Calcium-titanium-ore type composite oxide La1-xSrxMO3-0.5 beta F beta

A composite oxide and perovskite-type technology, applied in the direction of metal/metal oxide/metal hydroxide catalysts, chemical instruments and methods, chemical/physical processes, etc., can solve the problem of expanding reactor scale, high temperature gradient, Explosion hazard etc.

Inactive Publication Date: 2007-11-14
NANJING UNIV
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

The two main technical problems to be solved in the process of selective oxidation to synthesis gas are: 1. High temperature gradient; 2. CH 4 / O 2 Explosion hazard from co-feeds (usually within flammability and explosion limits)
Oxygen ion transport membrane (ITM) technology seems to meet the requirements of selective oxidation to synthesis gas [see Appl. Solve the problem of scaling up the reactor and sealing the reactor [see Solid State Ionics 86(1996) 1267]

Method used

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  • Calcium-titanium-ore type composite oxide La1-xSrxMO3-0.5 beta F beta
  • Calcium-titanium-ore type composite oxide La1-xSrxMO3-0.5 beta F beta

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Experimental program
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Effect test

Embodiment 1

[0027] 5.09g La(NO3 ) 3 ·6H 2 O, 0.73g Sr(NO 3 ) 2 , 7.05g Fe(NO 3 ) 3 9H 2 O was dissolved in 100ml of distilled water to obtain a mixed solution. 7.87 g of glycine was added to the above mixed solution. The above solution was stirred continuously at 70°C and evaporated slowly until a viscous colloidal liquid was obtained. The colloidal liquid was heated in a muffle furnace at 250°C for 0.5 h to make it react quickly to obtain a powdery precursor. The precursor was calcined in air at 900 °C for 5 h to obtain the activated oxygen carrier La 0.8 Sr 0.2 FeO 3 . Sample specific surface area 6.1m 2 / g, the crystal phase contained is mainly a perovskite structure composite oxide (see Figure 1a).

[0028] The oxidation performance of the composite oxide of the present invention was tested by methane pulse reaction. In the methane pulse reaction, the carrier gas was argon with a flow rate of 23.5 ml / min. Pulse injection gas is CH 4 / Ar mixed gas, wherein the methane c...

Embodiment 2

[0030] 4.00g La(NO 3 ) 3 ·6H 2 O, 1.53g Sr(NO 3 ) 2 , 7.38g Fe(NO 3 ) 3 9H 2 O was dissolved in 100ml of distilled water to obtain a mixed solution. 7.95 g of glycine was added to the above mixed solution. The above solution was stirred continuously at 70°C and evaporated slowly until a viscous colloidal liquid was obtained. The colloidal liquid was heated in a muffle furnace at 250°C for 0.5 h to make it react quickly to obtain a powdery precursor. The precursor was calcined in air at 900 °C for 5 h to obtain the activated oxygen carrier La 0.6 Sr 0.4 FeO 3 . Sample specific surface area 6.9m 2 / g, the crystal phase contained is mainly a perovskite structure composite oxide (see Figure 1b).

[0031] The oxidation performance of the composite oxide of the present invention was tested by methane pulse reaction. In the methane pulse reaction, the carrier gas was argon with a flow rate of 23.5 ml / min. Pulse injection gas is CH 4 / Ar mixed gas, wherein the methane...

Embodiment 3

[0033] 8.67g La(NO 3 ) 3 2H 2 O, 1.27g Sr(NO 3 ) 2 , 10.74g 50%Mn(NO 3 ) 2 The solution was added to 100 ml of distilled water to obtain a mixed solution. 10.81 g of glycine was added to the above mixed solution. The above solution was stirred continuously at 70°C and evaporated slowly until a viscous colloidal liquid was obtained. The colloidal liquid was heated in a muffle furnace at 250°C for 0.5 h to make it react quickly to obtain a powdery precursor. The precursor was calcined in air at 900 °C for 5 h to obtain the activated oxygen carrier La 0.8 Sr 0.2 MnO 3 . Sample specific surface area 13.4m 2 / g, the contained crystal phase is a perovskite structure composite oxide (see Figure 2b).

[0034] The oxidation performance of the composite oxide of the present invention was tested by methane pulse reaction. In the methane pulse reaction, the carrier gas was argon with a flow rate of 23.5 ml / min. Pulse injection gas is CH 4 / Ar mixed gas, wherein the methane...

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Abstract

The present invention relates to a kind of La1-x Srx MO3-0.5 beta F beta composite oxide, in which M-Mn or Fe or Ni, x=0-0.4, beta=0-0.1, x and beta are not zero at the same time. It is mainly formed from perovskite composite oxide, the phase composition is directly related to Sr content in the sample, and its specific surface area is 4.5-13.4 sq.m/g. The invented La1-x SrxMO3-0.5 beta F beta composite oxide can be used as an oxygen carrier, its lattice oxygen can be utilized for directly oxidate methane to prepare synthetic gas. In the reaction temperature range of 800-900deg.C its CH4 conversion rate is 15-55%, CO selectivity is 5-99%, and H2/CO (mol/mol)=1.9-10.5:1.0. Said invention also discloses its preparation method.

Description

technical field [0001] The invention relates to a perovskite type composite oxide and the synthesis gas produced by oxidizing methane with lattice oxygen on the composite oxide. Background technique [0002] Natural gas (contains >90% CH 4 ) will become the most important primary energy in the first half of this century. Sulfur compounds in natural gas are easier to remove than those in oil, making it a cleaner energy source. In addition to burning natural gas as a primary energy source, it can also be converted into synthesis gas, and then through F-T synthesis to produce liquid fuels and other high value-added chemical products, such as methanol, ammonia and dimethyl ether [see Catal.Today 64 (2001) 31]. The current rising oil price forces people to think about how to fully and effectively utilize natural gas resources. The H / C atomic ratio in natural gas is about twice that of petroleum, making it an ideal raw material for hydrogen production. Hydrogen energy has ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/34B01J23/83B01J23/02B01J27/12C01B3/36B01J37/04
Inventor 季伟捷魏昊娟李然家陈懿沈师孔
Owner NANJING UNIV
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