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Preparation method for oxygen permeation-hydrogen permeation-reaction three-effect tubular membrane reactor for partial methane oxidation hydrogen production

A technology of reactor and oxygen-permeable membrane, which is applied in the field of preparation of oxygen-permeable-hydrogen-permeable-reaction three-effect tubular membrane reactor, which can solve the problem that product separation cannot be carried out simultaneously in the same reactor

Active Publication Date: 2018-11-06
SHANDONG UNIV OF TECH
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  • Application Information

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Problems solved by technology

[0009] The purpose of the present invention is to provide a preparation method of an oxygen permeation-hydrogen permeation-reaction three-effect tubular membrane reactor for hydrogen production by partial oxidation of methane, which realizes the integration of air separation-hydrogen production by partial oxidation of methane-hydrogen separation and purification, and solves the problem of The problem that the raw material separation of methane partial oxidation reaction, methane reaction and product separation cannot be carried out simultaneously in the same reactor; the present invention provides its reactor simultaneously

Method used

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  • Preparation method for oxygen permeation-hydrogen permeation-reaction three-effect tubular membrane reactor for partial methane oxidation hydrogen production
  • Preparation method for oxygen permeation-hydrogen permeation-reaction three-effect tubular membrane reactor for partial methane oxidation hydrogen production
  • Preparation method for oxygen permeation-hydrogen permeation-reaction three-effect tubular membrane reactor for partial methane oxidation hydrogen production

Examples

Experimental program
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Effect test

Embodiment 1

[0043] 100g La 0.6 Sr 0.4 co 0.2 Fe 0.8 o 3 (LSCF) ceramic powder and 100g SrCe 0.9 Y 0.1 o 3 (SCY) ceramic powders are ball-milled and dispersed on a ball mill, passed through a 200-mesh sieve, and dried in an oven at 100°C; the dried LSCF ceramic powders and SCY ceramic powders are respectively added to 60g of 20wt.% polyethersulfone formazan In the base pyrrolidone solution, fully stir and disperse to obtain two kinds of film-forming liquids; extrude the film-forming liquids through an extruder and dry naturally to obtain LSCF tubular ceramic oxygen-permeable membrane blanks and SCY tubular ceramic hydrogen-permeable membrane blanks; and then The LSCF tubular ceramic oxygen-permeable membrane body was heated up to 1350°C at a heating rate of 5°C / min in a box-type high-temperature resistance furnace, kept for 5 hours, then cooled to 800°C at a cooling rate of 5°C / min, and then naturally cooled to room temperature , to obtain a LSCF tubular dense ceramic oxygen-permeab...

Embodiment 2

[0051] According to the method of Example 1, LSCF tubular dense ceramic oxygen permeable membrane and SCY tubular dense ceramic hydrogen permeable membrane were prepared.

[0052] The LSCF ceramic powder and the SCY ceramic powder with a mass ratio of 1:1 were used to prepare the catalyst carrier according to the method of Example 1 by physical mixing method; After calcining at 900°C for 4 hours, ball milling for 2 hours, and sieving with a 150-mesh sieve, the catalyst precursor was obtained, and then passed into H 2 The mixed gas of hydrogen and helium with a volume fraction of 5% was reduced at 800° C. for 4 hours to obtain a supported metal nickel catalyst.

[0053] The oxygen permeation-hydrogen permeation-reaction three-effect tubular membrane reactor for LSCF / SCY partial oxidation of methane to hydrogen was prepared according to the method in Example 1.

Embodiment 3

[0055] According to the method of Example 1, LSCF tubular dense ceramic oxygen permeable membrane, SCY tubular dense ceramic hydrogen permeable membrane and supported metal nickel catalyst were prepared.

[0056] Use concentrated hydrochloric acid to corrode and roughen the outer surface of the LSCF tubular dense ceramic oxygen permeable membrane and the inner surface of the SCY tubular dense ceramic hydrogen permeable membrane, increase the nickel catalyst and LSCF tubular dense ceramic oxygen permeable membrane, SCY tubular dense ceramic hydrogen permeable membrane The contact area also increases the gas transmission rate. Then, according to the method of Example 1, an oxygen permeation-hydrogen permeation-reaction three-effect tubular membrane reactor for LSCF / SCY partial oxidation of methane to hydrogen was prepared.

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Abstract

The invention belongs to the technical field of inorganic membrane reactors and in particular relates to a preparation method for an oxygen permeation-hydrogen permeation-reaction three-effect tubularmembrane reactor for partial methane oxidation hydrogen production. The preparation method comprises the following steps: firstly, preparing a tubular dense ceramic oxygen permeation membrane, a tubular dense ceramic hydrogen permeation membrane and a nickel catalyst; sleeving the tubular dense ceramic oxygen permeation membrane by the tubular dense ceramic hydrogen permeation membrane, mountingone end of the tubular dense ceramic hydrogen permeation membrane on a first sealing head, and filling interlayers of the two tubular membranes with the nickel catalyst; sleeving the hydrogen permeation membrane by a quartz tube, and mounting one end of the quartz tube on the first sealing head; further sealing the quartz tube and the other ends of the two tubular membranes by using second sealingheads, thereby forming a reactor. By adopting the preparation method, deep oxidation of methane can be prevented, real-time separation of hydrogen from carbon monoxide can be achieved, and reaction balance can also be promoted towards a product direction. By adopting the preparation method, the problem that raw material separation, methane reactions and product separation, of a partial methane oxidation reaction, cannot be carried out in a same reactor simultaneously can be solved.

Description

technical field [0001] The invention belongs to the technical field of inorganic membrane reactors, and in particular relates to a preparation method of an oxygen permeation-hydrogen permeation-reaction three-effect tubular membrane reactor for hydrogen production by partial oxidation of methane. Background technique [0002] Inorganic membranes have the incomparable advantages of organic membranes such as stable structure, high temperature resistance, acid and alkali resistance, organic solvent resistance, no leaching, low energy consumption, convenient operation and low cost. Inorganic membrane separation and reactor technology, especially the coupling of inorganic membrane separation function and catalytic reaction function, is an important technology to strengthen chemical process. Functional ceramic membranes with ion-electronic mixed conductivity can not only effectively couple separation and reaction, but also have good chemical and structural stability; especially th...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J19/24
CPCB01J19/2475
Inventor 孟波孟秀霞王晓斌庄淑娟谭小耀刘少敏
Owner SHANDONG UNIV OF TECH
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