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Low-temperature jet flow plasma and monatomic catalysis coupled nitrogen fixation device and low-temperature jet flow plasma and monatomic catalysis coupled nitrogen fixation method

A jet plasma and plasma technology, which is applied to nitrogen fixation devices and fields of low temperature jet plasma coupled with single-atom catalysis, can solve the problems of poor selectivity, high comprehensive cost, low ammonia yield and the like, so as to improve the yield and reaction rate , The effect of strong adjustability and uniform energy distribution

Active Publication Date: 2020-04-10
ZHEJIANG UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0005] The purpose of the present invention is to address the deficiencies of the prior art, to propose a nitrogen fixation method coupled with low-temperature jet plasma coupling single-atom catalysis, to solve the problems of low ammonia yield, poor selectivity, and high overall cost in the existing electrocatalytic nitrogen fixation process, and to use low-temperature Jet plasma technology activates air, nitrogen and water to generate active electrolyte, and then the single-atom catalytic active electrolyte is reduced to generate synthetic ammonia. This method has the advantages of simple process, high disposal efficiency, wide application range, flexible adjustability, high product value and Good compatibility with renewable energy, etc.

Method used

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  • Low-temperature jet flow plasma and monatomic catalysis coupled nitrogen fixation device and low-temperature jet flow plasma and monatomic catalysis coupled nitrogen fixation method
  • Low-temperature jet flow plasma and monatomic catalysis coupled nitrogen fixation device and low-temperature jet flow plasma and monatomic catalysis coupled nitrogen fixation method
  • Low-temperature jet flow plasma and monatomic catalysis coupled nitrogen fixation device and low-temperature jet flow plasma and monatomic catalysis coupled nitrogen fixation method

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Experimental program
Comparison scheme
Effect test

Embodiment 1-5

[0052] A tube furnace is used to calcine the precursor of the transition metal catalyst at a high temperature, the calcination temperature range is 800 degrees, and ammonia gas is passed into the tube furnace to prepare the Co single atom catalyst. The prepared load was 0.7 mg / cm 2 The Co single-atom catalyst, 0.7 μL of DuPont D520 (5% wt) nafion solution and 1 mL of absolute ethanol were dropped on carbon paper, and dried to prepare the working electrode of H-type electrolytic cell 6;

[0053] Get 160ml of 0.1M KOH in the reaction vessel, put the reaction vessel on the magnetic stirrer, set the rotating speed to 240rpm, adjust the distance between the discharge end of the jet plasma reactor 14 and the reaction liquid level in the reaction vessel to 1, 2, 3, 4, 5cm, connect the positive electrode 12 and the negative electrode 13 of the plasma power supply 2 to the jet plasma reactor 14, feed air into the jet plasma reactor 14 and adjust the flow rate to 7L / min through the mass...

Embodiment 6-10

[0059] A tube furnace is used to calcine the precursor of the transition metal catalyst at a high temperature, the calcination temperature range is 800 degrees, and ammonia gas is passed into the tube furnace to prepare the Co single atom catalyst. The prepared load was 0.7 mg / cm 2 The Co single-atom catalyst, 0.7 μL of DuPont D520 (5% wt) nafion solution and 1 mL of absolute ethanol were dropped on carbon paper, and dried to prepare the working electrode of H-type electrolytic cell 6;

[0060] Get 160ml of 0.1M KOH into the reaction vessel, place the reaction vessel on a magnetic stirrer, set the rotating speed to 240rpm, adjust the distance between the discharge end of the jet plasma reactor 14 and the reaction liquid level in the reaction vessel to 1cm, turn the plasma power supply 2 The positive electrode 12 of the power supply and the negative electrode 13 of the power supply are connected to the jet plasma reactor 14, the air is introduced into the jet plasma reactor 14 ...

Embodiment 11-15

[0066] A tube furnace is used to calcine the precursor of the transition metal catalyst at a high temperature, the calcination temperature range is 800 degrees, and ammonia gas is passed into the tube furnace to prepare the Co single atom catalyst. The prepared load was 0.7 mg / cm 2 The Co single-atom catalyst, 0.7 μL of DuPont D520 (5% wt) nafion solution and 1 mL of absolute ethanol were dropped on carbon paper, and dried to prepare the working electrode of H-type electrolytic cell 6;

[0067] Get 160ml of 0.1M KOH into the reaction vessel, place the reaction vessel on a magnetic stirrer, set the rotating speed to 240rpm, adjust the distance between the discharge end of the jet plasma reactor 14 and the reaction liquid level in the reaction vessel to 1cm, turn the plasma power supply 2 The positive electrode 12 of the power supply and the negative electrode 13 of the power supply are connected to the jet plasma reactor 14, and pure nitrogen, air, N 2 :O 2 =9:1, N 2 :O 2 =...

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Abstract

The invention discloses a low-temperature jet flow plasma and monatomic catalysis coupled nitrogen fixation device and a low-temperature jet flow plasma and monatomic catalysis coupled nitrogen fixation method. The nitrogen fixation device comprises an electrochemical workstation, a plasma power supply, an H-type electrolytic tank and a jet flow plasma reactor. The method comprises: preparing a transition metal monatomic catalyst, and then preparing a working electrode of an H-type electrolytic tank; directly introducing air, nitrogen or mixed gas of oxygen and nitrogen into a jet flow plasmareactor, turning on a plasma power supply to realize stable discharge of jet flow plasma, and turning off the plasma power supply after the jet flow plasma reactor discharges for 10 minutes; respectively transferring the discharged reaction solutions into the H-type electrolytic tank, starting an electrochemical workstation, carrying out an electrochemical catalysis process for 30 minutes, and collecting the NH4<+>-containing solution after the reaction in the H-type electrolytic tank. According to the invention, the method and the device are high in efficiency and environmentally friendly, plasma discharge and electrochemical catalytic reaction are combined, and the monatomic catalyst is beneficial to improving the yield and the reaction rate of synthetic ammonia.

Description

technical field [0001] The invention belongs to the technical fields of low-temperature jet plasma activation catalysis and single-atom catalysts in the synthesis of ammonia and energy storage, and particularly relates to a method of using low-temperature jet plasma to activate air, nitrogen and water, and coupling single-atom electrocatalysis to realize online / offline distributed Technical methods for synthesizing ammonia, synthesizing nitric acid, nitrogen oxides and other chemicals. Background technique [0002] Nitrogen fixation refers to the conversion of abundant nitrogen molecules in the atmosphere into nitrogen-containing compounds (such as ammonia, nitrate, nitrogen dioxide, etc.), which is one of the most basic biochemical reactions in nature, maintaining the global nitrogen cycle and the needs of animals and plants for survival . The electronic structure of free nitrogen in nature is stable (N≡N, 948kJ / mol), and it is difficult to be directly used. Nitrogen can o...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C25B1/00C25B9/04C25B9/08C25B11/06C25B11/12C25B15/02C25B9/19
CPCC25B1/00C25B15/02C25B9/65C25B11/051C25B9/19C25B11/075Y02P20/52
Inventor 吴昂键李晓东严建华郑佳庚张浩
Owner ZHEJIANG UNIV
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