Perovskite type composite metal oxide oxygen carrier as well as preparation method and application thereof

A composite metal, perovskite-type technology, applied in the field of oxygen carriers, can solve the problems of poor structural stability of composite oxides, low reactivity of oxygen carriers, low selectivity of oxidation products, etc., and is conducive to industrial promotion and use, Low cost and stable structure

Active Publication Date: 2020-03-13
TIANJIN UNIV +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0007] The present invention aims at the low reactivity of single oxide oxygen carrier, low selectivity of methane partial oxidation product (synthesis gas) and low hydrogen production efficiency commonly existing in the existing chemical chain methane reforming reaction; the reactivity of composite oxide oxygen carrier low, poor structural stability of doped composite oxides and other technical problems, a perovskite-type composite metal oxide oxygen carrier and its preparation method are provided, and its application in the chemical chain methane reforming reaction. La 3+ Trivalent ions of the same valence state pair LaFeO 3 A-site doping, without changing the perovskite lattice structure, can ensure that the oxygen carrier has high structural stability, and at the same time modulate its surface reactive site and oxygen ion migration ability, and prepare cycle Oxygen carrier with good stability and high selectivity for syngas

Method used

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  • Perovskite type composite metal oxide oxygen carrier as well as preparation method and application thereof
  • Perovskite type composite metal oxide oxygen carrier as well as preparation method and application thereof
  • Perovskite type composite metal oxide oxygen carrier as well as preparation method and application thereof

Examples

Experimental program
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Effect test

Embodiment 1

[0042] Step 1, weigh 4.3412g of cerium nitrate hexahydrate Ce (NO 3 ) 3 ·6H 2 O, 4.0399g of iron nitrate nonahydrate Fe (NO 3 ) 3 9H 2 O and complexing agent 4.6114g citric acid are dissolved in 50mL deionized water and are configured as a precursor solution, wherein the mol ratio of citric acid and the total amount of metal ions in the precursor solution is 1.2:1;

[0043] Step 2, the solution obtained in step 1 was evaporated to dryness at 90°C under stirring conditions until it became gelatinous, and the stirring rate was 600rpm; then it was aged in a constant temperature drying oven at 200°C for 24 hours, and the obtained precursor powder was dried at 1000°C in an air atmosphere Calcined for 6 hours to obtain the lanthanum cerium iron perovskite oxygen carrier, denoted as CeFeO 3 ;

[0044] Step 3, the CeFeO 3 The solid powder is compressed into tablets, sieved, and the granular oxygen carrier with a size of 20-40 mesh is taken.

Embodiment 2

[0046] Step 1, weigh 4.3412g of cerium nitrate hexahydrate Ce (NO 3 ) 3 ·6H 2 O, 4.0399g of iron nitrate nonahydrate Fe (NO 3 ) 3 9H 2 O and complexing agent 4.6114g citric acid are dissolved in 50mL deionized water and are configured as a precursor solution, wherein the mol ratio of citric acid and the total amount of metal ions in the precursor solution is 1.2:1;

[0047] Step 2, the solution obtained in step 1 was evaporated to dryness at 90°C under stirring conditions until it became gelatinous, and the stirring rate was 600rpm; then it was aged in a constant temperature drying oven at 200°C for 24 hours, and the obtained precursor powder was dried at 1000°C in a carbon dioxide atmosphere Calcined for 6 hours to obtain the lanthanum cerium iron perovskite oxygen carrier, denoted as CeFeO 3 ;

[0048] Step 3, the CeFeO 3 The solid powder is compressed into tablets, sieved, and the granular oxygen carrier with a size of 20-40 mesh is taken.

Embodiment 3

[0050] Prepared with the method of Example 2, the only difference is that the complexing agent in step (1) uses 1.4900g ethylene glycol, and the molar ratio of ethylene glycol to the total amount of metal ions in the precursor solution is 1.2:1.

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Abstract

The invention belongs to the technical field of oxygen carriers, and discloses a perovskite type composite metal oxide oxygen carrier and a preparation method and application thereof. The perovskite type composite metal oxide oxygen carrier is of a perovskite structure, the general formula of the oxygen carrier is La<1-x>Ce<x>FeO<3>, and x is greater than 0 and less than or equal to 1. A sol-gel method is adopted in the preparation method, and the preparation method comprises the following steps: firstly, taking lanthanum nitrate, cerium nitrate and ferric nitrate as precursors, and preparinga solution from the precursors and a complexing agent; then evaporating to remove water, and converting an obtained transparent sol into a viscous gel; and aging and roasting to obtain the composite metal oxide oxygen carrier with a perovskite structure. When the perovskite type composite metal oxide oxygen carrier is chemical-looping methane reforming reaction, methane can be partially oxidized with high activity and high selectivity to prepare synthesis gas; meanwhile, the oxygen carrier is reduced to be in a low valence state, the reduced oxygen carrier can react with carbon dioxide or water vapor to be oxidized to be in a high valence state, lattice oxygen is obtained again, cyclic regeneration of the oxygen carrier is achieved, and meanwhile carbon dioxide is converted into carbon monoxide or the water vapor is converted into hydrogen gas.

Description

technical field [0001] The present invention belongs to the technical field of oxygen carrier, and specifically relates to a perovskite type composite metal oxide oxygen carrier and a preparation method thereof, and the use of the perovskite type composite metal oxide oxygen carrier in chemical chain Application of methane reforming to synthesis gas and hydrogen. [0002] technical background [0003] With the rapid development of the global economy, the consumption of fossil energy such as coal and oil is accelerating, but their reserves are limited and will eventually be exhausted. In addition, the unclean use of fossil fuels has led to increasingly serious environmental pollution and the deterioration of the human living environment. Methane is the main component of natural gas and shale gas. my country's natural gas and shale gas resources are very rich, and the reserves of both rank among the top in the world. Compared with coal and petroleum petrochemical energy, how t...

Claims

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Application Information

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IPC IPC(8): B01J23/83B01J23/94C01B3/40
CPCB01J23/002B01J23/83B01J23/94C01B3/40B01J2523/00C01B2203/0227B01J2523/3706B01J2523/3712B01J2523/842Y02P20/584Y02P20/52
Inventor 巩金龙王宗宝张先华苏迎辉刘蕊肖海成王林王奕然李庆勋
Owner TIANJIN UNIV
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