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Method for preparing methyl alcohol, formaldehyde and CO used for methane direct selective oxidation

A methanol and formaldehyde technology, applied in the field of methane, can solve the problems of catalyst system, complex reaction process, unreported literature and patents, easy deactivation of catalyst, etc., achieve low catalyst cost, improve carbon resource utilization, and high C1 oxidation The effect of material selectivity

Active Publication Date: 2018-02-27
XIAMEN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Therefore, it is usually difficult to obtain the desired target product selectivity at a suitable methane conversion rate
For now, the yield of heterogeneous catalytic methane oxidation to methanol and formaldehyde, which has the most industrial application prospect, is generally less than 5%, and the catalyst is easily deactivated.
The process has so far been a batch reaction, limiting its further scale-up and even industrialization
However, in the Chinese patent CN 102285864 B, palladium noble metal and various organic solvents are used to catalyze and oxidize methane into methyl trifluoroacetate, and the methyl trifluoroacetate is hydrolyzed to produce methanol. The catalyst system and reaction process are complex and the reaction conditions Harsh (pressure 2 ~ 5MPa)
[0005] At present, the work of using BN as a catalyst to catalyze the dehydrogenation of alkanes above C2 to produce corresponding alkenes has been reported (Chinese patent CN 106140240 A; Chinese patent CN 106694017 A; Science 2016,354:1570; ChineseJ Catal.2017,38:389) , but the literature and patents for the direct catalytic oxidation of methane to prepare platform molecules such as methanol, formaldehyde, and CO have not been reported

Method used

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  • Method for preparing methyl alcohol, formaldehyde and CO used for methane direct selective oxidation
  • Method for preparing methyl alcohol, formaldehyde and CO used for methane direct selective oxidation
  • Method for preparing methyl alcohol, formaldehyde and CO used for methane direct selective oxidation

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Experimental program
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Effect test

Embodiment 1

[0038] With BN (400mg) as catalyst, the reactor adopts continuous flow fixed bed reactor (inner diameter=7mm), P 总 =0.1MPa, P(CH 4 ) = P(O 2 )=32kPa, the total flow rate of the reaction mixture is 15.5mL / min, and when the reaction temperature is 550°C, the conversion rate of methane is 12%, the selectivity of methanol and formaldehyde is respectively 8%, 18%, and the total yield of the two is 3.1 %, CO, CO 2 The selectivities were 66% and 4%, respectively.

Embodiment 2

[0040] With BN (200mg) as catalyst, the reactor adopts continuous flow fixed bed reactor (inner diameter=7mm), P 总 =0.1MPa, P(CH 4 ) = P(O 2 ) = 32kPa, T 反 =600°C, when the total flow rate of the reaction mixture gas is 31.1mL / min, the methane conversion rate is 28%, the selectivity of methanol and formaldehyde are 5% and 4%, respectively, and the total yield of the two is 2.5%, CO, CO 2 The selectivities were 74% and 8%, respectively.

Embodiment 3

[0042] With BN (150mg) as catalyst, the reactor adopts continuous flow fixed bed reactor (inner diameter=5mm), P 总 =0.1MPa, T 反 =600°C, the total flow rate of the reaction mixture is 46.7mL / min, P(CH 4 )=20kPa, when CH 4 :O 2 When =1:2 (mol), the conversion rate of methane is 21%, the selectivity of methanol and formaldehyde is 5%, 16% respectively, and the total yield of the two is 4.4%, CO, CO 2 The selectivities were 72% and 5%, respectively.

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Abstract

The invention discloses a method for preparing methyl alcohol, formaldehyde and CO used for methane direct selective oxidation. The method comprises the following steps: preparing a BN powder materialcatalyst, after mixing boric acid with urea, dissolving and stirring with a water and methyl alcohol mixed solvent, carrying out thermostatic waterbath standing for crystallization, and roasting under an inert atmosphere to obtain a BN powder material; tabletting and forming a roasted sample, smashing and sieving to obtain a BN powder material catalyst; catalyst activation: introducing oxygen-containing gas into a continuous flow reactor filled with the BN powder material catalyst for heating, activating, introducing inert gas, adjusting to a reaction temperature, and switching into a reaction gas; and preparing methyl alcohol, formaldehyde and CO.

Description

technical field [0001] The invention relates to methane, in particular to a method for preparing methanol, formaldehyde and CO by direct selective oxidation of methane. Background technique [0002] With the continuous discovery of new reserves of natural gas resources, especially the exploitation of shale gas and combustible ice, the effective utilization of natural gas with methane as the main component has attracted more and more attention. Methane conversion is divided into direct conversion and indirect conversion. In the indirect conversion, it is first converted into synthesis gas or methyl halide, and then generates oxygenated compounds such as methanol and formic acid or hydrocarbons such as alkanes and olefins. The indirect conversion process has a long process flow, high energy consumption or serious equipment corrosion, and high equipment investment. In the direct conversion of methane, oxidative coupling to ethane or ethylene, dehydroaromatization, etc., all r...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C07C27/14C07C29/50C07C31/04C07C45/33C07C47/048C01B32/40B01J27/24
CPCB01J27/24C01B2203/06C01B2203/061C07C29/50C07C45/33C07C31/04C07C47/04Y02P20/52
Inventor 张朝霞谈江乔田金树林敬东王帅王勇
Owner XIAMEN UNIV
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