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Preparation of manganese phthalocyanine modified oxhorn-shaped carbon-based catalyst and CO2 electric reduction method

A carbon-based catalyst, manganese phthalocyanine technology, applied in chemical instruments and methods, physical/chemical process catalysts, organic compound/hydride/coordination complex catalysts, etc., can solve the problem of low Faradaic efficiency and complex and diverse coordination structures , low metal loading rate, etc., to achieve high specific surface area, promote efficient reduction reaction, and promote the effect of conversion reaction

Active Publication Date: 2020-09-29
ZHEJIANG UNIV
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Problems solved by technology

However, transition metal single atoms also have problems such as low metal loading rate and complex and diverse coordination structures (for example: metal-carbon, metal-nitrogen), which lead to CO 2 Reduced Faraday is less efficient

Method used

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  • Preparation of manganese phthalocyanine modified oxhorn-shaped carbon-based catalyst and CO2 electric reduction method

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Effect test

Embodiment 1

[0034] Take 23.3g of ammonium bromide and 1g of melamine, add 30mL of deionized water, ultrasonicate for 1h, stir for 24h, and then dry in a vacuum oven at 100°C for 8h to obtain a mixture. Take this mixture and place it in a crucible, put the crucible into a muffle furnace at room temperature, control the heating rate to 1.8°C / min, raise the temperature to 500°C, and then calcine at a constant temperature for 2 hours to obtain carbon nitride. Then put the carbon nitride into the tube furnace and feed nitrogen gas, control the heating rate of the tube furnace to 5°C / min, heat it to 600°C and then pyrolyze it at a constant temperature for 2 hours, and centrifuge the pyrolysis product three times with deionized water, Then place it in a vacuum oven at 60°C and dry to obtain a horn-shaped carbon-based catalyst. Take 0.6g of horn-like carbon-based catalyst, disperse it in 200mL of N-N-dimethylformamide solution, after ultrasonic treatment for 30min, add 50mg of manganese phthalocy...

Embodiment 2

[0038] Take 23.3g of ammonium bromide and 1g of melamine, add 30mL of deionized water, ultrasonicate for 1h, stir for 24h, and then dry in a vacuum oven at 100°C for 8h to obtain a mixture. Take this mixture and place it in a crucible, put the crucible into a muffle furnace at room temperature, control the heating rate to 1.8°C / min, raise the temperature to 500°C, and then calcine at a constant temperature for 2 hours to obtain carbon nitride. Then put the carbon nitride into the tube furnace and feed nitrogen, control the heating rate of the tube furnace to 5°C / min, heat to 700°C and then pyrolyze at a constant temperature for 2 hours, and centrifuge the pyrolysis product three times with deionized water, Then place it in a vacuum oven at 60°C and dry to obtain a horn-shaped carbon-based catalyst. Take 0.6g of horn-like carbon-based catalyst, disperse it in 200mL of N-N-dimethylformamide solution, after ultrasonic treatment for 30min, add 60mg of manganese phthalocyanine mole...

Embodiment 3

[0042] Take 23.3g of ammonium bromide and 1g of melamine, add 30mL of deionized water, ultrasonicate for 1h, stir for 24h, and then dry in a vacuum oven at 100°C for 8h to obtain a mixture. Take this mixture and place it in a crucible, put the crucible into a muffle furnace at room temperature, control the heating rate to 1.8°C / min, raise the temperature to 500°C, and then calcine at a constant temperature for 2 hours to obtain carbon nitride. Then put the carbon nitride into the tube furnace and feed nitrogen gas, control the heating rate of the tube furnace to 5°C / min, heat to 800°C and then pyrolyze at a constant temperature for 2 hours, and centrifuge the pyrolysis product three times with deionized water, Then place it in a vacuum oven at 60°C and dry to obtain a horn-shaped carbon-based catalyst. Take 0.6g of horn-shaped carbon-based catalyst, disperse it in 200mL of N-N-dimethylformamide solution, after ultrasonic treatment for 30min, add 70mg of manganese phthalocyanin...

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Abstract

The invention relates to the technical field of building materials, and aims to provide a preparation method of a manganese phthalocyanine modified oxhorn-shaped carbon-based catalyst. The preparationmethod comprises the following steps: calcining a mixture of ammonium bromide and melamine to obtain carbon nitride, and pyrolyzing in a nitrogen atmosphere; and cleaning and drying the product to obtain the oxhorn-shaped carbon-based catalyst; dispersing the manganese phthalocyanine modified oxhorn-shaped carbon-based catalyst into an N-N-dimethylformamide solution, performing ultrasonic treatment, adding manganese phthalocyanine molecules, performing ultrasonic treatment, stirring, cleaning and drying to obtain the manganese phthalocyanine modified oxhorn-shaped carbon-based catalyst. The product provided by the invention has rich porous structure, high specific surface area, high content of pyridine nitrogen and pyrrole nitrogen active sites and good conductivity, and is an efficient cathode catalyst. The carbon-based catalyst with the horn-shaped structure has a tip effect to enrich charges under the action of an electric field, so that the efficient reduction reaction of CO2 is promoted. Manganese single atoms in phthalocyanine manganese molecules are used as active sites, so that the reaction energy barrier of reducing CO2 into an intermediate product COOH * is reduced, theconversion reaction of CO2 into a CO gas product is promoted, and the Faraday efficiency is high.

Description

technical field [0001] The present invention is about the greenhouse gas CO 2 conversion and utilization technology, especially the preparation of manganese phthalocyanine-modified horn-like carbon-based catalysts and the electroreduction of CO 2 method. Background technique [0002] Using wind power and photovoltaic energy storage to reduce and convert coal-fired flue gas CO 2 The production of renewable fuels is of great significance for energy saving, environmental protection and new energy development. Due to CO 2 Molecular chemical properties are stable, CO 2 The reduction process is accompanied by hydrogen evolution reaction, so it is difficult to catalytically reduce CO with high efficiency and high selectivity 2 . In order to solve these technical bottlenecks, it is urgent to develop efficient electrocatalysts to convert CO 2 Revert to renewable fuels. In recent years, researchers have improved the electrochemical reduction of CO 2 A lot of effort has been p...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/22B01J35/02C25B1/00C25B11/06B01J35/00
CPCB01J31/183C25B1/00B01J2531/72B01J2531/025B01J2231/62B01J35/33B01J35/00B01J35/30
Inventor 程军岑可法周俊虎刘建忠杨卫娟王智化张彦威周志军何勇
Owner ZHEJIANG UNIV
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