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Method for preparing two-phase compact oxygen permeable material with high oxygen permeability

A high oxygen permeability and dense technology, applied in the field of dense ceramic oxygen permeable membrane materials, can solve the problems that the membrane body cannot be dense, the electronic phase cannot be connected, and the oxygen permeability of the material is low, so as to achieve good chemical stability and fine particles , Improve the effect of oxygen permeability

Active Publication Date: 2012-07-25
UNIV OF SCI & TECH BEIJING
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Problems solved by technology

The United States "Chemical Engineering and Industrial Research" (J. Kim, Y. S. Lin, Palladium-Modified Yttria-Stabilized Zirconia Membranes, Ind Eng Chem Res 39 (2000) 2124-2126.) reported a new type of biphasic oxygen-permeable membrane, The electronic phase Pt is injected into the skeleton of the porous YSZ ion conductor, but the oxygen permeability of the material is low because the electronic phase cannot be connected and the membrane itself cannot be dense.
"Membrane Science" magazine (H.H. Wang, W.S. Yang, Y. Cong, X.F. Zhu, Y.S. Lin, Structure and oxygen permeability of a dual-phase membrane, J Membr Sci 224 (2003) 107-115.) reported that according to the dual-phase The melting points are different, and a solid phase method is used to obtain an oxygen ion phase La 0.15 Sr 0.85 Ga 0.3 Fe 0.7 o 3-δ As the skeleton, the electronic phase Ba 0.5 Sr 0.5 Fe 0.2 co 0.8 o 3-δ Through the dual-phase film, the obtained material has high oxygen permeability and excellent structural stability, but since the dual-phase is a perovskite structure, the problem of cation diffusion is unavoidable (A. L. Shaula, V. V. Kharton, F. M. B. Marques, A. V. Kovalevsky, A. P. Viskup, E. N. Naumovich, Oxygen permeability of mixed-conducting composite membranes: effects of phase interaction, J Solid State Electrochem 10 (2006) 28-40.)

Method used

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  • Method for preparing two-phase compact oxygen permeable material with high oxygen permeability
  • Method for preparing two-phase compact oxygen permeable material with high oxygen permeability
  • Method for preparing two-phase compact oxygen permeable material with high oxygen permeability

Examples

Experimental program
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Embodiment 1

[0017] Ce prepared by coating method with a volume ratio of 8:2 0.8 SM 0.2 o 2-δ –PrBaCo 2 o 5+δ Dual-phase dense oxygen-permeable membrane.

[0018] The fluorite-type oxygen ion conductor Ce used in this example 0.8 SM 0.2 o 2-δ Prepared by surfactant modulation synthesis method: CTAB(CH 3 (CH 2 ) 15 N + (CH 3 ) 3 Br – ) as an organic template was dissolved in deionized water, stirred to completely dissolve to form a solution (0.08 M), and then a certain amount of ammonia was added dropwise. At the same time, according to the proportion of the amount of the substance Ce 3+ :Sm 3+ =8:2 for batching, dissolved in deionized water and stirred evenly (1 mM), then slowly dropped into CTAB solution and stirred for 2 hours to obtain a precipitate. The precipitate was aged at room temperature for 24 hours, then washed by centrifugation and dried at 60°C. The resulting precipitate was sintered in two steps: heating up to 250 °C for 2 hours to remove organic matter; the...

Embodiment 2

[0024] The preparation method and preparation conditions of this example and the above-mentioned Example 1 are the same, the difference is that the Ce with a volume ratio of 7:3 is prepared by the liquid phase coating method. 0.8 SM 0.2 o 2-δ –PrBaCo 2 o 5+δ Dual-phase dense oxygen-permeable membrane. According to Ce 0.8 SM 0.2 o 2-δ :PrBaCo 2 o 5+δ The volume ratio is 7:3 preparation, the Ce 0.8 SM 0.2 o 2-δ The powder is ultrasonically dispersed in the PrBaCo described in Example 1 2 o 5+δ in the precursor solution.

[0025] Using the four-terminal lead method to measure Ce in the air atmosphere within the temperature range of 200~900℃ 0.8 SM 0.2 o 2-δ –PrBaCo 2 o 5+δ Conductivity of biphasic dense oxygen-permeable membranes. The experimentally measured conductivity reaches 6.67 S cm at 900 °C -1 . The oxygen permeability of the material is tested by a high temperature oxygen permeability test system. High-purity helium and synthetic air were blown into...

Embodiment 3

[0027] Preparation of Ce with a particle size of about 10 mm by solid-state method 0.8 SM 0.2 o 2-δ Ionically conductive phase powder according to Ce 0.8 SM 0.2 o 2-δ :PrBaCo 2 o5+δ The volume ratio is 8:2 preparation, the Ce 0.8 SM 0.2 o 2-δ Ultrasonic dispersion of the PrBaCo described in Example 1 2 o 5+δ in the precursor solution. Use a rotary evaporator to dry at 90° C. under reflux to form a gel, bake at 950° C. for 8 hours, and cool in the furnace to obtain a mixture of an electronically conductive phase coated with an ionically conductive phase.

[0028] The resulting mixture was ground in a mortar until homogeneous, (binder) polyvinyl alcohol was added, and then dry-pressed into discs in a stainless steel mold with a uniaxial pressure of 110 MPa, followed by sintering at 1193 °C for 10 h.

[0029] Measure Ce by four-terminal lead method in air atmosphere at a temperature of 200~900°C 0.8 SM 0.2 o 2-δ –PrBaCo 2 o 5+δ Conductivity of biphasic dense oxyge...

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Abstract

The invention relates to a method for preparing a Ce0.8Sm0.2O2 minus delta and PrBaCo2O5 plus delta two-phase compact oxygen permeable film and belongs to the field of a compact ceramic oxygen permeable film. The method comprises the following steps of: coating an electronic conductive phase PrBaCo2O5 plus delta on the surfaces of an ionic conductive phase, i.e. Ce0.8Sm0.2O2 minus delta particles, by a liquid phase method; and forming a two-phase oxygen permeable material with high ionic conductive phase content by high temperature sintering. Due to the special coating structure, the continuous and through threshold value of a surface to volume ratio of the ionic phase to the electronic phase is improved, which is beneficial for improving the oxygen permeability performance. The material has higher oxygen permeability, chemical stability and mechanical stability and can be used for oxygen separation in the air, a membrane reactor, oxygen enriched combustion and an electrode material of a fuel cell.

Description

[0001] technical field [0002] The invention belongs to the field of dense ceramic oxygen-permeable membrane materials, in particular to a high oxygen-permeable Ce 0.8 SM 0.2 o 2-δ –PrBaCo 2 o 5+δ A method for preparing a two-phase dense oxygen-permeable membrane material. Background technique [0003] Today in the 21st century, with the rapid development of social economy and rapid population growth, the shortage of resources and energy, and the deteriorating ecological environment, it is imminent to find clean and renewable energy. Hydrogen energy is an efficient, clean and easy-to-storage secondary energy source. The heat released by combustion is three times that of gasoline and five times that of coal. The mixed conductor oxygen permeable membrane can be used as a gas separation membrane to separate and produce oxygen from oxygen-containing gas due to its oxygen ion conductivity at high temperature, and then be used for partial oxidation of methane to produce hydr...

Claims

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Application Information

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IPC IPC(8): C04B35/50C04B35/624
CPCY02E60/50
Inventor 赵海雷陈婷谢志翔杜志鸿王捷
Owner UNIV OF SCI & TECH BEIJING
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