CN107673344A - The preparation method of three-dimensional graphene oxide - Google Patents

Abstract

The preparation method of the three-dimensional graphene oxide of the present invention is related to field of graphene, and in particular to the preparation method of three-dimensional graphene oxide, comprises the following steps：The measured 25mL concentrated sulfuric acids are poured into 100mL conical flask, are heated to 90 DEG C, 5g potassium peroxydisulfates and 5g phosphorus pentoxides is then added, is stirred continuously, until mixture is completely dissolved；The mixture of gained is cooled to 80 DEG C, 6g natural graphite powders is then added, foam occurs, foam gradually disappears in 30min；By mixture under 80 DEG C of water-baths agitating and heating 4.5h, mixture is then cooled to room temperature, and with 1L deionized water rinsings, the product of gained is stood overnight at room temperature；Products therefrom is filtered, and is washed with deionized, until the solution that last time filters gained is neutrality, it is then that the solid on miillpore filter is drying for one day at normal temperatures；Present invention process flow is simple, easy to operate, reaction safety, ensures product quality, substantially reduces production cost, improve production efficiency.

Description

The preparation method of three-dimensional graphene oxide

Technical field

The present invention relates to field of graphene, and in particular to the preparation method of three-dimensional graphene oxide.

Background technology

Graphene unique structure and excellent electronics, electrochemistry, optics, calorifics and mechanical performance, make it have wide Application prospect.But the graphene of structural integrity, reactivity is weak, and aggregation is easily produced between graphene film and piece, made Its dissolubility reduces, and this has had a strong impact on the further research and application of graphene.And three-dimensional grapheme corresponding thereto is gathered around Have unique three-dimensional network-like structure, excellent electric property and mechanical performance, allow three-dimensional grapheme in many fields all With very big application potential.

The content of the invention

Present invention aims at providing, a kind of technological process is simple, easy to operate, reaction safety, ensures product quality, greatly It is big to reduce production cost, improve the preparation method of the three-dimensional graphene oxide of production efficiency.

The preparation method of the three-dimensional graphene oxide of the present invention, comprises the following steps：

（1）The measured 25mL concentrated sulfuric acids are poured into 100mL conical flask, are heated to 90 DEG C, then add 5g over cures Sour potassium and 5g phosphorus pentoxides, are stirred continuously, until mixture is completely dissolved；

（2）The mixture of gained is cooled to 80 DEG C, 6g natural graphite powders is then added, foam occurs, foam in 30min by Fade；

（3）By mixture under 80 DEG C of water-baths agitating and heating 4.5h, mixture is then cooled to room temperature, and with 1L deionized waters Rinse, the product of gained is stood overnight at room temperature；

（4）Products therefrom is filtered, and is washed with deionized, until the solution that last time filters gained is neutrality, then will Solid on miillpore filter is drying for one day at normal temperatures；

（5）In the three-necked flask that above-mentioned product is put to people 500mL, the 230mL concentrated sulfuric acids and 30g permanganic acid are then slowly added into Potassium, it, which is asked, is continuously agitated, and keeping temperature is not higher than 10 degree, until being completely dissolved；

（6）Mixture is reacted 2h under 35 degree of water-bath, then add people 460mL deionized water, control inside three-necked flask The temperature of solution is less than 50 DEG C, and with being continuously added for dampening, the activity of reactant constantly reduces, until the deionization being eventually adding Water no longer causes obvious temperature change；

（7）Solution in three-necked flask is moved into 2L beaker, adds 1.4L deionized water, stirring reaction 2h, knot 25mL 30% hydrogen peroxide is added dropwise in Shu Houxiang mixtures, now, mixture solution will be changed into bright khaki, by it Stand a night；

（8）Supernatant is removed, is rinsed with substantial amounts of 5% hydrochloric acid solution, substantial amounts of deionized water rinsing is then used again, up to gained Solution for neutrality, finally by the mixture solution centrifuge of gained, obtain the graphite oxide of high concentration；

