CN114345388A - Modification method of graphite-like phase carbon nitride - Google Patents
Modification method of graphite-like phase carbon nitride Download PDFInfo
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- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 title claims abstract description 26
- 238000002715 modification method Methods 0.000 title claims abstract description 18
- FJDQFPXHSGXQBY-UHFFFAOYSA-L caesium carbonate Chemical compound [Cs+].[Cs+].[O-]C([O-])=O FJDQFPXHSGXQBY-UHFFFAOYSA-L 0.000 claims abstract description 27
- 229910000024 caesium carbonate Inorganic materials 0.000 claims abstract description 27
- 238000006243 chemical reaction Methods 0.000 claims abstract description 19
- -1 chlorocarbonyl Chemical group 0.000 claims abstract description 19
- 229910052581 Si3N4 Inorganic materials 0.000 claims abstract description 13
- 150000001491 aromatic compounds Chemical class 0.000 claims abstract description 13
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 claims abstract description 13
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- PASDCCFISLVPSO-UHFFFAOYSA-N benzoyl chloride Chemical compound ClC(=O)C1=CC=CC=C1 PASDCCFISLVPSO-UHFFFAOYSA-N 0.000 claims description 26
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 25
- NSNPSJGHTQIXDO-UHFFFAOYSA-N naphthalene-1-carbonyl chloride Chemical compound C1=CC=C2C(C(=O)Cl)=CC=CC2=C1 NSNPSJGHTQIXDO-UHFFFAOYSA-N 0.000 claims description 22
- 238000010438 heat treatment Methods 0.000 claims description 18
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- 238000000034 method Methods 0.000 claims description 12
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- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 3
- 239000004202 carbamide Substances 0.000 claims description 3
- XZMCDFZZKTWFGF-UHFFFAOYSA-N Cyanamide Chemical compound NC#N XZMCDFZZKTWFGF-UHFFFAOYSA-N 0.000 claims description 2
- 229920000877 Melamine resin Polymers 0.000 claims description 2
- 239000012459 cleaning agent Substances 0.000 claims description 2
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 claims description 2
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- 238000012986 modification Methods 0.000 abstract description 11
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- 229910052739 hydrogen Inorganic materials 0.000 description 13
- 238000004519 manufacturing process Methods 0.000 description 11
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 11
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- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
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- GSEJCLTVZPLZKY-UHFFFAOYSA-N Triethanolamine Chemical compound OCCN(CCO)CCO GSEJCLTVZPLZKY-UHFFFAOYSA-N 0.000 description 1
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Abstract
The invention belongs to the technical field of photocatalysis, and particularly discloses a modification method of graphite-like carbon nitride, which comprises the following steps: and (3) mixing the graphite-like phase silicon nitride with an organic solvent, adding cesium carbonate, dispersing, adding an aromatic compound containing chlorocarbonyl after dispersion is finished, reacting at 55-65 ℃, and obtaining the modified graphite-like phase silicon nitride after reaction is finished. The present invention modifies g-C by using an aromatic compound containing a chlorocarbonyl group3N4Can realize the redistribution of pi electrons, can effectively separate photoproduction electrons/holes, and g-C is modified under the irradiation of visible light3N4The excited electron can be better transferred to the cocatalyst through the accessed benzene ring to react with the proton to generate H2(ii) a The invention has mild modification reaction condition and is suitable for equipmentThe requirement is low, and the problem caused by modification under the harsh condition of high temperature or vacuum is solved.
Description
Technical Field
The invention relates to the technical field of photocatalysis, in particular to a modification method of graphite-like phase carbon nitride.
Background
With the emergence of the problem of energy crisis and environmental deterioration, hydrogen energy has been receiving increasing attention as a clean energy source. Photocatalytic water splitting is one of the hydrogen production methods, has the characteristics of strong oxidation capacity, no secondary pollution and the like, and is very suitable for the current situation. The method for preparing hydrogen by photocatalysis is particularly important for selecting the photocatalyst, and the current mainstream photocatalyst is graphite-like phase nitrogenCarbon (g-C)3N4) -a non-metallic conjugated semiconductor photocatalyst.
