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Application of cerium-based catalyst in methane oxyhalogenation methods used for preparing halogenated methane

A cerium-based catalyst, methane halogen oxidation technology, applied in physical/chemical process catalysts, carbon monoxide, halogenated hydrocarbon preparation and other directions, can solve the problems of easy deliquescence and complex preparation methods

Inactive Publication Date: 2012-02-08
XIAMEN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, LaCl 3 Very easy to deliquescence, it needs to use LaOCl as the precursor, react with HCl in situ at 400°C for more than 12 hours, and the preparation method is complicated

Method used

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  • Application of cerium-based catalyst in methane oxyhalogenation methods used for preparing halogenated methane
  • Application of cerium-based catalyst in methane oxyhalogenation methods used for preparing halogenated methane
  • Application of cerium-based catalyst in methane oxyhalogenation methods used for preparing halogenated methane

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0032] Catalyst preparation:

[0033] 3.47g Ce(NO 3 ) 2 *6H 2 Dissolve O in 20 mL of deionized water, add 140 ml of 9M NaOH solution under stirring, then transfer to an autoclave for 24 h at 100 ° C, cool, filter with suction, dry at 100 ° C, and roast at 550 ° C for 6 h to obtain CeO 2 .

[0034] Catalyst Test:

[0035] The reaction was carried out in a fixed-bed flow reactor at normal pressure, and the reactor was a quartz glass tube with an inner diameter of 10 mm. The reaction conditions are: catalyst dosage is 0.500g, reaction temperature is 480°C, CH 4 Flow 16.0mL / min, HCl flow 8.0mL / min, O 2 The flow rate is 8.0mL / min. The tail gas was analyzed by gas chromatography, with N 2 Do internal standard.

[0036] Experiments show that the conversion rate of methane is 27%, the selectivity of monochloromethane is 55%, the selectivity of dichloromethane is 14%, the selectivity of chloroform is 0.3%, the selectivity of carbon monoxide is 15%, and the selectivity of carbo...

Embodiment 2

[0038] Catalyst preparation:

[0039] 3.47g Ce(NO 3 ) 2 *6H 2 Dissolve O in 20 mL of deionized water, add 140 ml of 6M NaOH solution under stirring, then transfer to an autoclave for 24 h at 180 ° C, cool, filter with suction, dry at 100 ° C, and roast at 600 ° C for 6 h to obtain CeO 2 .

[0040] Catalyst Test:

[0041] The reaction was carried out in a fixed-bed flow reactor at normal pressure, and the reactor was a quartz glass tube with an inner diameter of 20 mm. The reaction conditions are: catalyst dosage is 2.000g, reaction temperature is 600°C, CH 4 Flow 10.0mL / min, O 2 Flow rate 5.0mL / min, 40wt% HBr / H 2 The O flow rate is 4.0 mL / min. Tail gas and liquid products were analyzed on a gas chromatograph.

[0042] Experiments show that the conversion rate of methane is 18%, the selectivity of methyl bromide is 75%, the selectivity of dibromomethane is 3.2%, the selectivity of carbon monoxide is 20%, and the selectivity of carbon dioxide is 1.4%.

Embodiment 3～8

[0044] Catalyst preparation:

[0045] 3.47g Ce(NO 3 ) 2 *6H 2 O and the corresponding metal nitrate solution were dissolved in 20mL of deionized water according to the mol composition of the catalyst in Table 1. After mixing evenly, 140ml of 9M NaOH solution was added under stirring, and then transferred to an autoclave for 24h at 100°C, cooled, and pumped. Filter, dry at 100°C, and calcined at 550°C for 6h.

[0046] Catalyst Test:

[0047] According to the test conditions in Example 1, see Table 1 for the experimental results of Examples 3-8.

[0048] Table 1

[0049]

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Abstract

The invention relates to a cerium-based catalyst, and relates to an application of the cerium-based catalyst in methane oxyhalogenation methods used for preparing halogenated methane. The methane oxyhalogenation methods used for preparing halogenated methane comprise a methane chlorine oxidation method used for preparing methyl chloride and a methane bromine oxidation method used for preparing methyl bromide. The cerium-based catalyst is suitable to be used in methane oxyhalogenation reactions. The cerium-based catalyst can be a CeO2 catalyst, a cerium-based bi-component composite oxide catalyst, a load-type cerium-based oxide catalyst, or the like. With the cerium-based catalyst, the methane oxyhalogenation reactions including a chlorine oxidation reaction and a bromine oxidation reaction can be effectively and stably catalyzed, and methyl chloride and methyl bromide can be prepared. With the cerium-based catalyst, reactants such as CH4, HCl and O2 can be catalytically converted with high efficiency for carrying out a chlorine oxidation reaction, such that products CH3Cl and CH2Cl2 are produced. Also, with the cerium-based catalyst, reactants such as CH4, HBr(H2O), and O2 can be converted with high efficiency for carrying out a bromine oxidation reaction, such that products CH3Br and CH2Br2 are produced.

Description

technical field [0001] The invention relates to a cerium-based catalyst, in particular to the application of a cerium-based catalyst in methane halooxidation to halide. Background technique [0002] With the long-term and large-scale development of oil resources, its reserves have gradually decreased, and oil prices have increased day by day. In contrast, gas resources such as natural gas, coalbed methane, and shale gas with relatively high reserve-production ratios have attracted people's attention. my country's natural gas resources account for about 10% of the world's total resources. In addition, coalbed methane and shale gas reserves are also very rich. The main components of these gas resources are methane (CH 4 ), its content is 60% to 99%. In addition to being directly used as energy (urban gas), methane is also a valuable carbon resource. Therefore, the development of effective ways to convert methane into high value-added chemicals such as aromatics, olefins, a...

Claims

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Application Information

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IPC IPC(8): C07C19/03C07C19/04C07C19/075C07C17/35B01J23/83B01J23/10B01J23/34C01B31/18C01B31/20C01B32/40C01B32/50
Inventor 张庆红王智慧何洁丽邓卫平孙振玲赵擂王野
Owner XIAMEN UNIV
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