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Method for preparing acetic acid by one-step conversion of CH4 and CO2 through cooperation of low-temperature plasma and modified molecular sieve catalyst

A technology of plasma and molecular sieve, which is applied in the field of conversion and utilization of CH4 and CO2, to achieve the effect of simple process, green method and increased added value

Active Publication Date: 2020-09-18
DALIAN MARITIME UNIVERSITY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0018] Obviously, the above-mentioned transformation of CH using plasma technology 4 and CO 2 In the reports of one-step synthesis of acetic acid, the research focuses on the plasma reaction parameters, plasma reactor and added gas, and no molecular sieve and plasma synergistic conversion of CH 4 and CO 2 One-step Synthesis of Acetic Acid

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0055]A plasma-catalyzed CH 4 / CO 2 The method of reforming acetic acid adopts the synergistic effect of dielectric barrier discharge plasma and modified HZSM-5 molecular sieve catalyst to activate CH 4 and CO 2 Selective generation of acetic acid;

[0056] The difference from Comparative Example 3 is: using the synergistic effect of the modified HZSM-5 molecular sieve catalyst and dielectric barrier discharge plasma to convert CH 4 and CO 2 ; The modified HZSM-5 molecular sieve catalyst is passivated by Si / Al of 30 HZSM-5 molecular sieve through 550°C water vapor for 3h, the influent flow rate is 3mL / h, and after passivation, use 0.6mol / L nitric acid solution Pickling for 3h, then washing with deionized water until neutral, drying, and in N 2 / O 2 (N 2 Accounting for 75%) in a plasma atmosphere at 450 ° C for 3 hours;

[0057] The reaction conditions are: the reaction temperature is 60°C, the CH 4 and CO 2 The molar ratio is 1:1, the CH 4 and CO 2 The residence ti...

Embodiment 2

[0060] A plasma-catalyzed CH 4 / CO 2 The difference between the method for reforming acetic acid and Example 1 is that the passivation temperature is 400°C.

Embodiment 3

[0062] A plasma-catalyzed CH 4 / CO 2 The difference between the method for reforming acetic acid and Example 1 is that the passivation temperature is 700°C.

[0063] Conclusion: Examples 1, 2, and 3 only change the water vapor passivation temperature, and the obtained feed gas conversion rate and acetic acid selectivity are significantly different, indicating that the water vapor passivation temperature has a significant effect on the reaction performance of the modified HZSM-5 molecular sieve catalyst. influences.

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PUM

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Abstract

The invention relates to a method for preparing acetic acid by one-step conversion of CH4 and CO2 through cooperation of low-temperature plasma and a modified molecular sieve catalyst, and belongs tothe field of CH4 and CO2 conversion and utilization. The preparation method comprises the following steps: (1) modifying a molecular sieve by at least one of a water vapor passivation method, an acidtreatment method, an alkali treatment method, an alkali metal modification method, an alkaline earth metal modification method and a rare earth metal modification method; and (2) roasting the productobtained in the step (1) in a plasma atmosphere at 350-500 DEG C for 0.5-3 hours. According to the method, CH4 and CO2 are converted into acetic acid with high additional value by using a one-step method under the conditions of low temperature and normal pressure, the process is simple, the method is green, the atom economy is high, the problem that the conventional catalytic CH4 and CO2 reactionneeds high temperature (generally higher than 700 DEG C) is solved, and meanwhile, the additional value of the product converted from CH4 and CO2 is increased.

Description

technical field [0001] The invention relates to a low-temperature plasma and a modified molecular sieve catalyst for synergistic one-step conversion of CH 4 and CO 2 The method of producing acetic acid belongs to CH 4 and CO 2 transform the field of use. Background technique [0002] CH 4 and CO 2 It is the two main greenhouse gases in the atmosphere, and it is the main cause of aggravating the greenhouse effect and global warming. It is also an important raw material for one-carbon chemistry. CH 4 Widely distributed in nature, it is the main component of natural gas, biogas, oilfield gas and coal mine tunnel gas, and it is also a cheap, easy-to-obtain and abundant carbon and hydrogen source. Atmospheric CO 2 It mainly comes from human activities such as fossil fuel combustion, and its concentration and average annual emissions show an increasing trend year by year. It is estimated that by 2040, CO 2 Global emissions are about 35.7 billion tons. Therefore, CH 4 an...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J37/10B01J37/34B01J29/40B01J29/89B01J29/85B01J29/03B01J29/18B01J29/70C07C51/15C07C53/08
CPCB01J37/10B01J37/349B01J29/405B01J29/89B01J29/85B01J29/03B01J29/185B01J29/7084C07C51/15B01J2229/186C07C53/08
Inventor 王丽杜晓敏徐红丽朱益民
Owner DALIAN MARITIME UNIVERSITY
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