CN113600169A - Solid solution photocatalyst for photocatalytic oxidation degradation of toluene and preparation method thereof - Google Patents
Solid solution photocatalyst for photocatalytic oxidation degradation of toluene and preparation method thereof Download PDFInfo
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- CN113600169A CN113600169A CN202110638510.1A CN202110638510A CN113600169A CN 113600169 A CN113600169 A CN 113600169A CN 202110638510 A CN202110638510 A CN 202110638510A CN 113600169 A CN113600169 A CN 113600169A
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- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 title claims abstract description 85
- 239000011941 photocatalyst Substances 0.000 title claims abstract description 37
- 239000006104 solid solution Substances 0.000 title claims abstract description 35
- 230000001699 photocatalysis Effects 0.000 title claims abstract description 22
- 230000003647 oxidation Effects 0.000 title claims abstract description 11
- 238000007254 oxidation reaction Methods 0.000 title claims abstract description 11
- 238000002360 preparation method Methods 0.000 title abstract description 10
- 230000015556 catabolic process Effects 0.000 title abstract description 5
- 238000006731 degradation reaction Methods 0.000 title abstract description 5
- 229910010252 TiO3 Inorganic materials 0.000 claims abstract description 21
- 239000000243 solution Substances 0.000 claims abstract description 16
- 150000001875 compounds Chemical class 0.000 claims abstract description 15
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 12
- 230000000593 degrading effect Effects 0.000 claims abstract description 7
- 238000003756 stirring Methods 0.000 claims abstract description 7
- 238000001027 hydrothermal synthesis Methods 0.000 claims abstract description 5
- 239000000203 mixture Substances 0.000 claims abstract description 5
- 239000000376 reactant Substances 0.000 claims abstract description 5
- 238000001035 drying Methods 0.000 claims abstract description 4
- 238000005406 washing Methods 0.000 claims abstract description 4
- 239000003513 alkali Substances 0.000 claims abstract description 3
- 239000007864 aqueous solution Substances 0.000 claims abstract description 3
- 239000011259 mixed solution Substances 0.000 claims abstract description 3
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 13
- 238000000034 method Methods 0.000 claims description 10
- 239000003054 catalyst Substances 0.000 claims description 7
- 238000004519 manufacturing process Methods 0.000 claims description 4
- 229910003074 TiCl4 Inorganic materials 0.000 claims description 2
- 229910001626 barium chloride Inorganic materials 0.000 claims description 2
- 239000012153 distilled water Substances 0.000 claims description 2
- 229910001631 strontium chloride Inorganic materials 0.000 claims description 2
- 238000010525 oxidative degradation reaction Methods 0.000 claims 5
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 claims 2
- 230000000694 effects Effects 0.000 abstract description 6
- 238000007146 photocatalysis Methods 0.000 abstract description 4
- 230000001089 mineralizing effect Effects 0.000 abstract description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 6
- 238000013033 photocatalytic degradation reaction Methods 0.000 description 5
- 239000012855 volatile organic compound Substances 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 4
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 239000001569 carbon dioxide Substances 0.000 description 3
- 229910002092 carbon dioxide Inorganic materials 0.000 description 3
- 230000036541 health Effects 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 239000000178 monomer Substances 0.000 description 2
- 239000002957 persistent organic pollutant Substances 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- VEALVRVVWBQVSL-UHFFFAOYSA-N strontium titanate Chemical compound [Sr+2].[O-][Ti]([O-])=O VEALVRVVWBQVSL-UHFFFAOYSA-N 0.000 description 2
- 206010007269 Carcinogenicity Diseases 0.000 description 1
- 229910002370 SrTiO3 Inorganic materials 0.000 description 1
- 238000003917 TEM image Methods 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 230000033558 biomineral tissue development Effects 0.000 description 1
- 230000007670 carcinogenicity Effects 0.000 description 1
- 231100000260 carcinogenicity Toxicity 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 238000005119 centrifugation Methods 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
- 230000005494 condensation Effects 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 239000010779 crude oil Substances 0.000 description 1
- 230000009849 deactivation Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 231100000086 high toxicity Toxicity 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- 238000009776 industrial production Methods 0.000 description 1
- 231100000053 low toxicity Toxicity 0.000 description 1
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
- 229910052753 mercury Inorganic materials 0.000 description 1
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- -1 polytetrafluoroethylene Polymers 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 230000036632 reaction speed Effects 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- 238000000985 reflectance spectrum Methods 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
Images
Classifications
-
- B01J35/39—
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/72—Organic compounds not provided for in groups B01D53/48 - B01D53/70, e.g. hydrocarbons
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/864—Removing carbon monoxide or hydrocarbons
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/02—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the alkali- or alkaline earth metals or beryllium
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
- B01D2257/708—Volatile organic compounds V.O.C.'s
Abstract
The application discloses a preparation method of a solid solution photocatalyst for photocatalytic oxidation degradation of toluene, which comprises the following steps: (1) dissolving a compound containing Sr element and a compound containing Ba element in water under the condition of stirring, dropwise adding an organic solution containing a compound containing Ti element into the aqueous solution, and obtaining a mixed solution after dropwise adding; (2) adjusting the pH of the system by using alkali; (3) stirring the mixture, and carrying out hydrothermal reaction at a certain temperature for a period of time; (4) washing and drying the reactant to obtain Sr1‑xBaxTiO3A solid solution photocatalyst. The preparation method is simple and easy to implement, and the prepared photocatalyst has higher activity of degrading toluene through photocatalysis and can be used for stably mineralizing toluene into CO2And can be used for removing toluene in the atmosphere.
