Preparation method of anti-carbon deposition methane dry gas reforming Ni-based alkaline earth metal modified catalyst

An alkaline earth metal, dry gas reforming technology, applied in catalyst activation/preparation, metal/metal oxide/metal hydroxide catalyst, catalyst carrier, etc., can solve serious carbon deposition, easy sintering of components, poor stability, etc. problem, to achieve the effect of small Ni particle size, improved carbon deposition resistance, and high Ni dispersion.

Pending Publication Date: 2021-11-05
NANCHANG UNIV
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0006] In view of the above-mentioned shortcomings of the existing methane dry gas reforming hydrogen production technology, the purpose of the present invention is to provide a high-dispersion, low-temperature methane reforming nickel-based catalyst with excellent anti-coking performance and its application to overcome the existing Methane dry gas reforming catalyst has the disadvantages of poor stability, easy sintering of components and serious carbon deposition

Method used

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  • Preparation method of anti-carbon deposition methane dry gas reforming Ni-based alkaline earth metal modified catalyst
  • Preparation method of anti-carbon deposition methane dry gas reforming Ni-based alkaline earth metal modified catalyst
  • Preparation method of anti-carbon deposition methane dry gas reforming Ni-based alkaline earth metal modified catalyst

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Embodiment 1

[0031] Present embodiment 1 is in the Ni / LaAlO of prior art 3 The catalyst was not modified with alkaline earth metals, but the Ni / LaAlO 3 Catalyst obtained by impregnation method to obtain 5%Ni / LaAlO 3 Ni-based alkaline earth metal modified catalyst, its preparation method is:

[0032] Prepare LaAlO by sol-gel method according to prior art 3 , and then prepared by impregnation method to obtain 5%Ni / LaAlO 3 catalyst. The specific synthesis process is as follows: 2.1650gLa(NO 3 ) 3 ·6H 2 O (lanthanum nitrate hexahydrate) and 1.8756gAl(NO 3 ) 3 9H 2 O is the base material and 3.1521g of citric acid monohydrate are mixed and dissolved, stirred at room temperature for 6h to obtain a mixed sol, and then evaporated to dryness in a water bath at 80°C until a gel is obtained, and the gel is transferred to an oven at 110°C for overnight drying , you can get fluffy dry glue; place the dry glue in a muffle furnace at 180 °C for pretreatment to prevent bumping during later roast...

Embodiment 2

[0034] 5%Ni / La 0.9 Mg 0.1 AlO 3 The preparation method of the Ni-based alkaline earth metal modified catalyst is as follows: use La(NO 3 ) 3 ·6H 2 O (lanthanum nitrate hexahydrate) and Al(NO 3 ) 3 9H 2 O and Mg(NO 3 ) 2 ·6H 2 O (magnesium alkaline earth metal salt) was mixed, and La was prepared by sol-gel method 0.9 Mg 0.1 AlO 3 , prepared by impregnation method to obtain 5%Ni / La 0.9 Mg 0.1 AlO 3 catalyst, the specific synthesis process is: 1.9485gLa(NO 3 ) 3 ·6H 2 O (lanthanum nitrate hexahydrate), 1.8756gAl(NO 3 ) 3 9H 2 O and 0.1282gMg(NO 3 ) 2 ·6H 2 O and 3.1521g citric acid monohydrate are mixed and dissolved, stirred at room temperature for 6h to obtain a mixed sol, which is then evaporated to dryness in a water bath at 80°C until a gel is obtained, and the gel is transferred to a 110°C oven for overnight drying to obtain Fluffy dry glue; place the dry glue in a muffle furnace at 180 °C for pretreatment to prevent bumping during post-baking, tran...

Embodiment 3

[0036] 5%Ni / La 0.8 Ca 0.2 AlO 3 The preparation method of Ni-based alkaline earth metal modified catalyst is as follows: prepare La with sol-gel method 0.8 Ca 0.2 AlO 3 Support, prepared by impregnation method to obtain 5%Ni / La 0.8 Ca 0.2 AlO 3 The Ni-based alkaline earth metal modified catalyst, the specific synthesis process is: 1.7320gLa (NO 3 ) 3 ·6H 2 O (lanthanum nitrate hexahydrate), 1.8756gAl(NO 3 ) 3 9H 2 O and 0.2362gCa(NO 3 ) 2 4H 2 O and 3.1521g citric acid monohydrate are mixed and dissolved, stirred at room temperature for 6h to obtain a mixed sol, which is then evaporated to dryness in a water bath at 80°C until a gel is obtained, and the gel is transferred to a 110°C oven for overnight drying to obtain Fluffy dry glue; place the dry glue in a muffle furnace at 180 °C for pretreatment to prevent bumping during post-baking, transfer the pretreated dry glue to a muffle furnace at 800 °C for 6 hours, and heat up at a rate of 2 ° C / min. Finally, the...

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Abstract

The invention discloses a preparation method of an anti-carbon deposition methane dry gas reforming Ni-based alkaline earth metal modified catalyst. The preparation method comprises the following steps of: mixing one of three alkaline earth metal raw materials according to a certain molar mass ratio to form a mixture, adding citric acid which is 1-2 times of the molar mass of metal ions in the mixture into the mixture, and mixing the citric acid with the mixtureand dissolving the newly obtained mixture to obtain mixed sol; evaporating the mixed sol to dryness to obtain gel, and then transferring the gel into a drying oven for drying the gel to obtain dry glue; pretreating the dry glue in a muffle furnace, carrying out heat preservation roasting on the dry glue in the muffle furnace, and cooling to obtain a perovskite carrier; and adding different perovskite carriers into a Ni (NO3) 3 solution to obtain Ni-based alkaline earth metal modified catalysts respectively. The catalyst has more active oxygen species, the oxygen species can eliminate carbon deposition on the surface of the catalyst and improve the carbon deposition resistance of the catalyst, the number of alkali centers of the catalyst modified by adding alkaline earth metal is obviously increased, and obtained Ni particles are smaller in size and higher in dispersity.

Description

technical field [0001] The invention relates to an alkaline earth metal modified Ni / La x m 1-x AlO 3 Preparation method of (M = Mg, Ca, Sr) catalytic material and its application in methane dry gas reforming. [0002] technical background [0003] As the cheapest and most abundant carbon resource in the C1 family, CO 2 Resource recycling is an important way to achieve a low-carbon economy. Looking for an efficient and cheap CO 2 Resource utilization method, large-scale CO 2 Using it to realize the harmonious coexistence between man and nature has become the most concerned research topic of scientists all over the world: methane dry gas reforming reaction can simultaneously convert two greenhouse gases, methane and carbon dioxide, into syngas, effectively mitigating the greenhouse effect. At the beginning of the 20th century, German scientists Tropsch and Fisher conducted research on the dry reforming of methane and carbon dioxide. Until 1991, Ashcroft et al. proposed t...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/83B01J37/02B01J37/03B01J37/18B01J32/00B01J23/10B01J35/02C01B3/40
CPCB01J23/83B01J37/0201B01J37/036B01J37/18B01J23/002B01J23/10B01J35/0066B01J35/026C01B3/40B01J2523/00C01B2203/0238C01B2203/1041B01J2523/22B01J2523/31B01J2523/3706B01J2523/23Y02P20/52
Inventor 王翔方修忠杨孟合
Owner NANCHANG UNIV
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