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Preparation method of amorphous C-N thin film electrocatalyst

An electrocatalyst, C-N technology, used in catalyst activation/preparation, chemical instruments and methods, physical/chemical process catalysts, etc., can solve problems such as difficulty in judging catalytic activity, complex operation process, inactivity, etc., to eliminate catalytic activity. effect, simple operation and low cost

Inactive Publication Date: 2013-11-13
JILIN UNIV
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AI Technical Summary

Problems solved by technology

The preparation methods of these nitrogen-doped carbon-based materials are mainly concentrated on high-temperature pyrolysis and chemical vapor deposition. to generate graphene and carbon nanotubes, and then dissolve and remove the metals with an acid solution
The problem with this material is that ① it is difficult to judge whether the final catalytic activity comes from the nitrogen-doped carbon-based material or the residual metal impurities; ② it is likely to protonate the active site pyridinic nitrogen into the inactive pyridinic nitrogen during the process of dissolving the metal. -hydrogen
At present, there is no report on the preparation of amorphous C-N thin film electrocatalysts by RF magnetron sputtering with substrate bias. This method is simple to operate, low in cost, and does not introduce any metal impurities during the entire preparation process. The test results show that its catalytic activity, stability and selectivity are comparable to those of Pt / C electrocatalysts

Method used

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preparation example Construction

[0028] The preparation of the C-N thin film in the present invention adopts the radio frequency magnetron sputtering deposition technology and uses polycrystalline titanium as the substrate. It is mainly divided into the following steps:

[0029] 1) The system is evacuated, and the sputtering gas and reaction gas are introduced, and wait for a period of time to make the gas mix evenly.

[0030] 2) A reasonable ratio of carbon source gas, nitrogen source gas, and sputtering gas, that is, CH 4 / N 2 / Ar=25 / 15 / 20, the unit is sccm, adjust the background pressure, set the RF power, sputtering time and substrate bias, the reaction raw materials are fully ionized, decomposed, and converted into active groups, in polycrystalline titanium The C-N film is finally deposited on the substrate.

[0031] 3) Cool down to below 100°C with protective gas.

[0032] In the present invention, a high-vacuum heat treatment furnace is used to heat-treat the film to obtain the final C-N catalyst. ...

Embodiment 1

[0043] 1) Using radio frequency magnetron sputtering equipment, deposit C-N thin films on polycrystalline titanium sheets, using high-purity carbon targets, when the background pressure reaches 1×10 -4 Pa, sequentially into CH 4 , N 2 and Ar gas, and adjust the gas flow to 25, 15, and 20 sccm respectively, and wait for a period of time to make the gas mix evenly.

[0044] 2) Adjust the reaction pressure to 0.5Pa, and after the pressure is stable, adjust the substrate bias to -150V.

[0045] 3) Turn on the RF power supply, the RF power is 150W, start sputtering, and the sputtering time is 40min.

[0046] 4) After the sputtering is over, take out the sample and wait for the next step.

[0047] 5) Put the sample into a high vacuum heat treatment furnace, when the background pressure reaches 1×10 -4 At Pa, the protective gas Ar is introduced, the heating time is 2h, the heat treatment temperature is 700°C, and the holding time is 5min.

[0048] 6) After the heat treatment, co...

Embodiment 2

[0051] Change the substrate bias value in Step 2) of Example 1 from the floating voltage to -50V, and the rest of the steps are the same as in Example 1, and the current density can reach 3.22mA cm -2 .

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Abstract

The invention relates to a preparation method of an amorphous C-N thin film electrocatalyst. The method comprises the following steps of: applying bias voltage on a substrate, depositing an amorphous C-N thin film on a titanium base, wherein the corresponding flow ratio of carbon source air, argon and nitrogen in the reaction process is 25 to 20 to15, and the unit refers to milliliter / per minute at a standard state; performing heat treatment at 700 DEG C on the deposited thin film by using a high-vacuum heat treatment furnace, thus realizing the preparation of the C-N thin film catalyst. The method is simple in preparation, has low cost and can not introduce metal impurities. For the prepared C-N catalyst, the starting potential is -0.02V, the limit current density is 5.46mA / cm<-2>, the specific current can keep 98% in a chronoamperometry test lasting for 18000 seconds, and the methanol poisoning can not be caused. The catalytic activity of the catalyst prepared by the method disclosed by the invention is comparable with that of a Pt / C catalyst, while the stability and the selectivity are better than those of the Pt / C catalyst, the catalyst is a non-noble metal catalyst with an excellent property.

Description

technical field [0001] The invention relates to a preparation method of an amorphous C-N thin film electrocatalyst material. It specifically involves the preparation of amorphous C-N thin films on titanium substrates by RF magnetron sputtering with substrate bias, and heat treatment of the films at 700°C to obtain C-N thin film electrocatalysts, which can be used to replace expensive Pt-based catalysts for Accelerates the oxygen reduction reaction at the fuel cell cathode. Background technique [0002] Energy is the foundation of economic development, without the development of the energy industry there would be no modern civilization. After several revolutionary industrial changes, people are looking for more efficient and environmentally friendly ways to use energy while developing the energy industry, so fuel cell technology has emerged. A fuel cell is a power-generating battery that converts chemical energy in fuel into electrical energy. Since the British Grove inven...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/24B01J37/34H01M4/90
CPCY02E60/50
Inventor 郑伟涛陈敬艳王欣石浩辰齐海燕
Owner JILIN UNIV
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