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

A technology for oxidative synthesis and catalyst, which is applied in the preparation of oxidation reaction, preparation of carbon-based compounds, chemical instruments and methods, etc., which can solve the requirements of high catalyst activity and stability, low selectivity of formaldehyde and methanol, and relatively high equipment safety requirements. Advanced problems, to achieve the effect of enhancing oxygen storage capacity and electron transfer capacity, high methane activation capacity, and improving conversion rate

Active Publication Date: 2015-12-16
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
However, the reaction pressure in this patent is too high, and the safety requirements for the equipment are relatively high.
[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] 4.9gSbCl 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 previo...

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] 4.9gSbCl 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 previou...

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] 4.9gSbCl 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 previo...

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PUM

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Abstract

The invention discloses a catalyst for the selective oxidation of methane to synthesize methanol and formaldehyde. It uses SiO2 modified by Nb and Ce as a carrier, Mo and Sb as active components. According to the weight content of the final catalyst, Mo? 5%~11%; Sb? 7%~20%; Nb? 1%~3.5%; Ce? 1%~3.5%; the balance is SiO2. A method for preparing a catalyst for the selective oxidation of methane to synthesize methanol and formaldehyde. The impregnation method is used to support Nb and Ce to prepare SiO2 modified by Nb and Ce; then the active components Sb and Mo are loaded; finally, the final catalyst is obtained by forming and sieving . The catalyst can be used in the selective oxidation of methane to produce methanol and formaldehyde under low pressure, and has the advantages of high methane conversion rate, high methanol and formaldehyde selectivity and the like.

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 Patents(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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