Simple and convenient method for preparing three-dimensional nitrogen-doped graphene

A nitrogen-doped graphene, three-dimensional technology, used in chemical instruments and methods, hybrid/electric double-layer capacitor manufacturing, electrodes, etc.

Active Publication Date: 2017-04-26
SHANDONG UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

There are also reports on the preparation of oxygen reduction catalysts by pyrolysis of melamine resin (Li M, Xue J. J PhysChem C (American Journal of Physical Chemistry), 2014, 118: 2507), but there is no PBI or ABPBI preparation of nitrogen-doped three-dimensional graphene catalysts. to report

Method used

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  • Simple and convenient method for preparing three-dimensional nitrogen-doped graphene

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0017] [Example 1] Preparation of ABPBI (method 1, solid-phase method): Take an appropriate amount of 3,4-diaminobenzoic acid (DABA) in a mortar, grind it thoroughly and transfer it to a three-necked flask with electric stirring and inert gas protection Inside, blow nitrogen for 15 minutes to exhaust the air in the flask. N 2 Under protection, under stirring, the oil bath was heated to 225°C and kept for 3h. Take it out after cooling, grind finely, N 2 Under protection, heat in an electric furnace, then raise the temperature to 270-275°C and keep for 3h. After cooling to room temperature, the product was taken out and finely ground to obtain ABPBI, and the molecular weight of ABPBI was measured with an Ubbelohde viscometer.

Embodiment 2

[0018] [Example 2] Preparation of ABPBI (method 2, liquid phase method): polyphosphoric acid (PPA) (50 g) was added into a three-necked flask, and stirred at 160° C. for 1 h under nitrogen protection to remove water and air. 3,4-diaminobenzoic acid (6 g, 39.5 mmol) was added and the temperature was raised to 190 °C, controlled by N 2Flow rate, to prevent DABA from being oxidized, continue to stir for 3h, add about 5g P in batches during the reaction 2 o 5 To absorb the water formed during the reaction. With the increase of reaction time, the polymerization system gradually became viscous. The reaction mixture was slowly transferred to deionized water, spinning to form a fibrous black solid, which was taken out and dried, crushed, and washed to remove polyphosphoric acid and unreacted raw materials in the reaction mixture. Get ABPBI products. The molecular weight of ABPBI was determined with an Ubbelohde viscometer.

Embodiment 3

[0019] [embodiment 3] SiO with particle diameter 30nm 2 Three-dimensional porous nitrogen-doped graphene was prepared by pyrolyzing the template agent mixed with ABPBI. With ABPBI and SiO 2 The template mass ratio is 1:1 as an example: In a 250mL beaker, add 1g of ABPBI (viscosity average molecular weight 20,000 to 30,000) and 20mL of DMAc, heat and stir to dissolve, and slowly add 1g of SiO while stirring 2 Nanoparticles with a particle size of 30nm make it uniformly dispersed. The obtained viscous liquid is heated and concentrated to nearly dryness under stirring, and dried in a vacuum oven at 100°C. The solid is ground in a mortar, transferred to a porcelain boat, and kept in a high-temperature electric furnace at 900°C under the protection of argon. Pyrolyze for 2-3 hours, wait for the furnace temperature to drop to room temperature, take it out, and grind it finely to obtain a black powdery solid, transfer it to a 250mL Erlenmeyer flask, add 70mL of hydrofluoric acid, h...

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Abstract

The invention discloses a simple and convenient method for preparing three-dimensional nitrogen-doped graphene through a poly(2,5-benzimidazole) (ABPBI) solution under the effect of a template agent, namely nano SiO2. An ABPBI macromolecular chain is composed of aromatic rigid benzimidazole, molecules contain imidazole rings and amino end groups which are rich in nitrogen element, and after pyrolysis is conducted under argon shield, a nitrogen-doped graphene structure can be easily formed. The specific preparation process for the three-dimensional nitrogen-doped graphene comprises the steps that the ABPBI solution is uniformly blended with the nano SiO2 of a certain particle diameter according to a certain proportion; drying by distillation and porphyrization are conducted under stirring; and high-temperature pyrolysis and template removing are conducted under argon shield. According to requirements, the ABPBI viscosity-average molar mass is 10 thousand-30 thousand, the particle diameter of the SiO2 is 5-50 nm; the mass ratio of ABPBI to the SiO2 is 3:1-1:3; the pyrolysis temperature is 600-1200 DEG C; the pyrolysis time is 2-3 h; and hydrofluoric acid washing is conducted for three times, and deionized water washing is conducted for three times. The prepared three-dimensional nitrogen-doped graphene is used for oxygen reduction catalysts, oxygen evolution catalysts, and electrochemistry energy storage and conversion parts including fuel cells, metal-air cells, super capacitors and the like.

Description

technical field [0001] It belongs to the field of nanomaterial preparation and is used in redox reaction catalysts in chemical production, fuel cells in the field of clean energy, metal-air battery cathode catalysts, electrolytic water catalysts, lithium-ion battery materials, supercapacitor electrode materials and electrochemical sensors. Background technique [0002] Graphene is a kind of nanomaterial with a regular hexagonal extended two-dimensional grid structure composed of carbon atoms. Due to its excellent performance and multiple potential applications, its development, research and application have attracted people's attention, and it has become a widely used material in today's society. A research hotspot of concern (Kim K S, et al. Nature (Nature), 2009, 457: 706). However, in the macroscopic world, two-dimensional graphene is very easy to overlap each other layer by layer to form a graphite structure, thus losing its excellent performance. Therefore, how to prev...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/02C25B11/06C25B1/04H01G11/44H01G11/86H01M4/88H01M4/96
CPCB01J31/0244B01J2231/60B01J2231/70C25B1/04C25B11/095H01G11/44H01G11/86H01M4/88H01M4/96Y02E60/13Y02E60/36Y02E60/50
Inventor 李忠芳王素文张廷尉岳攀峰
Owner SHANDONG UNIV OF TECH
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