CN104649254A - Method for rapidly preparing nitrogen-doped graphene by utilizing microwave-assisted solid phase method - Google Patents
Method for rapidly preparing nitrogen-doped graphene by utilizing microwave-assisted solid phase method Download PDFInfo
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- CN104649254A CN104649254A CN201410755442.7A CN201410755442A CN104649254A CN 104649254 A CN104649254 A CN 104649254A CN 201410755442 A CN201410755442 A CN 201410755442A CN 104649254 A CN104649254 A CN 104649254A
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Abstract
The invention relates to the technical field of inorganic chemistry application, and particularly relates to a method for rapidly preparing nitrogen-doped graphene by utilizing ethylene diamine as a nitrogen source through a microwave-assisted solid phase method. The method comprises the following steps: 1. preparing graphite oxide through low-temperature, medium-temperature and high-temperature stages; 2. preparing nitrogen-doped graphene: firstly preparing functional graphene, and then performing reflux reaction and microwave heating to complete the preparation of the nitrogen-doped graphene. The graphite oxide is functionalized by adopting ethylene diamine, and the nitrogen doping of graphene can be successfully realized by performing microwave treatment to ethylene diamine-functionalized graphene. Compared with the traditional nitrogen doping method, the method avoids the use of the high-corrosive and high-toxicity ammonia gas, and shows the environment-friendly characteristic. In addition, the method also has the characteristics of high efficiency, high doping quantity and the like.
Description
Technical field
The present invention relates to inorganic chemistry applied technical field, be specifically related to a kind of quadrol that utilizes and rapidly and efficiently prepare the method for nitrogen-doped graphene as the solid phase microwave-assisted of nitrogenous source.
Background technology
Prepare nitrogen-doped graphene mainly through directly synthesis and two approach such as aftertreatment.Direct synthesis refers to that passing into nitrogenous source when chemical vapour deposition synthesizing graphite alkene makes nitrogen-atoms enter its lattice in the process situ doping of graphene growth; Aftertreatment is then at high temperature utilize to process Graphene containing nitrogen molecule, makes nitrogen atom doping enter into the lattice of Graphene.At present, investigator has realized utilizing graphite oxide to prepare Graphene on a large scale for raw material, and therefore the approach of aftertreatment nitrating has more the potentiality of practical application.In order to realize, to the efficient N doping of Graphene, there is the NH of higher level of reactivity
3often be selected as nitrogenous source.But ammonia is poisonous and have strong corrodibility, very high requirement is proposed to equipment. and be unfavorable for realizing large-scale preparation.
Summary of the invention
The present invention is intended to propose a kind of quadrol that utilizes and rapidly and efficiently prepares the method for nitrogen-doped graphene as the solid phase microwave-assisted of nitrogenous source.
Technical program of the present invention lies in:
Microwave solid source prepares a method for nitrogen-doped graphene fast, adopts following steps:
Step 1: the preparation of graphite oxide:
(1) the low-temp reaction stage: add the 130mL vitriol oil and 5g crystalline flake graphite in the beaker of 1000mL, and under condition of ice bath mechanical stirring 2h; In above-mentioned system, slowly add 15g potassium permanganate, and continue under maintaining condition of ice bath to stir 2h, this one-phase is the low-temp reaction stage;
(2) warm step of reaction in: remove ice bath, continues to stir lh under 35 DEG C of water-baths;
(3) the pyroreaction stage: drip 230mL deionized water in beaker, and be warming up to 980 DEG C of continuation reaction 30min;
(4) pyroreaction adds 400mL deionized water after terminating wherein, and centrifuge washing obtains graphite oxide dispersion to neutrality;
Step 2: the preparation of nitrogen-doped graphene:
(1) graphite oxide dispersion of above-mentioned preparation is diluted to 1 mgmL
-1concentration, measure this dispersion liquid of 120mL and be added to 250mL single port flask back flow reaction 6 h at 95 DEG C with 1.5mL quadrol;
(2) solid phase FGS(functionalization graphene is obtained by lyophilize after having reacted);
(3) obtained FGS is placed in microwave oven. obtain nitrogen-doped graphene after full power microwave treatment l min under an ar atmosphere.
Technique effect of the present invention is:
The present invention adopts quadrol to carry out functionalization to graphite oxide, and successfully realizes the N doping to Graphene by the process of solid phase microwave treatment quadrol functionalization graphene.Relative to traditional N doping method, this method avoid and use highly corrosive and highly toxic ammonia, show eco-friendly feature.In addition, this method also feature such as combining efficient and highly doped amount.
