CN105461961B - A kind of flame retardant products and preparation method thereof - Google Patents
A kind of flame retardant products and preparation method thereof Download PDFInfo
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- CN105461961B CN105461961B CN201610005219.XA CN201610005219A CN105461961B CN 105461961 B CN105461961 B CN 105461961B CN 201610005219 A CN201610005219 A CN 201610005219A CN 105461961 B CN105461961 B CN 105461961B
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K9/00—Use of pretreated ingredients
- C08K9/02—Ingredients treated with inorganic substances
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/02—Elements
- C08K3/04—Carbon
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K5/00—Use of organic ingredients
- C08K5/16—Nitrogen-containing compounds
- C08K5/34—Heterocyclic compounds having nitrogen in the ring
- C08K5/3467—Heterocyclic compounds having nitrogen in the ring having more than two nitrogen atoms in the ring
- C08K5/3477—Six-membered rings
- C08K5/3492—Triazines
- C08K5/34922—Melamine; Derivatives thereof
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K5/00—Use of organic ingredients
- C08K5/49—Phosphorus-containing compounds
- C08K5/51—Phosphorus bound to oxygen
- C08K5/52—Phosphorus bound to oxygen only
- C08K5/521—Esters of phosphoric acids, e.g. of H3PO4
- C08K5/523—Esters of phosphoric acids, e.g. of H3PO4 with hydroxyaryl compounds
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K5/00—Use of organic ingredients
- C08K5/49—Phosphorus-containing compounds
- C08K5/5399—Phosphorus bound to nitrogen
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Abstract
The present invention relates to field of functional materials, disclose a kind of flame retardant products and preparation method thereof, the flame retardant products include the combustible material containing hydrophilic radical and the graphene oxide flame retardant coating coated in the combustible material surface, contain fire retardant and graphene oxide in the graphene oxide flame retardant coating, on the basis of the total amount of the graphene oxide flame retardant coating, the content of the fire retardant is 3 45 weight %, and the content of the graphene oxide is 55 97 weight %.Flame retardant products heat endurance provided by the invention is good, fire resistance is good, deformation is small, moreover, it is provided by the invention prepare flame retardant products method technique it is simple and cost is low, be adapted to large batch of industrialized production.
Description
Technical field
The present invention relates to field of functional materials, and in particular, to a kind of flame retardant products, a kind of preparation method of flame retardant products
And the flame retardant products being prepared by this method.
Background technology
In recent years since, the research in relation to graphene has obtained extensive concern.Graphene be one kind by carbon atom with sp2It is miscellaneous
Change the planar structure that track composition hexangle type is in honeycomb lattice, the two-dimensional material of only one carbon atom thickness.Since it has
High conductivity, high-specific surface area, high-termal conductivity and excellent mechanical performance so that graphene is widely used in super capacitor
The fields such as device, lithium ion battery, electronic component, memory device, erosion shield, absorbing material.
However, existing grapheme material is difficult the test for being resistant to fire, the anti-flammability of graphene has much room for improvement.
In existing disclosed patent application, graphene is added in the materials such as polymer generally as flame retardant to carry
Its high fire resistance.At present, fewer to research of the graphene as fire proofing in itself, Jong-Beom Baek report profit
The graphene containing phosphoric acid prepared with graphite and red phosphorus mixing and ball milling method has preferable anti-flammability.But for preparing contains phosphoric acid
Fire-retardant graphene mainly exist with powder, fire proofing or the flame retardant products that obtain morphology controllable are still relatively tired
It is difficult；Moreover, the aerial heat endurance of the material is poor, the residual quantity in 600 DEG C of air only has 30% or so.
The content of the invention
The purpose of the present invention is overcoming the aerial heat endurance of flame retardant products existing in the prior art poor, fire resistance
Difference, the defects of deformation is big, there is provided the flame retardant products that a kind of heat endurance is good, fire resistance is good, deformation is small.