Presence of sp in graphite-like phase carbon nitride structure2Hybridized nitrogen and carbon, which establish a pi-conjugated band structure to minimize the band gap, have excellent visible light response properties, but still have many defects in practical applications. Therefore, many modification techniques, such as doping, heterojunction construction, carbon material recombination, defect engineering, Surface Plasmon Resonance (SPR) modification, dye sensitization, and molecular modification, have been developed to enhance photocatalytic activity. However, many of the current modification methods need to be performed under a relatively harsh condition, such as a high-temperature or vacuum environment, which is not favorable for industrial production, and many groups cannot keep activity at high temperature, which also limits the selection space of materials.
Disclosure of Invention
In order to overcome the defects and shortcomings in the prior art, the invention aims to provide a modification method of graphite-like phase carbon nitride, which utilizes chemical reaction under mild conditions to graft small aromatic molecules into g-C3N4Further, the problem that modification reaction needs to be carried out under harsh conditions such as high temperature or vacuum environment is solved, and more selectable materials are expanded.
A modification method of graphite-like phase carbon nitride comprises the following steps:
and mixing the graphite-like phase silicon nitride, an organic solvent and cesium carbonate, dispersing, adding an aromatic compound containing chlorocarbonyl after dispersion is finished, reacting at 55-65 ℃, and obtaining the modified graphite-like phase silicon nitride after reaction is finished.
The method adopts cesium carbonate as a catalyst, wherein the cesium carbonate is dissolved in an organic solvent and can induce the reaction of graphite-like phase silicon nitride and a chlorocarbonyl-containing aromatic compound under mild conditions, and acyl chloride molecules are grafted to g-C3N4On the terminal amino group, a modified g-C is obtained3N4。
Preferably, the addition amount of the aromatic compound containing the chlorocarbonyl is 1 to 10 percent of the mass of the graphite-like phase silicon nitride; the molar ratio of the cesium carbonate to the aromatic compound containing the chlorocarbonyl group is (1-1.1): 1.
Preferably, the aromatic compound containing a chlorocarbonyl group is naphthoyl chloride and/or benzoyl chloride.
Both the naphthoyl chloride and the benzoyl chloride have strong conjugated structures, and the chlorine atoms in the acyl chloride are very active and are easy to hydrolyze, alcoholyze and aminolyze. Through research, the naphthoyl chloride and the benzoyl chloride are not only easy to react with g-C3N4The reaction is carried out and naphthoyl chloride and benzoyl chloride are grafted to g-C3N4The terminal amino group can realize the redistribution of pi electrons, can effectively separate photoproduction electrons/holes, and is g-C after modification under the irradiation of visible light3N4The excited electron can be better transferred to the cocatalyst through the accessed benzene ring to react with the proton to generate H2。
Preferably, the dispersion and the reaction are both carried out under a sealed condition, the dispersion time is 30-40 min, and the reaction time is 6-7 h.
Preferably, the organic solvent is N, N-dimethylformamide or tetrahydrofuran. Both N, N-dimethylformamide and tetrahydrofuran are soluble in g-C3N4。
Preferably, after the reaction is finished, the method further comprises the steps of filtering, washing and drying; the cleaning agent selected during washing is one or more of N, N-dimethylformamide, tetrahydrofuran and ethanol.
Preferably, the graphite-like phase silicon nitride is synthesized by the following steps: the nitrogen-containing compound is put into a muffle furnace, the muffle furnace is gradually heated from room temperature to 550 ℃ at the heating rate of 10 ℃/min, the nitrogen-containing compound is continuously calcined for 4 hours at 550 ℃ to obtain an intermediate, the obtained intermediate is ground into powder, the powder is put into the muffle furnace again, the temperature is gradually heated from room temperature to 550 ℃ at the heating rate of 10 ℃/min, and the intermediate is continuously calcined for 2 hours at 550 ℃ to obtain the graphite-like phase silicon nitride.
g-C prepared by the thermal polycondensation synthesis method3N4Thinner, and is more beneficial to photocatalytic reaction.
Preferably, the nitrogen-containing compound is one of melamine, cyanamide and urea.
Compared with the prior art, the invention has the beneficial effects that:
1. the invention adopts cesium carbonate as a catalyst and can react on g-C under mild conditions3N4The modification is carried out, the modification reaction condition is simple, the requirement on equipment is low, and the problem caused by modification under the harsh condition of high temperature or vacuum is solved.
