CN115340071B - Preparation method of hydrogen peroxide - Google Patents
Preparation method of hydrogen peroxide Download PDFInfo
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- CN115340071B CN115340071B CN202211161503.8A CN202211161503A CN115340071B CN 115340071 B CN115340071 B CN 115340071B CN 202211161503 A CN202211161503 A CN 202211161503A CN 115340071 B CN115340071 B CN 115340071B
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- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 title claims abstract description 104
- 238000002360 preparation method Methods 0.000 title claims abstract description 21
- 239000011941 photocatalyst Substances 0.000 claims abstract description 39
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 38
- 239000001301 oxygen Substances 0.000 claims abstract description 38
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 38
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 26
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 24
- 238000005286 illumination Methods 0.000 claims abstract description 22
- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 claims abstract description 20
- 239000007789 gas Substances 0.000 claims abstract description 17
- 238000000034 method Methods 0.000 claims abstract description 15
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 13
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 10
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 12
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 claims description 10
- 239000011261 inert gas Substances 0.000 claims description 9
- UMGDCJDMYOKAJW-UHFFFAOYSA-N thiourea Chemical compound NC(N)=S UMGDCJDMYOKAJW-UHFFFAOYSA-N 0.000 claims description 8
- 229910052724 xenon Inorganic materials 0.000 claims description 7
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 claims description 7
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 6
- 239000007795 chemical reaction product Substances 0.000 claims description 6
- 239000011541 reaction mixture Substances 0.000 claims description 6
- 229920000877 Melamine resin Polymers 0.000 claims description 5
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 claims description 5
- XAEFZNCEHLXOMS-UHFFFAOYSA-M potassium benzoate Chemical compound [K+].[O-]C(=O)C1=CC=CC=C1 XAEFZNCEHLXOMS-UHFFFAOYSA-M 0.000 claims description 5
- ZNNZYHKDIALBAK-UHFFFAOYSA-M potassium thiocyanate Chemical group [K+].[S-]C#N ZNNZYHKDIALBAK-UHFFFAOYSA-M 0.000 claims description 5
- CKUAXEQHGKSLHN-UHFFFAOYSA-N [C].[N] Chemical compound [C].[N] CKUAXEQHGKSLHN-UHFFFAOYSA-N 0.000 claims description 4
- 239000004202 carbamide Substances 0.000 claims description 4
- QGBSISYHAICWAH-UHFFFAOYSA-N dicyandiamide Chemical compound NC(N)=NC#N QGBSISYHAICWAH-UHFFFAOYSA-N 0.000 claims description 4
- 230000005587 bubbling Effects 0.000 claims description 3
- 239000007788 liquid Substances 0.000 claims description 3
- 239000012467 final product Substances 0.000 claims description 2
- 238000010438 heat treatment Methods 0.000 claims description 2
- 238000002156 mixing Methods 0.000 claims description 2
- 239000000203 mixture Substances 0.000 claims description 2
- BDERNNFJNOPAEC-UHFFFAOYSA-N propan-1-ol Chemical compound CCCO BDERNNFJNOPAEC-UHFFFAOYSA-N 0.000 claims description 2
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical compound CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 claims 2
- 230000002194 synthesizing effect Effects 0.000 abstract description 5
- 238000006243 chemical reaction Methods 0.000 description 30
- 230000001699 photocatalysis Effects 0.000 description 20
- 239000012295 chemical reaction liquid Substances 0.000 description 7
- 238000005516 engineering process Methods 0.000 description 5
- 238000005259 measurement Methods 0.000 description 5
- 238000007146 photocatalysis Methods 0.000 description 5
- 239000010453 quartz Substances 0.000 description 5
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 5
- 230000001678 irradiating effect Effects 0.000 description 4
- 238000007789 sealing Methods 0.000 description 4
- 239000003054 catalyst Substances 0.000 description 3
- 239000000498 cooling water Substances 0.000 description 3
- 230000007613 environmental effect Effects 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- 238000000862 absorption spectrum Methods 0.000 description 2
- PYKYMHQGRFAEBM-UHFFFAOYSA-N anthraquinone Natural products CCC(=O)c1c(O)c2C(=O)C3C(C=CC=C3O)C(=O)c2cc1CC(=O)OC PYKYMHQGRFAEBM-UHFFFAOYSA-N 0.000 description 2
