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Ni-N-C catalyst for electroreduction reaction of carbon dioxide and preparation and application thereof

A carbon dioxide and catalyst technology, applied in electrodes, electrolytic processes, electrolytic components, etc., can solve the problems of insufficient carbon dioxide electroreduction activity and increased current density of CO, and achieve excellent carbon dioxide electroreduction activity and high current density.

Active Publication Date: 2019-04-19
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0006] The technical problem of the present invention is to overcome the insufficient carbon dioxide electroreduction activity of the existing Ni-N-C catalytic material, and provide a preparation method of Ni-N-C catalytic material with high carbon dioxide electroreduction reaction activity. The CO Faraday efficiency of the catalyst can be in a very wide potential range 92%, and the CO partial current density increases with the increase of the overpotential, up to 71.5mA cm -2

Method used

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  • Ni-N-C catalyst for electroreduction reaction of carbon dioxide and preparation and application thereof
  • Ni-N-C catalyst for electroreduction reaction of carbon dioxide and preparation and application thereof
  • Ni-N-C catalyst for electroreduction reaction of carbon dioxide and preparation and application thereof

Examples

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Effect test

Embodiment 1

[0046] Weigh 2.45g Zn(NO 3 ) 2 ·6H 2 O and 2.39g Ni(NO 3 ) 2 ·6H 2 O was dissolved in 300mL of methanol, and 300mL of methanol solution containing 10.82g of 2-dimethylimidazole was added under stirring, and the stirring was continued at room temperature for 12 hours; centrifuged and washed with methanol for 3 times, and dried in vacuum to obtain a solid powder; take 0.2g of the solid powder Placed in a quartz boat, placed in a tube furnace, 50mLmin -1 Under argon protection, 5°C min -1 Heating to 900°C and maintaining it for 4 hours, cooling to room temperature to obtain a Ni-N-C catalyst. like figure 1 As shown, the Ni-N-C catalyst was in the form of a porous carbon layer, and no metal particles were observed.

[0047] Weigh 4.4 mg of Ni-N-C catalyst, add appropriate amount of deionized water and ethanol, mix ultrasonically for 10 minutes, add 9.8 mg of 5% Nafion solution, and mix ultrasonically for 20 minutes to obtain catalyst slurry. The catalyst slurry was brushe...

Embodiment 2

[0051] Weigh 2.94g Zn(NO 3 ) 2 ·6H 2 O and 11.47g Ni(NO 3 ) 2 ·6H 2 O was dissolved in 300mL of methanol, and 300mL of methanol solution containing 32.45g of 2-dimethylimidazole was added under stirring, and the stirring was continued at room temperature for 24 hours; centrifuged and washed 3 times with methanol, and dried in vacuo to obtain a solid powder; 0.4g of the solid powder was obtained Placed in a quartz boat, placed in a tube furnace, 100mLmin -1 Under nitrogen protection, 10°C min -1 Heating to 600°C and maintaining it for 12 hours, cooling to room temperature to obtain a Ni-N-C catalyst. like image 3 As shown, the near-edge absorption peak profile of Ni-N-C is between that of simple nickel and nickel phthalocyanine, which proves that the valence state of Ni is between +2 and 0. like Figure 4 As shown, the Ni-N-C catalyst obtained by this method can also electroreduce carbon dioxide to carbon monoxide, but the highest CO Faradaic efficiency is only 65%, a...

Embodiment 3

[0053] Weigh 2.94g Zn(NO 3 ) 2 ·6H 2 O and 1.43g Ni(NO 3 ) 2 ·6H 2 O was dissolved in 300mL of methanol, and 300mL of methanol solution containing 4.86g of 2-dimethylimidazole was added under stirring, and the stirring was continued at room temperature for 24 hours; centrifuged and washed 3 times with methanol, and dried in vacuo to obtain a solid powder; 0.6g of the solid powder was obtained Placed in a quartz boat, placed in a tube furnace, 80mL min -1 Under nitrogen protection, 1°C min -1 Heating to 1000°C and maintaining it for 4 hours, cooling to room temperature to obtain Ni-N-C catalyst.

[0054] The working electrode preparation process and test conditions are the same as in Example 1. like Figure 5 As shown, the Ni-N-C catalyst is in the potential range of -1.2V to -1.6V vs.Ag / AgCl, the CO faradaic efficiency is maintained above 91%, and the highest can reach 95.6%, and the CO sub-current density is -1.7V vs.Ag / AgCl up to 45.6mA cm -2 .

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Abstract

The invention discloses a preparation method of a Ni-N-C catalyst for a carbon dioxide electroreduction reaction. The method comprises the following steps: dissolving zinc nitrate and nickel nitrate in methanol according to a certain ratio, adding a certain amount of 2-methylimidazole methanol solution while stirring, and stirring the mixture at room temperature for 12-36 hours; centrifuging and washing with methanol for 3 times, drying under vacuum to obtain a solid powder; taking a certain amount (0.1-0.8g) of the solid powder in a tube furnace, heating to 600-1000 DEG C at a certain flow velocity and under the protection of inert gas, maintaining for 1 to 12 hours, and cooling to room temperature to obtain the Ni-N-C catalyst. The catalyst body is amorphous carbon with N and Ni uniformly doped in a carbon skeleton, is applied to carbon dioxide electroreduction, and has high CO Faraday efficiency and current density.

Description

technical field [0001] The invention relates to a carbon dioxide electroreduction reaction, in particular to a Ni-N-C catalyst which can be used in the carbon dioxide electroreduction reaction and a preparation method thereof. Background technique [0002] According to the "World Energy Outlook 2016" report released by the US Energy Information Administration, fossil energy will still occupy a dominant position in the energy structure in the next ten years. The extensive exploitation and use of fossil energy is accompanied by a large amount of carbon dioxide emissions. The concentration of carbon dioxide in the atmosphere has reached 400ppm. Excessively high carbon dioxide concentration will bring about a series of environmental problems such as global warming and ocean acidification. Therefore, technologies for capturing, storing, converting, and utilizing carbon dioxide have received extensive attention. Carbon dioxide electroreduction technology can use the electric ener...

Claims

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Application Information

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IPC IPC(8): C25B11/06C25B3/04C25B1/00C22C1/05C22C1/10C25B3/25
CPCC22C1/058C25B1/00C25B11/04C25B3/25
Inventor 汪国雄阎程程叶益凡包信和
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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