2. The present invention modifies g-C by using an aromatic compound containing a chlorocarbonyl group3N4Incorporating chlorocarbonyl-containing aromatic compounds into g-C3N4The terminal amino group can realize the redistribution of pi electrons, can effectively separate photoproduction electrons/holes, and is g-C after modification under the irradiation of visible light3N4The excited electron can be better transferred to the cocatalyst through the accessed benzene ring to react with the proton to generate H2。
Drawings
FIG. 1 shows g-C of blank groups in an example of the present invention3N4Modification of (DCN) with benzoyl chloride group (a) g-C3N4A graph comparing the hydrogen production efficiency of (DCN-BC 1%, DCN-BC 2%, DCN-BC 5%, DCN-BC 10%);
FIG. 2 shows g-C of blank set in example of the present invention3N4Modified g-C of (DCN) with naphthoyl chloride group (b)3N4(DCN-NC 1%, DCN-NC 2%, DCN-NC 1%, DCN-NC 1%) in comparison with the hydrogen production efficiency.
Detailed Description
The present invention will be described in further detail with reference to examples, but the embodiments of the present invention are not limited thereto. Reagents, methods and apparatus used in the present invention are conventional in the art unless otherwise indicated. In the present specification, "part" and "%" represent "part by mass" and "% by mass", respectively, unless otherwise specified.
Example 1
A synthetic method of graphite-like phase carbon nitride comprises the following steps:
using a thermal polycondensation synthesis method, 50g of urea is put into a muffle furnace, heated from room temperature to 550 ℃ at the heating rate of 10 ℃/min, calcined and reacted for 4h at 550 ℃, the obtained sample is ground into powder, put into the muffle furnace again for secondary calcination, heated from room temperature to 550 ℃ at the heating rate of 10 ℃/min, calcined and reacted for 2h at 550 ℃, and g-C is obtained3N4(blank group, named DCN).
Example 2
A modification method of graphite-like phase carbon nitride comprises the following steps:
0.5g of g-C obtained in step S1 was weighed3N4(DCN) adding 50mL of dehydrated DMF solution serving as a solvent into a beaker, weighing 11.6mg of cesium carbonate, adding the cesium carbonate into the beaker, sealing, and ultrasonically dispersing for 30min at normal temperature; after the ultrasonic resolution and the stagnation, 5mg of benzoyl chloride is added, after sealing, the temperature is gradually increased from room temperature to 60 ℃ at the temperature increase rate of 5 ℃/min, the mixture is stirred and reacts for 6 hours in a water bath at the temperature of 60 ℃, after the reaction is finished, the filtrate is filtered, the filter residue is washed by DMF and absolute ethyl alcohol for three times, and the dosage of the DMF and the absolute ethyl alcohol is 20mL each time. After washing, transferring the sample to a watch glass, putting the watch glass into an oven, setting the temperature of the oven to be 60 ℃, and drying the watch glass overnight to finally obtain modified g-C3N4(benzoyl chloride group, named DCN-BC 1%).
Example 3
A modification method of graphite-like phase carbon nitride comprises the following steps:
0.5g of g-C obtained in step S1 was weighed3N4(DCN) adding 50mL of dehydrated DMF solution serving as a solvent into a beaker, weighing 23.1mg of cesium carbonate, adding the cesium carbonate into the beaker, sealing, and ultrasonically dispersing for 30min at normal temperature; after the ultrasonic resolution and the stagnation, 10mg of benzoyl chloride is added, after sealing, the temperature is gradually increased from room temperature to 60 ℃ at the temperature increase rate of 5 ℃/min, the mixture is stirred and reacted for 6 hours in a water bath at the temperature of 60 ℃, after the reaction is finished, the filtrate is filtered, the filter residue is washed by DMF and absolute ethyl alcohol for three times, and the dosage of the DMF and the absolute ethyl alcohol is 20mL each time. After being washed cleanTransferring the sample to a watch glass, putting the watch glass into an oven, setting the temperature of the oven to be 60 ℃, and drying the watch glass overnight to obtain modified g-C3N4(benzoyl chloride group, named DCN-BC 2%).
