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Catalyst for carbon dioxide hydrogenation synthesis of low-carbon alcohols, preparation method and application thereof

A carbon dioxide and catalyst technology, applied in the field of catalysts, can solve problems such as low catalyst activity, achieve the effects of high activity, avoid raw material loss, and low cost

Active Publication Date: 2019-03-19
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Considering CO hydrogenation and CO 2 similarity to hydrogenation, we apply this catalyst to CO 2 In the reaction of hydrogenation to low-carbon alcohols, but the catalyst activity is low, and high pressure is required to achieve high activity. Regarding the understanding of the active species of this type of catalyst, it is generally accepted that the layered MoS 2 Ni-Mo-K-S species formed with Ni(Co) and K at the edge of the layer, and stacked on M oS 2 Ni(Co) on the layer forms hydrocarbons, so how to control the MoS 2 The height of layer stacking becomes the core issue restricting the improvement of the catalyst activity

Method used

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  • Catalyst for carbon dioxide hydrogenation synthesis of low-carbon alcohols, preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0024] Ni 4.2 Mo 1 K 0.5 Catalyst preparation and its catalytic performance for carbon dioxide hydrogenation to low-carbon alcohols:

[0025] Take by weighing 12.21g nickel nitrate (Ni(NO 3 )·6H 2 O) was dissolved in 200mL deionized water, under stirring, the rotation speed was 500r / min, heated to 80°C, and 7.25g of anhydrous potassium carbonate (K 2 CO 3 ) was dissolved in 250mL deionized water, and slowly added dropwise to the above-mentioned nickel nitrate solution, and the dripping was completed in about 2 hours. After the obtained precipitate was aged for 24 hours, the supernatant was poured off to obtain a slurry-like precipitate. Heat this slurry precipitate to 80 ℃ under stirring, weigh 1.8g ammonium molybdate ((NH 4 ) 6 Mo 7 o 24 4H 2 O) dissolved in 200mL of deionized water, slowly added dropwise, and continued to stir at 80°C for 5h to allow the two to fully complete the ion exchange. Suction filtration, the obtained solid was dried at 60°C for 12h, and ...

Embodiment 2

[0028] Ni 4.2 Mo 1 K 1 Catalyst preparation and its catalytic performance for carbon dioxide hydrogenation to low-carbon alcohols:

[0029] The catalyst preparation process and activity evaluation were the same as in Example 1, except that the amount of potassium carbonate was changed to 0.44g during impregnation. At 5.0MPa, 320°C, V(H 2 ) / V(CO 2 ) / V(Ar)=72 / 24 / 4, under the reaction conditions of GHSV=3000mL / (h g), Ni 4.2 Mo 1 K 1 CO on catalyst 2 The conversion rate was 27.7%, the selectivity of total alcohol was 73% (excluding CO), wherein the selectivity of ethanol was 18%, and the space-time yield of total alcohol was 25.2 mg / (h g). The detailed results are shown in Table 1, Sequence 2.

Embodiment 3

[0031] Ni 4.2 Mo 1 K 1.5 Catalyst preparation and its catalytic performance for carbon dioxide hydrogenation to low-carbon alcohols:

[0032] The catalyst preparation process and activity evaluation were the same as in Example 1, except that the amount of potassium carbonate was changed to 0.67g during impregnation. At 5.0MPa, 320°C, V(H 2 ) / V(CO 2 ) / V(Ar)=72 / 24 / 4, under the reaction conditions of GHSV=3000mL / (h g), Ni 4.2 Mo 1 K 1.5 CO on catalyst 2 The conversion rate reached 28.2%, the selectivity of total alcohol was 66% (excluding CO), wherein the selectivity of ethanol was 22%, and the space-time yield of total alcohol was 23.8 mg / (h g). The detailed results are shown in Table 1, Sequence 3.

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Abstract

The invention relates to a catalyst for synthesis of low carbon alcohol by hydrogenation of carbon dioxide as well as a preparation method and an application thereof, and more specifically relates to a ternary metal sulfide catalyst with a layered structure as well as a preparation method and an application thereof. The catalyst employs basic nickel carbonate which is prepared by coprecipitation of nickel salt and base as a template, an ion exchange method is used for introducing transition metal molybdenum, alkali metal potassium is dipped, and sulfuration is carried out in order to obtain the catalyst. Hydrogenation for carbon dioxide is carried out on the catalyst in order to directly obtain ethanol, propanol and other alcohol fuel with high added values, and proportioning of each metal in the catalyst can be changed in order to adjust distribution of alcohol products. In an optimum condition, the mol fraction of ethanol in total alcohol reaches 43% and far exceeds the mol fraction of ethanol in total alcohol which is synthesized on a rhodium-based catalyst. Compared with a traditional coprecipitation immersion method, raw material loss due to different pH conditions of nickel and molybdenum precipitation is avoided, and utilization rate of raw material is substantially improved.

Description

technical field [0001] The invention belongs to the field of catalysts, and in particular relates to a catalyst for carbon dioxide hydrogenation to synthesize low-carbon alcohols, a preparation method and application thereof. Background technique [0002] carbon dioxide (CO 2 ) The environmental problems brought about by it are becoming increasingly prominent, while CO 2 It is also the largest carbon resource pool on earth. CO 2 Catalytic conversion into chemicals and fuels needed by human beings is the most fundamental way to solve environmental and energy problems. [0003] Currently for CO 2 Most of the research on catalytic conversion is CO 2 Hydrogenation of methanol, while ethanol and low-carbon alcohols have higher added value than methanol, and also have obvious price advantages (methanol 2,500 yuan / ton, ethanol 6,000 yuan / ton, propanol 10,000 yuan / ton), and more People love it. Although ethanol can be produced by CO 2 Hydrogenation is used to synthesize meth...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J27/051B01J37/03B01J37/30C07C29/156C07C31/04C07C31/08C07C31/10
CPCY02P20/52
Inventor 李灿王集杰蒋宗轩陈燕蝶
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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