CN114700103B - Immobilization preparation method of metal-free carbon-based catalyst, product and application of product - Google Patents
Immobilization preparation method of metal-free carbon-based catalyst, product and application of product Download PDFInfo
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- CN114700103B CN114700103B CN202210378344.0A CN202210378344A CN114700103B CN 114700103 B CN114700103 B CN 114700103B CN 202210378344 A CN202210378344 A CN 202210378344A CN 114700103 B CN114700103 B CN 114700103B
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 45
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 45
- 239000003054 catalyst Substances 0.000 title claims abstract description 40
- 238000002360 preparation method Methods 0.000 title claims description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 60
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 53
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims abstract description 51
- 239000006004 Quartz sand Substances 0.000 claims abstract description 46
- 239000007787 solid Substances 0.000 claims abstract description 34
- 238000000034 method Methods 0.000 claims abstract description 26
- VYFYYTLLBUKUHU-UHFFFAOYSA-N dopamine Chemical compound NCCC1=CC=C(O)C(O)=C1 VYFYYTLLBUKUHU-UHFFFAOYSA-N 0.000 claims abstract description 24
- CIWBSHSKHKDKBQ-JLAZNSOCSA-N Ascorbic acid Chemical compound OC[C@H](O)[C@H]1OC(=O)C(O)=C1O CIWBSHSKHKDKBQ-JLAZNSOCSA-N 0.000 claims abstract description 22
- 239000008367 deionised water Substances 0.000 claims abstract description 19
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 19
- 229960003638 dopamine Drugs 0.000 claims abstract description 12
- 229960005070 ascorbic acid Drugs 0.000 claims abstract description 11
- 235000010323 ascorbic acid Nutrition 0.000 claims abstract description 11
- 239000011668 ascorbic acid Substances 0.000 claims abstract description 11
- QGBSISYHAICWAH-UHFFFAOYSA-N dicyandiamide Chemical compound NC(N)=NC#N QGBSISYHAICWAH-UHFFFAOYSA-N 0.000 claims abstract description 11
- 238000001035 drying Methods 0.000 claims abstract description 11
- 239000000203 mixture Substances 0.000 claims abstract description 10
- 239000008055 phosphate buffer solution Substances 0.000 claims abstract description 9
- 238000003756 stirring Methods 0.000 claims abstract description 9
- 239000011259 mixed solution Substances 0.000 claims abstract description 8
- 238000001914 filtration Methods 0.000 claims abstract description 6
- 238000011010 flushing procedure Methods 0.000 claims abstract description 6
- 239000007788 liquid Substances 0.000 claims abstract description 6
- 238000001354 calcination Methods 0.000 claims description 6
- 239000000356 contaminant Substances 0.000 claims description 6
- 230000000593 degrading effect Effects 0.000 claims description 3
- 239000002184 metal Substances 0.000 abstract description 12
- 239000002957 persistent organic pollutant Substances 0.000 abstract description 8
- 230000007774 longterm Effects 0.000 abstract description 4
- 230000008569 process Effects 0.000 abstract description 4
- 238000001723 curing Methods 0.000 abstract description 3
- 238000009776 industrial production Methods 0.000 abstract description 2
- FHHJDRFHHWUPDG-UHFFFAOYSA-L peroxysulfate(2-) Chemical compound [O-]OS([O-])(=O)=O FHHJDRFHHWUPDG-UHFFFAOYSA-L 0.000 description 14
- 239000002351 wastewater Substances 0.000 description 9
- 239000000243 solution Substances 0.000 description 7
- 238000005406 washing Methods 0.000 description 6
- CQPFMGBJSMSXLP-ZAGWXBKKSA-M Acid orange 7 Chemical compound OC1=C(C2=CC=CC=C2C=C1)/N=N/C1=CC=C(C=C1)S(=O)(=O)[O-].[Na+] CQPFMGBJSMSXLP-ZAGWXBKKSA-M 0.000 description 5
- 230000000694 effects Effects 0.000 description 5
- 230000003213 activating effect Effects 0.000 description 4
- 239000003575 carbonaceous material Substances 0.000 description 4
- 239000003622 immobilized catalyst Substances 0.000 description 4
- 230000004913 activation Effects 0.000 description 3
- 230000015556 catabolic process Effects 0.000 description 3
- 238000006731 degradation reaction Methods 0.000 description 3
- 238000005303 weighing Methods 0.000 description 3
- 239000007853 buffer solution Substances 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 238000001704 evaporation Methods 0.000 description 2
- 238000011049 filling Methods 0.000 description 2
- 239000002638 heterogeneous catalyst Substances 0.000 description 2
- 239000008363 phosphate buffer Substances 0.000 description 2
- 239000010865 sewage Substances 0.000 description 2
- 208000033830 Hot Flashes Diseases 0.000 description 1
- 206010060800 Hot flush Diseases 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 230000003100 immobilizing effect Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012544 monitoring process Methods 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000004576 sand Substances 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 238000004065 wastewater treatment Methods 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