- 150000004056 anthraquinones Chemical class 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- VZGDMQKNWNREIO-UHFFFAOYSA-N tetrachloromethane Chemical compound ClC(Cl)(Cl)Cl VZGDMQKNWNREIO-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- WCUXLLCKKVVCTQ-UHFFFAOYSA-M Potassium chloride Chemical compound [Cl-].[K+] WCUXLLCKKVVCTQ-UHFFFAOYSA-M 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 230000002939 deleterious effect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000004134 energy conservation Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 230000031700 light absorption Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000004076 pulp bleaching Methods 0.000 description 1
- 238000001878 scanning electron micrograph Methods 0.000 description 1
- 238000004659 sterilization and disinfection Methods 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B15/00—Peroxides; Peroxyhydrates; Peroxyacids or salts thereof; Superoxides; Ozonides
- C01B15/01—Hydrogen peroxide
- C01B15/022—Preparation from organic compounds
- C01B15/026—Preparation from organic compounds from alcohols
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B15/00—Peroxides; Peroxyhydrates; Peroxyacids or salts thereof; Superoxides; Ozonides
- C01B15/01—Hydrogen peroxide
- C01B15/027—Preparation from water
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- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Catalysts (AREA)
Abstract
The invention discloses a preparation method of hydrogen peroxide, which comprises the steps of firstly adding water, alcohol and a photocatalyst into a container, wherein the weight ratio of the water to the alcohol to the photocatalyst is 200-500:10-50:0.3-1, wherein the photocatalyst is a K-doped marginal nitrogen vacancy carbon nitride photocatalyst; then oxygen-containing gas is introduced into the container under illumination, so that hydrogen peroxide can be generated; or the container is irradiated by light after being emptied of oxygen, and then oxygen-containing gas is introduced under the dark condition after the irradiation is finished, so that hydrogen peroxide can be generated. The method can be used for efficiently synthesizing hydrogen peroxide under the illumination condition and synthesizing hydrogen peroxide under the dark condition, and the whole process is simple in operation, energy-saving and environment-friendly.
Description
Technical Field
The invention relates to a preparation method of hydrogen peroxide, in particular to a method for preparing hydrogen peroxide under the condition of illumination or darkness by utilizing a photocatalyst.
Background
Hydrogen peroxide (H) 2 O 2 ) As a multifunctional environment-friendly oxidant and reducer, the catalyst has been widely applied to the fields of disinfection, pollutant degradation, pulp bleaching, organic synthesis and the like. H 2 O 2 The characteristics of easy storage, safe handling and transportation also enable H 2 O 2 Becomes H in the fuel cell 2 Is a promising alternative energy carrier. Currently, for H 2 O 2 The industrial anthraquinone process of preparation faces sustainability challenges such as high energy consumption, complex industrial routes, and deleterious byproducts. Photocatalytic production of H compared to the anthraquinone process 2 O 2 Has remarkable sustainability and environmental friendliness.
The solar energy is widely paid attention to as a representative green energy source because of no pollution, abundant reserves and the like, and the photocatalysis technology can effectively utilize the solar energy. The photocatalysis technology converts solar energy into chemical energy, thereby being beneficial to solving the energy and environmental problems, but the existing photocatalysis technology still has the defects of low catalysis efficiency, poor stability and the like, and particularly is difficult to play a role under dark and dark conditions. This defect greatly restricts the practical application of the photocatalysis technology. Therefore, how to synthesize hydrogen peroxide not only under light, but also under dark conditions is a new challenge to hydrogen peroxide preparation technology.
Disclosure of Invention
The invention aims to provide a preparation method of hydrogen peroxide, which can be used for efficiently synthesizing hydrogen peroxide under illumination conditions and synthesizing hydrogen peroxide under dark conditions, and has the advantages of simple operation, energy conservation and environmental protection.
