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Nano-copper base catalyst used for methanol aqueous vapour reforming hydrogen producing and its preparation method

A technology of steam reforming and copper-based catalysts, which is applied in the chemical industry, can solve the problems of inability to meet the hydrogen production requirements of vehicle-mounted fuel cells, high carbon monoxide content, and reduced catalyst activity, so as to improve hydrogen production activity and service life, and be easy to operate , easy industrial amplification effect

Inactive Publication Date: 2006-06-14
FUDAN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Although the CuO / ZnO / Al prepared by this method is usually 2 o 3 The catalyst has good hydrogen production activity and hydrogen selectivity in steam reforming of methanol, but the catalyst usually needs to be used at a temperature > 280°C to achieve a high methanol conversion rate, which obviously cannot meet the actual needs of vehicle-mounted fuel cells. Hydrogen demand
In addition, this method not only requires a large amount of solvent, but also has a long preparation period, complex process parameters and is very easy to introduce alkali metal impurities, resulting in a decrease in catalyst activity.
Recently, it has been reported that oxides of transition metal elements such as Mn, Cr, and Zr were used as promoters to prepare oxide-modified CuO / ZnO / Al 2 o 3 Catalyst, which can realize methanol conversion of more than 95% under the condition of about 250 ° C, but the content of carbon monoxide in the reformed gas obtained by this type of catalyst is still high

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0033] Accurately weigh 7.26g Cu(NO 3 ) 2 ·3H 2 O, 8.91g Zn(NO 3 ) 2 ·6H 2 O, 2.50g Al(NO 3 ) 3 9H 2 O (AR grade) and 10.1g of AR grade oxalic acid (H 2 C 2 o 4 2H 2 O, in terms of metal salts, oxalic acid excess 20%), placed in a ball mill (QM-1SP04 planetary ball mill, Nanjing University Instrument Factory), after ball milling for 4h, the gained oxalate solid-phase precursor was dried at 120°C for 12h and placed in a The oxidized state precursor of the catalyst was obtained after calcination at 350°C for 4 hours in an air atmosphere, and the molar ratio of copper, zinc and aluminum components in the sample was 45 / 45 / 10.

Embodiment 2

[0040] Accurately weigh 7.26g Cu(NO 3 ) 2 ·3H 2 O, 8.91g Zn(NO 3 ) 2 ·6H 2 O (AR grade) and 9.1g of AR grade oxalic acid (H 2 C 2 o 4 2H 2 O, based on the metal salt, oxalic acid excess 20%), placed in an agate mortar, after grinding for 3 hours, the resulting oxalate solid phase precursor was dried at 120°C for 12h and roasted at 350°C for 4h in an air atmosphere to obtain the catalyst. Oxidation state precursor, the molar ratio of copper and zinc components in the sample is 50 / 50. Catalyst methanol steam reforming hydrogen production activity evaluation is the same as embodiment 1, test result shows: at normal pressure, temperature 260 ℃, n(H 2 O) / n(CH 3 OH)=1.3 / 1.0, WHSV=5.8h -1 Under the reaction conditions, the methanol conversion rate was 92.4%, the hydrogen selectivity was 98.7%, and the CO 2 The selectivity is 98.3%, and the CO content in the reformed gas is 0.35%.

Embodiment 3

[0042] Accurately weigh 7.26g Cu(NO 3 ) 2 ·3H 2 O, 8.91g Zn(NO 3 ) 2 ·6H 2 O (AR grade) and 9.1g of AR grade oxalic acid (H 2 C 2 o 4 2H 2 O, in terms of metal salts, oxalic acid excess 20%), placed in a ball mill (QM-1SP04 planetary ball mill), after grinding for 0.5h, the resulting oxalate solid phase precursor was dried at 120°C for 12h and heated in an air atmosphere for 350 After calcination at ℃ for 4 hours, the oxidized precursor of the catalyst was obtained, and the molar ratio of copper and zinc components in the sample was 50 / 50. Catalyst activity evaluation is the same as embodiment 1, and test result shows: at normal pressure, temperature 260 ℃, n (H 2 O) / n(CH 3 OH)=1.3 / 1.0, WHSV=5.8h -1 Under the reaction conditions, methanol conversion rate is 96.8%, hydrogen selectivity is 99.0%, CO 2 The selectivity is 99.0%, and the CO content in the reformed gas is 0.32%.

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Abstract

A Cu-based nano-catalyst for preparing H2 by reforming the vapor of methanol contains CuO (30-70 mole %), ZnO (20-60), and Al2O3 (0-15). It is proportionally prepared from copper nitrate, zinc nitrate, aluminium nitrate and oxalic acid through grinding, drying and calcining. Its advantages are high low-temp activity, high stability and high selectivity to H2.

Description

technical field [0001] The invention belongs to the technical field of chemical industry, and in particular relates to a novel high-efficiency nano-copper-based catalyst for hydrogen production by steam reforming of methanol and a preparation method thereof. technical background [0002] As one of the most promising high-energy-carrying liquid fuels, methanol has the advantages of low cost, high energy density, low carbon content, and convenient transportation and storage. The instant generation of hydrogen through catalytic conversion can effectively solve various technical problems in the utilization of hydrogen energy, and become an ideal hydrogen carrier. It is currently the hydrogen source for high-power fuel cells (used to drive electric vehicles, submarines, etc.) Research hotspots in the field of energy catalysis. Achieving on-board hydrogen production is key to making fuel cells competitive with other portable power sources. As a hydrogen source for fuel cells, th...

Claims

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Application Information

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IPC IPC(8): B01J23/80C01B3/40
CPCY02P20/52
Inventor 曹勇王路存戴维林范康年
Owner FUDAN UNIV
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