CN110339853A - C3N5Material and its preparation method and application - Google Patents
C3N5Material and its preparation method and application Download PDFInfo
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- CN110339853A CN110339853A CN201910661674.9A CN201910661674A CN110339853A CN 110339853 A CN110339853 A CN 110339853A CN 201910661674 A CN201910661674 A CN 201910661674A CN 110339853 A CN110339853 A CN 110339853A
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- 238000002360 preparation method Methods 0.000 title claims abstract description 30
- 239000000463 material Substances 0.000 claims abstract description 80
- KLSJWNVTNUYHDU-UHFFFAOYSA-N Amitrole Chemical compound NC1=NC=NN1 KLSJWNVTNUYHDU-UHFFFAOYSA-N 0.000 claims abstract description 30
- ZFSLODLOARCGLH-UHFFFAOYSA-N isocyanuric acid Chemical compound OC1=NC(O)=NC(O)=N1 ZFSLODLOARCGLH-UHFFFAOYSA-N 0.000 claims abstract description 20
- 125000004070 6 membered heterocyclic group Chemical group 0.000 claims abstract description 19
- 239000000843 powder Substances 0.000 claims abstract description 19
- 239000003054 catalyst Substances 0.000 claims abstract description 18
- 229940125717 barbiturate Drugs 0.000 claims abstract description 14
- 238000002156 mixing Methods 0.000 claims abstract description 14
- 238000010438 heat treatment Methods 0.000 claims abstract description 13
- 238000001816 cooling Methods 0.000 claims abstract description 10
- 238000004321 preservation Methods 0.000 claims abstract description 4
- IOLCXVTUBQKXJR-UHFFFAOYSA-M potassium bromide Chemical compound [K+].[Br-] IOLCXVTUBQKXJR-UHFFFAOYSA-M 0.000 claims description 20
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical group [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 15
- 238000001035 drying Methods 0.000 claims description 14
- 239000012752 auxiliary agent Substances 0.000 claims description 12
- 238000003756 stirring Methods 0.000 claims description 11
- 239000003795 chemical substances by application Substances 0.000 claims description 7
- 238000013329 compounding Methods 0.000 claims description 7
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
- 206010013786 Dry skin Diseases 0.000 claims description 5
- 239000011812 mixed powder Substances 0.000 claims description 3
- 239000002253 acid Substances 0.000 claims 2
- JMANVNJQNLATNU-UHFFFAOYSA-N glycolonitrile Natural products N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 claims 2
- 238000009210 therapy by ultrasound Methods 0.000 claims 1
- 230000001699 photocatalysis Effects 0.000 abstract description 26
- 238000000034 method Methods 0.000 abstract description 20
- 238000007146 photocatalysis Methods 0.000 abstract description 11
- 239000002994 raw material Substances 0.000 abstract description 7
- 238000005516 engineering process Methods 0.000 abstract description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 10
- 230000000052 comparative effect Effects 0.000 description 9
- 239000012153 distilled water Substances 0.000 description 8
- 238000001228 spectrum Methods 0.000 description 8
- 239000000725 suspension Substances 0.000 description 8
- 230000005284 excitation Effects 0.000 description 7
- 230000000630 rising effect Effects 0.000 description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- 238000005303 weighing Methods 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- 238000001354 calcination Methods 0.000 description 3
- 230000015556 catabolic process Effects 0.000 description 3
- 238000006555 catalytic reaction Methods 0.000 description 3
- XLJMAIOERFSOGZ-UHFFFAOYSA-N cyanic acid Chemical compound OC#N XLJMAIOERFSOGZ-UHFFFAOYSA-N 0.000 description 3
- 238000006731 degradation reaction Methods 0.000 description 3
- 229960000935 dehydrated alcohol Drugs 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 239000003344 environmental pollutant Substances 0.000 description 3
- 231100000719 pollutant Toxicity 0.000 description 3
- 239000004065 semiconductor Substances 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- 238000005406 washing Methods 0.000 description 3
- JYEUMXHLPRZUAT-UHFFFAOYSA-N 1,2,3-triazine Chemical group C1=CN=NN=C1 JYEUMXHLPRZUAT-UHFFFAOYSA-N 0.000 description 2
- NSPMIYGKQJPBQR-UHFFFAOYSA-N 4H-1,2,4-triazole Chemical compound C=1N=CNN=1 NSPMIYGKQJPBQR-UHFFFAOYSA-N 0.000 description 2
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 2
- 230000031709 bromination Effects 0.000 description 2