In order to achieve the above purpose, the present invention adopts the following technical scheme:
a preparation method of hydrogen peroxide comprises the following steps:
step S1: adding water, alcohol and a photocatalyst into a container, wherein the weight ratio of the water to the alcohol to the photocatalyst is 200-500:10-50:0.3-1, wherein the photocatalyst is a K-doped marginal nitrogen vacancy carbon nitride photocatalyst;
step S2: introducing oxygen-containing gas into the container under illumination to generate hydrogen peroxide; or the container is irradiated by light after being emptied of oxygen, and then oxygen-containing gas is introduced under the dark condition after the irradiation is finished, so that hydrogen peroxide can be generated.
Preferably, in the step S2, the illumination is illumination by a solar simulator such as a xenon lamp or the like.
Preferably, the oxygen in the container is exhausted by introducing inert gas such as nitrogen or vacuumizing the container.
Preferably, in the step S1, a plurality of containers are provided, the water, the ethanol and the photocatalyst are added according to the weight ratio, in the step S2, the containers are irradiated with light after being emptied of oxygen, and after the irradiation is completed, oxygen-containing gas is sequentially introduced into the containers according to the sequence under the dark condition, and hydrogen peroxide is produced in the containers according to the sequence.
Preferably, in the step S2, the plurality of containers are irradiated with light for 0.5 to 4 hours after being emptied of oxygen, and the oxygen-containing gas is introduced into the plurality of containers at regular intervals, such as 1 to 4 hours, in sequence under a dark condition after the irradiation is completed.
Preferably, in the step S1, the K-doped marginal nitrogen-vacancy carbon nitride photocatalyst is prepared by:
step S11: mixing a carbon-nitrogen source, potassium salt and LiCl according to a weight ratio of 1:1-2:1-2 to obtain a reaction mixture, wherein the carbon-nitrogen source is one or more of melamine, urea, thiourea and dicyandiamide;
step S12: the reaction mixture is reacted under inert gas and CCl 4 Heating the mixture of gases to 450-600 ℃ to react to obtain a reaction product;
step S13: and (3) carrying out post-treatment on the reaction product to obtain the K-doped marginal nitrogen vacancy carbon nitride photocatalyst.
Further, in the step S11, the potassium salt is KSCN, KCl, KNO 3 One or more of the following.
Further, in the step S12, the inert gas sum CCl 4 The mixed gas is obtained by passing inert gas such as nitrogen through liquid CCl 4 Bubbling to obtain the final product.
According to the technical scheme, the K-doped marginal nitrogen vacancy carbon nitride photocatalyst is utilized to realize that oxygen, water and alcohol are used for preparing hydrogen peroxide, the reaction can be directly carried out under the illumination condition, or can be carried out under the dark condition after being irradiated by light in advance when no oxygen exists, so that conditions are created for succinctly synthesizing hydrogen peroxide at night or under other dark conditions, the preparation of hydrogen peroxide can be realized under other dark conditions after the reaction system is irradiated by oxygen in daytime or under the light condition, and a wider application range is provided for preparing hydrogen peroxide by photocatalysis. The carbon nitride photocatalyst adopted by the method is prepared by calcining melamine, urea, thiourea, dicyandiamide and other carbon and nitrogen sources, potassium salt and LiCl at high temperature in the atmosphere of inert gas and carbon tetrachloride gas, has a carbon nitride structure of K-doped marginal nitrogen vacancy, is easier to generate photo-generated electrons-holes and smoothly realize transfer, has good photocatalytic performance, can generate and store high-energy electrons under illumination to be used in darkness, and provides guarantee for preparing hydrogen peroxide under darkness.
Drawings
FIG. 1 is a graph showing the performance of hydrogen peroxide preparation in example 1 of the present invention;
FIG. 2 is a graph showing the performance of the hydrogen peroxide preparation in example 4 of the present invention;
FIG. 3 is a graph showing the performance of the hydrogen peroxide preparation according to examples 5-7 of the present invention;
FIG. 4 is a color chart of the reaction system in example 4 of the present invention;
FIG. 5 is a graph showing the ultraviolet absorption spectrum of the reaction system in example 4 of the present invention;
FIG. 6 is an SEM image of the photocatalyst used in the present invention.
