Catalyst for hydrogen production from methanol reforming as well as preparation method and application of catalyst

A technology for reforming hydrogen production and catalysts, which is applied in chemical instruments and methods, metal/metal oxide/metal hydroxide catalysts, physical/chemical process catalysts, etc. It can achieve the effect of simple preparation process, eliminating washing process and good catalytic performance.

Active Publication Date: 2012-09-26
SHANXI INST OF COAL CHEM CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

According to the literature, the existing reforming catalysts are mostly prepared by the carbonate liquid-phase co-precipitation method, but this method not only requires a large amount of solvent, but also has a long preparation period, complex process parameters and easy introduction of alkali metal impurities, resulting in a decline in catalyst performance.

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0021] Accurately weigh 21.44g copper nitrate [Cu(NO 3 ) 2 ·3H 2 O], 38.89g zinc nitrate [Zn(NO 3 ) 2 ·6H 2 O], 8.09g aluminum nitrate [Al(NO 3 ) 3 9H 2 O] and 42.54g oxalic acid [H 2 C 2 o 4 2H 2 O] (the molar mass of oxalic acid is 1.4 times the total molar mass of Cu, Zn, and Al), add it to a round-bottomed flask, add 300ml of distilled water, heat it to 70°C in a water bath, stir for 6.5h, centrifuge and separate the solid phase at 100°C Drying under air for 15 hours, calcining at 350°C for 8 hours in an air atmosphere, adding 1.2 g of graphite and punching into flakes to obtain a finished catalyst, the composition (mass fraction): CuO=35.3%, ZnO=53.2%, Al 2 o 3 =5.5%, graphite=6.0%.

[0022] Crush the catalyst, take 3.0g of 8-14 mesh and put it into the reactor, pass H at 30ml / min 2 , reduced at 230°C for 3h, then stopped the hydrogen, and started the reaction, at a reaction temperature of 250°C and a mass space velocity of 1.2h -1 , Reaction pressure 0.8MP...

Embodiment 2

[0024] Accurately weigh 33.18g copper nitrate [Cu(NO 3 ) 2 ·3H 2 O], 26.76g zinc nitrate [Zn(NO 3 ) 2 ·6H 2 O], 8.54g aluminum nitrate [Al(NO 3 ) 3 9H 2 O] and 50.41g oxalic acid [H 2 C 2 o 4 2H 2 O] (the molar weight of oxalic acid is 1.6 times the total molar weight of Cu, Zn, and Al), add it to a round bottom flask, add 300ml of distilled water, heat it in a water bath to 50°C, stir and react for 9h, centrifuge and separate the solid phase at 120°C Dry for 10 hours, bake at 540°C for 3 hours in an air atmosphere, add 0.6 g of graphite to form a pellet, and obtain a finished catalyst. The composition is (mass fraction): CuO=54.6%, ZnO=36.6%, Al 2 o 3 =5.8%, graphite=3.0%.

[0025] Break the catalyst, take 3.0g of 8-14 mesh and put it into the reactor, flow hydrogen at 20ml / min, reduce at 260°C for 2h, then stop the hydrogen, raise the temperature to 280°C, and start the reaction. 2.0 hours -1 , the reaction pressure is 1.4MPa, H 2 O / CH 3 Under the condition ...

Embodiment 3

[0027] Accurately weigh 24.78g copper nitrate [Cu(NO 3 ) 2 ·3H 2 O], 29.68g zinc nitrate [Zn(NO 3 ) 2 ·6H 2 O], 14.13g aluminum nitrate [Al(NO 3 ) 3 9H 2 O] and 36.30 g oxalic acid [H 2 C 2 o 4 2H 2 O] (the molar mass of oxalic acid is 1.2 times the total molar mass of Cu, Zn, and Al), add it to a round bottom flask, add 300ml of distilled water, heat it to 90°C in a water bath, stir for 5h, and centrifuge to separate the solid phase at 110°C Dry for 12 hours, bake at 450°C for 5 hours in a nitrogen atmosphere, add 1.8g of graphite to form a pellet, and obtain a finished catalyst. The composition is (mass fraction): CuO=40.8%, ZnO=40.6%, Al 2 o 3 =9.6%, graphite=9.0%.

[0028] Break the catalyst, take 3.0g of 8-14 mesh and put it into the reactor, flow hydrogen at 15ml / min, reduce at 200°C for 5h, then stop the hydrogen, raise the temperature to 220°C, and start the reaction. 0.2 hours -1 , the reaction pressure is normal pressure, H 2 O / CH 3 Under the conditi...

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Abstract

The invention relates to a catalyst for hydrogen production from methanol reforming as well as a preparation method and an application of the catalyst. The catalyst comprises the following components in percentage by mass: 35.0-55.0% of CuO, 35.0-55.0% of ZnO, 5.0-15.0% of Al2O3, and 3.0-10.0% of graphite. The method comprises the steps as follows: precursors of Cu, Zn and Al and oxalic acid solid are added into water solution at the same time and stirred, wherein the molar weight of oxalic acid is 1.2-1.6 times of the total molar weight of Cu, Zn and Al, the reaction temperature is 50-90 DEG C, and the reaction time is 5-9 hours; after the reaction, the mixture is separated and dried for 10-15 hours at 100-120 DEG C; the mixture is calcinated for 3-8 hours at 350-550 DEG C and with air or nitrogen as calcination atmosphere; after calcination, graphite is added for beating into pieces and molding, and then the finished catalyst is obtained. The preparation method has the advantages of simple preparation process and high efficiency, and reduces the cost greatly; and the catalyst has good catalytic performance on hydrogen production from methanol reforming.

Description

technical field [0001] The invention belongs to the field of hydrogen production from methanol, and in particular relates to a catalyst for hydrogen production by reforming methanol and its preparation method and application. Background technique [0002] Methanol is a bulk raw material with a wide range of sources. It has the characteristics of high energy density, low carbon content, and convenient storage and transportation. It is considered to be the most promising high-energy-carrying fuel. Methanol is converted into hydrogen by catalysis, which can meet the demand for on-site hydrogen use in many occasions, and solve the problem of difficult hydrogen transportation and storage. [0003] The methanol conversion method includes three methods: methanol cracking, methanol reforming and methanol partial oxidation. Among them, methanol reforming is the reaction with the highest hydrogen content, and has the characteristics of low cost, mild conditions, no corrosion, and few ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/72C01B3/32
Inventor 高志贤庆绍军郗宏娟侯晓宁赵金珍谷传涛李光俊李林东胡蕴青董凌曜王海荣
Owner SHANXI INST OF COAL CHEM CHINESE ACAD OF SCI
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