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Zinc-containing series perovskite mixing conductor oxygen-penetrating film and its preparation method and application

A hybrid conductor, oxygen-permeable membrane technology, applied in the fields of oxygen preparation, chemical instruments and methods, inorganic chemistry, etc., can solve the problems of large difference in ionic radius, membrane rupture, inability to operate stably for a long time, and achieve high operational stability. , the effect of small thermal expansion coefficient

Inactive Publication Date: 2010-12-08
SOUTH CHINA UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, because Co is easily reduced in a reducing atmosphere, the cobalt (Co) perovskite or perovskite-like structure cannot operate stably for a long time in the partial oxidation of methane to synthesis gas and hydrogen; State like Co 2+ ,Co 3+ ,Co 4+ , the ionic radii of these valence states are quite different. During the heating and cooling process, these valence states will transform into each other, resulting in large expansion and contraction, which will lead to the rupture of the membrane.

Method used

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  • Zinc-containing series perovskite mixing conductor oxygen-penetrating film and its preparation method and application
  • Zinc-containing series perovskite mixing conductor oxygen-penetrating film and its preparation method and application
  • Zinc-containing series perovskite mixing conductor oxygen-penetrating film and its preparation method and application

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0027] Preparation of 0.1 mol Ba by EDTA-citric acid joint complexation 0.5 Sr 0.5 Zn 0.2 Fe 0.8 o 3-δ Powder: weigh Ba(NO 3 ) 2 , Sr(NO 3 ) 2 , Zn(NO 3 ) 2 , Fe(NO 3 ) 3 The four raw materials are dissolved in water to make 0.5mol / lBa(NO 3 ) 2 , 0.4mol / lSr(NO 3 ) 2 , 0.2mol / l Zn(NO 3 ) 2 , 0.8mol / lFe(NO 3 ) 3 solution, take 100ml 0.5mol / lBa(NO 3 ) 2 , 125ml 0.4mol / lSr(NO 3 ) 2 , 100ml 0.2mol / l Zn(NO 3 ) 2 , 100ml 0.8mol / l Fe(NO 3 ) 3 Stir in a heat-resistant beaker for 30 minutes, then add 0.1mol of EDTA and stir for 30 minutes, then add 0.15mol of citric acid and stir for 30 minutes, add 250ml of analytical reagent NH 3 ·H 2 O adjust the pH of the mixed solution to 8, heat and evaporate the mixed solution at 80°C to form a gel, and finally sinter the gel at 950°C for 8 hours to obtain Ba 0.5 Sr 0.5 Zn 0.2 Fe 0.8 o 3-δ Powder, where δ=0~0.5. The obtained powder was subjected to phase analysis, and the results were as follows: figure 1 shown....

Embodiment 2

[0029] Preparation of 0.1 mol Ba by EDTA-citric acid joint complexation 0.2 Sr 0.8 Zn 0.2 Fe 0.8 o 3-δ Powder: weigh Ba(NO 3 ) 2 , Sr(NO 3 ) 2 , Zn(NO 3 ) 2 , Fe(NO 3 ) 3 The four raw materials are dissolved in water to form 0.2mol / lBa(NO 3 ) 2 , 0.8mol / lSr(NO 3 ) 2, 0.2mol / l Zn(NO 3 ) 2 , 0.8mol / lFe(NO 3 ) 3 solution, take 100ml 0.2mol / lBa(NO 3 ) 2 , 100ml 0.8mol / lSr(NO 3 ) 2 , 100ml 0.2mol / l Zn(NO 3 ) 2 , 100ml 0.8mol / l Fe(NO 3 ) 3 Stir in a heat-resistant beaker for 30 minutes, then add 0.1mol of EDTA and stir for 30 minutes, then add 0.15mol of citric acid and stir for 30 minutes, add 250ml of analytical reagent NH 3 ·H 2 O adjust the pH of the mixed solution to 9, heat and evaporate the mixed solution at 100°C to form a gel, and finally sinter the gel at 900°C for 7 hours to obtain Ba 0.5 Sr 0.5 Zn 0.2 Fe 0.8 o 3-δ Powder, where δ=0~0.5. The obtained powder was subjected to phase analysis, and the results were as follows: figure 1 shown....

Embodiment 3

[0031] Preparation of 0.1 mol SrZn by EDTA-citric acid joint complexation 0.2 Fe 0.8 o 3-δ Powder: weigh Sr(NO 3 ) 2 , Zn(NO 3 ) 2 , Fe(NO 3 ) 3 The three raw materials are dissolved in water to make 1mol / lSr(NO 3 ) 2 , 0.2mol / l Zn(NO 3 ) 2 , 0.8mol / l Fe(NO 3 ) 3 solution, take 100ml 1mol / lSr(NO 3 ) 2 , 100ml 0.2mol / l Zn(NO 3 ) 2 , 100ml 0.8mol / l Fe(NO 3 ) 3 Stir in a heat-resistant beaker for 30 minutes, then add 0.1mol of EDTA and stir for 30 minutes, then add 0.15mol of citric acid and stir for 30 minutes, add 250ml of analytical reagent NH 3 ·H 2 O adjust the mixed solution to PH≈8, heat and evaporate the mixed solution at 80°C to form a gel, and finally sinter the gel at 950°C for 8h to obtain SrZn 0.2 Fe 0.8 o 3-δ Powder, where δ=0~0.5. The obtained powder was subjected to phase analysis, and the results were as follows: figure 1 shown.

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Abstract

The invention relates to a zind-based perovskite mixed conducting oxygen-permeable membrane. The chemical formula of the membrane is as follows: BaySr1-yZnxB1-xO3-Delta, wherein B is at least one selected from Fe, Mn, V and Ni; x is more than 0 but less than or equal to 0.2; y is more than or equal to 0 but less than or equal to 1; and Delta is in the range of 0-0.5. The membrane is produced by EDTA-citric acid combined complexation method, including: compression-molding synthetic powders under 10-40 MPa to form a membrane and calcining at 1100-1300 DEG C for 5-12 hours. The zind-based perovskite mixed conducting oxygen-permeable membrane, provided in the invention, is a cobalt-free perovskite oxide, has high oxygen permeability and high stability in reducing atmosphere, can be used for the selective separation of oxygen from an oxygen-containing mixed gas and also for the conversion of synthetic gases and hydrogen from natural gas.

Description

technical field [0001] The invention relates to the design, preparation and structure of a zinc-containing series perovskite mixed conductor oxygen-permeable membrane and its use for separating and preparing pure oxygen from oxygen-containing mixed gas, especially from air, and converting natural gas to produce synthetic gas and hydrogen. Background technique [0002] Mixed conductor oxygen permeable membrane is a kind of ceramic membrane with both electronic and oxygen ion conductivity. Since oxygen is not transmitted in the form of molecular oxygen but in the form of ionized oxygen through oxygen holes in the process of oxygen transmission, the theoretical diffusion selectivity to oxygen is 100%, and the oxygen transmission rate of some materials can be compared with micro The permeation of the porous membrane is comparable. Since the mid-1980s, Professor Teraoka of Japan was the first to study La(A)Co(B)O with a perovskite structure. 3-δ Since the oxygen permeability of...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C04B35/26C04B35/495C04B35/622C01B13/02C01B3/24C01B3/34
Inventor 王海辉罗惠霞刘桥生蔡明雅
Owner SOUTH CHINA UNIV OF TECH