Embodiment
Microwave solid source prepares a method for nitrogen-doped graphene fast, adopts following steps:
Step 1: the preparation of graphite oxide:
(1) the low-temp reaction stage: add the 130mL vitriol oil and 5g crystalline flake graphite in the beaker of 1000mL, and under condition of ice bath mechanical stirring 2h; In above-mentioned system, slowly add 15g potassium permanganate, and continue under maintaining condition of ice bath to stir 2h, this one-phase is the low-temp reaction stage;
(2) warm step of reaction in: remove ice bath, continues to stir lh under 35 DEG C of water-baths;
(3) the pyroreaction stage: drip 230mL deionized water in beaker, and be warming up to 980 DEG C of continuation reaction 30min;
(4) pyroreaction adds 400mL deionized water after terminating wherein, and centrifuge washing obtains graphite oxide dispersion to neutrality;
Step 2: the preparation of nitrogen-doped graphene:
(1) graphite oxide dispersion of above-mentioned preparation is diluted to 1 mgmL
-1concentration, measure this dispersion liquid of 120mL and be added to 250mL single port flask back flow reaction 6 h at 95 DEG C with 1.5mL quadrol;
(2) solid phase FGS(functionalization graphene is obtained by lyophilize after having reacted);
(3) obtained FGS is placed in microwave oven. obtain nitrogen-doped graphene after full power microwave treatment l min under an ar atmosphere.
Claims (1)
1. microwave solid source prepares a method for nitrogen-doped graphene fast, it is characterized in that: adopt following steps:
Step 1: the preparation of graphite oxide:
(1) the low-temp reaction stage: add the 130mL vitriol oil and 5g crystalline flake graphite in the beaker of 1000mL, and under condition of ice bath mechanical stirring 2h; In above-mentioned system, slowly add 15g potassium permanganate, and continue under maintaining condition of ice bath to stir 2h, this one-phase is the low-temp reaction stage;
(2) warm step of reaction in: remove ice bath, continues to stir lh under 35 DEG C of water-baths;
(3) the pyroreaction stage: drip 230mL deionized water in beaker, and be warming up to 980 DEG C of continuation reaction 30min;
(4) pyroreaction adds 400mL deionized water after terminating wherein, and centrifuge washing obtains graphite oxide dispersion to neutrality;
Step 2: the preparation of nitrogen-doped graphene:
(1) graphite oxide dispersion of above-mentioned preparation is diluted to 1 mgmL
-1concentration, measure this dispersion liquid of 120mL and be added to 250mL single port flask back flow reaction 6 h at 95 DEG C with 1.5mL quadrol;
(2) solid phase FGS(functionalization graphene is obtained by lyophilize after having reacted);
(3) obtained FGS is placed in microwave oven. obtain nitrogen-doped graphene after full power microwave treatment l min under an ar atmosphere.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201410755442.7A CN104649254A (en) | 2014-12-11 | 2014-12-11 | Method for rapidly preparing nitrogen-doped graphene by utilizing microwave-assisted solid phase method |
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| Application Number | Priority Date | Filing Date | Title |
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| CN201410755442.7A CN104649254A (en) | 2014-12-11 | 2014-12-11 | Method for rapidly preparing nitrogen-doped graphene by utilizing microwave-assisted solid phase method |
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| CN104649254A true CN104649254A (en) | 2015-05-27 |
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| CN201410755442.7A Pending CN104649254A (en) | 2014-12-11 | 2014-12-11 | Method for rapidly preparing nitrogen-doped graphene by utilizing microwave-assisted solid phase method |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105271203A (en) * | 2015-11-18 | 2016-01-27 | 深圳大学 | Porous co-doped graphene and preparation method thereof |
| CN105293484A (en) * | 2015-12-10 | 2016-02-03 | 太原理工大学 | Preparation method of nitrogen-doped graphene and nitrogen-doped graphene loaded nanocrystalline catalyst |
| CN111099578A (en) * | 2018-10-27 | 2020-05-05 | 中国石油化工股份有限公司 | Nitrogen-doped three-dimensional graphene material |
-
2014
- 2014-12-11 CN CN201410755442.7A patent/CN104649254A/en active Pending
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105271203A (en) * | 2015-11-18 | 2016-01-27 | 深圳大学 | Porous co-doped graphene and preparation method thereof |
| CN105293484A (en) * | 2015-12-10 | 2016-02-03 | 太原理工大学 | Preparation method of nitrogen-doped graphene and nitrogen-doped graphene loaded nanocrystalline catalyst |
| CN111099578A (en) * | 2018-10-27 | 2020-05-05 | 中国石油化工股份有限公司 | Nitrogen-doped three-dimensional graphene material |
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Application publication date: 20150527 |