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/40—Organic compounds containing sulfur
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
Abstract
The invention discloses a method for preparing an immobilization catalyst without metal carbon, a product and application thereof, wherein the method comprises the following steps: (1) Dissolving dicyandiamide and ascorbic acid in methanol, placing the mixture in an oven until the methanol is completely volatilized, and then roasting to obtain a metal-free carbon-based catalyst; (2) Adding dopamine, a metal-free carbon-based catalyst and quartz sand into a phosphate buffer solution, and stirring in a water bath to obtain a first mixed solution; (3) Filtering the first mixed solution, removing the liquid part to obtain semi-solidified quartz sand and suspended solids, flushing the semi-solidified quartz sand and suspended solids with deionized water for a plurality of times, and drying the semi-solidified quartz sand and suspended solids to obtain first solids; (4) And (3) placing the first solid in a muffle furnace for roasting to obtain the metal-free carbon-based catalyst-supported quartz sand. The catalyst prepared by the invention has long-term stability in the process of removing organic pollutants, the curing condition is easy to achieve, the method is simple, the equipment requirement is low, the industrial production is easy, the price is low, and the wide popularization and application are convenient.
Description
Technical Field
The invention relates to the field of water treatment, in particular to a method for preparing an immobilization catalyst without a metal carbon base, a product and application thereof.
Background
Catalytic activation of Peroxymonosulfate (PMS) to degrade organic pollutants in sewage and wastewater is an emerging advanced oxidation technology, and causes research hot flashes at home and abroad. It is known that the metal-based catalyst has excellent effect of activating PMS, but this increases the preparation cost of the catalyst, and in the process of activating PMS to degrade pollutants, the stability of the catalyst is poor due to the change of the pH of the system, and metal ions are dissolved into water again, so that secondary pollution is caused, which severely limits the application of PMS activation in actual sewage and wastewater treatment.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides a method for preparing the metal-free carbon-based catalyst by immobilization, which is used for preparing the metal-free carbon-based catalyst which is low in cost and easy to obtain, and successfully immobilizing the catalyst on quartz sand, so that PMS can be continuously and stably activated, and the quick removal of organic matters in water is realized.
The invention adopts the following technical scheme:
in a first aspect, the invention discloses a method for preparing an immobilization catalyst without a metal carbon base, which comprises the following steps:
(1) Dissolving dicyandiamide and ascorbic acid in methanol, placing the mixture in an oven until the methanol is completely volatilized, and then roasting to obtain a metal-free carbon-based catalyst;
(2) Adding dopamine, a metal-free carbon-based catalyst and quartz sand into a phosphate buffer solution, and stirring in a water bath to obtain a first mixed solution;
(3) Filtering the first mixed solution, removing the liquid part to obtain semi-solidified quartz sand and suspended solids, flushing the semi-solidified quartz sand and suspended solids with deionized water for a plurality of times, and drying the semi-solidified quartz sand and suspended solids to obtain first solids;
(4) And (3) placing the first solid in a muffle furnace for roasting to obtain the metal-free carbon-based catalyst-supported quartz sand.
Preferably, in the step (1), the roasting temperature is 500 ℃ and the roasting time is 4 hours.
Preferably, in the step (1), dicyandiamide: ascorbic acid: the molar ratio of methanol is 100:3:750.
preferably, in the step (2), the concentration of the phosphate buffer solution is 0.05-0.5mol/L, and the pH value is 7.5-8.5.
More preferably, the pH of the phosphate buffer is 8.0.
Preferably, in the step (2), the time is 5-15 hours, and the temperature is 15-35 ℃.
More preferably, in the step (2), the time is 10 hours and the temperature is 25 ℃.
Preferably, in the step (3), the obtained mixed solid is washed with deionized water and dried before the calcination.
Preferably, in the step (3), the deionized water is washed 3-5 times, and the drying temperature is 60-100 ℃.
Preferably, in the step (4), the roasting time is 0.5-2h, and the temperature is 300-400 ℃.
More preferably, in the step (4), the roasting time is 1h and the temperature is 350 ℃.
Preferably, in the step (4), the obtained first solid needs to be washed by deionized water after being calcined, so as to remove suspended solids and be dried.
More preferably, in the step (4), deionized water is washed 3 to 5 times, and the temperature of drying and dewatering is 60 ℃.
