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Catalyst for preparing hydrocarbons by one-step hydrogenation of carbon dioxide and preparation method thereof

A carbon dioxide and catalyst technology, which is applied to the catalyst for preparing hydrocarbons by one-step hydrogenation of carbon dioxide and the field of preparation thereof, can solve problems such as unfavorable methanol and low methane, and achieve the effects of reducing production cost, small particle size and high target product selectivity.

Active Publication Date: 2021-03-12
SHANGHAI ADVANCED RES INST CHINESE ACADEMY OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

The reaction to generate hydrocarbons is an endothermic reaction, and the higher the temperature, the more favorable it is. However, the reaction to generate methanol or corresponding intermediate species is an exothermic reaction, and the higher the temperature, the more unfavorable the formation of methanol. Therefore, how to break through the thermodynamic equilibrium is guaranteed Under the premise of low methane selectivity, it is the key to obtain target hydrocarbons with high selectivity

Method used

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  • Catalyst for preparing hydrocarbons by one-step hydrogenation of carbon dioxide and preparation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0044] 40.4g Fe(NO 3 ) 3 9H 2 O was added to 1L deionized water to prepare a mixed metal salt solution with a metal ion concentration of 0.1mol / L, and 5.30g of sodium carbonate was added to a mixed solution of 0.25L deionized water and 0.25L absolute ethanol to prepare a 0.1mol / L solution. L of precipitant solution, add the precipitant solution dropwise to the metal salt solution at 20°C, the dropping process needs to be fully stirred, the final pH value is kept at 9, and the resulting product is stirred at 70°C after the precipitation reaction After aging for 4 hours under high temperature, the resulting precipitate was washed several times with deionized water, then dried at 80°C for 12 hours, and then calcined at 350°C for 4 hours to obtain a metal oxide, which was characterized by a particle size of 20nm and a specific surface area of ​​75m 2 / g. Set the specific surface area to 500m 2 / g, the mesopore diameter is 4.1nm, and the mesopore volume is 0.41cm 3 / g of hiera...

Embodiment 2

[0047] 13.32g Cr(NO 3 ) 2 9H 2 O and 28.62g Zr(NO 3 ) 4 ·5H 2 O was added to a mixed solution of 0.1L water and 0.025L absolute ethanol to prepare a mixed metal salt solution with a metal ion concentration of 0.8mol / L, and 3.3mL ammonia water was added to a mixed solution of 0.05L absolute ethanol to make 1mol / L of precipitant solution, add the precipitant solution dropwise to the metal salt solution at 25°C, the dropping process needs to be fully stirred, the final pH value is kept at 10, and the resulting product is stirred at 60°C after the precipitation reaction is completed Aged for 6 hours under the same conditions, then the obtained precipitate was washed several times with deionized water, then dried at 60°C for 18 hours, and then calcined at 300°C for 3 hours to obtain a metal oxide, which was characterized by a particle size of 10nm and a specific surface area of 136m 2 / g, tableted and sieved into 20-40 mesh. The specific surface area is 340m 2 / g, the meso...

Embodiment 3

[0050] 41.79g Ga(NO 3 ) 3 ·xH 2 O was added to the mixed solution of 0.12L water and 0.08L absolute ethanol to prepare a metal ion concentration of 0.5mol / L mixed metal salt solution, and 3.3mL ammonia water was added to the mixture of 0.01L deionized water and 0.02L absolute ethanol Prepare a 1.67mol / L precipitant solution in the mixed solution, and add the precipitant solution dropwise to the metal salt solution at 15°C. The dropping process needs to be fully stirred, and the final pH value is kept at 11. After the precipitation reaction is completed, the The obtained product was aged at 100°C for 1.5h, then the obtained precipitate was washed several times with deionized water, then dried at 60°C for 24h, and then calcined at 300°C for 7h to obtain a metal oxide. The diameter is 23nm and the specific surface area is 112m 2 / g. The specific surface area of ​​molecular sieve is 445m 2 / g, the mesopore diameter is 4.39nm, and the mesopore volume is 0.49cm 3 / g Hierarchic...

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Abstract

The invention provides a catalyst for one-step hydrogenation of carbon dioxide to prepare hydrocarbons and a preparation method thereof. The catalyst for one-step hydrogenation of carbon dioxide to prepare hydrocarbons includes nanometer metal oxides and hierarchically porous zeolite molecular sieves. The nanometer metal oxides The mass fraction of the multi-stage zeolite molecular sieve in the catalyst is 10%-90%, and the mass fraction of the multi-stage zeolite molecular sieve in the catalyst is 10%-90%. The catalyst obtained by the present invention has excellent catalytic performance, good reaction stability, high selectivity of the target product, C in hydrocarbon products 2 = ~C 4 = Up to 80%, C 5+ Up to 85%, aromatics up to 65%.

Description

technical field [0001] The invention relates to the technical field of catalysts, in particular to a catalyst for one-step hydrogenation of carbon dioxide to prepare hydrocarbons and a preparation method thereof. Background technique [0002] carbon dioxide (CO 2 ) as a "carbon source" compound that exists in abundance in nature, converting it into valuable chemicals or fuels can not only solve the problem of excessive CO 2 Environmental problems caused by emissions can also alleviate the problem of excessive dependence on fossil fuels. The use of hydrogen produced by new energy sources for CO 2 Hydroconversion can convert CO 2 Conversion into products such as chemicals (methanol, formic acid and dimethyl ether, etc.), synthesis gas, materials and liquid fuels. Among many products, hydrocarbons are considered to be more potential target products due to reasons such as economic value and wide application, such as low-carbon olefins (C 2 ＝ ~C 4 ＝ ), higher carbon hydro...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J29/08B01J29/40B01J29/46B01J29/70B01J29/72B01J29/85C10G2/00B01J35/00
CPCC10G2/50B01J29/088B01J29/405B01J29/46B01J29/7007B01J29/7092B01J29/7215B01J29/85B01J29/084B01J37/031B01J23/745B01J23/26B01J23/08B01J23/10B01J21/066B01J23/06B01J37/04B01J2229/38B01J29/40B01J29/7015B01J29/70B01J37/0036B01J37/009B01J37/06B01J37/16B01J37/18B01J37/08B01J35/19B01J35/40B01J35/23B01J35/613B01J35/615B01J19/14B01J20/3021B01J29/7057B01J29/7615B01J37/0063B01J37/082
Inventor 孙予罕党闪闪高鹏卜宪昵刘子玉王慧钟良枢邱明煌石志彪
Owner SHANGHAI ADVANCED RES INST CHINESE ACADEMY OF SCI
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