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Multi-layer composite ceramic oxygen permeation film as well as preparation and application thereof

An oxygen permeable membrane and multilayer composite technology, which is applied in the field of multilayer composite ceramic oxygen permeable membrane and its preparation and application, can solve the problems of thermal expansion matching oxygen flux decline, development limitation, high chemical stability, etc.

Active Publication Date: 2013-09-04
NANJING TECH UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Compared with Co-containing materials, the stability of dual-phase mixed conductors has been improved, but considering the thermal expansion matching between the two phases and the decrease in oxygen flux caused by the decrease in the ratio of the oxygen ion conductor phase to the electron conductor phase, such materials development is limited
In the actual membrane reaction process, such as: partial oxidation of methane to synthesis gas, methane oxidative steam reforming, carbon dioxide decomposition, methane partial oxidation coupled with carbon dioxide decomposition, and bioethanol oxidative steam reforming coupled with water splitting, etc., these reaction processes all involve Direct contact of the membrane surface with the reaction atmosphere, which leads to a decrease in the chemical stability of these monolayer membrane reactors
Therefore, for single-layer membrane reactors, there is a certain contradiction between high oxygen permeability and excellent chemical stability. How to achieve a balance between these two aspects is a huge challenge.

Method used

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  • Multi-layer composite ceramic oxygen permeation film as well as preparation and application thereof
  • Multi-layer composite ceramic oxygen permeation film as well as preparation and application thereof
  • Multi-layer composite ceramic oxygen permeation film as well as preparation and application thereof

Examples

Experimental program
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Effect test

Embodiment 1

[0035] Dense layer material is 0.5wt%Nb 2 o 5 Doped SrCo 0.8 Fe 0.2 o 3-δ(SCF), the porous layer is Ba 0.3 Sr 0.7 Fe 0.9 Mo 0.1 o 3-δ (BSFM). SCF and BSFM mixed conductor materials were prepared by citric acid-EDTA complexation method, Nb 2 o 5 Doped SCF (SCFNb) was synthesized by a solid-phase method. The particle sizes of BSFM and SCFNb powder particles are 500nm and 260nm, respectively. The dense SCFN layer is a sheet structure with a thickness of 1 mm. Polyvinyl alcohol is used as a binder in the process of preparing the green body, and the content is 5%. 8.41wt.% BSFM powder, 6.43wt.% glycerol, 18.91wt.% ethylene glycol, 60wt.% isopropanol and 6.25wt.% terpineol were mixed to obtain a suspension for preparing a porous BSFM layer. The suspension is sprayed on one side surface of the dense SCFNb membrane by spraying method. The sprayed double-layer film was kept at 1000°C for 2 hours at a heating rate of 2°C / min, and then cooled at a rate of 2°C / min. The desi...

Embodiment 2

[0037] Dense layer material is Ba 0.5 Sr 0.5 co 0.8 Fe 0.2 o 3-δ , Prepared by improved citric acid method. The porous layer is a dual-phase material 40wt.%Pr 0.6 Sr 0.4 FeO 3-δ -60wt.%Ce 0.9 PR 0.1 o 2-δ , prepared by solid-phase reaction method. The particle diameters of the dense layer and the porous layer are 100nm and 150nm, respectively, and the thicknesses are 2.0mm and 10μm, respectively. Polysulfone was used as a binder in the process of preparing the dense layer green body with a content of 1.2%. 5.68wt.% of 40wt.%Pr 0.6 Sr 0.4 FeO 3-δ -60wt.%Ce 0.9 PR 0.1 o 2-δ The powder, 6wt.% glycerin, 40.3wt.% ethanol, 40wt.% polyvinylpyrrolidone and 8.02wt.% epoxy resin were mixed to obtain a suspension for preparing the porous layer. Apply the suspension to the dense Ba 0.5 Sr 0.5 co 0.8 Fe 0.2 o 3-δ one side of the diaphragm. The double-layer film after spraying was kept at 900°C for 5h at a heating rate of 5°C / min, and then cooled at a rate of 5°C / min...

Embodiment 3

[0039] Dense layer material is 3wt.%ZrO 2 Doped SrCo 0.8 Fe 0.2 o 3-δ , prepared by solid phase reaction method, its particle size is 500nm. The material of the porous layer is the ionic electronic material La 0.85 Ce 0.1 Ga 0.3 Fe 0.65 al 0.05 o 3-δ and proton-electron mixed conductor material BaCe 0.95 Y 0.05 o 3-δ . The two are synthesized by the improved citric acid method, and the particle sizes are 50nm and 60nm respectively. The dense layer is prepared by isostatic pressing into a sheet-type green body with a thickness of 2 mm, wherein the binder is polyvinyl alcohol with a content of 10%. After calcining, a sheet-like dense layer is obtained. The proportion of the porous layer suspension is 9.5wt.% porous layer powder, 8.5wt.% glycerin, 50.5wt.% ethylene glycol, 25wt.% polyvinylpyrrolidone and 6.5wt.% polysulfone. La 0.85 Ce 0.1 Ga 0.3 Fe 0.65 al 0.05 o 3-δ and BaCe 0.95 Y 0.05 o 3-δ Porous layer, the thicknesses of the two porous layers are 50 ...

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Abstract

The invention relates to a multi-layer composite ceramic oxygen permeation film as well as preparation and an application thereof. The composite film is composed of a porous layer which is resistant to a reaction atmosphere and has a protective function, and a compact layer which has high oxygen permeation performance. Methods such as a spraying method are adopted for combining the porous layer with the compact layer, and the multi-layer composite ceramic oxygen permeation film is prepared through certain degree of thermal treatment. According to the invention, the design is reasonable, the structure is compact, the traditional design concept is broken through, and the practicability of an oxygen permeation film reactor can be effectively enhanced. The invention is applicable to a film reaction process, particularly the multiple-reaction coupling, and solves the problem that a traditional single-layer reactor is hardly balanced between the high oxygen permeation performance and excellent chemical stability.

Description

technical field [0001] The invention relates to a multilayer composite ceramic oxygen permeable membrane and its preparation and application. It specifically relates to a multi-layer composite ceramic membrane and its preparation, and the composite membrane is used for membrane reaction, which can simultaneously obtain high oxygen permeability and good chemical stability. technical background [0002] Mixed Ionic Electronic Conductor (MIEC) oxygen permeable membrane is a kind of ceramic membrane with oxygen ion and electronic conductivity at high temperature. This kind of membrane material can continuously carry out oxygen transfer process without external circuit. Because it realizes the transfer of oxygen through lattice vibration, it has 100% selectivity to oxygen in theory and can be directly used for oxygen separation. As an important gas separation membrane, since the mid-1980s, after years of research, a large number of excellent mixed conductor oxygen permeable memb...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01D71/02B01D69/12B32B18/00B01D53/22C01B13/02
Inventor 金万勤姜威张广儒刘郑堃张凯徐南平
Owner NANJING TECH UNIV
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