In a second aspect, the invention provides metal-free carbon-based catalyst-supported quartz sand, which is prepared by the method.
In a third aspect, the invention provides an application of metal-free carbon-based catalyst immobilized quartz sand prepared by the preparation method in degrading organic pollutants in water.
Preferably, the organic contaminants include acid orange 7 organic contaminants.
Preferably, the metal-free carbon-based catalyst-supported quartz sand is filled in a fixed bed reactor as a heterogeneous catalyst and used for treating acid orange 7 (AO 7) wastewater, the fixed bed reactor is in a continuous flow mode of water inflow at the bottom end and water outflow at the upper end, the water inflow of the fixed bed reactor comprises AO7 wastewater and PMS, and the water inflow residence time is 10-60min.
More preferably, the inlet water residence time is 10 minutes.
Compared with the prior art, the invention has the beneficial effects that:
(1) The catalyst prepared by the invention has long-term stability in the process of removing organic pollutants.
(2) The preparation and curing method has the advantages of easy achievement of conditions, simple method, low equipment requirement and easy industrialized production.
(3) The quartz sand used in the invention is easy to obtain in the environment, has low price in the market, and is convenient for wide popularization and application.
Drawings
The invention will be further described with reference to the accompanying drawings, in which embodiments do not constitute any limitation of the invention, and other drawings can be obtained by one of ordinary skill in the art without inventive effort from the following drawings.
FIG. 1 is a schematic diagram showing the degradation effect of the metal-free carbon-based catalyst-supported quartz sand prepared in example 2 of the present invention on acid orange 7 (AO 7) in wastewater.
Detailed Description
The technical features, objects and advantages of the present invention will be more clearly understood from the following detailed description of the technical aspects of the present invention, but should not be construed as limiting the scope of the invention.
The starting materials, reagents or apparatus used in the following examples are all available from conventional commercial sources or may be obtained by methods known in the art unless otherwise specified.
The invention is further described below with reference to the drawings and examples.
The method for preparing the metal-free carbon-based catalyst by immobilization provided by the embodiment comprises the following steps:
(1) Dissolving dicyandiamide and ascorbic acid in methanol, placing the mixture in an oven until the methanol is completely volatilized, and then roasting to obtain a metal-free carbon-based catalyst; roasting at 500 ℃ for 4 hours; dicyandiamide: ascorbic acid: the molar ratio of methanol is 100:3:750.
(2) Adding dopamine, a metal-free carbon-based catalyst and quartz sand into a phosphate buffer solution, and stirring in a water bath to obtain a first mixed solution; the concentration of the phosphate buffer solution is 0.05-0.5mol/L, and the pH value is 7.5-8.5; more preferably, the pH of the phosphate buffer is 8.0. The water bath stirring time is 5-15h, and the temperature is 15-35 ℃. More preferably, the water bath is stirred for 10 hours at 25 ℃.
(3) Filtering the first mixed solution, removing the liquid part to obtain semi-solidified quartz sand and suspended solids, flushing the semi-solidified quartz sand and suspended solids with deionized water for a plurality of times, and drying the semi-solidified quartz sand and suspended solids to obtain first solids; the washing times of deionized water are 3-5 times, and the drying temperature is 60-100 ℃; washing the obtained mixed solid by deionized water and drying the mixed solid before calcining;
(4) And (3) placing the first solid in a muffle furnace for roasting to obtain the metal-free carbon-based catalyst-supported quartz sand. After calcining the obtained first solid, washing the first solid by deionized water to remove suspended solid and drying the first solid; washing with deionized water for 3-5 times, and drying at 60deg.C; roasting for 0.5-2h at 300-400 ℃; more preferably, in the step (4), the roasting time is 1h and the temperature is 350 ℃.
The embodiment of the invention also provides the metal-free carbon-based catalyst immobilized quartz sand which is prepared by the method.
The embodiment of the invention also provides an application of the metal-free carbon-based catalyst immobilized quartz sand prepared by the preparation method in degrading organic pollutants in water. The organic contaminants include acid orange 7 organic contaminants.
The application comprises the following steps: and filling the metal-free carbon-based catalyst immobilized quartz sand into a fixed bed reactor as a heterogeneous catalyst and used for treating acid orange 7 (AO 7) wastewater, wherein the fixed bed reactor is in a continuous flow mode of water inflow at the bottom end and water outflow at the upper end, and the water inflow of the fixed bed reactor comprises AO7 wastewater and PMS, and the water inflow residence time is 10-60min. More preferably, the inlet water residence time is 10 minutes.
