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A nickel-molybdenum carbide composite catalyst for dry reforming of methane to synthesis gas

A technology for dry reforming of methane and composite catalyst, which is applied in the fields of physical/chemical process catalyst, inorganic chemistry, bulk chemical production, etc., can solve the problems of complicated operation, catalyst deactivation, long carbonization time, etc. The effect of increasing the number of catalytic active centers and reducing the thermal effect

Inactive Publication Date: 2017-04-19
CHENGDU UNIVERSITY OF TECHNOLOGY
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0006] The technical problem to be solved by the present invention is that the sintering and oxidation of the catalyst active components that are prone to occur in the existing nickel-based catalyst and molybdenum carbide catalyst in the methane dry reforming process, resulting in the problem of catalyst deactivation, and the use of hydrogen and methane to preheat Carbonization to obtain molybdenum carbide active species has problems such as long carbonization time and cumbersome operation. The present invention uses nickel and molybdenum dual components to synthesize nickel molybdenum oxide precursor by one-step synthesis of urea combustion method, and then dry reforms the raw material gas with methane. In situ temperature programming, the nickel component in the catalyst is used to dissociate methane to generate carbon intermediate species, and in situ convert molybdenum oxide to molybdenum carbide to form Ni-Mo 2 C composite structure while establishing Mo 2 Carbonization-oxidation cycle of C to obtain a Ni-Mo with high specific surface area, sintering resistance, oxidation resistance and stable structure 2 C / Al 2 o 3 Catalysts for dry methane reforming processes

Method used

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  • A nickel-molybdenum carbide composite catalyst for dry reforming of methane to synthesis gas
  • A nickel-molybdenum carbide composite catalyst for dry reforming of methane to synthesis gas

Examples

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Effect test

example 2

[0027] Weigh 25.79 grams of Al(NO 3 ) 3 .9H 2 O and 10.32 g CO(NH 2 ) 2 , add 20 ml of deionized water and mix to form solution #1, and place it in a constant temperature water bath at 80°C under magnetic stirring. Weigh 2.94 g of starch and add 5 mL of deionized water to form solution #2. Weigh 4.25 g (NH 4 ) 6 Mo 7 o 24 .4H 2 O and 1.08 g of citric acid were added to 10 mL of deionized water to form solution #3. Slowly drop #2 into solution #1 to form a homogeneous mixture, then drop into solution #3 and stir for 2.5h to form a gel. Dry at 105°C for 12h, and bake at 550°C for 5h; then in 50ml / min of CH 4 / CO 2 =1 in the mixed gas at 5°C / min to 800°C for carbonization to obtain the CDUT-M5A catalyst, the nitrogen adsorption / desorption test results show that its specific surface area is 32.6m 2 / g. The weight composition of the catalyst is as follows: the content of molybdenum carbide is 12.4%, and the content of aluminum oxide is 87.6%.

[0028] The catalyst wa...

Embodiment 1

[0030] Weigh 22.56 grams of Al(NO 3 ) 3 .9H 2 O and 9.03 g CO(NH 2 ) 2 , add 20 milliliters of deionized water and mix to form solution #1, place it in a constant temperature water bath at 80°C under magnetic stirring; weigh 2.57 grams of starch, add 5 milliliters of deionized water to form solution #2; weigh 2.81 grams of Ni ( NO 3 ).6H 2 O, 2.23 g (NH 4 ) 6 Mo 7 o 24 .4H 2 0 and 3.41 grams of citric acid, add 10 milliliters of deionized water to form solution #3; #2 is slowly dropped into solution #1 to form a uniform mixture, and solution #3 is added dropwise, and stirred for 2.5h to form a gel; Dry at 105°C for 12h, and bake at 550°C for 5h to obtain the oxide precursor, whose typical nickel-molybdenum oxide structure is as attached figure 1 shown; then, at 50ml / min of CH 4 / CO 2 =1 in the mixed gas at 5°C / min to 800°C for carbonization to obtain CDUT-NM3A catalyst, the typical Ni-Mo 2 C / Al 2 o 3 Composite figure 2 shown. After nitrogen adsorption / desorp...