Example 4
A modification method of graphite-like phase carbon nitride comprises the following steps:
0.5g of g-C from step S1 was weighed3N4(DCN) adding 50mL of dehydrated DMF solution serving as a solvent into a beaker, weighing 57.9mg of cesium carbonate, adding the cesium carbonate into the beaker, sealing, and ultrasonically dispersing for 30min at normal temperature; after the ultrasonic dispersion is finished, adding 25mg of benzoyl chloride, sealing, gradually heating from room temperature to 60 ℃ at the heating rate of 5 ℃/min, stirring and reacting for 6 hours under the condition of water bath at 60 ℃, filtering to remove filtrate after the reaction is finished, washing filter residue with DMF (dimethyl formamide) and absolute ethyl alcohol for three times, wherein the dosage of the DMF and the absolute ethyl alcohol is 20mL each time. After washing, transferring the sample to a watch glass, putting the watch glass into an oven, setting the temperature of the oven to be 60 ℃, and drying the watch glass overnight to finally obtain modified g-C3N4(benzoyl chloride group, named DCN-BC 5%).
Example 5
A modification method of graphite-like phase carbon nitride comprises the following steps:
0.5g of g-C obtained in step S1 was weighed3N4Adding 50mL of dewatered DMF solution serving as a solvent into a beaker, weighing 115.9mg of cesium carbonate, adding the cesium carbonate into the beaker, sealing, and ultrasonically dispersing for 30min at normal temperature; after the ultrasonic dispersion is finished, adding 50mg of benzoyl chloride, sealing, gradually heating from room temperature to 60 ℃ at the heating rate of 5 ℃/min, stirring and reacting for 6 hours under the condition of water bath at 60 ℃, filtering to remove filtrate after the reaction is finished, washing filter residue with DMF (dimethyl formamide) and absolute ethyl alcohol for three times, wherein the dosage of the DMF and the absolute ethyl alcohol is 20mL each time. After washing, transferring the sample to a watch glass, putting the watch glass into an oven, setting the temperature of the oven to be 60 ℃, and drying the watch glass overnight to finally obtain modified g-C3N4(benzoyl chloride group, named DCN-BC 10%).
Example 6
A modification method of graphite-like phase carbon nitride comprises the following steps:
0.5g of g-C obtained in step S1 was weighed3N4(DCN) adding 50mL of dehydrated DMF solution serving as a solvent into a beaker, weighing 57.9mg of cesium carbonate, adding the cesium carbonate into the beaker, sealing, and ultrasonically dispersing for 40min at normal temperature; after the ultrasonic dispersion is finished, adding 25mg of benzoyl chloride, sealing, gradually heating from room temperature to 55 ℃ at the heating rate of 5 ℃/min, stirring and reacting for 7 hours under the condition of water bath at 55 ℃, filtering to remove filtrate after the reaction is finished, washing filter residue with DMF (dimethyl formamide) and absolute ethyl alcohol for three times, wherein the dosage of the DMF and the absolute ethyl alcohol is 20mL each time. After washing, transferring the sample to a watch glass, putting the watch glass into an oven, setting the temperature of the oven to be 60 ℃, and drying the watch glass overnight to finally obtain modified g-C3N4(benzoyl chloride group, named DCN-BC 5% -1).
Example 7
A modification method of graphite-like phase carbon nitride comprises the following steps:
0.5g of g-C obtained in step S1 was weighed3N4(DCN) adding 50mL of dehydrated DMF solution serving as a solvent into a beaker, weighing 63.7mg of cesium carbonate, adding the cesium carbonate into the beaker, sealing, and ultrasonically dispersing for 35min at normal temperature; after the ultrasonic dispersion is finished, adding 25mg of benzoyl chloride, sealing, gradually heating from room temperature to 65 ℃ at the heating rate of 5 ℃/min, stirring and reacting for 6 hours under the condition of water bath at 65 ℃, filtering to remove filtrate after the reaction is finished, washing filter residue with DMF (dimethyl formamide) and absolute ethyl alcohol for three times, wherein the dosage of the DMF and the absolute ethyl alcohol is 20mL each time. After washing, transferring the sample to a watch glass, putting the watch glass into an oven, setting the temperature of the oven to be 60 ℃, and drying the watch glass overnight to finally obtain modified g-C3N4(benzoyl chloride group, named DCN-BC 5% -2).