Description
Technical Field
The invention relates to a catalyst, in particular to a solid solution catalyst for photocatalytic oxidation degradation of atmospheric pollutants, and especially relates to Sr for photocatalytic oxidation degradation of toluene1-xBaxTiO3Solid solution photocatalyst and a preparation method thereof.
Background
Volatile Organic Compounds (VOCs) are one of the main causes of the greenhouse effect, are mainly discharged by vehicle emissions in industrial production of chemical industry, coating, petroleum and the like and transportation, and pose great threat to human health. Various methods such as adsorption, condensation, biological treatment, and catalysis have been applied to the treatment of volatile organic compounds. Among them, photocatalysis is a very economical and efficient method for mineralizing VOCs contaminants into carbon dioxide under mild conditions. The photocatalysis technology is a new process for treating organic pollutants difficult to degrade developed in the later stage of the 20 th century, and is characterized in that hydroxyl free radicals (OH) with extremely strong activity are generated under the action of a semiconductor catalyst, and the OH can oxidize and degrade the organic pollutants difficult to degrade in the air into small molecular substances without toxicity or low toxicity, and even directly mineralize the small molecular substances into carbon dioxide and water to achieve the aim of harmlessness. The technology has the advantages of no selectivity, strong oxidation capability, high reaction speed, high treatment efficiency, no secondary pollution and the like. Toluene is a common, typical volatile organic compound, mainly produced during crude oil processing, and is difficult to naturally degrade in the environment. Toluene molecules have high toxicity and carcinogenicity, seriously affect the atmospheric environment and threaten the health of people. The photocatalytic degradation of toluene has received much attention, but in the reports, the low mineralization rate of the photocatalytic degradation of toluene and the easy deactivation of the catalyst are common problems, so the development and preparation of the photocatalyst capable of efficiently and stably degrading toluene is the focus of the current research.
Strontium titanate has enough band gap and proper valence conduction band position, and has certain activity in photocatalytic degradation of toluene. The monomer has high electron-hole recombination efficiency, so that the photocatalytic performance is adversely affected, and the practical application of the monomer in photocatalysis is severely restricted. Therefore, it is one of the important issues in the field of photocatalytic research to make a strontium titanate-based photocatalyst have sufficient photocatalytic performance by modification.
Disclosure of Invention
The invention aims to provide Sr aiming at the defects of the prior art1-xBaxTiO3The solid solution photocatalyst has better performance of oxidizing and degrading toluene, the preparation method of the catalyst simplifies the production process, and the prepared Sr simplifies the production process1-xBaxTiO3The solid solution can stabilize the toluene in the air removed by photocatalytic oxidation.
In order to achieve the purpose, the technical scheme of the invention is as follows:
a solid solution photocatalyst for degrading toluene through photocatalytic oxidation is characterized in that the molar ratio of Sr element to Ba element in the catalyst is Sr: ba ═ 1-x: x (x is less than or equal to 0.2) Sr1-xBaxTiO3A solid solution photocatalyst.
Further, the molar ratio of the Sr element to the Ba element is 2: 1. 5: 1 or 8: 1, preferably 5: 1, the total amount of Sr element and Ba element is 12 mmol.