In a first aspect, the present invention provides a kind of flame retardant products, which includes the combustible material containing hydrophilic radical
With the graphene oxide flame retardant coating coated in the combustible material surface, contain fire retardant in the graphene oxide flame retardant coating
And graphene oxide, on the basis of the total amount of the graphene oxide flame retardant coating, the content of the fire retardant is 3-45 weights
% is measured, the content of the graphene oxide is 55-97 weight %.
Second aspect, the present invention provide a kind of method for preparing flame retardant products, and this method includes：
(1) in the presence of solvent, graphene oxide is contacted with fire retardant, obtains solution A；
(2) solution A is coated on the surface of the combustible material containing hydrophilic radical and is dried；
Wherein, the dosage of the graphene oxide and the fire retardant to obtain after step (2) is dry fire-retardant
The content of the fire retardant in graphene oxide flame retardant coating in product is 3-45 weight %, and the content of the graphene is
55-97 weight %.
The third aspect, the present invention provide the flame retardant products being prepared by preceding method.
Flame retardant products heat endurance provided by the invention is good, fire resistance is good, deformation is small, moreover, system provided by the invention
The method technique of standby flame retardant products is simple and cost is low, is adapted to large batch of industrialized production.
Other features and advantages of the present invention will be described in detail in subsequent specific embodiment part.
Embodiment
The embodiment of the present invention is described in detail below.It is it should be appreciated that described herein specific
Embodiment is merely to illustrate and explain the present invention, and is not intended to limit the invention.
In a first aspect, the present invention provides a kind of flame retardant products, which includes the combustibles containing hydrophilic radical
Matter and the graphene oxide flame retardant coating coated in the combustible material surface, containing fire-retardant in the graphene oxide flame retardant coating
Agent and graphene oxide, on the basis of the total amount of the graphene oxide flame retardant coating, the content of the fire retardant is 3-45 weights
% is measured, the content of the graphene oxide is 55-97 weight %.
To the species of the combustible material containing hydrophilic radical, there is no particular limitation, such as can be the easy fuel woods such as paper
Material or material.
Preferably, on the basis of the total amount of the graphene oxide flame retardant coating, the content of the fire retardant is 8-35 weights
% is measured, the content of the graphene oxide is 65-92 weight %.
Preferably, load capacity of the graphene oxide flame retardant coating on the combustible material surface is 0.1-10mg/
cm2；Preferably 0.5-5mg/cm2。
Preferably, the fire retardant is selected from least one of nitrogenated flame retardant and phosphorus flame retardant；Preferably, the resistance
Fire agent and be selected from least one of hexa chloro cyclotripolyphosphazene, melamine and triphenyl phosphate；It is further preferred that the fire retardant
For hexa chloro cyclotripolyphosphazene.It was found by the inventors of the present invention that using fire retardant of the hexa chloro cyclotripolyphosphazene as the present invention and institute
State graphene oxide carry out with the use of when, the fire resistance for the flame retardant products being prepared is more preferable, and heat endurance higher.
According to a kind of preferred embodiment, in the graphene oxide flame retardant coating of flame retardant products of the present invention
In hexa chloro cyclotripolyphosphazene containing graphene oxide and as fire retardant, using the total amount of the graphene oxide flame retardant coating as
Benchmark, the content of the hexa chloro cyclotripolyphosphazene is 8-35 weight %, and the content of the graphene oxide is 65-92 weight %.
It was found by the inventors of the present invention that the fire proofing that the technical solution of this embodiment using the present invention is prepared
Fire resistance and heat endurance are optimal.
Second aspect, the present invention provides a kind of method for preparing flame retardant products, this method includes：
(1) in the presence of solvent, graphene oxide is contacted with fire retardant, obtains solution A；
(2) solution A is coated on the surface of the combustible material containing hydrophilic radical and is dried；
Wherein, the dosage of the graphene oxide and the fire retardant to obtain after step (2) is dry fire-retardant
The content of the fire retardant in graphene oxide flame retardant coating in product is 3-45 weight %, and the content of the graphene is
55-97 weight %.
It is further preferred that the dosage of the graphene oxide and the fire retardant to obtain after step (2) is dry
Flame retardant products in graphene oxide flame retardant coating in the content of the fire retardant be 8-35 weight %, the graphite oxide
The content of alkene is 65-92 weight %.