Example 8
A modification method of graphite-like phase carbon nitride comprises the following steps:
0.5g of g-C obtained in step S1 was weighed3N4(DCN) in a beaker, 50mL of dehydrated DMF solution was added as a solvent, and 8.5mg of cesium carbonate was weighed in the beaker and sealedThen ultrasonically dispersing for 30min at normal temperature; after the ultrasonic resolution and the stagnation, 5mg of naphthoyl chloride is added, after sealing, the temperature is gradually increased from room temperature to 60 ℃ at the temperature increase rate of 5 ℃/min, the mixture is stirred and reacts for 6 hours in a water bath at the temperature of 60 ℃, after the reaction is finished, the filtrate is filtered, filter residue is washed by DMF and absolute ethyl alcohol for three times, and the dosage of the DMF and the absolute ethyl alcohol is 20mL each time. After washing, transferring the sample to a watch glass, putting the watch glass into an oven, setting the temperature of the oven to be 60 ℃, and drying the watch glass overnight to finally obtain modified g-C3N4(naphthoyl chloride group, named DCN-NC 1%).
Example 9
A modification method of graphite-like phase carbon nitride comprises the following steps:
0.5g of g-C obtained in step S1 was weighed3N4(DCN) adding 50mL of dehydrated DMF solution serving as a solvent into a beaker, weighing 17mg of cesium carbonate, adding the cesium carbonate into the beaker, sealing, and ultrasonically dispersing for 30min at normal temperature; after the ultrasonic resolution and the stagnation, 10mg of naphthoyl chloride is added, after sealing, the temperature is gradually increased from room temperature to 60 ℃ at the temperature increase rate of 5 ℃/min, the mixture is stirred and reacts for 6 hours in a water bath at the temperature of 60 ℃, after the reaction is finished, the filtrate is filtered, filter residue is washed by DMF and absolute ethyl alcohol for three times, and the dosage of the DMF and the absolute ethyl alcohol is 20mL each time. After washing, transferring the sample to a watch glass, putting the watch glass into an oven, setting the temperature of the oven to be 60 ℃, and drying the watch glass overnight to finally obtain modified g-C3N4(naphthoyl chloride group, named DCN-NC 2%).
Example 10
A modification method of graphite-like phase carbon nitride comprises the following steps:
0.5g of g-C obtained in step S1 was weighed3N4(DCN) adding 50mL of dehydrated DMF solution serving as a solvent into a beaker, weighing 42.7mg of cesium carbonate, adding the cesium carbonate into the beaker, sealing, and ultrasonically dispersing for 30min at normal temperature; after the ultrasonic dispersion is finished, adding 25mg of naphthoyl chloride, sealing, gradually heating from room temperature to 60 ℃ at the heating rate of 5 ℃/min, stirring and reacting for 6 hours under the condition of water bath at 60 ℃, filtering to remove filtrate after the reaction is finished, and washing filter residue with DMF (dimethyl formamide) and absolute ethyl alcoholWashing and washing three times, wherein the dosage of DMF and absolute ethyl alcohol is 20mL each time. After washing, transferring the sample to a watch glass, putting the watch glass into an oven, setting the temperature of the oven to be 60 ℃, and drying the watch glass overnight to finally obtain modified g-C3N4(naphthoyl chloride group, named DCN-NC 5%).
Example 11
A modification method of graphite-like phase carbon nitride comprises the following steps:
0.5g of g-C obtained in step S1 was weighed3N4(DCN) adding 50mL of dehydrated DMF solution serving as a solvent into a beaker, weighing 85mg of cesium carbonate, adding the cesium carbonate into the beaker, sealing, and ultrasonically dispersing for 30min at normal temperature; after the ultrasonic dispersion is finished, adding 50mg of naphthoyl chloride, sealing, gradually heating from room temperature to 60 ℃ at the heating rate of 5 ℃/min, stirring and reacting for 6 hours under the condition of water bath at 60 ℃, filtering to remove filtrate after the reaction is finished, washing filter residue with DMF (dimethyl formamide) and absolute ethyl alcohol for three times, wherein the dosage of the DMF and the absolute ethyl alcohol is 20mL each time. After washing, transferring the sample to a watch glass, putting the watch glass into an oven, setting the temperature of the oven to be 60 ℃, and drying the watch glass overnight to finally obtain modified g-C3N4(naphthoyl chloride group, named DCN-NC 10%).