The invention also provides a preparation method of the solid solution photocatalyst for degrading toluene through photocatalytic oxidation, which comprises the following steps:
(1) dissolving a compound containing Sr element and a compound containing Ba element in water under the condition of stirring, dropwise adding an organic solution containing a compound containing Ti element into the aqueous solution, and obtaining a mixed solution after dropwise adding;
(2) adjusting the pH of the system by using alkali;
(3) stirring the mixture, and carrying out hydrothermal reaction at a certain temperature for a period of time;
(4) washing and drying the reactant to obtain Sr1-xBaxTiO3A solid solution photocatalyst.
Further, the compound of Sr element in the step (1) is selected from Sr (NO)3)3And SrCl2Preferably Sr (NO)3)3(ii) a The compound of Ba element is selected from Ba (CH)3COO)2And BaCl2Any one of them, preferably Ba (CH)3COO)2(ii) a The compound of Ti element is selected from C16H36O4Ti and TiCl4Any one of (1), preferably C16H36O4Ti。
Further, the water in step (1) is distilled water, and the amount of water is 15 to 20mL, for example, 15mL, 16mL, 17mL, 18mL, 19mL, 20mL, preferably 20 mL.
Further, the organic solution in step (1) is ethylene glycol solution, and the amount of the ethylene glycol solution is 15-20mL, such as 15mL, 16mL, 17mL, 18mL, 19mL, 20mL, preferably 20 mL.
Further, in step (2) the pH is 9-12, such as 9, 10, 11, 12, preferably 12.
Further, after the mixture is stirred in the step (3), performing hydrothermal reaction at the temperature of 160-180 ℃ for 12-48h, for example, the temperature is 160, 180, 200 ℃, preferably 200 ℃; for example, the reaction time is 12, 24, 48h, preferably 48 h.
Further, in the step (4), the reaction product is washed and then dried at a temperature of 60 to 80 ℃ such as 60 ℃, 65 ℃, 70 ℃, 75 ℃, 80 ℃, preferably 60 ℃.
Further, the reaction is washed and dried at a temperature of 60-80 ℃ for 3-24h, for example, for 3h, 6h, 9h, 12h, 24h, preferably 12 h.
Compared with the prior art, the invention has the following beneficial effects:
(1) the invention optimizes the preparation process of the photocatalyst and achieves the aim of simplifying the production flow;
(2) the photocatalyst has a solid solution structure, so that the photocatalytic activity is improved;
(3) sr of the invention1-xBaxTiO3Solid solution, for gaseous toluene with initial concentration of 45ppm, the removal rate reaches 74% within 60 min;
(4) the invention adopts nontoxic and harmless components, and reduces the harm to human health and ecological environment.
Drawings
FIG. 1 shows Sr of the present invention1-xBaxTiO3A transmission electron micrograph of a solid solution photocatalyst;
FIG. 2 shows Sr of the present invention1-xBaxTiO3An X-ray diffraction pattern of a solid solution photocatalyst;
FIG. 3 shows Sr of the present invention1-xBaxTiO3An ultraviolet-visible diffuse reflectance pattern of a solid solution photocatalyst;
FIG. 4 shows Sr of the present invention1-xBaxTiO3Performance diagram of solid solution photocatalyst for degrading toluene.
Detailed Description
To better illustrate the invention and to facilitate the understanding of the technical solutions thereof, typical but non-limiting examples of the invention are as follows:
example 1
Preparation of Sr1-xBaxTiO3Solid solution photocatalyst
2.1633g Sr (NO) are weighed out by an analytical balance3)3、0.5108g Ba(CH3COO)2Dissolving in 20mL deionized water to obtain solution A, and measuring 8.509mL C16H36O4Dissolving Ti in ethylene glycol to obtain a solution B, dropwise adding the solution B into the solution A, adjusting the pH of the system to 12 by using 2.5mM NaOH, stirring for 30min, transferring the reaction solution to a 70mL stainless steel reaction kettle with a polytetrafluoroethylene lining, and heating to 200 ℃ in an oven for 48 h. After the reaction is finished, the Sr is obtained by centrifugation, water washing and drying for 24h at the temperature of 60 DEG C1-xBaxTiO3A solid solution photocatalyst.
FIG. 1 is a photograph taken by transmission electron microscope of a solid solution photocatalyst prepared in this example, and it can be seen from the photograph that Sr was prepared1-xBaxTiO3The solid solution photocatalyst is spherical and has good dispersibility.