- 238000005893 bromination reaction Methods 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 230000005611 electricity Effects 0.000 description 2
- 238000000695 excitation spectrum Methods 0.000 description 2
- 238000002189 fluorescence spectrum Methods 0.000 description 2
- 229910021389 graphene Inorganic materials 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- 239000002957 persistent organic pollutant Substances 0.000 description 2
- 229910052700 potassium Inorganic materials 0.000 description 2
- 239000011591 potassium Substances 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- 150000003852 triazoles Chemical group 0.000 description 2
- 238000005829 trimerization reaction Methods 0.000 description 2
- ULRPISSMEBPJLN-UHFFFAOYSA-N 2h-tetrazol-5-amine Chemical compound NC1=NN=NN1 ULRPISSMEBPJLN-UHFFFAOYSA-N 0.000 description 1
- 238000000862 absorption spectrum Methods 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 238000004821 distillation Methods 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- IDGUHHHQCWSQLU-UHFFFAOYSA-N ethanol;hydrate Chemical compound O.CCO IDGUHHHQCWSQLU-UHFFFAOYSA-N 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- LELOWRISYMNNSU-UHFFFAOYSA-N hydrogen cyanide Chemical compound N#C LELOWRISYMNNSU-UHFFFAOYSA-N 0.000 description 1
- 238000005286 illumination Methods 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000011941 photocatalyst Substances 0.000 description 1
- 125000002924 primary amino group Chemical group [H]N([H])* 0.000 description 1
- 230000001681 protective effect Effects 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 238000006479 redox reaction Methods 0.000 description 1
- 238000006722 reduction reaction Methods 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 238000001338 self-assembly Methods 0.000 description 1
- 238000010025 steaming Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/24—Nitrogen compounds
-
- B01J35/39—
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Catalysts (AREA)
Abstract
The present invention relates to C3N5Material preparation method and its application belong to photocatalysis technology field.The technical problem to be solved by the present invention is to provide a kind of C3N5The preparation method of material, this method comprises the following steps: a, mixing 3- amino-1,2,4-triazole and six-membered heterocycle by weight 1:0.8~1.2, the powder after being mixed, wherein six-membered heterocycle is at least one of cyanuric acid and barbiturates；B, the powder heating after mixing is taken out after cooling, is washed in 480~520 DEG C of 2.5~3.5h of heat preservation, it is dry, obtain C3N5Material.The present invention is in preparation C3N5When material, raw material is used as using 3- amino-1,2,4-triazole and the mixing of specific six-membered heterocycle, preparation method is simple, thus obtained C3N5Material, photocatalytic activity is preferable, is widely used as photochemical catalyst.
Description
Technical field
The present invention relates to C3N5Material and its preparation method and application belongs to photocatalysis technology field.
Background technique
Photocatalysis technology is a kind of technology that catalysis reaction occurs under light illumination using photochemical catalyst, is one kind in the energy
There is the green technology of important application prospect with environmental area.Photochemical catalyst is the key that photocatalysis technology, is swashing in photon
The general designation that can play the chemical substance of catalytic action is given, semiconductor light-catalyst can excite generation electricity under the irradiation of light
Son and hole occur redox reaction in semiconductor surface, to realize the decomposition of water or the decomposition of organic pollutant, realize
The utilization and conversion of luminous energy.
As a kind of novel semiconductor material, C3N5It unique is formed with structure and visible light catalysis activity etc. with its
Feature has become a hot topic of research.More C is more studied with existing3N4Material is compared, C3N5With higher limit of diffusion electricity
Current density and lower overpotential, make its photocatalysis performance more preferably.Currently, C3N5Preparation method have some reports, but to it
The report of specific structure is seldom, and the C that different methods is prepared3N5Material, photocatalytic activity is not identical, this may
It is since method difference causes brought by the difference of its structure.
C3N5Preparation can using the preparation of 5- amino -1H-TETRAZOLE (5-ATTZ) self assembly, such as: In Young Kim etc.
In document " the order mesoporous C with triazole and triazine skeleton3N5And its graphene complex " in report (Dr.In Young
Kim,Sungho Kim,Dr.Xiaoyan Jin,Dr.Selvarajan Premkumar,Dr.Goutam Chandra,
Dr.Nam-Suk Lee,Prof.Gurudas P.Mane,Prof.Seong-Ju Hwang,Prof.Siva Umapathy,
Prof.Ajayan Vinu.Ordered Mesoporous C3N5with a Combined Triazole and Triazine
Framework and Its Graphene Hybrids for the Oxygen Reduction Reaction(ORR)[J]
.Angewandte Chemie,2018,130(52).)
C3N5Preparation 3- amino-1,2,4-triazole can also be used for raw material preparation, such as patent CN109562940A
In, use 3- amino-1,2,4-triazole that C is prepared for raw material3N5Material.The material that this method is prepared, photocatalytic
It can need to be further improved.
And Hunan Normal University Zhang Youyu etc. has studied under the auxiliary of NaOH, 3- amino-1,2,4-triazole is raw material system
It is standby to obtain C3N5Material, increase of the discovery with NaOH concentration, g-C3N5The vacancy N be gradually increased, show excellent photocatalysis
And photoelectrochemical behaviour.(it is detailed in document " the porous graphite carbonitride with controllable nitrogen vacancy: enhancing pollutant Visible Light Induced Photocatalytic
Ideal catalyst ", Haiyan Wang, Mingxia Li, Huan Li, Qiujun Lu, Youyu Zhang, Shouzhuo
Yao.Porous graphitic carbon nitride with controllable nitrogen vacancies:As
promising catalyst for enhanced degradation of pollutant under visible light
[J].Materials&；Design, 2018.) in addition, they are investigated under the auxiliary of KBr, and 3- amino -1,2,4- tri-
Azoles is that C is prepared in raw material3N5Material finds compared with the material being directly prepared, the obtained C under KBr auxiliary3N5Material
Material also shows that significant excellent photocatalysis performance.(it is detailed in document " the mesoporous rodlike g-C of salt guiding synthesis3N5: have as degradation
The excellent photochemical catalyst of machine pollutant ", Wang, Haiyan, Li, Mingxia, Lu, Qiujun, et al.A mesoporous
rod-like g-C3N5synthesized by salt-guided strategy:as a superior
photocatalyst for degradation of organic pollutant[J].ACS Sustainable
Chemistry&Engineering.)
Summary of the invention
First technical problem that the present invention solves is to provide a kind of C3N5The preparation method of material, is prepared using this method
Obtained material shows more preferably photocatalysis performance compared with the existing methods.
C of the present invention3N5The preparation method of material, includes the following steps:
A, mixing: 3- amino-1,2,4-triazole and six-membered heterocycle are mixed by weight 1:0.8~1.2, mixed
Powder afterwards, wherein six-membered heterocycle is at least one of cyanuric acid and barbiturates；
B, it calcines: the powder after mixing is heated up, in 480~520 DEG C of 2.5~3.5h of heat preservation, take out, wash after cooling,
It is dry, obtain C3N5Material.
Preferably, the concrete operations of a step are as follows: dehydrated alcohol is added in 3- amino-1,2,4-triazole and six-membered heterocycle
In, 1~3h is stirred, 0.5~1.5h, 60~80 DEG C of dryings, the powder after being mixed then are ultrasonically treated.More preferably stirring
Then 2h is ultrasonically treated 1h, 70 DEG C of dryings.
Preferably, in a step, six-membered heterocycle is cyanuric acid.It is furthermore preferred that 3- amino-1,2,4-triazole and trimerization
Cyanic acid is mixed by weight 1:1.
Another preferred, in a step, six-membered heterocycle is cyanuric acid and barbiturates.It is furthermore preferred that by weight,
3- amino -1,2,4- triazole: cyanuric acid: barbiturates=1:1:0.1.
Preferably, in b step, heating rate is 3~8 DEG C/min, and preferably heating rate is 5 DEG C/min.
Preferably, step c, the step c are carried out after a step are as follows: it is molten that auxiliary agent is added in the powder after mixing
It in liquid, and stirs evenly, then dries, then the powder after drying is subjected to b step；The auxiliary agent is sodium hydroxide or bromination
Potassium.
Preferably, the concentration of the compounding agent solution is 0.05~0.15g/mL, and the concentration of the more preferable compounding agent solution is
0.1g/mL。
Preferably, the weight ratio of auxiliary agent and 3- amino-1,2,4-triazole is 1:10~20, more preferable auxiliary agent and 3- amino-
The weight ratio of 1,2,4- triazole is 1:15.
Second technical problem that the present invention solves is to provide a kind of C3N5Material.
C of the present invention3N5Material is prepared using the above method.It can be seen by uv drs and fluorescence emission spectrum
Out, the C that the material and existing method are prepared3N5Material is compared, and photocatalytic activity is more preferable.
The present invention also provides C of the present invention3N5Application of the material in photochemical catalyst.
C of the invention3N5Material, photocatalytic activity is preferable, can be used in photochemical catalyst.C of the present invention3N5Material can be with
It uses, can also be used in mixed way with other photochemical catalysts separately as photochemical catalyst.
Compared with prior art, the invention has the following beneficial effects:
The present invention is in preparation C3N5When material, using 3- amino-1,2,4-triazole and specific six-membered heterocycle mixing conduct
Raw material, preparation method is simple, thus obtained C3N5Material, photocatalytic activity is preferable, is widely used as photochemical catalyst.
Detailed description of the invention
Fig. 1 is the C that the embodiment of the present invention 1~4 and comparative example 1~2 are prepared3N5XRD spectrum.
Fig. 2 is the C that the embodiment of the present invention 1~4 and comparative example 1~2 are prepared3N5Uv drs map.
Fig. 3 is the C that the embodiment of the present invention 1~4 and comparative example 1~2 are prepared3N5Fluorescent emission under 366nm excitation
Map.
Specific embodiment
C of the present invention3N5The preparation method of material, includes the following steps:
A, mixing: 3- amino-1,2,4-triazole and six-membered heterocycle are mixed by weight 1:0.8~1.2, mixed
Powder afterwards, wherein six-membered heterocycle is at least one of cyanuric acid and barbiturates；
B, it calcines: by the powder heating after mixing in 480~520 DEG C of 2.5~3.5h of heat preservation, taking out, wash after cooling, do
It is dry, obtain C3N5Material.
A step is primarily to raw material is mixed according to the ratio, it is preferred that the concrete operations of a step are as follows: by amino -1 3-,
2,4- triazoles and six-membered heterocycle are added to absolute ethanol, and stir 1~3h, are then ultrasonically treated 0.5~1.5h, and 60~80 DEG C dry
It is dry, the powder after being mixed；It is preferred that stirring 2h, is then ultrasonically treated 1h, 70 DEG C of dryings.
As one of embodiment, in a step, six-membered heterocycle is cyanuric acid.Preferably, 3- amino -1,2,
4- triazole and cyanuric acid are mixed by weight 1:1.
As another embodiment, in a step, six-membered heterocycle is cyanuric acid and barbiturates.Studies have shown that plus
Enter the C obtained after 3- amino -1,2,4- triazole, cyanuric acid and barbiturates3N5The photocatalytic activity of material is better than in the preparation
3- amino-1,2,4-triazole and cyanuric acid is only added, i.e. the addition of barbiturates is conducive to the light for improving the material of synthesis
Catalytic performance.Preferably, by weight, 3- amino-1,2,4-triazole: cyanuric acid: barbiturates=1:1:0.1.
B step is that calcining obtains C3N5The process of material.The calcining of the step is not necessarily to protective gas, can carry out in air,
It is easy to operate, there is no special requirement to calciner, is carried out for example, directly the powder after mixing can be put into Muffle furnace
Heating calcining.
Preferably, in b step, heating rate is 3~8 DEG C/min, and preferably heating rate is 5 DEG C/min.
Preferably, step c, the step c are carried out after a step are as follows: it is molten that auxiliary agent is added in the powder after mixing
It in liquid, and stirs evenly, then dries, then the powder after drying is subjected to b step；The auxiliary agent is sodium hydroxide or bromination
Potassium.After auxiliary agent is added, obtained C3N5The performance of material is more preferably.
Preferably, the concentration of the compounding agent solution is 0.05~0.15g/mL, and the concentration of the more preferable compounding agent solution is
0.1g/mL。
Preferably, the weight ratio of auxiliary agent and 3- amino-1,2,4-triazole is 1:10~20, more preferable auxiliary agent and 3- amino-
The weight ratio of 1,2,4- triazole is 1:15.
C of the present invention3N5Material is prepared using the above method.It can be seen by uv drs and fluorescence emission spectrum
Out, the C that the material and existing method are prepared3N5Material is compared, and photocatalytic activity is more preferable.
The present invention also provides C of the present invention3N5Application of the material in photochemical catalyst.
C of the invention3N5Material, photocatalytic activity is preferable, can be used in photochemical catalyst.C of the present invention3N5Material can be with
It uses, can also be used in mixed way with other photochemical catalysts separately as photochemical catalyst.
A specific embodiment of the invention is further described below with reference to embodiment, is not therefore limited the present invention
System is among the embodiment described range.
Embodiment 1
The cyanuric acid of the 3- amino -1,2,4- triazole and 5g that weigh 5g respectively is packed into beaker and the anhydrous second of 100mL is added
Suspension is then stirred 2h at ambient temperature, is then ultrasonically treated 1h at room temperature by alcohol.Then suspension is put into 70 DEG C
Baking oven in it is dry after obtain powder, be loaded into the crucible with cover of 50mL, move to Muffle furnace with the heating rate of 5 DEG C/min
3h is kept the temperature after rising to 500 DEG C.Sample is fitted into the distilled water that 100mL in beaker and is added after cooling, is then placed in ultrasonic machine
Ultrasonic disperse 3h, sample then be centrifuged and dried, and obtains C3N5Material is denoted as 3-C-1.The XRD spectrum of the material is shown in Fig. 1, purple
Outer diffusing reflection map is shown in that Fig. 2, the fluorescent emission map under 366nm excitation are shown in Fig. 3.
Embodiment 2
The barbiturates for weighing the 3- amino -1,2,4- triazole of 5g, the cyanuric acid of 5g and 0.5g respectively is packed into beaker simultaneously
100mL dehydrated alcohol is added, then suspension is stirred into 2h at ambient temperature, is then ultrasonically treated 1h at room temperature.Then
Suspension is put into 70 DEG C of baking oven and obtains white powder after drying, is loaded into the crucible with cover of 50mL, move to Muffle
Furnace keeps the temperature 3h after rising to 500 DEG C with the heating rate of 5 DEG C/min.Sample is fitted into the steaming that 100mL in beaker and is added after cooling
Distilled water is then placed in ultrasonic disperse 3h in ultrasonic machine, then sample is centrifuged and is dried, obtains C3N5Material is denoted as 3-C-1-2.
The XRD spectrum of the material is shown in that Fig. 1, uv drs map are shown in that Fig. 2, the fluorescent emission map under 366nm excitation are shown in Fig. 3.
Embodiment 3
Weigh respectively 4.5g 3- amino -1,2,4- triazole and 4.5g cyanuric acid be packed into beaker and be added 100mL without
Suspension is then stirred 2h at ambient temperature, is then ultrasonically treated 1h at room temperature by water-ethanol.Then suspension is put into
Powder is obtained in 70 DEG C of baking oven after drying, KBr solution (3mL distilled water is added in the KBr of 0.3g) is added and simultaneously stirs evenly, then
It is put into 80 DEG C of drying in oven and obtains solid, move it into the crucible with cover of 50mL, move to Muffle furnace with the liter of 5 DEG C/min
Warm rate keeps the temperature 3h after rising to 500 DEG C.Sample is fitted into the distilled water that 100mL in beaker and is added after cooling, is then placed in super
Sample washing is centrifuged and dry afterwards for several times, obtains C by ultrasonic disperse 3h in sound machine3N5Material is denoted as 3-C-K-1.The material
XRD spectrum is shown in that Fig. 1, uv drs map are shown in that Fig. 2, the fluorescent emission map under 366nm excitation are shown in Fig. 3.
Embodiment 4
The barbiturates for weighing the 3- amino -1,2,4- triazole of 4.5g, the cyanuric acid of 4.5g and 0.45g respectively, which is packed into, to be burnt
Simultaneously 100mL dehydrated alcohol is added in cup, then suspension is stirred 2h at ambient temperature, is then ultrasonically treated 1h at room temperature.
Then suspension is put into 70 DEG C of baking oven and obtains powder after drying, KBr solution is added, and (3mL distillation is added in the KBr of 0.3g
Water) and stir evenly, it is subsequently placed into 80 DEG C of drying in oven and obtains solid, move it into the crucible with cover of 50mL, move to
Muffle furnace keeps the temperature 3h after rising to 500 DEG C with the heating rate of 5 DEG C/min.Sample is fitted into beaker after cooling and 100mL is added
Distilled water, be then placed in ultrasonic disperse 3h in ultrasonic machine, sample washing be centrifuged and dry afterwards for several times, obtain C3N5Material, note
For 3-C-K-1-2.The XRD spectrum of the material is shown in that Fig. 1, uv drs map are shown in Fig. 2, the fluorescent emission figure under 366nm excitation
Spectrum is shown in Fig. 3.
Comparative example 1
The 3- amino-1,2,4-triazole for weighing 6g is fitted into the crucible with cover of 50mL, moves to Muffle furnace with the liter of 5 DEG C/min
Warm rate keeps the temperature 3h after rising to 500 DEG C.Sample is fitted into the distilled water that 100mL in beaker and is added after cooling, is then placed in super
Ultrasonic disperse 3h, sample then be centrifuged and dried in sound machine, obtains C3N5Material is denoted as 3-C.The XRD spectrum of the material is shown in figure
1, uv drs map is shown in that Fig. 2, the fluorescent emission map under 366nm excitation are shown in Fig. 3.
Comparative example 2
The 3- amino-1,2,4-triazole for weighing 4.5g is fitted into beaker, and KBr solution is added, and (KBr of 0.3g is added 3mL and steams
Distilled water) and stir evenly, it is subsequently placed into 80 DEG C of drying in oven and obtains solid, move it into the crucible with cover of 50mL, move
3h is kept the temperature after rising to 500 DEG C to Muffle furnace with the heating rate of 5 DEG C/min.Sample is fitted into beaker and is added after cooling
The distilled water of 100mL is then placed in ultrasonic disperse 3h in ultrasonic machine, sample washing is centrifuged and dry afterwards for several times, obtains C3N5Material
Material, is denoted as 3-C-K.The XRD spectrum of the material is shown in that Fig. 1, uv drs map are shown in Fig. 2, the fluorescent emission figure under 366nm excitation
Spectrum is shown in Fig. 3.
Fig. 1 is the C that the embodiment of the present invention 1~4 and comparative example 1~2 are prepared3N5XRD spectrum, can from Fig. 1
Out, the C being prepared with existing method3N5Material (i.e. comparative example 1~3) is compared, and the material that the method for the present invention is prepared is surveyed
Try the C of diffraction maximum and existing way preparation when XRD3N5Material diffraction maximum position consistency, it is seen then that the present invention is successfully prepared
C3N5Material, and present invention gained C3N5The XRD diffraction maximum of material is than the C that existing method is prepared3N5Material diffraction maximum is wider,
Illustrate that crystal form is declined, specific surface area increases, conducive to the raising of photocatalysis performance.