Example 12
Testing the photocatalytic hydrogen production effect:
blanks g-C, obtained in example 1 respectively3N4(DCN), modification g-C of benzoyl chloride group obtained in example 2-example 53N4(DCN-BC 1%, DCN-BC 2% DCN-BC 5%, DCN-BC 10%), modified g-C of naphthoyl chloride groups obtained in examples 8 to 113N4(DCN-NC 1%, DCN-NC 2%, DCN-NC 5% and DCN-NC 10%) is added with a triethanolamine aqueous solution as a sacrificial agent, and photocatalytic hydrogen production experiments are respectively carried out under visible light to test photocatalytic performance.
As can be seen from FIGS. 1 and 2, the modification g-C of the benzoyl chloride group and the naphthoyl chloride group3N4The hydrogen production efficiency of the catalyst is higher than that of the g-C of the blank group3N4The hydrogen production effect is high, which shows that the g-C is obviously increased by the insertion of benzoyl chloride or naphthoyl chloride3N4The hydrogen production efficiency of (2) is enhanced by g-C3N4The photocatalytic performance of (a). And, the amount of naphthoyl chloride or benzoyl chloride added is less than g-C3N4At 5% by mass, g-C is modified3N4The hydrogen production efficiency of (a) increases with the addition of the naphthoyl chloride or the benzoyl chloride, but the addition amount of the naphthoyl chloride or the benzoyl chloride is higher than g-C3N4At 5% by mass, g-C is modified3N4The hydrogen production effect of the catalyst is reduced along with the increase of the addition amount of the naphthoyl chloride or the benzoyl chloride, and the addition amount of the naphthoyl chloride or the benzoyl chloride is g-C through research3N4At 5% by mass, g-C is modified3N4The hydrogen production effect is best, and the photocatalytic performance is best.
The above-described embodiments are preferred implementations of the present invention, and the present invention may be implemented in other ways without departing from the spirit of the present invention.
Claims (8)
1. A modification method of graphite-like phase carbon nitride is characterized by comprising the following steps:
and mixing the graphite-like phase silicon nitride, an organic solvent and cesium carbonate, dispersing, adding an aromatic compound containing chlorocarbonyl after dispersion is finished, reacting at 55-65 ℃, and obtaining the modified graphite-like phase silicon nitride after reaction is finished.
2. The method for modifying graphite-like phase carbon nitride according to claim 1, wherein the amount of the aromatic compound containing a chlorocarbonyl group is 1 to 10% by mass of the graphite-like phase silicon nitride; the molar ratio of the cesium carbonate to the aromatic compound containing the chlorocarbonyl group is (1-1.1): 1.
3. The method for modifying graphite-like carbon nitride according to claim 2, wherein the aromatic compound containing a chlorocarbonyl group is naphthoyl chloride and/or benzoyl chloride.
4. The method for modifying graphite-like phase carbon nitride according to claim 3, wherein the dispersing and the reacting are both performed under a sealed condition, the dispersing time is 30min to 40min, and the reacting time is 6h to 7 h.
5. The method for modifying graphite-like phase carbon nitride according to claim 4, wherein the organic solvent is N, N-dimethylformamide or tetrahydrofuran.
6. The method for modifying graphite-like-phase carbon nitride according to claim 5, further comprising the steps of filtering, cleaning, and drying after the reaction; the cleaning agent selected during cleaning is one or more of N, N-dimethylformamide, tetrahydrofuran and ethanol.
7. The method for modifying graphite-like phase carbon nitride according to any one of claims 1 to 6, wherein the graphite-like phase silicon nitride is synthesized by the following steps: the nitrogen-containing compound is put into a muffle furnace, the muffle furnace is gradually heated from room temperature to 550 ℃ at the heating rate of 10 ℃/min, the nitrogen-containing compound is continuously calcined for 4 hours at 550 ℃ to obtain an intermediate, the obtained intermediate is ground into powder, the powder is put into the muffle furnace again, the temperature is gradually heated from room temperature to 550 ℃ at the heating rate of 10 ℃/min, and the intermediate is continuously calcined for 2 hours at 550 ℃ to obtain the graphite-like phase silicon nitride.
8. The method for modifying graphite-like phase carbon nitride according to claim 7, wherein the nitrogen-containing compound is one of melamine, cyanamide and urea.
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