FIG. 2 shows the solid prepared in this exampleThe X-ray diffraction pattern of the solution photocatalyst shows that Sr is successfully prepared1-xBaxTiO3A solid solution photocatalyst.
FIG. 3 is a graph of the UV-visible diffuse reflectance spectrum of the solid solution photocatalyst prepared in this example, from which Sr can be seen1-xBaxTiO3Compared with SrTiO3There was little change.
Example 2
Sr1-xBaxTiO3Photocatalytic degradation activity of solid solution photocatalyst on toluene
Sr prepared in example 1 was used as a light source in a 300W mercury lamp1-xBaxTiO3The solid solution photocatalyst is uniformly coated on a glass sheet, the initial concentration of toluene is controlled to be 50ppm, and the concentrations of the toluene and carbon dioxide after catalytic oxidation are measured by a light spectrometer. Sr1-xBaxTiO3The photocatalytic degradation activity of solid solution photocatalyst on toluene is shown in fig. 4.
Claims (10)
1. A solid solution photocatalyst for degrading toluene through photocatalytic oxidation is characterized in that the catalyst is prepared by mixing Sr: ba ═ 1-x: x (x is less than or equal to 0.2) Sr1-xBaxTiO3A solid solution photocatalyst.
2. The solid solution photocatalyst for photocatalytic oxidative degradation of toluene as claimed in claim 1, wherein the molar ratio of Sr element and Ba element is 2: 1. 5: 1 or 8: 1, the total amount of Sr element and Ba element is 12 mmol.
3. The method of preparing a solid solution photocatalyst for photocatalytic oxidative degradation of toluene according to claim 1 or 2, comprising the steps of:
(1) dissolving a compound containing Sr element and a compound containing Ba element in water under the condition of stirring, dropwise adding an organic solution containing a compound containing Ti element into the aqueous solution, and obtaining a mixed solution after dropwise adding;
(2) adjusting the pH of the system by using alkali;
(3) stirring the mixture, and carrying out hydrothermal reaction at a certain temperature for a period of time;
(4) washing and drying the reactant to obtain Sr1-xBaxTiO3A solid solution photocatalyst.
4. The method for producing a solid solution photocatalyst for photocatalytic oxidative degradation of toluene as claimed in claim 3, wherein said Sr compound in the step (1) is selected from Sr (NO)3)3And SrCl2Any one of the above; the compound of Ba element is selected from Ba (CH)3COO)2And BaCl2Any one of the above; the compound of Ti element is selected from C16H36O4Ti and TiCl4Any one of them.
5. The method of claim 3, wherein the water used in step (1) is distilled water, and the amount of water is 15-20 mL.
6. The method of claim 3, wherein the organic solution in step (1) is a glycol solution, and the amount of glycol solution is 15-20 mL.
7. The method of preparing a solid solution photocatalyst for photocatalytic oxidative degradation of toluene as claimed in claim 3, wherein said pH in the step (2) is 9 to 12.
8. The method as claimed in claim 3, wherein the mixture is stirred in step (3) and then undergoes hydrothermal reaction at 160-180 ℃ for 12-48 h.
9. The method for preparing a solid solution photocatalyst for photocatalytic oxidative degradation of toluene as claimed in claim 3, wherein in the step (4), the reactants are washed and then dried at a temperature of 60 to 80 ℃.
10. The method of claim 9 wherein the reactants are washed and dried at a temperature of 60-80 ℃ for 3-24 hours.
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| Application Number | Priority Date | Filing Date | Title |
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| CN202110638510.1A CN113600169A (en) | 2021-06-08 | 2021-06-08 | Solid solution photocatalyst for photocatalytic oxidation degradation of toluene and preparation method thereof |
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| CN202110638510.1A CN113600169A (en) | 2021-06-08 | 2021-06-08 | Solid solution photocatalyst for photocatalytic oxidation degradation of toluene and preparation method thereof |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115888676A (en) * | 2022-09-28 | 2023-04-04 | 电子科技大学长三角研究院(湖州) | Composition for inhibiting decomposition of nitrate and preparation method thereof |
| CN115888676B (en) * | 2022-09-28 | 2024-05-14 | 电子科技大学长三角研究院(湖州) | Composition for inhibiting nitrate decomposition and preparation method thereof |
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