Fig. 2 is the C that the embodiment of the present invention 1~4 and comparative example 1~2 are prepared3N5Uv drs map, from map
It is upper to can be seen that the C being prepared with existing method3N5Material is compared, the material absorption spectrum model that the method for the present invention is prepared
It encloses wider, is more advantageous to and realizes photocatalysis under visible light or daylight.
Fig. 3 is the C that the embodiment of the present invention 1~4 and comparative example 1~2 are prepared3N5Fluorescent emission under 366nm excitation
Map.It is well known to those skilled in the art, electrons and holes, a portion electronics and sky can be generated after the excitation of photochemical catalyst light
Redox is played in cave, and another part then can be compound, and energy releases in the form of light, and in general, electrons and holes
Compound tense can issue fluorescence, and therefore, fluorescent emission intensity is lower, and electron-hole recombination rate is then lower, show that photocatalytic activity is got over
It is high.And from figure 3, it can be seen that the C that the method for the present invention is prepared3N5Material, fluorescent emission intensity are below existing method preparation
Obtained C3N5Material shows the C that the method for the present invention obtains3N5The photocatalytic activity of material is higher.The photocatalysis of 3-C-1-2 is living
Property be better than 3-C-1, the photocatalytic activity of 3-C-K-1-2 is better than 3-C-K-1, shows to joined barbiturates and trimerization in the preparation
The C of cyanic acid3N5Material light catalysis activity, which is higher than, only joined cyanuric acid.In addition, the photocatalytic activity of 3-C-K-1 is better than 3-
The photocatalytic activity of C-1,3-C-K-1-2 are better than 3-C-1-2, show that the addition of auxiliary agent potassium bromide helps to improve the light of material and urges
Change activity.
Claims (10)
1.C3N5The preparation method of material, which comprises the steps of:
A, mixing: 3- amino-1,2,4-triazole and six-membered heterocycle are mixed by weight 1:0.8~1.2, after being mixed
Powder, wherein six-membered heterocycle is at least one of cyanuric acid and barbiturates；
B, it calcines: the powder after mixing is heated up, in 480~520 DEG C of 2.5~3.5h of heat preservation, take out, wash after cooling, it is dry,
Obtain C3N5Material.
2. C according to claim 13N5The preparation method of material, it is characterised in that: the concrete operations of a step are as follows: by 3-
Amino-1,2,4-triazole and six-membered heterocycle are added to absolute ethanol, and stir 1~3h, then 0.5~1.5h of ultrasonic treatment, and 60
~80 DEG C of dryings, the powder after being mixed；It is preferred that stirring 2h, is then ultrasonically treated 1h, 70 DEG C of dryings.
3. C according to claim 13N5The preparation method of material, it is characterised in that: in a step, six-membered heterocycle three
Paracyanogen acid, preferably 3- amino-1,2,4-triazole and cyanuric acid are mixed by weight 1:1.
4. C according to claim 13N5The preparation method of material, it is characterised in that: in a step, six-membered heterocycle three
Paracyanogen acid and barbiturates, preferably by weight, 3- amino-1,2,4-triazole: cyanuric acid: barbiturates=1:1:0.1.
5. C according to claim 13N5The preparation method of material, it is characterised in that: in b step, heating rate is 3~8
DEG C/min, preferably heating rate is 5 DEG C/min.
6. described in any item C according to claim 1~53N5The preparation method of material, it is characterised in that: c is carried out after a step
Step, the step c are as follows: the powder after mixing is added in compounding agent solution, and stirs evenly, then dries, then will be after drying
Powder carry out b step；The auxiliary agent is sodium hydroxide or potassium bromide.
7. C according to claim 63N5The preparation method of material, it is characterised in that: the concentration of the compounding agent solution is
0.05~0.15g/mL, the concentration of the preferably described compounding agent solution are 0.1g/mL.
8. C according to claim 63N5The preparation method of material, it is characterised in that: auxiliary agent and 3- amino-1,2,4-triazole
Weight ratio be 1:10~20, the weight ratio of preferred promoter and 3- amino-1,2,4-triazole is 1:15.
9. C according to any one of claims 1 to 83N5The C that the preparation method of material is prepared3N5Material.
10. C as claimed in claim 93N5Application of the material in photochemical catalyst.
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