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Aluminum-based MOFs (Metal-Organic Frameworks) derived Ni-based catalyst as well as preparation method and application thereof in CO methanation reaction

A catalyst, aluminum-based technology, applied in the field of aluminum-based MOFs derived Ni-based catalyst and its preparation and application in CO methanation reaction, can solve the problems of catalyst sintering deactivation, concentration of reduction temperature, aggregation of catalyst active metal particles, etc. Achieve the effects of not easy to aggregate, improve utilization rate, and not easy to sinter and deactivate

Active Publication Date: 2021-07-20
INNER MONGOLIA UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0008] The purpose of the present invention is to solve the problem that the CO methanation reaction catalysts in the prior art can only be reduced at a certain temperature, and the active metals reduced by these catalysts cannot meet the requirements of the low temperature and high temperature at the same time. Technical issues of thermal stability
[0009] Another object of the present invention is to solve the difficulty of reducing the nickel-aluminum catalyst formed by traditional high-temperature roasting, the reduction temperature is too concentrated, and in the high-temperature region, the utilization rate of the active metal Ni is reduced, which easily leads to the aggregation of catalyst active metal particles, resulting in catalyst Technical problems of sintering deactivation

Method used

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  • Aluminum-based MOFs (Metal-Organic Frameworks) derived Ni-based catalyst as well as preparation method and application thereof in CO methanation reaction
  • Aluminum-based MOFs (Metal-Organic Frameworks) derived Ni-based catalyst as well as preparation method and application thereof in CO methanation reaction
  • Aluminum-based MOFs (Metal-Organic Frameworks) derived Ni-based catalyst as well as preparation method and application thereof in CO methanation reaction

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preparation example Construction

[0049] The aluminum-based MOFs derived Ni-based catalyst of the present invention is prepared by the following method, and the preparation method comprises the following steps:

[0050] Step 1: Prepare metal-organic framework support MOF-Al using soluble aluminum salt, dicarboxylic acid and water;

[0051] Step 2: impregnating the metal organic framework support MOF-Al in the mixed solution of soluble nickel salt and alcohol, and then roasting to prepare the catalyst precursor NiO / NiAl 2 o 4 ,

[0052] Step 3: the catalyst precursor NiO / NiAl 2 o 4 The Ni-based catalyst derived from the Al-based MOFs was obtained by reduction in a hydrogen atmosphere.

[0053] Examples of the soluble aluminum salt include, but are not limited to, aluminum nitrate nonahydrate, aluminum trichloride, aluminum sulfate, and the like.

[0054] Examples of the dicarboxylic acid include: aliphatic hydrocarbon dicarboxylic acid, malonic acid, succinic acid, azelaic acid (AZA), sebacic acid, etc.; a...

Embodiment 1

[0066] Preparation of Al-based MOFs

[0067] First weigh 15g aluminum nitrate nonahydrate (Al(NO 3 ) 3 9H 2 O) and 4 g of organic ligand (terephthalic acid) were dispersed in deionized water. The above solution was transferred to a 100 mL polytetrafluoroethylene-lined stainless steel reaction kettle, sealed and placed in an oven at 200°C for 72 hours. After the reaction was completed, it was slowly lowered to room temperature, the sample was transferred to a beaker, washed repeatedly with distilled water, filtered with suction, and then dried overnight in an oven at 80°C. After drying, wash with DMF at room temperature, stir for 8 hours, filter with absolute ethanol, and dry in an oven at 120°C for 12 hours to obtain the product MIL-53(Al).

[0068] Preparation of Al-based MOFs-derived Ni-based catalysts

[0069] Add 10mL of ethanol to a 100mL beaker, weigh 0.24g of nickel nitrate, and stir with a glass rod until completely dissolved (dark green). Then weigh 2g of MI...

Embodiment 2

[0071] In addition to weighing 0.36g of nickel nitrate, the catalyst precursor NiO / NiAl was prepared in the same manner as in Example 1 2 o 4 , with a porosity of 48% and a Ni loading of 15wt%, and finally reduced in a hydrogen atmosphere at 600 °C to finally obtain an aluminum-based MOFs-derived Ni-based catalyst, referred to as the catalyst Ni / Al-2.

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Abstract

The invention relates to an aluminum-based MOFs (Metal-Organic Frameworks) derived Ni-based catalyst as well as a preparation method and application thereof in CO methanation reaction. A precursor of the catalyst is composed of a carrier and a nickel component, the carrier is NiAl2O4 which is derived from MOF-Al and has a micropore and mesoporous structure with the porosity of 45-55%, and the total content of Ni in the precursor is 5-20 wt%. The catalyst can realize progressive reduction of NiO through controllable reduction, and is used for methanation reaction of synthesis gas. The catalyst provided by the invention can be used in a wide reaction temperature range, and can meet the requirements of activity and thermal stability at low temperature and high temperature at the same time. The catalyst also improves the utilization rate of the active metal Ni in the use period of the catalyst, active metal particles of the catalyst are not easy to aggregate, and sintering inactivation of the catalyst is not easy to cause.

Description

technical field [0001] The invention relates to an aluminum-based MOFs-derived Ni-based catalyst, a preparation method thereof and an application in a CO methanation reaction. Background technique [0002] In the field of heterogeneous catalytic technology and composite material technology, syngas methanation is a key technology for coal-to-natural gas. At present, coal-to-natural gas methanation catalysts (technology) are mainly provided by foreign companies such as David in the UK and Topsoe in Denmark. However, the above-mentioned catalysts that have been used in industry still have problems such as low low-temperature activity, easy carbon deposition, and easy sintering of high-temperature active components. Atmospheric pressure partial methanation technology and trace CO / CO 2 There is no catalyst for industrial application in the methanation section of the coal-to-natural gas process. [0003] The CO methanation reaction is a strongly exothermic and volume-shrinking r...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/755C07C1/04C07C9/04
CPCB01J23/755C07C1/0435C07C2523/755C07C9/04Y02P20/52
Inventor 王红张二桐王晓燕包亚莉吴俊霞纪利春
Owner INNER MONGOLIA UNIV OF TECH