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Supported copper-based catalysts for hydrogen production by methanol steam reforming as well as preparation method and application of supported copper-based catalysts

A copper-based catalyst, reforming hydrogen production technology, applied in the direction of catalyst activation/preparation, metal/metal oxide/metal hydroxide catalyst, chemical instruments and methods, etc., can solve problems such as stability to be improved, easy sintering, etc. , to overcome activity and selectivity bottlenecks, increase methanol conversion, and simplify the method

Inactive Publication Date: 2020-12-22
EAST CHINA UNIV OF SCI & TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, copper-based catalysts are easy to sinter at high temperatures, and their stability needs to be improved. There is also a large room for improvement in reducing CO production.

Method used

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  • Supported copper-based catalysts for hydrogen production by methanol steam reforming as well as preparation method and application of supported copper-based catalysts
  • Supported copper-based catalysts for hydrogen production by methanol steam reforming as well as preparation method and application of supported copper-based catalysts
  • Supported copper-based catalysts for hydrogen production by methanol steam reforming as well as preparation method and application of supported copper-based catalysts

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0038] A hydrogen production catalyst for methanol steam reforming was prepared by co-precipitation method using sodium carbonate and sodium hydroxide as precipitants. A certain amount of sodium carbonate and sodium hydroxide was added to the nitrate mixed solution of copper, magnesium and aluminum at a constant rate. , aging after precipitation, and after suction filtration, drying, grinding and calcination, the catalyst was obtained. by Cu-Al 2 o 3 The addition of magnesium oxide to the catalyst improves the activity and stability of the original copper-based catalyst.

[0039] In this example, it is CuO-MgO-Al 2 o 3 Preparation of catalyst, copper oxide mass content 20wt%, molar ratio Mg:Al=2:5

[0040] making process:

[0041] S1: 1.522g Cu(NO 3 )2 ·3H 2 O, 11.254g Al(NO 3 ) 3 9H 2 O and 3.077g Mg(NO 3 ) 2 ·6H 2 Dissolve O in 100mL deionized water, and dissolve it with a magnetic stirrer;

[0042] S2: 100mL of 1.6 ([M 2+ ]+[Al 3+ ]) Sodium Hydroxide 2[Al 3...

Embodiment 2

[0056] In this example, it is CuO-MgO-Al 2 o 3 Catalyst preparation, molar ratio Mg:Al=3:4

[0057] making process:

[0058] S1: 1.468g Cu(NO 3 ) 2 ·3H 2 O, 9.003g Al(NO 3 ) 3 9H 2 O and 4.615g Mg(NO 3 ) 2 ·6H 2 Dissolve O in 100mL deionized water, and dissolve it with a magnetic stirrer;

[0059] S2: 100mL of 1.6 ([M 2+ ]+[Al 3+ ]) Sodium Hydroxide 2[Al 3+ ] The mixed solution of sodium carbonate is added to the solution obtained in step S1, and the dropping rate is 1-2mL / min;

[0060] S3: After continuing to stir the mixture obtained in step S2 for 1 hour, let it stand for 18 hours;

[0061] S4: Suction filter and wash the mixture obtained in step S3, and the washing water volume is 8L;

[0062] S5: put the solid matter obtained in step S4 into an oven for 12 hours, and set the temperature at 100°C;

[0063] S6: Grinding the solid obtained in step S5 into powder, and calcining in a muffle furnace at 400-500° C. for 3-5 hours to obtain a final product.

[00...

Embodiment 3

[0071] In this example, it is CuO-MgO-Al 2 o 3 Preparation of catalyst, CuO mass content 20wt%, molar ratio Mg:Al=4:3

[0072] making process:

[0073] S1: 1.417g Cu(NO 3 ) 2 ·3H 2 O, 6.752g Al(NO 3 ) 3 9H 2 O and 6.153g Mg(NO 3 ) 2 ·6H 2 Dissolve O in 100mL deionized water, and dissolve it with a magnetic stirrer;

[0074] S2: 100mL of 1.6 ([M 2+ ]+[Al 3+ ]) Sodium Hydroxide 2[Al 3+ ] The mixed solution of sodium carbonate is added to the solution obtained in step S1, and the dropping rate is 1-2mL / min;

[0075] S3: After continuing to stir the mixture obtained in step S2 for 1 hour, let it stand for 18 hours;

[0076] S4: Suction filter and wash the mixture obtained in step S3, and the washing water volume is 8L;

[0077] S5: put the solid matter obtained in step S4 into an oven for 12 hours, and set the temperature at 100°C;

[0078] S6: Grinding the solid obtained in step S5 into powder, and calcining in a muffle furnace at 400-500° C. for 3-5 hours to obt...

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Abstract

The invention relates to supported copper-based catalysts for hydrogen production by methanol steam reforming as well as a preparation method and application of the supported copper-based catalysts. According to the invention, magnesium-and-aluminum-supported copper-based catalysts with different magnesium-to-aluminum molar ratios are prepared by roasting a hydrotalcite precursor, wherein the supported copper-based catalyst is a Cu-Mg-Al composite oxide, a molar ratio of Mg to Al in the Cu-Mg-Al composite oxide is 2: 5 to 5: 2, and the mass fraction of CuO is 10%-30%. Compared with the prior art, the catalyst provided by the invention has the advantages that through doping modification of a single oxide carrier, a methanol conversion rate is greatly improved on the basis of keeping high hydrogen selectivity, and particularly, the methanol conversion rate is improved by nearly one time at a low-temperature section (225 DEG C) without generation of CO, so a basis is provided for application of the catalyst to a fuel cell; the stability of the catalyst is higher than the stability of commercial Cu / ZnO / Al2O3, and the bottleneck that the activity, selectivity and stability of an existing catalytic system cannot be obtained at the same time is overcome; and the preparation method is simple, the magnesium / aluminum ratio is adjustable, and the method is suitable for large-scale industrial production.

Description

technical field [0001] The invention relates to the field of hydrogen production from methanol, in particular to a supported copper-based catalyst for steam reforming of methanol to produce hydrogen, a preparation method and application thereof. Background technique [0002] Today, when environmental issues have become the focus of the world, it is imperative to find and develop new clean energy sources. Among them, hydrogen is an ideal clean energy because it can be effectively converted into energy without producing toxic substances or greenhouse gases. Especially its use in fuel cell vehicles has made the world see the feasibility and Inevitability, its development and utilization has become one of the future world development trends. However, to date, the direct application of hydrogen in fuel cell vehicles has been limited by hydrogen storage technologies, namely: hydrogen storage containers and hydrogen storage materials. Based on this, using hydrogen storage materia...

Claims

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Application Information

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IPC IPC(8): B01J23/78B01J37/03B01J37/08C01B3/32
CPCB01J23/002B01J23/78B01J37/031B01J37/088B01J2523/00C01B3/326B01J2523/17B01J2523/22B01J2523/31
Inventor 徐至朱明辉李迪迪
Owner EAST CHINA UNIV OF SCI & TECH
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