Those skilled in the art the common knowledge of aforementioned definition and this area can determine preparing according to the present invention
The dosage of graphene oxide and fire retardant in the step of method of flame retardant products (1).Under preferable case, fire-retardant production is prepared described
In the method for product, in step (1), the graphene oxide relative to every g weight, the dosage of the fire retardant is 0.05-
0.7g。
The method of flame retardant products is prepared described, the graphene oxide is usually solution form, such as can be oxygen
Graphite aqueous solution, the tetrahydrofuran solution of graphene oxide, the solution of N,N-dimethylformamide etc. of graphene oxide.
The method of flame retardant products is prepared described, in the step (1), the graphene oxide can be by commercially available
Arrive, can also be prepared using various methods well known in the art.Such as chemical oxidation graphite method can be used
(Hummers methods), the Hummers methods of modification prepare graphene oxide.Chemical oxygen is exemplarily used in the preparation example of the present invention
Graphite method prepares graphene oxide.
Preferably, in step (1), the fire retardant is selected from least one of nitrogenated flame retardant and phosphorus flame retardant；
Preferably, the fire retardant is selected from least one of hexa chloro cyclotripolyphosphazene, melamine and triphenyl phosphate；More preferably
Ground, the fire retardant are hexa chloro cyclotripolyphosphazene.
Preferably, in step (1), the solvent in n,N-Dimethylformamide, water and tetrahydrofuran at least
It is a kind of.The water is preferably distilled water or deionized water.
In the case of more preferably, the method for flame retardant products is prepared described, in the step (1), the graphene oxide
The graphene oxide solution being prepared for preceding method using the present invention, and the fire retardant with the graphene oxide
Before contact, it is first dissolved in solvent (such as in n,N-Dimethylformamide).That is, the present invention is preferably described " in solvent
In the presence of, graphene oxide is contacted with fire retardant " the step of be：By graphene oxide solution with containing the molten of fire retardant
Liquid is contacted.Concentration of the invention to the graphene oxide solution, and do not have to the concentration of the solution containing fire retardant
There are special limitation, the flame retardant products that those skilled in the art can obtain according to ordinary skill in the art means and needs
Adjust the concentration of the graphene oxide solution and the concentration of the solution containing fire retardant.For example, the graphene oxide solution
In the concentration of graphene oxide can be 0.1-8mg/mL, the concentration of the fire retardant in the solution containing fire retardant can be with
For 0.1-30mg/mL.
Preferably, in step (2), the coated weight of the solution A is the graphite oxide in obtained flame retardant products
Load capacity of the alkene flame retardant coating on the combustible material surface is 0.1-10mg/cm2。
It is further preferred that in step (2), the coated weight of the solution A is the oxidation in obtained flame retardant products
Load capacity of the graphene flame retardant coating on the combustible material surface is 0.5-5mg/cm2。
Preferably, in step (2), the condition of the drying includes：Temperature is 30-60 DEG C, time 24-72h.
The third aspect, the present invention provides the flame retardant products being prepared by preceding method.
The present invention will be described in detail by way of examples below.
In case of no particular description, a variety of materials used below is all from commercially available.
Preparation example 1 is used to prepare graphene oxide water solution.
Embodiment 1-9 is used to prepare flame retardant products of the present invention.
Preparation example 1
The reaction bulb of 250mL is assembled in ice-water bath, adds the 80mL concentrated sulfuric acids, stirs lower addition 3g graphite powders and 1.5g
The solid mixture of sodium nitrate, then 9g potassium permanganate is added portionwise, controlling reaction temperature is no more than 10 DEG C, stirs 30min, then
35 DEG C or so are warming up to, continues to stir 30min, is slow added into the deionized water of 150mL, is continued after stirring 20min, is added suitable
Measure hydrogen peroxide and reduce remaining oxidant, solution is changed into glassy yellow.Filter while hot, and with the HCl solution of 5 weight % and go from
Sub- water washing loads bag filter dialysis untill sulfate radical-free is detected into filtrate, obtains the oxidation that concentration is 10.5mg/mL
Graphene solution.Prepared graphene oxide solution is diluted, obtain concentration be respectively 1mg/mL, 2mg/mL and
The graphene oxide solution of 3.5mg/mL, it is spare.