Detailed Description
The invention is further described below with reference to the accompanying drawings:
example 1 preparation of Hydrogen peroxide under illumination example 1
Step S1: 50 mg of K-doped marginal nitrogen-vacancy carbon nitride photocatalyst is reacted with 45g of H 2 O and 5g ethanol are added into the photocatalytic reactor after being uniformly mixed.
Step S2: introducing oxygen into the reaction system through a hose, wherein the flow rate of the oxygen is 100 sccm, and the cooling water is turned on to control the temperature of the reactor to 15 ℃, using a 300W xenon lamp as a light source, irradiating the photoreactor, generating hydrogen peroxide, taking 1.5 mL reaction liquid every 15 min, measuring, and measuring H 2 O 2 As shown in FIG. 1, the solubility of the catalyst is high, and the catalyst used in the reaction system has high photocatalytic activity and can smoothly generate hydrogen peroxide.
Example 2 preparation of Hydrogen peroxide under illumination example 2
Step S1: 50 mg K-doped marginal nitrogen-vacancy carbon nitride photocatalyst with 33 gH 2 O and 1.6. 1.6 g methanol are added into a photocatalytic reactor after being uniformly mixed.
Step S2: introducing oxygen into the reaction system through a hose, wherein the flow rate of the oxygen is 200 sccm, and the cooling water is turned on to control the temperature of the reactor at 18 ℃, irradiating the reactor with 400W xenon lamp as a light source, generating hydrogen peroxide, taking 1.5 mL reaction liquid every 15 min, measuring, and measuring H 2 O 2 Solubility, similar to example 1.
Example 3 preparation of Hydrogen peroxide under illumination example 3
Step S1: will be 50mg K doped marginal nitrogen vacancy carbon nitride photocatalyst and 25g H 2 O and 2.5 g propanol are added into the photocatalytic reactor after being uniformly mixed.
Step S2: introducing oxygen into the reaction system through a hose, wherein the flow rate of the oxygen is 150 sccm, and the cooling water is turned on to control the temperature of the reactor to 20 ℃, irradiating the photoreactor by using a 200W xenon lamp (or sunlight) as a light source, generating hydrogen peroxide, taking 1.5 mL reaction liquid every 15 min, measuring, and measuring H 2 O 2 Solubility, similar to example 1.
Example 4 preparation of Hydrogen peroxide under dark conditions example 1
Step S1: 50 mg K-doped marginal nitrogen-vacancy carbon nitride photocatalyst with 45g H 2 O and 4 g ethanol are added into the photocatalytic reactor after being uniformly mixed.
Step S2: introducing N into the photocatalytic reactor 2 After the air is discharged, a sealing cover is covered, then the reaction system 2H is irradiated under the sunlight, then the reaction system is directly put into a dark environment and is filled with 30mL oxygen for reaction, hydrogen peroxide is produced, 1.5 mL reaction liquid is taken per minute for measurement, and H is measured 2 O 2 The concentration is shown in FIG. 2, and it can be seen from FIG. 2 that the photocatalyst used in the reaction system has photocatalytic activity under dark condition after illumination, and can generate hydrogen peroxide.
Example 5 preparation of Hydrogen peroxide under dark conditions example 2
Step S1: 50 mg of K-doped marginal nitrogen-vacancy carbon nitride photocatalyst is reacted with 40 g of H 2 O and 4 g ethanol are added into the photocatalytic reactor after being uniformly mixed.
Step S2: introducing argon into the photocatalytic reactor to remove air, covering a sealing cover, irradiating the reaction system 3H under sunlight, placing the reaction system in a dark environment after illumination for 4 hours, and then charging 20 mL oxygen into the reaction system for reaction, wherein hydrogen peroxide is produced, 1.5 mL reaction liquid is taken every minute for measurement, and H is measured 2 O 2 Concentration.
Example 6 preparation of Hydrogen peroxide under dark conditions example 3
Step S1: 50 mg K-doped marginal nitrogen-vacancy carbon nitride photocatalyst with 25g H 2 O and 2.5 g ethanol are added into the photocatalytic reactor after being uniformly mixed.
Step S2: introducing N into the photocatalytic reactor 2 After the air is discharged, a sealing cover is covered, then the reaction system is irradiated under a 200W xenon lamp for 4H, after the irradiation, the reaction system is put into a dark environment for 8 hours, then 40 mL oxygen is filled into the reaction system for reaction, the hydrogen peroxide is produced, 1.5 mL reaction liquid is taken every minute for measurement, and H is measured 2 O 2 Concentration.
Example 7 preparation of Hydrogen peroxide under dark conditions example 4
Step S1: 50 mg of K-doped marginal nitrogen-vacancy carbon nitride photocatalyst is reacted with 25g of H 2 O and 2.5 g ethanol are added into the photocatalytic reactor after being uniformly mixed.
Step S2: introducing N into the photocatalytic reactor 2 After the air is discharged, a sealing cover is covered, then the reaction system is irradiated under a 200W xenon lamp for 4H, after the irradiation, the reaction system is put into a dark environment for 12 hours, 30mL of oxygen is filled into the reaction system for reaction, hydrogen peroxide is produced, 1.5 mL reaction liquid is taken every minute for measurement, and H is measured 2 O 2 Concentration.
The results of the measurements of examples 5-7 are shown in FIG. 3, which shows the concentration of hydrogen peroxide produced in the dark, and the shorter the waiting time in the dark after illumination, the higher the activity of the photocatalyst in producing oxygen, compared with example 4.
FIG. 4 shows the color change of the reaction system in example 4, wherein FIG. A shows yellow color before illumination, FIG. B shows green color after illumination after oxygen removal, and FIG. C shows yellow color after oxygen introduction under dark conditions. Fig. 4 illustrates that the photocatalyst generates high-energy electrons after illumination, and can catalyze a reaction system to rapidly generate hydrogen peroxide.
FIG. 5 is a graph showing the ultraviolet absorption spectrum of the reaction system of example 4 before irradiation, 1min and 2min after removal of oxygen irradiation and 10s after addition of oxygen under dark conditions, and it can be seen from FIG. 6 that the reaction system after irradiation has absorbed light (actually, absorption after generation of high-energy electrons by the photocatalyst) in the wavelength range of 400-1200nm compared with the original sample, and the reaction system after addition of oxygen no longer has light absorption performance in the corresponding region (the high-energy electrons of the photocatalyst disappear due to the reaction).
Example 8 preparation of marginal nitrogen vacancy doped carbon nitride photocatalyst
The doped marginal nitrogen-vacancy carbon nitride photocatalysts used in examples 1-6 above were prepared by the following method:
step S11: after 10 mmol of melamine, 10 mmol of KSCN and 15 mmol of LiCl were ground and mixed uniformly, a reaction mixture was obtained, and the reaction mixture was placed in a quartz boat, and then the quartz boat was placed in a quartz tube.
Step S12: the quartz tube was placed in a tube furnace and then heated at 50 sccm N 2 /CCl 4 （N 2 From liquid CCl by bubbling machine 4 Inner bulge thus bringing out CCl 4 Gas) was heated at 520 c for 10, 10 h to obtain a reaction product.
Step S13: and grinding reaction products in the quartz boat into powder, and washing unreacted KSCN and LiCl by using deionized water to obtain the K-doped and nitrogen vacancy carbon nitride photocatalyst.
By urea, thiourea, dicyandiamide, KCl and KNO 3 A photocatalyst with similar properties can be obtained by replacing melamine and KSCN correspondingly.
An SEM picture of the photocatalyst obtained in example 8 is shown in fig. 6.
The present embodiments are merely illustrative of the present invention and are not intended to be limiting, and the technical solutions that are not substantially transformed under the present invention are still within the scope of protection.
