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Catalyst for autothermal reformation of methanol to prepared hydrogen and its prepn process and application

A technology of autothermal reforming and catalysts, which is applied in chemical instruments and methods, metal/metal oxide/metal hydroxide catalysts, physical/chemical process catalysts, etc. Expensive and other issues, to achieve good heat stability, high activity, good strength

Inactive Publication Date: 2005-09-28
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

The thermal stability and activity of this type of catalyst are greatly enhanced, and it is more convenient to use than copper-based catalysts. However, the CO content in the reformed gas gradually increases with the progress of the reaction, that is, the CO selectivity becomes worse. At the same time, the amount of precious metal larger and more expensive
In addition, Chinese patents CN1305867 and CN1305868 once reported a copper-free non-precious metal catalyst used in the autothermal reforming process of methanol to obtain higher methanol conversion and hydrogen selectivity, but this catalyst lacks sufficient Thermal stabilization aids, structural stabilization aids, and supports for active components, the catalyst is easily powdered and broken during use, so it is difficult to meet the catalyst strength requirements of fuel cell hydrogen source systems, especially vehicle-mounted hydrogen source systems during long-term operation. and stability requirements

Method used

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  • Catalyst for autothermal reformation of methanol to prepared hydrogen and its prepn process and application
  • Catalyst for autothermal reformation of methanol to prepared hydrogen and its prepn process and application
  • Catalyst for autothermal reformation of methanol to prepared hydrogen and its prepn process and application

Examples

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Effect test

example 1

[0032] Example 1: ZnO-Cr prepared by coprecipitation method 2 o 3 -CeO 2 -La 2 o 3 -ZrO 2 composite oxide catalyst

[0033] a) Weigh industrial grade Ce(NO 3 ) 3 ·6H 2 O 90.90g, technical grade Zr(OH) 4 8.45g, La(NO 3 ) 3 ·6H 2 O6.35g. Will weigh Zr(OH) 4 Put it into a beaker, add 65-68% concentrated nitric acid and heat to react until there are no visible particles and the solution is transparent. The dissolved Zr(NO 3 ) 4 The solution was poured into the dissolved Ce(NO 3 ) 3 and La(NO 3 ) 3 The mixed solution was filtered for later use.

[0034] b) Weighing analytically pure Zn(NO 3 ) 2 ·6H 2 O 18.90g, (NH 4 ) 2 Cr 2 o 7 5.55g, add deionized water to dissolve, then mix the Ce-Zr solution in step a with it, and in the case of constant stirring, use a separatory funnel to drop 25-28% ammonia water into the above mixed solution, the amount of ammonia water depends on the pH Control the value until the pH value reaches 7-8. The formed Zn-Cr-Ce-Zr c...

example 2

[0035] Example 2: ZnO-Cr prepared by impregnation method 2 o 3 / CeO 2 composite oxide catalyst

[0036] a) Weigh industrial grade Ce(NO 3 ) 3 ·6H 2 O 90.90g, add deionized water to dissolve, filter, drop 25-28% ammonia water into the above solution with a separatory funnel, the amount of ammonia water is controlled according to the pH value, until the pH value reaches 8-9. Formed CeO 2 The precipitate was thoroughly stirred, vacuum filtered and washed, and then put into an oven for drying at 110°C for 15 hours, and then put into a muffle furnace for calcination at 500°C for 2 hours. Grind the roasted product to below 200 mesh, add 1.5g of pseudo-boehmite and 1.5ml of 10% nitric acid, mix well, extrude with extruder, air-dry and cut into cylinders about 3×4mm. Dry the cylinder in an oven at 110°C for 4 hours, then put it in a muffle furnace and bake it at 500°C for 2 hours to obtain CeO 2 carrier. Grind it to 12-16 mesh and measure its water absorption.

[0037] b) W...

example 3

[0038] Example 3: ZnO-Cr prepared by thermal decomposition 2 o 3 -CeO 2 -ZrO 2 composite oxide catalyst

[0039] a) Weigh industrial grade Ce(NO 3 ) 3 ·6H 2 O 90.90g, technical grade Zr(OH) 4 8.45g, analytically pure Zn(NO 3 ) 2 ·6H 2 O 18.90g, (MH 4 ) 2 Cr 2 o 7 5.55g, urea 0.5g. Mix the above reagents well, put them into a muffle furnace, conduct thermal decomposition at 500°C for 30 minutes, and cool down to room temperature rapidly after the decomposition is completed.

[0040] b) Grind the decomposition product to below 200 mesh, add 2.5g of pseudo-boehmite, mix well, extrude with extruder, air-dry and cut into cylinders of about 3×4mm. Dry the cylinder at 110°C for 4 hours in an oven, and then bake it in a muffle furnace at 800°C for 2 hours to obtain ZnO-Cr 2 o 3 -CeO 2 -ZrO 2 Composite oxide catalyst (C).

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Abstract

The catalyst has metal oxide without copper and noble metal as main active component and the composite oxide of RE and transition metal as the catalytic assistant, heat stabilizing assistant, structure stabilizing assistant and active catalyst component support. The addition of the composite oxide of RE and transition metal raises the reaction activity of the catalyst as well as its strength and stability greatly. The preparation process may be co-precipitation one, isometric soaking one or hot decomposition one. In the co-precipitation process or soaking process, adhesive and pore creating agent are added, and the adhesive and pore creating agent is mixture water solution of organic acids, inorganic acids, pseudo-thin diasphore and polymer. The catalyst may be used in hydrogen source system of fuel cell with unstable operation.

Description

technical field [0001] The invention relates to a methanol autothermal reforming hydrogen production catalyst. [0002] The present invention also relates to a method for preparing the above-mentioned catalyst. [0003] The invention also relates to the use of the catalysts described above. Background technique [0004] Since the development of proton exchange membrane fuel cell (PEMFC) technology, the battery fuel, that is, the hydrogen source, has become one of the technical bottlenecks hindering its commercialization, which has attracted more and more attention and extensive research. It is the most realistic and feasible way to supply hydrogen by reforming hydrocarbons such as methanol, gasoline, natural gas, or on-site to generate hydrogen for fuel cell power generation. The preferred solution. At present, many countries in the world have carried out research and development work in this field, made a lot of research progress, and launched a number of fuel cell demons...

Claims

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Application Information

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IPC IPC(8): B01J23/80B01J23/83C01B3/32
Inventor 王树东袁中山付桂芝张纯希王淑娟刘娜李德意
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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