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Noble metal catalyst for high temperature steam reforming preparing hydrogen from methyl alcohol

A precious metal catalyst, reforming hydrogen production technology, applied in the direction of metal/metal oxide/metal hydroxide catalyst, catalyst activation/preparation, physical/chemical process catalyst, etc., can solve the problem of low space velocity and poor thermal stability of catalyst use , poor stability and other problems, to achieve the effect of overcoming limitations, high activity and good stability

Inactive Publication Date: 2010-03-24
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

However, due to the poor thermal stability of Cu itself, the use temperature of the catalyst is limited.
Another class of methanol steam reforming catalyst is a Pd-Zn catalyst [such as patent CN1334141; Applied Catalysis A: General 248 (2003): 153; Catalysis Today 77 (2002): 79 etc.] with noble metals as active components. The catalyst discards the disadvantages of poor stability and spontaneous combustion of the Cu system, and has good activity and selectivity in the reaction, but the high content of precious metals limits its application
For the above two types of catalysts, their service temperature is lower than 300°C, so they are difficult to apply in palladium membrane reactors
[0007] At present, there are relatively few catalysts for steam reforming of methanol at higher temperatures. Patent WO2004 / 002616 and patent CN1504403 have developed Cu-free catalysts. WO2004 / 002616 can react at 325°C-425°C. But the stability is poor, and the Zn provided by CN1504403 a Ca b Si c o d The space velocity of the type composite oxide catalyst is too low, and the stability data after repeated use is not given

Method used

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  • Noble metal catalyst for high temperature steam reforming preparing hydrogen from methyl alcohol
  • Noble metal catalyst for high temperature steam reforming preparing hydrogen from methyl alcohol

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0028]Embodiment 1: Catalyst A: 0.6% Ir / Ce x Zr 1-x o 2 , (X=0.8)

[0029] 1) Weigh zirconium nitrate Zr (NO 3 ) 4 ·5H 2 O 42.9g and cerium nitrate Ce (NO 3 ) 3 ·6H 2 O173.6g was dissolved in a beaker with deionized water.

[0030] 2) Weigh 180g of urea in a 2000ml beaker, add the Zr(NO 3 ) 4 -Ce(NO 3 ) 3 Mix the solution while adding deionized water to 1600ml. Heat and stir the above solution until boiling to decompose urea to form a precipitate. After heating for 2 hours, age at room temperature for 2 hours. The precipitate washed with boiling water and isopropanol is vacuum-dried at 68°C for 24 hours, and roasted at 500°C for 2 hours. Hours, that is, cerium-zirconium composite oxide.

[0031] 3) Grind the above-mentioned composite oxides to a size below 200 meshes, press into tablets, and crush them to 20-30 meshes. Determine water absorption.

[0032] 4) take by weighing chloroiridic acid (H 2 IrCl 6 ·6H 2 (0) 0.32g, dissolved in deionized water, fixed v...

Embodiment 2

[0033] Example 2: Catalyst B: 0.1% Ir / 5% La 2 o 3 / C x Zr 1-x o 2 , (X=0.75)

[0034] 1) Weigh the Zr(NO 3 ) 4 ·5H 2 O 42.9g, Ce(NO 3 ) 3 ·6H 2 O130.2g, prepare composite oxide particle, method is with the step 1-3 of embodiment 1.

[0035] 2) Weigh lanthanum nitrate (La(NO 3 ) 2 ·nH 2 O, containing ≥44% La 2 o 3 ) 6.8g, dissolved in deionized water, fixed volume 12ml, adopt the step 4 method of embodiment 1 to impregnate 60g above-mentioned composite oxides in equal amounts.

[0036] 3) Weigh H 2 IrCl 6 ·6H 2 O 0.16g, dissolved with deionized water, fixed volume 12ml, adopts the method for equal impregnation to impregnate the composite oxide that step 2 obtains, and method is the same as step 4 of embodiment 1, obtains catalyst B.

Embodiment 3

[0037] Embodiment 3: Catalyst C: 0.3% Ir / Ce x Zr 1-x o 2 (X=0.5)

[0038] 1) Weigh the Zr(NO 3 ) 4 ·5H 2 O 85.8g, Ce(NO 3 ) 3 ·6H 2 O 86.8g, dissolved, made into 100ml Zr(NO 3 ) 4 and Ce(NO 3 ) 3 mixed solution.

[0039] 2) Add 200ml of 1:1 ammonia water into a 1000ml beaker, drop the mixed solution of step 1) into the ammonia water, stir at the same time, age at room temperature for 2 hours, wash and filter, dry, roast and shape, the method is the same as Step 3 of Example 1.

[0040] 3) Weigh H 2 IrCl 6 ·6H 2 O 0.32g, dissolved in deionized water, fixed volume 8ml, using the step 4 method of Example 1 to impregnate 40g of the above-mentioned composite oxide in equal amounts to obtain catalyst C.

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Abstract

The invention provides a noble metal catalyst which is used for hydrogen preparation by a water steam reforming of methanol at high temperature. The catalyst has one or several noble metals from platinum, palladium, rhodium, ruthenium, and iridium as active ingredients, and has composite oxides of lanthanide elements comprising lanthanum, cerium, gadolinium and samarium, and transition metal suchas titanium, chromium, zirconium, molybdenum, vanadium, manganese, nickel, etc. as high temperature stability adjuvants and carriers, wherein weight content of the noble metals is lower than 0.6%. Thecatalyst of the invention can perform the water steam reforming reaction of methanol under a higher reaction temperature of 350-450 DEG C. and an unstable operation state. Hydrogen content of the reforming gas is more than 70mol%, and the conversion of the methanol is over 90% after 100 hours. The invention has high activity, good stability and good maneuverability, thus is especially suitable toapplication in a hydrogen-production reactor for separating and purifying hydrogen by palladium film.

Description

technical field [0001] The invention relates to a noble metal catalyst for high-temperature steam reforming of methanol to produce hydrogen, which can carry out reforming reaction under relatively high temperature and unsteady conditions, has high methanol conversion rate, good stability and good operability It is especially suitable for application in small-scale high-efficiency hydrogen production reactors that use palladium membranes to separate and purify hydrogen. [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] Hydrogen energy is an important secondary energy that is currently being researched, exploited and utilized worldwide. At present, commercial hydrogen is mainly obtained through large-scale hydrogen production using fossil resources such as natural gas, oil, and coal as raw materials. Due to the grad...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/38B01J23/54B01J37/02C01B3/32
Inventor 王树东张纯希刘娜袁中山王淑娟高典楠
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI