CN111994903A - Synthetic method of 3-aminopropyltriethoxysilane modified graphene oxide - Google Patents
Synthetic method of 3-aminopropyltriethoxysilane modified graphene oxide Download PDFInfo
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Abstract
The invention discloses a synthesis method of 3-aminopropyl triethoxysilane modified graphene oxide. Adding graphene oxide into tetrahydrofuran, wherein the dosage ratio of the graphene oxide to the tetrahydrofuran is 20-100 mg: 35.6-222.5 g, ultrasonically dispersing for 1-2 hours at the temperature of 20-35 ℃, and then adding 3-aminopropyltriethoxysilane, wherein the dosage ratio of the graphene oxide, the tetrahydrofuran and the 3-aminopropyltriethoxysilane is 20-100 mg: 35.6 g-222.5 g: 3.76*10‑3mg～2.82*10‑2And mg, stirring and reacting for 6-8 h at the temperature of 60-70 ℃, centrifuging, washing and drying to obtain black powder 3-aminopropyltriethoxysilane modified graphene oxide.
Description
Technical Field
The invention belongs to the field of organic synthesis, and particularly relates to a synthesis method of 3-aminopropyl triethoxysilane modified graphene oxide.
Background
Graphene oxide is an important graphene derivative, and has unique application in the field of composite materials. A large number of oxygen-containing groups such as hydroxyl, carboxyl, epoxy and the like exist on the surface of the graphene oxide, functionalized modification can be carried out on the surface of the graphene oxide through a covalent or non-covalent method to obtain functionalized graphene oxide, and the functionalized modified graphene oxide can form acting force with high polymers such as rubber, polyvinyl alcohol, chitosan and the like, is used for modifying the characteristics of high polymer materials, can also act with nano metal oxides, and is used for solar cells.
3-aminopropyltriethoxysilane is an important siloxane compound, and intramolecular alkoxy groups can react with functional groups on the surface of graphene oxide to form the 3-aminopropyltriethoxysilane-modified graphene oxide compound. At present, a method for mainly preparing 3-aminopropyltriethoxysilane modified graphene oxide is reported in the chemical schools of higher schools, 2013, 31(10), by using marfan and Zhoujun: 1982-1986 preparation of dispersible graphene A article discloses a method for modifying graphene oxide by 3-aminopropyltriethoxysilane, which comprises the steps of dispersing graphene oxide in an ethanol-water mixed solvent, adding 3-Aminopropyltriethoxysilane (APTES), and stirring for 24 hours at room temperature. However, after the 3-aminopropyltriethoxysilane modified graphene oxide prepared by the method is reduced and dried by hydrazine hydrate, the obtained corresponding modified graphene cannot be dispersed in an organic solvent (such as DMF, ethanol, acetone and the like) by ultrasonic, the dried aggregate has high hardness, is difficult to grind and is not beneficial to subsequent use, and electron microscope images of the graphene oxide and the reduced graphene are not given by the method.
Disclosure of Invention
The invention overcomes the defects or shortcomings of the prior art, and provides a synthesis method of 3-aminopropyltriethoxysilane modified graphene oxide, wherein THF is used for replacing toluene, the reaction temperature is reduced, and the reaction time is shortened, and after the 3-aminopropyltriethoxysilane modified graphene oxide prepared by the synthesis method is reduced by hydrazine hydrate and dried, the 3-aminopropyltriethoxysilane modified graphene oxide can be stably dispersed in organic solvents such as N, N-Dimethylformamide (DMF), dimethyl sulfoxide (DMSO), ethanol, THF and the like by ultrasonic treatment for 0.5-2 h.
In order to realize the technical task, the invention adopts the following technical scheme to realize:
a synthetic method of 3-aminopropyl triethoxysilane modified graphene oxide takes graphene oxide as a raw material, and comprises the following steps:
step 1, mixing graphene oxide and tetrahydrofuran according to a mass ratio of 20-100 mg: 35.6g to 222.5 g;
and 2, ultrasonically dispersing the mixture obtained in the step 1 at the temperature of 20-35 ℃ for 1-2 h, and then adding 3-aminopropyltriethoxysilane, wherein the mass ratio of graphene oxide to tetrahydrofuran is 20-100 mg: 35.6 g-222.5 g: 3.76*10-3mg～2.82*10-2mg；
And 3, stirring the mixed reactant obtained in the step 2 at the temperature of 60-70 ℃ for 6-8 hours, centrifuging, washing and drying to obtain powdery 3-aminopropyltriethoxysilane modified graphene oxide.
Compared with the prior art, the invention has the following beneficial technical effects:
compared with the prior art, THF is used for replacing toluene in the method, the reaction temperature is reduced, the reaction time is shortened, and the prepared 3-aminopropyltriethoxysilane modified graphene oxide can be stably dispersed in organic solvents such as N, N-Dimethylformamide (DMF), dimethyl sulfoxide (DMSO), ethanol, Tetrahydrofuran (THF) and the like by ultrasonic treatment for 0.5-2 h after reduction and drying by hydrazine hydrate.
Drawings
FIG. 1 is an infrared image of 3-aminopropyltriethoxysilane-modified graphene oxide prepared in example 1 of the present invention.
FIG. 2 is an XPS diagram of 3-aminopropyltriethoxysilane-modified graphene oxide prepared in example 1 of the present invention.
FIG. 3 is an SEM image of 3-aminopropyltriethoxysilane-modified graphene oxide prepared in example 1 of the present invention.
Fig. 4 is a raman diagram of 3-aminopropyltriethoxysilane-modified graphene oxide prepared in example 1 of the present invention.
Fig. 5 is a dispersion diagram of 3-aminopropyltriethoxysilane-modified graphene oxide prepared in example 1 of the present invention and 3-aminopropyltriethoxysilane-modified graphene prepared in the background art after being respectively reduced, dispersed in DMSO, and precipitated for 24 hours.
FIG. 6 is an SEM image of reduced 3-aminopropyltriethoxysilane-modified graphene of example 1.
The technical contents of the present invention will be described in further detail below with reference to the accompanying drawings and embodiments.
Detailed Description
The overall thought of the invention is as follows: by controlling reaction conditions, firstly dispersing graphene oxide in an organic solvent, then adding 3-aminopropyltriethoxysilane, reacting the 3-aminopropyltriethoxysilane with hydroxyl on the graphene oxide, removing ethoxy groups to generate corresponding ether, and finally preparing the 3-aminopropyltriethoxysilane modified graphene oxide.
It should be noted that the graphene oxide used in the synthesis process of the present invention is purchased from the dealers beijing carbofuran technologies ltd, and the other reagents are commercially available analytical purifiers.
The present invention will be described in further detail with reference to specific examples, but the scope of the present invention is not limited thereto.
Example 1
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 20mg of graphene oxide into 35.6g of tetrahydrofuran, ultrasonically dispersing for 1.5h at 25 ℃, and then adding 3.76 to 10-3And (3) mg of 3-aminopropyltriethoxysilane, reacting for 8.0h at 70 ℃, centrifuging, washing and drying to obtain black powder, namely 30mg of 3-aminopropyltriethoxysilane modified graphene oxide.
And (3) structural identification:
1. infrared analysis
1740cm in graphite oxide can be seen in the infrared spectrum of the target compound 3-aminopropyltriethoxysilane modified graphene oxide-1The absorption peak of carbonyl stretching vibration at the position has been shifted to 1636cm-11248cm in the corresponding graphite oxide-1The characteristic absorption peak of epoxy group becomes very weak and even disappears, which shows that part of amino groups in 3-aminopropyl triethoxysilane and epoxy groups in graphite oxide have addition reaction. The modified graphite oxide is 1040cm-1The absorption peak of stretching vibration of Si-O-Si bond is formed by hydrolytic condensation of partial alkoxy in 3-aminopropyl triethoxy silane. The surface of the graphene oxide is modified by 3-aminopropyltriethoxysilane. FIG. 1 is an infrared image of 3-mercaptopropyltriethoxysilane-modified graphene oxide prepared in example 1.
X-ray photoelectron spectroscopy (XPS) analysis
The XPS spectrum shows that the graphene oxide only contains two characteristic peaks of C1s and O1s, namely 289eV and 535 eV. Comparing the graphene oxide with the characterization results of 3-aminopropyltriethoxysilane-modified graphene oxide, the 3-aminopropyltriethoxysilane-modified graphene oxide is found to have new N1s and Si2p spectral peaks at 402eV and 102eV in addition to the C1s and O1s characteristic peaks. The results demonstrate that 3-aminopropyltriethoxysilane was successfully grafted in the graphene oxide structure. FIG. 2 is an XPS plot of 3-aminopropyltriethoxysilane-modified graphene oxide prepared in example 1.
3. Scanning Electron Microscope (SEM) analysis
Analysis of electron microscope results show that the flaky structure of the 3-aminopropyltriethoxysilane-modified graphene oxide obviously exists, and large-scale agglomeration does not occur. And after functionalization, folds on the 3-aminopropyltriethoxysilane-modified graphene oxide sheet layer are obviously increased. FIG. 3 is an SEM image of 3-aminopropyltriethoxysilane modified graphene oxide prepared in example 1.
4. Raman analysis
The Raman spectrum of NH-Si-FGO showed that the D peak and the G peak appeared at 1355cm-1 and 1599cm-1, respectively. The intensity ratio of the D band to the G band of the Raman spectrum also represents the sp3/sp2 carbon atom ratio. Wherein, the ID/IG of NH-Si-FGO is 1.119, and is higher than the ID/IG of GO is 1.027. This is due to the increase in sp3 heterocyclic carbon atoms after GO is functionalized. Fig. 4 is a raman diagram of 3-aminopropyltriethoxysilane-modified graphene oxide prepared in example 1.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain 15mg of 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. Fig. 5 shows the dispersion of 3-aminopropyltriethoxysilane modified graphene prepared by the applied method and the background art method, respectively, after 24h of precipitation in DMSO (wherein the left side is the method of the present application and the right side is the method of makinsonite and the periwinian). As can be seen from the SEM image of the 3-aminopropyltriethoxysilane modified graphene, the reduced graphene does not have an agglomeration phenomenon. FIG. 6 is an SEM image of reduced 3-aminopropyltriethoxysilane-modified graphene of example 1.
Example 2
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 40mg of graphene oxide into 100g of tetrahydrofuran, performing ultrasonic dispersion at 25 ℃ for 1h, and then adding 9 x 10-3And (3) mg of 3-aminopropyltriethoxysilane, reacting for 7.0h at 60 ℃, centrifuging, washing and drying to obtain black powder of 58mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image results of the 3-aminopropyltriethoxysilane-modified graphene of this example, it was also found that the reduced graphene did not exhibit the agglomeration phenomenon.
Example 3
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 60mg of graphene oxide into 140g of tetrahydrofuran, performing ultrasonic dispersion at 30 ℃ for 2 hours, and then adding 1.00 x 10-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 7 hours at 65 ℃, centrifuging, washing and drying to obtain black powder, namely 85mg of 3-aminopropyltriethoxysilane modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image results of the 3-aminopropyltriethoxysilane-modified graphene of this example, it is also seen that no agglomeration phenomenon occurs in the reduced graphene.
Example 4
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 80mg of graphene oxide into 190g of tetrahydrofuran, and carrying out ultrasonic separation at the temperature of 35 DEG CDispersing for 1.0h, and adding 1.63 x 10-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 7.5h at 68 ℃, centrifuging, washing and drying to obtain black powder of 114mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image results of the 3-aminopropyltriethoxysilane-modified graphene of this example, it is also seen that the reduced graphene does not undergo agglomeration.
Example 5
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 100mg of graphene oxide into 222.5g of tetrahydrofuran, ultrasonically dispersing for 1.0h at 30 ℃, and then adding 2.82 x 10-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 7.0h at 69 ℃, centrifuging, washing and drying to obtain 149mg of black powder 3-aminopropyltriethoxysilane modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image results of the 3-aminopropyltriethoxysilane-modified graphene of this example, it is also seen that the reduced graphene does not undergo agglomeration.
Example 6
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 90mg of graphene oxide into 200g of tetrahydrofuran, ultrasonically dispersing for 1.2h at 32 ℃, and then adding 2.69 x 10-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 7.5h at 67 ℃, centrifuging, washing and drying to obtain black powder, namely 130mg of 3-aminopropyltriethoxysilane modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 6
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 85mg of graphene oxide into 184g of tetrahydrofuran, ultrasonically dispersing for 1.6h at 33 ℃, and then adding 2.47 x 10-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 7.2h at 68 ℃, centrifuging, washing and drying to obtain black powder of 124mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 7
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 95mg of graphene oxide into 217g of tetrahydrofuran, performing ultrasonic dispersion at 22 ℃ for 1.4h, and then adding 2.64 x 10-2And (3) reacting the 3-aminopropyltriethoxysilane for 7.3h at 66 ℃, centrifuging, washing and drying to obtain black powder, namely 140mg of the 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. As can be seen from the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, the reduced graphene does not undergo agglomeration.
Example 8
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
80mg of graphene oxide was added to 174.9g of tetrahydrofuran and sonicated at 21 deg.CDisperse for 1.3h, then add 2.01 x 10-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 6.4h at 64 ℃, centrifuging, washing and drying to obtain black powder of 114mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 10
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 77mg of graphene oxide into 180g of tetrahydrofuran, ultrasonically dispersing for 1.0h at 24 ℃, and then adding 1.99 x 10-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 7.0h at 64 ℃, centrifuging, washing and drying to obtain black powder of 106mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 11
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 73mg of graphene oxide into 177g of tetrahydrofuran, ultrasonically dispersing for 1.1h at 26 ℃, and then adding 1.80 x 10-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 6.5h at 62 ℃, centrifuging, washing and drying to obtain black powder of 105mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 12
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
69mg of graphene oxide was added to 174g of tetrahydrofuran, ultrasonically dispersed at 27 ℃ for 1.2h, and then 1.74 x 10 was added-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 6.3h at 61 ℃, centrifuging, washing and drying to obtain black powder, namely 103mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 14
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 64mg of graphene oxide into 169g of tetrahydrofuran, ultrasonically dispersing at 34 ℃ for 1.6h, and then adding 1.71 x 10-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 7.6h at 64 ℃, centrifuging, washing and drying to obtain black powder 93mg of 3-aminopropyltriethoxysilane modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the example 3-aminopropyltriethoxysilane-modified graphene, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 15
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 56mg of graphene oxide into 150g of tetrahydrofuran, and carrying out ultrafiltration at 35 DEG CThe sound was dispersed for 1.4h, then 1.34 x 10 was added-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 7.1h at 69 ℃, centrifuging, washing and drying to obtain black powder, namely 80mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the example 3-aminopropyltriethoxysilane-modified graphene, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 16
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 50mg of graphene oxide into 130g of tetrahydrofuran, ultrasonically dispersing for 1.4h at 20 ℃, and then adding 1.01 x 10-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 7.0h at 60 ℃, centrifuging, washing and drying to obtain black powder of 72mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 17
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 44mg of graphene oxide into 100g of tetrahydrofuran, performing ultrasonic dispersion at 25 ℃ for 2.0h, and then adding 1.01 x 10-2And (3) mg of 3-aminopropyltriethoxysilane, reacting for 6.4h at 66 ℃, centrifuging, washing and drying to obtain black powder of 60mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 18
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 36mg of graphene oxide into 89g of tetrahydrofuran, ultrasonically dispersing for 1.6h at 21 ℃, and then adding 8.8 x 10- 3And (3) mg of 3-aminopropyltriethoxysilane, reacting for 6.4h at 64 ℃, centrifuging, washing and drying to obtain black powder, namely 51mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 19
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
32mg of graphene oxide was added to 74g of tetrahydrofuran, ultrasonically dispersed at 26 ℃ for 1.9h, and then 7.48 x 10 was added- 3And (3) mg of 3-aminopropyltriethoxysilane, reacting for 7.0h at 65 ℃, centrifuging, washing and drying to obtain black powder, namely 44mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 20
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
28mg of graphene oxide was added to 51g of tetrahydrofuranDispersing in furan by ultrasonic wave at 30 deg.C for 1.5h, and adding 6.17 x 10- 3And (3) mg of 3-aminopropyltriethoxysilane, reacting for 6.8h at 67 ℃, centrifuging, washing and drying to obtain black powder, namely 37mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Example 21
Synthesis of 3-aminopropyltriethoxysilane modified graphene oxide
Adding 24mg of graphene oxide into 41g of tetrahydrofuran, ultrasonically dispersing for 1.1h at 34 ℃, and then adding 5.04 x 10- 3And (3) mg of 3-aminopropyltriethoxysilane, reacting for 6.5h at 64 ℃, centrifuging, washing and drying to obtain black powder, namely 33mg of 3-aminopropyltriethoxysilane-modified graphene oxide.
Reduction of 3-aminopropyltriethoxysilane modified graphene oxide
Dispersing 20mg of washed and dried 3-aminopropyltriethoxysilane modified graphene oxide in 40mL of tetrahydrofuran, carrying out ultrasonic treatment for 0.5h, adding 0.5g of hydrazine hydrate, and reducing at 70 ℃ for 6 h; and washing the obtained product with absolute ethyl alcohol and distilled water, and drying to obtain the 3-aminopropyl triethoxysilane modified graphene. Weighing 10mg of dried 3-aminopropyltriethoxysilane modified graphene, respectively dispersing in DMF, DMSO, ethanol, THF and acetone, and performing ultrasonic treatment for 0.5-2 h to obtain a stable dispersion liquid, wherein precipitation and delamination do not occur after 24 h. From the SEM image of the 3-aminopropyltriethoxysilane-modified graphene of this example, it can also be seen that the reduced graphene does not undergo agglomeration.
Claims (1)
1. A synthetic method of 3-aminopropyl triethoxysilane modified graphene oxide takes graphene oxide as a raw material, and is characterized in that: the method comprises the following steps:
step 1, mixing graphene oxide and tetrahydrofuran according to a mass ratio of 20-100 mg: 35.6g to 222.5 g;
and 2, ultrasonically dispersing the mixture obtained in the step 1 at the temperature of 20-35 ℃ for 1-2 h, and then adding 3-aminopropyltriethoxysilane, wherein the mass ratio of graphene oxide to tetrahydrofuran is 20-100 mg: 35.6 g-222.5 g: 3.76*10-3mg～2.82*10-2mg；
And 3, stirring the mixed reactant obtained in the step 2 at the temperature of 60-70 ℃ for 6-8 hours, centrifuging, washing and drying to obtain powdery 3-aminopropyltriethoxysilane modified graphene oxide.
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