Embodiment 2

[0033] Weigh 21.63 grams of Al(NO 3 ) 3 .9H 2 O and 8.66 g CO(NH 2 ) 2 , add 20 milliliters of deionized water and mix to form solution #1, place it in a constant temperature water bath at 80°C under magnetic stirring; weigh 2.37 grams of starch, add 5 milliliters of deionized water to form solution #2; weigh 2.52 grams of Ni ( NO 3 ).6H 2 O, 3.56 g (NH 4 ) 6 Mo 7 o 24 .4H 2 0 and 3.63 grams of citric acid, add 10 milliliters of deionized water to form solution #3; #2 is slowly dropped into solution #1 to form a uniform mixture, and solution #3 is added dropwise, and stirred for 2.5h to form a gel; Dry at 105°C for 12h, and bake at 550°C for 5h to obtain the oxide precursor, whose typical nickel-molybdenum oxide structure is as attached figure 1 shown; then, at 50ml / min of CH 4 / CO 2 =1 in the mixed gas at 5°C / min to 800°C for carbonization to obtain CDUT-NM5A catalyst, its typical Ni-Mo 2 C / Al 2 o 3 Composite figure 2 shown. After nitrogen adsorption / desorp...

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Abstract

The invention relates to a nickel-molybdenum carbide composite catalyst for preparing a synthesis gas through dry reforming of methane, and aims at solving the problem that catalyst deactivation is caused by the situation that active components in the conventional nickel-based catalyst and molybdenum-based catalyst are easy to oxidize and sinter during the process of preparing the synthesis gas through dry reforming of methane. The preparation method of the nickel-molybdenum carbide composite catalyst comprises the following steps: a nickel molybdenum oxide precursor is synthesized through a one-step synthesis urea combustion method by adopting the double components, namely nickel and molybdenum; the virgin gas is subjected to dry reforming through methane, and an Ni-Mo2C composite structure is compounded in situ; carbonization-oxidation circulation of Mo2C is established during the process of dry reforming of methane at the same time, so as to obtain the nickel-molybdenum carbide composite catalyst which is sintering-resistant, oxidation-resistant and stable in structure. According to the nickel-molybdenum carbide composite catalyst, the stability and hydrogen selectivity of the process of preparing the synthesis gas through dry reforming of methane are improved; the chemical composition of the catalyst provided by the invention is Nia (Mo2C)b (Al2O3 )c in which the a is 0.09-0.19, the b is 0.03-0.10 and the c is 0.75-0.88.

Description

technical field [0001] The invention relates to a nickel-molybdenum carbide composite catalyst for producing synthesis gas by dry reforming of methane, more specifically, to a nickel-molybdenum carbide composite catalyst synthesized in situ for producing synthesis gas by dry reforming of methane The catalyst of composite phase belongs to the technical field of preparing synthesis gas by methane dry reforming. Background technique [0002] Syngas, i.e. H 2 The mixture of CO and CO can be adjusted by adjusting different hydrogen-carbon ratios (H 2 / CO), used as raw material gas to synthesize methanol, acetic acid and hydrocarbon fuels and other products, and can also be used as fuel for solid oxide fuel cells. Synthesis gas (CH 4 +CO 2 =2CO+2H 2 ), that is, the methane dry reforming process, on the one hand, fully utilizes the two greenhouse gases methane and carbon dioxide, and on the other hand, produces a hydrogen-carbon ratio (H 2 / CO) is close to 1, which provides i...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/883B01J35/10C01B3/40
CPCY02P20/52
Inventor 黄利宏段义平钟心燕尚锐淑谢伟周庆杨浩牛飞兴
Owner CHENGDU UNIVERSITY OF TECHNOLOGY
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