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Method for promoting electro-catalytic oxidation of methane to generate chloromethane by using chloride ions

A technology for electrocatalytic oxidation and chloromethane, which can be used in methane capture, electrolytic organic production, electrodes, etc., and can solve problems such as high price

Active Publication Date: 2021-07-30
FUDAN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, this type of method must use expensive oxidizing agents, such as H 2 o 2 , NO x and oleum

Method used

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  • Method for promoting electro-catalytic oxidation of methane to generate chloromethane by using chloride ions
  • Method for promoting electro-catalytic oxidation of methane to generate chloromethane by using chloride ions
  • Method for promoting electro-catalytic oxidation of methane to generate chloromethane by using chloride ions

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Experimental program
Comparison scheme
Effect test

Embodiment 1

[0024] Embodiment 1, the preparation of cobalt-nickel oxide electrocatalyst, concrete steps are as follows:

[0025] Cobalt-nickel mixed oxide nanoparticles with a ratio of 1:1 were synthesized by a hydrothermal method, and the morphology of the nanoparticles was as follows figure 2 shown. 1mmolCo(OAc) 2 4H 2 O and 1 mmol Ni(OAc) 2 4H 2 O was dissolved in 25 mL of deionized water. Add 2.5 mL of 30% ammonia water to the solution, and stir vigorously with oxygen for at least 10 min. The solution was then transferred to a 50 mL autoclave at 150 o C under reaction 3h. The precipitate was separated by centrifugation and washed several times with deionized water. at 80 o After drying at C, the catalyst was heated at 350 o C was calcined in air for 2h.

Embodiment 2

[0026] Embodiment 2, the preparation of cobalt oxide electrocatalyst, concrete steps are as follows:

[0027] Cobalt oxide nanoparticles were synthesized by a hydrothermal method. 2 mmol Co(OAc) 2 4H 2 O was dissolved in 25 mL of deionized water. Add 3.0 mL of 30% ammonia water to the solution, and stir vigorously with oxygen for at least 10 min. The solution was then transferred to a 50 mL autoclave at 120 o C for 4 h. The precipitate was separated by centrifugation and washed several times with deionized water. at 100 o After drying at C, the catalyst was heated at 300 o C was calcined in air for 2 h.

Embodiment 3

[0028] Embodiment 3, using chlorine ions in the electrolyte to promote the electrocatalytic oxidation of methane to generate methyl chloride, the specific steps are as follows:

[0029] The above catalysts were ultrasonically dispersed in isopropanol solution. Spray polytetrafluoroethylene emulsion, catalyst dispersion and conductive carbon black evenly on the carbon paper layer by layer, and control the catalyst loading to 1mg / cm 2 , and dry the electrode under an infrared lamp as a catalytic reaction electrode. The electrodes were then installed in the electrolytic cell, and the tests were performed at room temperature and pressure. With this electrode as the anode, the flow rate of methane gas was controlled to be 20 mL / min. Saturated NaCl was used as the electrolyte, and the flow rate of the electrolyte was controlled at 10 mL / min. With silver / silver chloride as the reference electrode, a controlled voltage of 1.8–2.5 V was applied. Methane is selectively oxidized to m...

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Abstract

The invention belongs to the technical field of methane electro-catalytic oxidation, and particularly relates to a method for promoting electro-catalytic oxidation of methane to generate chloromethane by using chloride ions. According to the preparation method, firstly, an electrocatalyst, namely cobalt-nickel composite spinel oxide nanoparticles for generating chloromethane is prepared through electrocatalytic oxidation of methane; and then the electrocatalyst is used as a catalytic reaction anode, an electrolyte containing chloride ions is adopted, and cobalt-nickel composite oxide nanoparticles electrically catalyzes methane oxidation in the presence of the chloride ions in the electrolyte, chloromethane is selectively generated, and meanwhile, side reactions such as carbon dioxide and oxygen are inhibited. According to the invention, a traditional chlorine and methane gas phase conversion method is improved, and an electrochemical in-situ active chlorine generation method is expanded into a gas-liquid phase interface reaction. The method is wide in raw material source, simple in preparation method, environmentally friendly, low in price and beneficial to application and popularization.

Description

technical field [0001] The invention belongs to the technical field of electrocatalytic oxidation of methane, and in particular relates to a method for electrocatalytically oxidizing methane to generate methyl chloride. Background technique [0002] Methane is a by-product of oil extraction and widely exists in natural gas, shale gas and combustible ice. Due to its abundance and low price, methane is becoming an important precursor of chemicals and fuels replacing coal and petroleum. Therefore, the rational utilization of methane provides conditions for the decarbonization of the current petroleum industry. Although methane is emitted to a lesser extent than carbon dioxide, it is thirty times more capable of absorbing and emitting infrared radiation than carbon dioxide. Over the last two decades, methane has contributed eighty-six times more to global warming than carbon dioxide. The tetrahedral configuration of methane shows high symmetry and low polarity. At the same t...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C25B11/091C25B3/11C25B3/27
CPCY02C20/20
Inventor 郑耿锋王启豪
Owner FUDAN UNIV