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Catalyst for synthesis of methanol and formaldehyde through selective oxidation of methane, and preparation method and application thereof

A technology of oxidation synthesis and selectivity, which is applied in the direction of oxidation reaction preparation, carbon-based compound preparation, chemical instruments and methods, etc. It can solve the problems of high catalyst activity and stability, low selectivity of formaldehyde and methanol, and high reaction pressure. , to achieve the effects of enhancing oxygen storage capacity and electron transfer capacity, high methane activation capacity, and improving conversion rate

Active Publication Date: 2014-05-14
CHINA PETROLEUM & CHEM CORP +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0004] CN1621150A discloses a silica-loaded antimony oxide catalyst and its preparation method for the selective oxidation of methane to formaldehyde. Its examples show that the highest formaldehyde selectivity of the reaction at 600 ° C is 30.2%, and the methane conversion rate at this time is Only 0.7%, but the reaction temperature is too high, which requires high catalyst activity and stability
[0005] In short, the above-mentioned catalysts generally have one or more deficiencies such as the need to further increase the methane conversion rate, the low selectivity of formaldehyde and methanol, and the relatively high reaction pressure.

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0021] Weigh 1.9g niobium oxalate and 1.6g Ce(NO 3 ) 3 ·6H 2 O dissolved in water, 20.0g SiO 2 Immerse the carrier in the solution, let it stand at room temperature for 12 hours, remove water by rotary evaporation at 60°C, dry at 120°C for 12 hours, and bake at 500°C for 5 hours to prepare Nb and Ce modified SiO 2 carrier.

[0022] 4.9g SbCl 5 Add an appropriate amount of ethanol, and after the dissolution is complete, add the Nb and Ce-modified SiO prepared in the previous step 2 The carrier was impregnated with an equal volume for 4 hours, dried at room temperature for 12 hours, added to 100mL ammonia water and stirred for 2 hours, filtered, washed with water until the pH value was 6~7, dried at room temperature for 24 hours, and dried in an oven at 120°C for 24 hours.

[0023] Weigh 2.8g (NH 4 ) 6 Mo 7 o 24 .4H 2 O was completely dissolved in an appropriate amount of water; then the solution was impregnated with an equal volume on the carrier prepared in the previ...

Embodiment 2

[0026] Weigh 1.9g niobium oxalate and 1.6g Ce(NO 3 ) 3 ·6H 2 O dissolved in water, 20.0g SiO 2 Immerse the carrier in the solution, let it stand at room temperature for 12 hours, remove water by rotary evaporation at 60°C, dry at 120°C for 12 hours, and bake at 500°C for 5 hours to prepare Nb and Ce modified SiO 2 carrier.

[0027] 4.9g SbCl 5 Add an appropriate amount of ethanol, and after the dissolution is complete, add the Nb and Ce-modified SiO prepared in the previous step 2 The carrier was impregnated with an equal volume for 4 hours, dried at room temperature for 12 hours, added to 100mL ammonia water and stirred for 2 hours, filtered, washed with water until the pH value was 6~7, dried at room temperature for 24 hours, and dried in an oven at 120°C for 24 hours.

[0028] Weigh 2.8g (NH 4 ) 6 Mo 7 o 24 .4H 2O was completely dissolved in an appropriate amount of water; then the solution was impregnated with an equal volume on the carrier prepared in the previo...

Embodiment 3

[0031] Weigh 1.9g niobium oxalate and 1.6g Ce(NO 3 ) 3 ·6H 2 O dissolved in water, 20.0g SiO 2 Immerse the carrier in the solution, let it stand at room temperature for 12 hours, remove water by rotary evaporation at 60°C, dry at 120°C for 12 hours, and bake at 500°C for 5 hours to prepare Nb and Ce modified SiO 2 carrier.

[0032] 4.9g SbCl 5 Add an appropriate amount of ethanol, and after the dissolution is complete, add the Nb and Ce-modified SiO prepared in the previous step 2 The carrier was impregnated with an equal volume for 4 hours, dried at room temperature for 12 hours, added to 100mL ammonia water and stirred for 2 hours, filtered, washed with water until the pH value was 6~7, dried at room temperature for 24 hours, and dried in an oven at 120°C for 24 hours.

[0033] Weigh 2.8g (NH 4 ) 6 Mo 7 o 24 .4H 2 O was completely dissolved in an appropriate amount of water; then the solution was impregnated with an equal volume on the carrier prepared in the previ...

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PUM

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Abstract

The invention discloses a catalyst for synthesis of methanol and formaldehyde through selective oxidation of methane. According to the invention, SiO2 modified by Nb and Ce is used as a carrier, and Mo and Sb are used as active components; in terms of the weight of the finished catalyst, Mo accounts for 5 to 11%, Sb accounts for 7 to 20%, Nb accounts for 1 to 3.5%, and Ce accounts for 1 to 3.5%, with the balance being SiO2. A preparation method for the catalyst used for synthesis of methanol and formaldehyde through selective oxidation of methane comprises the following steps: loading Nb and Ce by using an impregnation method so as to prepare SiO2 modified by Nb and Ce; then loading the active components--Sb and Mo; and finally, carrying out molding and screening so as to prepare the finished catalyst. The catalyst can be used for a selective oxidation reaction of methane for preparation of methanol and formaldehyde at a low pressure and has the advantages of a high methane conversion rate, high methanol and formaldehyde selectivity, etc.

Description

technical field [0001] The invention relates to a catalyst for the selective oxidation of methane to synthesize methanol and formaldehyde and its preparation method and application, in particular to a catalyst for the selective oxidation of methane to synthesize methanol and formaldehyde with silicon dioxide modified by multiple additives as a carrier and its Preparation methods and applications. Background technique [0002] With the increasing shortage of fossil resources such as oil and coal, the use of natural gas as a high-quality, clean energy and chemical raw material has attracted more and more attention from all countries. The main component of natural gas is methane. The development of methane direct production of methanol and formaldehyde technology, compared with the current industrialized indirect method, has the advantages of simple route and low cost. Therefore, Shell, Sasol, Exxon-Mobil, BP and other major oil companies Has invested heavily in research. The...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/28C07C27/14C07C31/04C07C29/50C07C47/048C07C45/33
CPCY02P20/52
Inventor 张信伟张舒东方向晨尹泽群张喜文刘全杰
Owner CHINA PETROLEUM & CHEM CORP
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