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Nonmetal-ion-doped perovskite type mixed conductor hydrogen permeation membrane, and preparation method and application of same

A perovskite-type, mixed-conductor technology, applied in separation methods, non-metallic elements, chemical instruments and methods, etc., can solve the problems of limiting membrane material input, permeability and stability at the same time, and achieve the improvement of hydrogen gas permeability , The effect of small powder particle diameter and low powder phase formation temperature

Active Publication Date: 2018-12-07
SOUTH CHINA UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

The hydrogen permeability of the hydrogen permeable membrane can be increased by doping metal ions at the B site, but the metal ions will be reduced to a certain extent in the hydrogen atmosphere, which limits the investment of membrane materials in practical applications.
[0004] At present, the permeability and stability of hydrogen permeable membranes are two major problems that limit the practical industrial application of membrane materials. Existing materials cannot give consideration to both permeability and stability at the same time.

Method used

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  • Nonmetal-ion-doped perovskite type mixed conductor hydrogen permeation membrane, and preparation method and application of same
  • Nonmetal-ion-doped perovskite type mixed conductor hydrogen permeation membrane, and preparation method and application of same
  • Nonmetal-ion-doped perovskite type mixed conductor hydrogen permeation membrane, and preparation method and application of same

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0033] A phosphorus ion-doped perovskite-type mixed hydrogen permeable material BaCe of the present embodiment 0.8 P 0.2 o 3-δ (δ = 0.2) (BCP20) and undoped perovskite-type hybrid hydrogen permeable material BaCeO 3-δ (δ = 0) (BCO), the preparation method comprises the following steps:

[0034] (1) Weigh BCP20 raw material: 12.91g Ba (NO 3 ) 2 , 9.33g Ce (NO 3 ) 4 ·6H 2 O, 1.14g NH 4 h 2 PO 4 Dissolve in deionized water, add 8.89g glycine to the mixture;

[0035] (2) Weigh BCO raw material: 12.91g Ba (NO 3 ) 2 , 11.66g Ce (NO 3 ) 4 ·6H 2 O was dissolved in deionized water, and 9.88g glycine was added to the mixture;

[0036] (3) Heat the nitrate mixture obtained in steps (1) and (2) to 100°C and stir for 40 hours until the solution becomes gelatinous, then put the gel in an electric furnace, heat to 350°C and roast to obtain The precursor of the powder; the powder is placed in a muffle furnace, and the temperature is kept at a rate of 2.5 ° C to 850 ° C per ...

Embodiment 2

[0043] A kind of phosphorus ion-doped perovskite type mixed conductor hydrogen permeable film material Ba of the present embodiment 5.3 Zr 0.7 P 0.3 o 3-δ (δ =0.3) (BZP30) preparation method includes the following steps:

[0044] (1) Weigh BZP30 raw material: 10.11g Ba (NO 3 ) 2 , 11.63g Zr (NO 3 ) 4 ·5H 2 O, 1.33g NH 4 h 2 PO 4 Dissolve in deionized water, add 6.72g glycine to the mixture;

[0045] (2) Heat the nitrate mixture obtained in step (1) to 250°C and stir for 32 hours until the solution takes on the form of a gel, then put the gel into an electric furnace, heat to 200°C and bake to obtain the precursor of the powder ; Put the powder in a muffle furnace, keep the temperature at a rate of 5° C. to 950° C. per minute for 12 hours, and obtain the powder BZP30.

[0046] (3) Weigh 2g of powder BZP30 and put it into a cast iron mold, keep it under 15MPa pressure for 5 minutes to obtain a green body; put the green body into a high-temperature muffle furnace at ...

Embodiment 3

[0049] A kind of sulfide-doped perovskite type mixed conductor hydrogen permeable membrane material SrCe of the present embodiment 0.5 S 0.5 o 3-δ (δ =0.5) (SCS50) preparation method comprises the following steps:

[0050] (1) Weigh SCS50 raw material: 12.79g Sr (NO 3 ) 2 4H 2 O, 5.32g Ce (NO 3 ) 4 ·6H 2 O, 2.62g NH 4 h 2 SO 4 Dissolve in deionized water, add 8.05g glycine to the mixture;

[0051] (2) Heat the nitrate mixture obtained in step (1) to 350°C and stir for 25 hours until the solution takes on the form of a gel, then put the gel into an electric furnace, heat to 500°C and bake to obtain the precursor of the powder ; Put the powder in a muffle furnace, keep the temperature at a rate of 1° C. to 750° C. per minute for 5 hours, and obtain the powder SCS50.

[0052] (3) Weigh 0.5g of the phase-forming powder SCS50 and put it into a cast iron mold, and keep it under 10MPa pressure for 10 minutes to obtain a green body; put the green body into a high-temperat...

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Abstract

The invention discloses a nonmetal-ion-doped perovskite type mixed conductor hydrogen permeation membrane, and a preparation method and an application of same. The chemical general formula of the perovskite type mixed conductor hydrogen permeation membrane is AB<1-x>MxO<3-delta>, wherein A is one of Sr, Ba and Ca, B is one of Ce and Zr, M is one of nonmetal elements P and S and the delta refers tonon-stoichiometry, 0 <= delta <= 0.5 and 0 <= x <= 0.5. The material can be prepared through a glycine-nitrate combustion process. The electronic conductivity of the membrane is enhanced by doping the nonmetal ions, and further the hydrogen permeation capacity is increased. The material, in a hydrogen-containing atmosphere, has excellent separation performance and can be used for separating hydrogen from a hydrogen-containing gas mixture.

Description

technical field [0001] The invention belongs to the technical field of application of energy separation materials, and in particular relates to a perovskite-type mixed conductor hydrogen permeable membrane doped with non-metal ions and its preparation method and application. Background technique [0002] Mixed conductor hydrogen permeable membrane can occupy a certain position in the field of hydrogen separation because it can conduct protons and electrons at the same time. Among the many types of mixed conductor hydrogen permeable membranes, perovskite-type inorganic metal oxides are the most common and studied. [0003] The general structural formula of perovskite inorganic metal oxides is ABO3, and most hydrogen permeable materials are based on BaCeO 3-δ and SrCeO 3-δ system, the conductivity of the perovskite-type mixed conductor hydrogen permeable film can reach 10 -2 ~10 -3 S cm -1 . Although BaCeO 3-δ and SrCeO 3-δ Compared with the proton conductivity, the e...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01D71/02B01D67/00B01D53/22C01B3/50
CPCB01D53/228B01D67/0039B01D71/024B01D2256/16C01B3/503C01B2203/0405
Inventor 王海辉庄丽彬薛健李家祺
Owner SOUTH CHINA UNIV OF TECH
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