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Pyridine nitrogen enriched carbon nanotube catalyst as well as preparation method and application thereof

A carbon nanotube and pyridine nitrogen technology, applied in the field of electrocatalysis, can solve the problems of application limitation, low percentage of pyridine nitrogen, etc., and achieve the effects of good stability, high current density and good application prospect.

Active Publication Date: 2019-03-22
TECHNICAL INST OF PHYSICS & CHEMISTRY - CHINESE ACAD OF SCI +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0004] Many previous reports have shown that pyridinic nitrogen is the main active site of metal radical nitrogen-doped carbon materials, but the percentage of pyridinic nitrogen in nitrogen-doped carbon tubes currently available is relatively low, which limits its application.

Method used

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  • Pyridine nitrogen enriched carbon nanotube catalyst as well as preparation method and application thereof
  • Pyridine nitrogen enriched carbon nanotube catalyst as well as preparation method and application thereof
  • Pyridine nitrogen enriched carbon nanotube catalyst as well as preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0041] The preparation method of pyridine nitrogen-enriched carbon nanotube catalyst comprises the following steps:

[0042] 600 mg of 1-10 phenanthroline and 200 mg of multi-walled carbon nanotubes were dispersed in a mixed solution of 25 ml of ethanol and 25 ml of deionized water, stirred at room temperature for 12 hours, then evaporated to dryness at 105 °C, and ground in an agate mortar Then, the electrocatalyst precursor was obtained; the electrocatalyst precursor was taken and placed in a porcelain boat, heat-treated in a tube furnace, heated from room temperature to 700°C at 5°C / min, held for 3 hours, and then cooled at 3.3°C / min At room temperature, the heat treatment atmosphere is an ammonia gas atmosphere to obtain the pyridine nitrogen-enriched carbon nanotube catalyst.

[0043] The X-ray diffraction curve of the catalyst prepared in this example is as follows figure 1 As can be seen from the figure, the catalyst prepared in this example has three typical crystal p...

Embodiment 2

[0054] Example 1 was repeated, except that the heat treatment temperature was changed from 700 °C to 500 °C, and the morphology of the obtained electrocatalyst was similar to that of the electrocatalyst obtained in Example 1, but the total nitrogen content was reduced to 2.0%, and the percentage of pyridine nitrogen was 58.7 %.

[0055] The catalyst prepared in this example was prepared in 0.5M NaHCO saturated with carbon dioxide 3 The Faradaic efficiency-voltage diagram of carbon monoxide obtained by electrolysis in aqueous solution is as follows Image 6 The resulting electrocatalyst product selectivity is shown to be similar to the electrocatalyst obtained in Example 1.

[0056] The catalyst prepared in this example was prepared in 0.5M NaHCO saturated with carbon dioxide 3 The carbon monoxide current density-voltage diagram obtained by electrolysis in aqueous solution is as follows Figure 7 shown. The maximum current density of carbon monoxide is 13 mA / cm 2 .

Embodiment 3

[0058] Example 1 was repeated, except that the heat treatment temperature was changed from 700 °C to 300 °C, and the morphology of the obtained electrocatalyst was similar to that of the electrocatalyst obtained in Example 1, but the total nitrogen content was reduced to 1.0%, and the percentage of pyridine nitrogen was 79.6%.

[0059] The catalyst prepared in this example was prepared in 0.5M NaHCO saturated with carbon dioxide 3 Carbon monoxide Faradaic efficiency-voltage obtained by electrolysis in aqueous solution as Image 6 shown. The product selectivity of the obtained electrocatalyst is not much different from that of the electrocatalyst obtained in Example 1.

[0060] The catalyst prepared in this example was prepared in 0.5M NaHCO saturated with carbon dioxide 3 The carbon monoxide current density-voltage diagram obtained by electrolysis in aqueous solution is as follows Figure 7 shown. The maximum current density of carbon monoxide is 8 mA / cm 2 .

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Abstract

The invention discloses a pyridine nitrogen enriched carbon nanotube catalyst which is prepared from carbon nanotube and nitrogen atoms doped in the carbon nanotube, wherein the doping amount of the nitrogen atoms is 1-2.5wt%, the nitrogen atoms contain pyridine nitrogen, and the pyridine nitrogen accounts for 55-80wt% of the total amount of the nitrogen atoms. The catalyst is high in pyridine nitrogen content; when the catalyst is used for performing electrocatalytic reduction on carbon dioxide to obtain carbon monoxide, the product selectivity of the carbon monoxide is high, the current density is large; and the catalyst is relatively high in stability. The invention also discloses a preparation method and application of the catalyst.

Description

technical field [0001] The present invention relates to the technical field of electrocatalysis. More specifically, it relates to a pyridine nitrogen-enriched carbon nanotube catalyst and its preparation method and application. Background technique [0002] Carbon dioxide is one of the main gases causing the greenhouse effect, and its massive emission has gradually intensified the greenhouse effect, which has brought about a series of problems such as sea level rise and land desertification. At the same time, carbon dioxide is an abundant carbon source. If it can be converted into carbon-containing compounds to obtain fuels and chemicals, it will alleviate the two important problems of energy and environment at the same time. Therefore, the conversion of carbon dioxide is very meaningful. [0003] Noble metal-based electrocatalysts such as gold and silver can electrocatalytically reduce carbon dioxide with high selectivity and high stability at low overpotentials. However...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/24C25B1/00C25B11/06
CPCC25B1/00C25B11/04B01J27/24B01J35/33
Inventor 马晨康鹏
Owner TECHNICAL INST OF PHYSICS & CHEMISTRY - CHINESE ACAD OF SCI
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