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Catalyst for carbon dioxide methanation and preparation method thereof

A technology of carbon dioxide and catalyst, which is applied in the field of carbon dioxide methanation catalyst and its preparation, achieving the effects of low energy consumption, small particle size and uniform dispersion

Inactive Publication Date: 2012-07-25
SICHUAN UNIV
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Problems solved by technology

Chinese patent CN101884927 discloses a catalyst for complete methanation of carbon dioxide and its preparation method. The mass percentage of each component in the catalyst is composed of: γ-Al 2 o 3 : 60-80%; NiO: 10-20%; Fe 2 o 3 : 5-15%; MgO: 1-10%; La 2 o 3 or CeO 2 : 1-10%, but this catalyst is mainly suitable for the complete methanation of carbon dioxide under medium pressure 3.0-5.0MPa, we report the catalyst of this patent embodiment 1 (this catalyst main component and its proportioning are: 16.9%NiO- 6.5% Fe 2 o 3 -3.3%MgO-2.8%CeO 2 -70.5% γ-Al 2 o 3 ) was applied to carbon dioxide methanation reaction under normal pressure conditions, and it was found that at 360°C CO 2 The conversion rate is 87.5%, methane selectivity is 100%, but after 100h stability test, CO 2 The conversion dropped to 80.3%, CH 4 The selectivity is also reduced to 99.4%, indicating that the catalyst for the complete methanation of carbon dioxide disclosed in Chinese patent CN101884927 is only suitable for CO under medium pressure. 2 Methanation reaction, and due to the aggregation of catalyst active components and the formation of carbon on the surface during the reaction, the activity of the catalyst decreases, and the reaction stability of this catalyst is poor

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  • Catalyst for carbon dioxide methanation and preparation method thereof
  • Catalyst for carbon dioxide methanation and preparation method thereof
  • Catalyst for carbon dioxide methanation and preparation method thereof

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preparation example Construction

[0034] The concrete steps of the catalyst preparation method for carbon dioxide methanation of the present invention are:

[0035] 1) Prepare the composite support by impregnation-precipitation method: impregnate the salt solution corresponding to the water-soluble metal oxide in γ-Al by stirring at room temperature 2 o 3 On the carrier, the immersion time is 4-6 hours, so that the salt solution corresponding to the water-soluble metal oxide can completely enter the γ-Al 2 o 3 In the carrier; reintroduce precipitating agent to solution pH value is 8-10 (Ce(OH) when pH value ≥ 8 3 Precipitation begins to form. In an alkaline environment with a pH value of 8-10, it is easy to form small grains with better dispersion. If the pH value is too high, the particles will be agglomerated sharply). The purpose of adding a precipitant is to better The salt solution corresponding to the water-soluble metal oxide is uniformly loaded on the base carrier γ-Al 2 o 3 Surface: After the sol...

Embodiment 1

[0046] Example 1 12.7wt% NiO / 6.0wt% CeO 2 -81.3wt% γ-Al 2 o 3 Catalyst preparation

[0047] A First, CeO was prepared by impregnation-precipitation method 2 / γ-Al 2 o 3 Composite carrier: weigh 1.06g Ce(NO 3 ) 3 ·6H 2 Put O in a beaker, add 20ml of deionized water and stir to dissolve; weigh 4.65g of γ-Al 2 o 3 Place in the above solution, stir at room temperature for 60min, then slowly add the precipitating agent NH 3 ·H 2 O (0.8mol / L) to pH = 9, stirred for 2 hours to make the precipitate uniform, aged (aged means standing at room temperature) for 2 hours, filtered, washed, dried overnight at 120°C, and then roasted at 550°C for 5 hours. Get CeO 2 / γ-Al 2 o 3 Composite support, where CeO 2 The mass fraction of is 6.0wt%;

[0048] The preparation of B catalyst precursor: weigh 2.83g Ni(NO 3 ) 2 (Analytical pure, commercially available) is placed in a beaker, add 20ml of deionized water and stir to dissolve it; weigh 5g of CeO prepared in step A 2 / γ-Al 2 o...

Embodiment 2-11

[0052] Compared with Example 1, only the content of catalyst components or the types of nickel salt and water-soluble metal salt used are different, and other processes are the same as in Example 1 to obtain various finished catalysts. The catalyst compositions of Examples 2 to 11 and the nickel salts and water-soluble metal salts used are shown in Table 1.

[0053] Table 1 Catalyst Composition Table

[0054]

[0055] The catalyst obtained in Examples 1-11 was pressed into tablets and sieved to obtain 60-80 mesh catalyst particles, and 200 mg was filled in a fixed-bed reactor, and hydrogen was used for in-situ reduction. The reduction temperature was 450 ° C, and the reaction pressure was normal pressure. Raw material gas ratio is n(H 2 ):n(CO 2 )=4:1, gas volume space velocity 10000ml / h g cat , the investigation temperature range is 240-360°C, the tail gas composition is analyzed by TDX01 chromatographic column of GC-1690 gas chromatograph (TCD), and the data is recorde...

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Abstract

The invention discloses a catalyst for carbon dioxide methanation and a preparation method of the catalyst, belonging to the technical field of carbon dioxide methanation. The catalyst for carbon dioxide methanation is composed of a composite carrier and an active ingredient at a ratio of 84-90wt%:10-16wt%, wherein the composite carrier is composed of gamma-Al2O3 and water soluble metal oxide at a mass ratio of 77-86:2-10; and the active ingredient is Ni which exists in the catalyst in a form of NiO. The catalyst is high in activity, low in cost and better in stability, and can be used for carbon dioxide methanation reaction under normal pressure condition.

Description

technical field [0001] The invention belongs to the technical field of carbon dioxide methanation, and in particular relates to a catalyst for carbon dioxide methanation and a preparation method thereof. Background technique [0002] Carbon dioxide is one of the most abundant carbon sources on earth. With the increasing depletion of petroleum resources and the serious ecological and environmental problems caused by the massive emission of carbon dioxide into the atmosphere, the greenhouse gas CO 2 Transformation into high value-added chemical products has become a hot topic of research and discussion in domestic and foreign industries and academic circles. In 1902, the French chemist Paul Sabatier first reported the catalytic hydrogenation reduction technology of carbon dioxide (ie CO 2 methanation reaction): CO 2 (g)+4H 2 (g)=CH 4 (g)+2H 2 O(g)Δ R h 0 298K=-252.9KJ·mol -1 , with CO 2 Hydrogenation to synthesize methane gas, on the one hand CO 2 Turning waste into...

Claims

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Application Information

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IPC IPC(8): B01J23/83B01J23/755B01J37/34C07C1/12C07C9/04
Inventor 蔡梦蝶江成发成雪清李泽军
Owner SICHUAN UNIV
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