Embodiment 1
The hexa chloro cyclotripolyphosphazene of 2.2mg is dissolved in the n,N-Dimethylformamide of 0.5mL, is then with 20mL concentration
The graphene oxide solution of 1mg/mL is uniformly mixed, dry at 30 DEG C by uniformly mixed solution drop coating to the surface of filter paper
60h, it is 1.0mg/cm to obtain load capacity2Flame retardant filter paper Z1, wherein, the content of the graphene oxide in coating is 90.1 weights
% is measured, surplus is fire retardant.
By blank filter paper, load capacity 1.0mg/cm2The filter paper of graphite oxide ene coatings and obtained flame retardant filter paper
Z1 burns on alcolhol burner flame, as a result：Blank filter paper does not just remain after the 5s that burns；Load 1.0mg/cm2Aoxidize stone
The filter paper of black ene coatings does not just remain after 15s；Flame retardant filter paper Z1 can also keep the overwhelming majority after the 120s that burns, and only be
Some curlings of edge.
Embodiment 2
The hexa chloro cyclotripolyphosphazene of 10mg is dissolved in the n,N-Dimethylformamide of 1mL, is then with 20mL concentration
The graphene oxide solution of 2mg/mL is uniformly mixed, dry at 40 DEG C by uniformly mixed solution drop coating to the surface of filter paper
50h, it is 1.5mg/cm to obtain load capacity2Flame retardant filter paper Z2, wherein, the content of the graphene oxide in coating is 80.0 weights
% is measured, surplus is fire retardant.
It is 1.5mg/cm by load capacity2The filter paper of graphite oxide ene coatings and obtained flame retardant filter paper Z2 are in alcolhol burner
Burn on flame, as a result：Load 1.5mg/cm2The filter paper of graphite oxide ene coatings does not just remain after 18s；Flame retardant filter paper
Z2 can also keep the overwhelming majority after the 130s that burns, and only be some curlings of edge.
Embodiment 3
The hexa chloro cyclotripolyphosphazene of 30mg is dissolved in the n,N-Dimethylformamide of 3mL, is then with 20mL concentration
The graphene oxide solution of 3.5mg/mL is uniformly mixed, and uniformly mixed solution drop coating to the surface of filter paper is done at 60 DEG C
Dry 24h, it is 2.0mg/cm to obtain load capacity2Flame retardant filter paper Z3, wherein, the content of the graphene oxide in coating is 70.0 weights
% is measured, surplus is fire retardant.
It is 2.0mg/cm by load capacity2The filter paper of graphite oxide ene coatings and obtained flame retardant filter paper Z3 are in alcolhol burner
Burn on flame, as a result：Load 2.0mg/cm2The filter paper of graphite oxide ene coatings does not just remain after 23s；Flame retardant filter paper
Z3 can also keep the overwhelming majority after the 140s that burns, and only be some curlings of edge.
Embodiment 4
The present embodiment is carried out using method similar to Example 1, except that：
The fire retardant used in the present embodiment is melamine.
Remaining is in the same manner as in Example 1, obtains flame retardant filter paper Z4.
It is 1.0mg/cm by load capacity2The filter paper of graphite oxide ene coatings and obtained flame retardant filter paper Z4 are in alcolhol burner
Burn on flame, as a result：Load 1.0mg/cm2The filter paper of graphite oxide ene coatings does not just remain after 15s；Flame retardant filter paper
Z4 can also keep the overwhelming majority after the 90s that burns, and only be some curlings of edge.
Embodiment 5
The present embodiment is carried out using method similar to Example 2, except that：
The fire retardant used in the present embodiment is triphenyl phosphate.
Remaining is in the same manner as in Example 2, obtains flame retardant filter paper Z5.
It is 1.5mg/cm by load capacity2The filter paper of graphite oxide ene coatings and obtained flame retardant filter paper Z5 are in alcolhol burner
Burn on flame, as a result：Load 1.5mg/cm2The filter paper of graphite oxide ene coatings does not just remain after 18s；Flame retardant filter paper
Z5 can also keep the overwhelming majority after the 100s that burns, and only be some curlings of edge.
Embodiment 6
The present embodiment is carried out using method similar to Example 3, except that：
The fire retardant used in the present embodiment is that (and both weight ratios are 1 for melamine and triphenyl phosphate：1).
Remaining is in the same manner as in Example 3, obtains flame retardant filter paper Z6.
It is 2.0mg/cm by load capacity2The filter paper of graphite oxide ene coatings and obtained flame retardant filter paper Z6 are in alcolhol burner
Burn on flame, as a result：Load 2.0mg/cm2The filter paper of graphite oxide ene coatings does not just remain after 23s；Flame retardant filter paper
Z6 can also keep the overwhelming majority after the 110s that burns, and only be some curlings of edge.
Embodiment 7
The present embodiment is carried out using method similar to Example 1, except that：
The chlordene ring trimerization that the fire retardant used in the present embodiment is the 13.3mg for the N,N-dimethylformamide for being dissolved in 1mL
Phosphonitrile.
Remaining is in the same manner as in Example 1, obtains flame retardant filter paper Z7, wherein, the content of graphene oxide is in coating
60.1 weight %, surplus are fire retardant.
It is 1.0mg/cm by load capacity2The filter paper of graphite oxide ene coatings and obtained flame retardant filter paper Z7 are in alcolhol burner
Burn on flame, as a result：Load 1.0mg/cm2The filter paper of graphite oxide ene coatings does not just remain after 15s；Flame retardant filter paper
Z7 can also keep the overwhelming majority after the 90s that burns, and only be some curlings of edge.
Embodiment 8
The present embodiment is carried out using method similar to Example 2, except that：
The chlordene ring three that the fire retardant used in the present embodiment is the 2.5mg for the N,N-dimethylformamide for being dissolved in 0.5mL
Polyphosphazene.
Remaining is in the same manner as in Example 2, obtains flame retardant filter paper Z8, wherein, the content of graphene oxide is in coating
94.2 weight %, surplus are fire retardant.
It is 1.5mg/cm by load capacity2The filter paper of graphite oxide ene coatings and obtained flame retardant filter paper Z8 are in alcolhol burner
Burn on flame, as a result：Load 1.5mg/cm2The filter paper of graphite oxide ene coatings does not just remain after 18s；Flame retardant filter paper
Z8 can also keep the overwhelming majority after the 100s that burns, and only be some curlings of edge.
Embodiment 9
The present embodiment is carried out using method similar to Example 7, except that：
The fire retardant used in the present embodiment is the melamine of the 13.3mg for the N,N-dimethylformamide for being dissolved in 1mL.
Remaining is in the same manner as in Example 7, obtains flame retardant filter paper Z9.
It is 1.0mg/cm by load capacity2The filter paper of graphite oxide ene coatings and obtained flame retardant filter paper Z9 are in alcolhol burner
Burn on flame, as a result：Load 1.0mg/cm2The filter paper of graphite oxide ene coatings does not just remain after 15s；Flame retardant filter paper
Z9 can also keep the overwhelming majority after the 80s that burns, and only be some curlings of edge.
From the result of above-described embodiment can be seen that flame retardant products provided by the invention heat endurance is good, fire resistance
It is good, deformation is small, moreover, it is provided by the invention prepare flame retardant products method technique it is simple and cost is low, be adapted to large batch of work
Industry metaplasia is produced.
The preferred embodiment of the present invention described in detail above, still, during present invention is not limited to the embodiments described above
Detail, in the range of the technology design of the present invention, a variety of simple variants can be carried out to technical scheme, this
A little simple variants belong to protection scope of the present invention.
It is further to note that each particular technique feature described in above-mentioned embodiment, in not lance
In the case of shield, can be combined by any suitable means, in order to avoid unnecessary repetition, the present invention to it is various can
The combination of energy no longer separately illustrates.
In addition, various embodiments of the present invention can be combined randomly, as long as it is without prejudice to originally
The thought of invention, it should equally be considered as content disclosed in this invention.
Claims (11)
1. a kind of flame retardant products, which includes the combustible material containing hydrophilic radical and coated in the combustible material table
The graphene oxide flame retardant coating in face, it is characterised in that contain fire retardant and graphite oxide in the graphene oxide flame retardant coating
Alkene, on the basis of the total amount of the graphene oxide flame retardant coating, the content of the fire retardant is 3-45 weight %, the oxidation
The content of graphene is 55-97 weight %, and the fire retardant is hexa chloro cyclotripolyphosphazene.
2. flame retardant products according to claim 1, wherein, on the basis of the total amount of the graphene oxide flame retardant coating,
The content of the fire retardant is 8-35 weight %, and the content of the graphene oxide is 65-92 weight %.
3. flame retardant products according to claim 2, wherein, the graphene oxide flame retardant coating is in the combustible material table
The load capacity in face is 0.1-10mg/cm2。
4. flame retardant products according to claim 2, wherein, the graphene oxide flame retardant coating is in the combustible material table
The load capacity in face is 0.5-5mg/cm2。
5. a kind of method for preparing flame retardant products, this method include：
(1) in the presence of solvent, graphene oxide is contacted with fire retardant, obtains solution A；
(2) solution A is coated on the surface of the combustible material containing hydrophilic radical and is dried；
Wherein, the dosage of the graphene oxide and the fire retardant causes the flame retardant products obtained after step (2) is dry
In graphene oxide flame retardant coating in the content of the fire retardant be 3-45 weight %, the content of the graphene is 55-
97 weight %, the fire retardant are hexa chloro cyclotripolyphosphazene.
6. according to the method described in claim 5, wherein, in step (1), the solvent be selected from n,N-Dimethylformamide,
At least one of water and tetrahydrofuran.
7. according to the method described in claim 5, wherein, in step (2), the coated weight of the solution A obtains
Load capacity of the graphene oxide flame retardant coating on the combustible material surface in flame retardant products is 0.1-10mg/cm2。
8. according to the method described in claim 7, wherein, in step (2), the coated weight of the solution A obtains
Load capacity of the graphene oxide flame retardant coating on the combustible material surface in flame retardant products is 0.5-5mg/cm2。
9. according to the method described in claim 5, wherein, in step (2), the condition of the drying includes：Temperature is 30-60
DEG C, time 24-72h.
10. according to the method described in claim 5, wherein, the dosage of the graphene oxide and the fire retardant to pass through
The content of the fire retardant in graphene oxide flame retardant coating in the flame retardant products obtained after step (2) is dry is 8-35 weights
% is measured, the content of the graphene is 65-92 weight %.
11. the flame retardant products being prepared as the method described in any one in claim 5-10.
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| CN201510835710.0A CN105273237A (en) | 2015-11-25 | 2015-11-25 | Anti-flaming product and preparation method thereof |
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| CN201610005219.XA CN105461961B (en) | 2015-11-25 | 2016-01-06 | A kind of flame retardant products and preparation method thereof |
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| CN103241735A (en) * | 2013-05-17 | 2013-08-14 | 南京理工大学 | Hybrid nanomaterial of melamine chemically-modified graphene oxide and preparation method of hybrid nanomaterial |
| CN105037801A (en) * | 2015-08-03 | 2015-11-11 | 苏州大学 | Phosphorus-containing hybridization graphene oxide and preparation method thereof |
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| ITMI20131391A1 (en) * | 2013-08-14 | 2015-02-15 | Directa Plus Spa | DELAYING COMPOSITION OF GRAFENE INCLUDING FLAME |
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Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103241735A (en) * | 2013-05-17 | 2013-08-14 | 南京理工大学 | Hybrid nanomaterial of melamine chemically-modified graphene oxide and preparation method of hybrid nanomaterial |
| CN105037801A (en) * | 2015-08-03 | 2015-11-11 | 苏州大学 | Phosphorus-containing hybridization graphene oxide and preparation method thereof |
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