Preparation method and application of copper modified molecular sieve catalyst

A catalyst and molecular sieve technology, applied in the field of catalytic chemistry, can solve the problems of discontinuous reaction process, low methanol yield, uneconomical oxidant and catalyst, etc., to achieve optimized methane activation effect, excellent catalytic activity, and good hydrothermal stability Effect

Pending Publication Date: 2021-06-18
NANKAI UNIV
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0005] In order to solve the problems of excessive oxidation of methane, low yield of methanol, discontinuous reaction process, and uneconomical oxidant and catalyst used in the reaction in the existing technology, the purpose of the present invention is to provide a kind of catalyst with excellent catalytic performance and good hydrothermal stability. , green economy, molecular sieve catalyst with simple synthesis process

Method used

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  • Preparation method and application of copper modified molecular sieve catalyst
  • Preparation method and application of copper modified molecular sieve catalyst
  • Preparation method and application of copper modified molecular sieve catalyst

Examples

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Embodiment 1-6

[0030] This embodiment provides the preparation method of the copper-modified molecular sieve catalyst that is used for the selective oxidation of methane to produce methanol,

[0031] Step 1. Mix 85% orthophosphoric acid as the phosphorus source in water, stir for five minutes, add 67% pseudo-boehmite and stir for 1.5 hours at room temperature to obtain the first mixed solution;

[0032] Step 2, another CuSO 4 ·5H 2 O is mixed in a certain amount of water, and after it is completely dissolved, tetraethylenepentamine is added and stirred for 30 minutes, then morpholine is added for stirring, and 50% silica sol is added after 30 minutes to obtain a second mixed solution;

[0033] Step 3. The second mixed solution is mixed with the first mixed solution, stirred at room temperature for 6-12 hours, mixed evenly, put into a stainless steel reactor lined with polytetrafluoroethylene, and crystallized at 200°C for 2-4 hours. day; after the crystallization was completed, the reactor...

Embodiment 7-12

[0045] The above-mentioned Cu / SAPO-34-3 was used as the catalyst. Except that the reaction temperature was controlled at 200-400° C., other operating conditions were the same as in Examples 1-6. See Table 3 for specific analysis results.

[0046] Table 3 Effect of reaction temperature on the reaction of methane selective oxidation to methanol

[0047] Example 7 8 9 10 11 12 Reaction temperature (°C) 200 250 270 300 350 400 Methane conversion rate (%) 0 0.0017 0.0045 0.0126 0.0416 0.0505 Methanol selectivity (%) 0 100 100 86 52 19 Methanol productivity (μmol / g / h) 0 20 62 176 503 196

[0048] As can be seen from Table 3, as the reaction temperature increases, the conversion rate of methane increases and the selectivity of methanol decreases. At 270 ° C, the selectivity of methanol is 100%, after which the peroxidation product carbon dioxide appears, lead to a decrease in selectivity.

Embodiment 13-16

[0050] The catalyst is the above-mentioned Cu / SAPO-34-3. Take 0.1-0.3g sample and put it into a quartz reactor. After pretreatment, feed methane gas, water vapor, and oxygen reaction gas. Carry out below, the total flow of control inlet gas is 60ml / min, change the ratio of feeding reaction gas, wherein the volume content of methane is 99% in the reaction gas of example 13, without oxygen; The volume content of methane in the reaction gas of example 13 98%, the volume content of oxygen is 0.04%; the volume content of methane in the reaction gas of example 14 is 78%, and the volume content of oxygen is 0.2%;

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Abstract

The invention discloses a preparation method of a copper modified molecular sieve catalyst applied to preparation of methanol by selective oxidation of methane, which comprises the following step of placing a certain amount of molecular sieve catalyst sample in a quartz tube of a fixed bed reactor, introducing inert gas, and pretreating at 500 DEG C, cooling to a reaction temperature, introducing a reaction gas mixture of methane, water vapor and oxygen in a certain proportion into the fixed bed reactor, reacting at 200-400 DEG C, introducing a product into a gas chromatograph for analysis and detection, preferably, enabling the selectivity of methanol to be 93%, and the yield to be 184 mol/kgcat/h. The copper modified molecular sieve catalyst provided by the invention is Cu/SAPO-34 which is synthesized in situ by utilizing a one-step method and controls the gradient change of the content of loaded metal copper. The molecular sieve catalyst obtained by the invention has the characteristics of simple synthesis process, good hydrothermal stability and excellent catalytic performance. When the catalyst is applied to methanol preparation through methane oxidation, continuous production of methanol can be realized, the reaction process is simple, the process is green and economical, the methanol yield is high, and the industrial application value is high.

Description

technical field [0001] The invention belongs to the field of catalytic chemistry, and relates to a preparation method and application of a copper-modified molecular sieve catalyst used for selective oxidation of methane to methanol. Background technique [0002] As a widely distributed and abundant fossil energy, methane has a great advantage in mass calorific value compared with other hydrocarbons. It is found in abundance in natural gas, can be extracted cost-effectively from shale gas, tight oil, and methane can be used for heating, electricity generation and as a power source for vehicles. However, this methane is usually burned, producing large amounts of carbon dioxide. Therefore, finding an efficient process to convert methane into high value-added fuels or chemicals is of great economic and sustainable significance. Methanol has extremely high application value. It can be used not only as an energy source for hydrogen production, but also as a vehicle fuel or direc...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/85C07C29/50C07C31/04
CPCB01J29/85C07C29/50B01J2229/18C07C31/04Y02P20/52
Inventor 李兰冬王玉武光军戴卫理关乃佳
Owner NANKAI UNIV
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