（9）Graphite oxide is diluted with water, after sonicated, obtains homogeneous scattered yellowish-brown graphite oxide solution；

（10）Resorcinol, formaldehyde, natrium carbonicum calcinatum are taken, it is 1 to make the mol ratio of resorcinol and formaldehyde：2；

（11）0.025g natrium carbonicum calcinatums are dissolved in standby in 40g water；

（12）Graphene oxide, formaldehyde and Carbon Dioxide sodium solution are weighed, is put into ultrasonic more than 0.5h in ultrasonic instrument；

（13）Three-necked flask is put up on thermostat water bath, 150mL hexamethylenes is measured, 5mL sorbester p17s, is put into three mouthfuls put up In flask, stirring is opened, and is warming up to 60 degree, water-bath mouth is sealed with preservative film, prevents water loss；

（14）Mixture after ultrasound is added in the three-necked flask for having been preheated with 60 degree, be kept stirring for, after reacting 2h, taken The resorcinol of precalculated amount, 3mL solution is configured to, is added to three-necked flask, continue to stir, reaction is taken out two days later；

（15）Liquid is stood, after it has been settled, filtered, ethanol wash and constant pressure and dry, obtains three-dimensional grapheme.

Present invention process flow is simple, easy to operate, reaction safety, ensures product quality, substantially reduces production cost, carry High efficiency.

Embodiment

The preparation method of the three-dimensional graphene oxide of the present invention, comprises the following steps：

（1）The measured 25mL concentrated sulfuric acids are poured into 100mL conical flask, are heated to 90 DEG C, then add 5g over cures Sour potassium and 5g phosphorus pentoxides, are stirred continuously, until mixture is completely dissolved；

（2）The mixture of gained is cooled to 80 DEG C, 6g natural graphite powders is then added, foam occurs, foam in 30min by Fade；

（3）By mixture under 80 DEG C of water-baths agitating and heating 4.5h, mixture is then cooled to room temperature, and with 1L deionized waters Rinse, the product of gained is stood overnight at room temperature；

（4）Products therefrom is filtered, and is washed with deionized, until the solution that last time filters gained is neutrality, then will Solid on miillpore filter is drying for one day at normal temperatures；

（5）In the three-necked flask that above-mentioned product is put to people 500mL, the 230mL concentrated sulfuric acids and 30g permanganic acid are then slowly added into Potassium, it, which is asked, is continuously agitated, and keeping temperature is not higher than 10 degree, until being completely dissolved；

（6）Mixture is reacted 2h under 35 degree of water-bath, then add people 460mL deionized water, control inside three-necked flask The temperature of solution is less than 50 DEG C, and with being continuously added for dampening, the activity of reactant constantly reduces, until the deionization being eventually adding Water no longer causes obvious temperature change；

（7）Solution in three-necked flask is moved into 2L beaker, adds 1.4L deionized water, stirring reaction 2h, knot 25mL 30% hydrogen peroxide is added dropwise in Shu Houxiang mixtures, now, mixture solution will be changed into bright khaki, by it Stand a night；

（8）Supernatant is removed, is rinsed with substantial amounts of 5% hydrochloric acid solution, substantial amounts of deionized water rinsing is then used again, up to gained Solution for neutrality, finally by the mixture solution centrifuge of gained, obtain the graphite oxide of high concentration；

（9）Graphite oxide is diluted with water, after sonicated, obtains homogeneous scattered yellowish-brown graphite oxide solution；

（10）Resorcinol, formaldehyde, natrium carbonicum calcinatum are taken, it is 1 to make the mol ratio of resorcinol and formaldehyde：2；

（11）0.025g natrium carbonicum calcinatums are dissolved in standby in 40g water；

（12）Graphene oxide, formaldehyde and Carbon Dioxide sodium solution are weighed, is put into ultrasonic more than 0.5h in ultrasonic instrument；

