for 4 hours. Then centrifuge, wash, dry overnight at 120°C, and bake at 600°C for 4 hours in an air atmosphere. The molar ratio of cerium and nickel in the prepared nanocomposite catalyst is 1:1. The reaction condition of oxidative dehydrogenation of propane to propylene is: the ratio of reaction gas is C 3 h 8 :O 2 :N 2 =16:16:68, reaction temperature 300°C, catalyst consumption 0.15g, space velocity 6000h -1 . Analysis of the reaction tail gas shows that the conversion rate of propane is 34.6%, the selectivity to propylene is 25.7%, and the yield of propylene is 8.9%.

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Abstract

The present invention belongs to the field of chemical technology, and is one kind of composite nano RE oxide catalyst with low temperature activity for propane oxidizing dehydrogenation process to prepare propylene and its preparation process. The catalyst consists of cerium oxide and transition metal oxide, and has cerium content of 10-90 mol%. The catalyst is prepared through oxalate co-precipitation process including dissolving certain amount of oxalic acid in water or alcohol solution, dripping in solution of soluble salt of cerium and transition metal, ageing in stirring, centrifugal separation, drying, roasting and other steps. The prepared catalyst has unique nano solid solution structure and rather high catalytic activity at low temperature of 300 deg.c, and is used for propane oxidizing dehydrogenation process to prepare propylene to result in propylene yield as high as 15 %.

Description

technical field [0001] The invention belongs to the technical field of chemical industry, and in particular relates to a nano-rare-earth composite oxide catalyst with low-temperature catalytic activity and a preparation method thereof for propane oxidative dehydrogenation to propylene. technical background [0002] my country is a country rich in propane resources, such as Daqing, Zhongyuan, Tarim and other oil fields, the gas is rich in about 6% propane, and the condensate oil contains about 3%-6% (volume fraction, the same below) propane. Propane makes up about 60% of liquefied petroleum gas and up to 15% of natural gas wet gas. Under the action of a suitable catalyst, propane can be selectively oxidized to more useful chemical raw materials such as propylene and acrolein. Among them, propylene is an extremely important basic chemical raw material, which is widely used in the production of acrylonitrile, oxo alcohol, etc. At present, propylene is mainly produced by catal...

Claims

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Application Information

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IPC IPC(8): B01J23/70B01J23/80C07C5/48C07C11/06
CPCY02P20/52
Inventor 曹勇刘永梅伊楠戴维林范康年
Owner FUDAN UNIV
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