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Preparation of functionalized carbon material based on Schiff base-MOF and application of functionalized carbon material as electrocatalyst

A technology of -MOF and Schiff base, applied in the field of preparation of nitrogen-functionalized carbon materials, can solve the problems of ORR and OER catalytic performance degradation, high raw material prices, poor catalyst stability, etc., and achieve excellent methanol tolerance, preparation method Simple, long-lasting results

Active Publication Date: 2018-05-29
NORTHWEST NORMAL UNIVERSITY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0004] However, the above-mentioned catalysts usually use expensive raw materials, low efficiency, and even cause certain pollution to the environment.
On the other hand, the stability of many catalysts is poor, especially under acidic conditions, which may be due to the fact that under acidic conditions, some transition metals in the catalyst do not produce the expected products, but produce peroxides through electronic pathway reactions. , the strong oxidation of these generated peroxides will seriously corrode the catalyst, resulting in the reduction of catalytic sites, resulting in a decrease in the catalytic performance of ORR and OER

Method used

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  • Preparation of functionalized carbon material based on Schiff base-MOF and application of functionalized carbon material as electrocatalyst
  • Preparation of functionalized carbon material based on Schiff base-MOF and application of functionalized carbon material as electrocatalyst
  • Preparation of functionalized carbon material based on Schiff base-MOF and application of functionalized carbon material as electrocatalyst

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0041] (1) NH 2 - Preparation of MOF-Ni: Take 1.81g (0.01mol) of 2-aminoterephthalic acid and NiCl 2 ·6H 2 O 14.26g (0.06mol), added to 50ml DMF and mixed into a uniform and stable solution; then the mixed solution was placed in a hydrothermal box, and reacted hydrothermally at 200°C for 18 hours, and the obtained product was washed 6 times with DMF, centrifuged, Vacuum drying at 60°C for 12 hours to obtain the product NH 2 -MOF-Ni;

[0042] (2) Preparation of Schiff base-MOF precursor: Weigh NH 2 -MOF-Ni 0.2g and L-cysteine ​​(L-Cysteine) 1.2g, (NH 2 -MOF-Ni and L-cysteine ​​mass ratio is 1:6), respectively added to 30mlCH 2 Cl 2 in, mix and stir, stir and heat to reflux at 60°C for 6h, centrifuge, and use CH 2 Cl 2 Wash 3~5 times, dry in vacuum at 60°C for 24 hours to obtain the precursor L-cysteine-NH 2 -MOF-Ni;

[0043] (3) Preparation of nitrogen-doped functionalized carbon materials: the precursor L-cysteine-NH 2 -MOF-Ni is carbonized at a high temperature of ...

Embodiment 2

[0046] (1) NH 2 - Preparation of MOF-Ni: Take 1.81g (0.01mol) of 2-aminoterephthalic acid and FeCl 3 ·6H 2 O 16.21g (0.06mol), added to 50ml DMF and mixed into a uniform stable solution; then the mixed solution was placed in a hydrothermal box, and hydrothermally reacted at 200°C for 18 hours, and the obtained product was washed 6 times with DMF, centrifuged, Vacuum drying at 60°C for 12 hours to obtain the product NH 2 -MOF-Fe;

[0047] (2) Preparation of Schiff base-MOF precursor: Weigh NH 2 -MOF-Fe 0.2g and L-cysteine ​​(L-Cysteine) 1.2g, (NH 2 -MOF-Fe and L-cysteine ​​mass ratio is 1:6), respectively added to 30mlCH 2 Cl 2 in, mix and stir, stir and heat to reflux at 60°C for 6h, centrifuge, and use CH 2 Cl 2 Wash 3~5 times, dry in vacuum at 60°C for 24h to obtain the precursor L-cysteine-NH 2 -MOF-Fe;

[0048] (3) Preparation of nitrogen-doped functionalized carbon materials: the precursor L-cysteine-NH 2 -MOF-Fe was carbonized at 500°C for 3 hours in a nitroge...

Embodiment 3

[0051] (1) NH 2 - Preparation of MOF-Ni: Take 1.81g (0.01mol) of 2-aminoterephthalic acid and NiCl 2 ·6H 2 O 14.26g (0.06mol), added to 50ml DMF and mixed into a uniform stable solution; then the mixed solution was placed in a hydrothermal box, and hydrothermally reacted at 200°C for 18 hours, and the obtained product was washed 6 times with DMF, centrifuged, Vacuum drying at 60°C for 12 hours to obtain the product NH 2 -MOF-Ni;

[0052] (2) Preparation of Schiff base-MOF precursor: Weigh NH 2 -MOF-Ni 0.2g and L-Lysine (L-Lysine) 1.2g, (NH 2 -MOF-Ni and L-lysine mass ratio is 1:6), respectively added to 30mlCH 2 Cl 2 in, mix and stir, stir and heat to reflux at 60°C for 6h, centrifuge, and use CH 2 Cl 2 Wash 3~5 times, dry in vacuum at 60°C for 24 hours to obtain the precursor L-lysine-NH 2 -MOF-Ni;

[0053] (3) Preparation of nitrogen-doped functionalized carbon materials: the precursor L-lysine-NH 2 -MOF-Ni is carbonized at a high temperature of 500°C for 3 hours ...

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Abstract

The invention provides a preparation method of a functionalized carbon material based on Schiff base-MOF. 2-aminoterephthalic acid and transition metal salt are taken as initial materials and firstlysubjected to a hydrothermal reaction to produce a metal-organic framework compound, the metal-organic framework compound reacts with amino acid or salicylaldehyde derivatives to produce a Schiff baseprecursor, finally, high-temperature carbonization is performed, and the nitrogen-doped functionalized carbon material is obtained. The carbon material is applied to an electrocatalytic cathode ORR (oxygen reduction reaction) and a water electrolysis OER (oxygen evolution reaction), has catalytic activity equivalent to that of 20wt% of commercial Pt / C and shows excellent methanol tolerance, good conductivity and durable stability. The raw materials contain no precious metal and have low cost, the preparation method is simple and easy to control and operate, and the functionalized carbon material has good application prospects as a cathode catalyst of fuel cells.

Description

technical field [0001] The present invention relates to a nitrogen-doped functionalized carbon material, in particular to the preparation of a nitrogen-functionalized carbon material based on Schiff base-MOF, which is mainly used as an electrocatalyst for the electrocatalytic oxygen reduction reaction (ORR) in alkaline media. ) and electrolytic water oxygen evolution reaction (OER). Background technique [0002] A fuel cell is an energy conversion device that directly converts chemical energy stored in fuel and oxidant into electrical energy. Among them, the cathode oxygen reduction reaction (ORR) affects the working efficiency of the battery. It is well known that the noble metal Pt is the most commonly used class of catalysts in ORR reactions. However, the metal Pt is expensive and scarce, and it is easily poisoned by methanol in the experiment, and its chemical stability is poor. Therefore, it is necessary to develop a new catalyst to replace the noble metal Pt, so as ...

Claims

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Application Information

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IPC IPC(8): B01J27/24C25B11/06C25B1/04
CPCB01J27/24C25B1/04C25B11/04Y02E60/36
Inventor 童金辉李文艳马文梅
Owner NORTHWEST NORMAL UNIVERSITY
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