Claims (9)
1. The preparation method of the hydrogen peroxide is characterized by comprising the following steps:
step S1: adding water, alcohol and a photocatalyst into a container, wherein the weight ratio of the water to the alcohol to the photocatalyst is 200-500:10-50:0.3-1, wherein the photocatalyst is a K-doped marginal nitrogen vacancy carbon nitride photocatalyst;
step S2: introducing oxygen-containing gas into the container under illumination to generate hydrogen peroxide; or the container is irradiated by light after being emptied of oxygen, and oxygen-containing gas is introduced under the dark condition after the irradiation is finished, so that hydrogen peroxide can be generated;
in the step S1, the K-doped marginal nitrogen-vacancy carbon nitride photocatalyst is prepared by:
step S11: mixing a carbon-nitrogen source, potassium salt and LiCl according to a weight ratio of 1:1-2:1-2 to obtain a reaction mixture, wherein the carbon-nitrogen source is one or more of melamine, urea, thiourea and dicyandiamide;
step S12: the reaction mixture is reacted under inert gas and CCl 4 Heating the mixture of gases to 450-600 ℃ to react to obtain a reaction product;
step S13: and (3) carrying out post-treatment on the reaction product to obtain the K-doped marginal nitrogen vacancy carbon nitride photocatalyst.
2. The method according to claim 1, wherein in the step S2, the illumination is solar light illumination or solar simulated light source illumination.
3. The method according to claim 1, wherein in the step S2, oxygen in the container is exhausted by introducing an inert gas into the container or evacuating the container.
4. The method for preparing hydrogen peroxide according to claim 1, wherein in the step S1, a plurality of containers are provided and the water, ethanol and photocatalyst are added according to the weight ratio, in the step S2, the containers are irradiated with light after being emptied of oxygen, and after the irradiation is completed, oxygen-containing gas is sequentially introduced into the containers in sequence under dark conditions, and the hydrogen peroxide is produced in the containers in the sequence.
5. The method for preparing hydrogen peroxide according to claim 4, wherein in the step S2, the plurality of containers are irradiated with light for 0.5 to 4 hours after being emptied of oxygen, and the plurality of containers are sequentially introduced with oxygen-containing gas at intervals of 1 to 4 hours in sequence under a dark condition after the irradiation is completed.
6. The method according to claim 1, wherein in the step S11, the potassium salt is KSCN, KCl, KNO 3 One or more of the following.
7. The method according to claim 6, wherein in the step S12, the inert gas and CCl are mixed with each other 4 The mixed gas of the gases is obtained by passing inert gas through liquid CCl 4 Bubbling to obtain the final product.
8. The method according to claim 1, wherein in the step S1, the alcohol is ethanol, methanol, propanol or butanol.
9. The method for preparing hydrogen peroxide according to claim 2, wherein the solar simulated light source is a xenon lamp.
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| CN113401876A (en) * | 2021-07-05 | 2021-09-17 | 中山大学 | Method for producing hydrogen peroxide through photocatalysis without sacrificial agent |
| CN113426470A (en) * | 2021-07-02 | 2021-09-24 | 中国科学技术大学 | Potassium, chlorine and iodine co-doped carbon nitride, preparation method thereof and method for preparing hydrogen peroxide through photocatalysis |
| CN115007182A (en) * | 2022-04-20 | 2022-09-06 | 东南大学 | Preparation method of potassium-oxygen co-doped graphite-phase carbon nitride photocatalyst |
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- 2022-09-23 CN CN202211161503.8A patent/CN115340071B/en active Active
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109607499A (en) * | 2018-12-17 | 2019-04-12 | 山东大学 | A kind of limit nitrogen vacancy g-C3N4Photochemical catalyst and preparation method thereof |
| CN111992236A (en) * | 2020-09-01 | 2020-11-27 | 福州大学 | Carbon nitrogen catalyst prepared by molten salt thermal polymerization method and having function of photocatalytic oxidation of hydrogen sulfide gas, and preparation method and application thereof |
| CN113426470A (en) * | 2021-07-02 | 2021-09-24 | 中国科学技术大学 | Potassium, chlorine and iodine co-doped carbon nitride, preparation method thereof and method for preparing hydrogen peroxide through photocatalysis |
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