（13）Three-necked flask is put up on thermostat water bath, 150mL hexamethylenes is measured, 5mL sorbester p17s, is put into three mouthfuls put up In flask, stirring is opened, and is warming up to 60 degree, water-bath mouth is sealed with preservative film, prevents water loss；

（14）Mixture after ultrasound is added in the three-necked flask for having been preheated with 60 degree, be kept stirring for, after reacting 2h, taken The resorcinol of precalculated amount, 3mL solution is configured to, is added to three-necked flask, continue to stir, reaction is taken out two days later；

（15）Liquid is stood, after it has been settled, filtered, ethanol wash and constant pressure and dry, obtains three-dimensional grapheme.

Present invention process flow is simple, easy to operate, reaction safety, ensures product quality, substantially reduces production cost, carry High efficiency.

Claims (1)

1. a kind of preparation method of three-dimensional graphene oxide, it is characterised in that comprise the following steps：

（1）The measured 25mL concentrated sulfuric acids are poured into 100mL conical flask, are heated to 90 DEG C, then add 5g over cures Sour potassium and 5g phosphorus pentoxides, are stirred continuously, until mixture is completely dissolved；

（2）The mixture of gained is cooled to 80 DEG C, 6g natural graphite powders is then added, foam occurs, foam in 30min by Fade；

（3）By mixture under 80 DEG C of water-baths agitating and heating 4.5h, mixture is then cooled to room temperature, and with 1L deionized waters Rinse, the product of gained is stood overnight at room temperature；

（4）Products therefrom is filtered, and is washed with deionized, until the solution that last time filters gained is neutrality, then will Solid on miillpore filter is drying for one day at normal temperatures；

（5）In the three-necked flask that above-mentioned product is put to people 500mL, the 230mL concentrated sulfuric acids and 30g permanganic acid are then slowly added into Potassium, it, which is asked, is continuously agitated, and keeping temperature is not higher than 10 degree, until being completely dissolved；

（6）Mixture is reacted 2h under 35 degree of water-bath, then add people 460mL deionized water, control inside three-necked flask The temperature of solution is less than 50 DEG C, and with being continuously added for dampening, the activity of reactant constantly reduces, until the deionization being eventually adding Water no longer causes temperature change；

（7）Solution in three-necked flask is moved into 2L beaker, adds 1.4L deionized water, stirring reaction 2h, knot 25mL 30% hydrogen peroxide is added dropwise in Shu Houxiang mixtures, now, mixture solution will be changed into bright khaki, by it Stand a night；

（8）Supernatant is removed, is rinsed with substantial amounts of 5% hydrochloric acid solution, substantial amounts of deionized water rinsing is then used again, up to gained Solution for neutrality, finally by the mixture solution centrifuge of gained, obtain the graphite oxide of high concentration；

（9）Graphite oxide is diluted with water, after sonicated, obtains homogeneous scattered yellowish-brown graphite oxide solution；

（10）Resorcinol, formaldehyde, natrium carbonicum calcinatum are taken, it is 1 to make the mol ratio of resorcinol and formaldehyde：2；

（11）0.025g natrium carbonicum calcinatums are dissolved in standby in 40g water；

（12）Graphene oxide, formaldehyde and Carbon Dioxide sodium solution are weighed, is put into ultrasonic more than 0.5h in ultrasonic instrument；

（13）Three-necked flask is put up on thermostat water bath, 150mL hexamethylenes is measured, 5mL sorbester p17s, is put into three mouthfuls put up In flask, stirring is opened, and is warming up to 60 degree, water-bath mouth is sealed with preservative film, prevents water loss；

（14）Mixture after ultrasound is added in the three-necked flask for having been preheated with 60 degree, be kept stirring for, after reacting 2h, taken The resorcinol of precalculated amount, 3mL solution is configured to, is added to three-necked flask, continue to stir, reaction is taken out two days later；

（15）Liquid is stood, after it has been settled, filtered, ethanol wash and constant pressure and dry, obtains three-dimensional grapheme.