Example 1
This embodiment
The provided embodiment provides a method for preparing the immobilized catalyst without metal carbon, which is used for preparing the immobilized quartz sand without metal carbon catalyst and applying the immobilized quartz sand to PMS for activating and removing organic pollutants in water, and the method for preparing the immobilized catalyst comprises the following steps:
(1) Preparing 100mL of phosphate buffer solution with the pH value of 7.5-8.5 and 0.05-0.5 mol/L; dicyandiamide and ascorbic acid are dissolved in methanol, dicyandiamide: ascorbic acid: the molar ratio of methanol is 100:3:750, placing the mixture in an oven until methanol is completely volatilized, and roasting the mixture at 500 ℃ for more than 4 hours to obtain a metal-free carbon-based catalyst;
(2) Weighing 0.36g of dopamine, dissolving in 100mL of PBS buffer solution, and stirring until the dopamine is completely dissolved to obtain a dopamine solution; weighing 0.3g of the metal-free carbon-based catalyst, 20g of quartz sand, dissolving in a dopamine solution, and placing in a water bath at 15-35 ℃ for stirring for more than 5-15 h. Filtering the stirred solid-liquid mixture to obtain semi-solidified quartz sand, flushing with deionized water for 3-5 times, and placing at 60-100deg.C until water is completely evaporated;
(3) And (3) placing the evaporated semi-solid quartz sand in a muffle furnace, and roasting for 0.5-2h at 300-400 ℃ to obtain the modified quartz sand. And (3) washing the obtained modified quartz sand with deionized water for 3-5 times, removing suspended matters suspended in water, and completely evaporating the water at 60 ℃ until the water is completely evaporated, thus obtaining the quartz sand without metal carbon material load.
(4) Filling the obtained quartz sand without metal carbon material load into a column, and introducing 10ppm AO7 and 2mM PMS organic wastewater into the column; the fixed bed reactor is in a continuous flow mode with water inlet at the bottom end and water outlet at the upper end, the water inlet of the fixed bed reactor comprises AO7 wastewater and PMS, and the water inlet residence time is 10-60min.
Example 2
The provided embodiment provides a method for preparing the immobilized catalyst without metal carbon, which is used for preparing the immobilized quartz sand without metal carbon catalyst and applying the immobilized quartz sand to PMS for activating and removing organic pollutants in water, and the method for preparing the immobilized catalyst comprises the following steps:
(1) Preparing 100mL of phosphate buffer solution with the pH of 0.2mol/L and the pH of 8; dicyandiamide and ascorbic acid are dissolved in methanol, dicyandiamide: ascorbic acid: the molar ratio of methanol is 100:3:750, placing the mixture in an oven until methanol is completely volatilized, and roasting the mixture at 500 ℃ for more than 4 hours to obtain a metal-free carbon-based catalyst;
(2) Weighing 0.36g of dopamine, dissolving in 100mL of PBS buffer solution, and stirring until the dopamine is completely dissolved to obtain a dopamine solution; 0.3g of metal-free carbon-based catalyst, 20g of quartz sand and dissolved in dopamine solution are respectively weighed and placed in a water bath at 25 ℃ for stirring for more than 10 hours. Filtering the stirred solid-liquid mixture to obtain semi-solidified quartz sand, flushing with deionized water for 3 times, and placing at 60 ℃ until the water is completely evaporated;
(3) And (3) placing the evaporated semi-solid quartz sand in a muffle furnace, and roasting for 1h at 350 ℃ to obtain the modified quartz sand. Washing the obtained modified quartz sand with deionized water to remove suspended matters suspended in water, and completely evaporating the water at 60 ℃ until the water is completely evaporated to obtain quartz sand without metal carbon material load;
(4) The resulting metal carbon material loaded silica sand was packed into a column and 10ppm AO7,2mM PMS organic wastewater was passed into the column.
(5) The degradation effect of AO7 in water is detected by the water inlet and outlet, and the obtained effect is shown in figure 1.
Experimental example
Catalytic degradation Properties
As shown in fig. 1, the effect of the metal-free material of example 1 immobilized on quartz sand for PMS activation to remove organic contaminants in water is schematically shown for long term monitoring. In the short period of 10 minutes, over 90 percent of AO7 can be removed rapidly, and in the detection of 600 hours continuously, the reactor still keeps good stability, so that the scientific bottleneck problem of poor catalyst stability is broken, and the method has very practical application significance.
The preparation and curing method provided by the invention has the advantages of easy achievement of conditions, simple method, low equipment requirement and easy industrial production; the prepared catalyst has long-term stability in the process of removing organic pollutants, is low in price and is convenient for wide popularization and application.
Finally, it should be noted that the above embodiments are only for illustrating the technical solution of the present invention, and not for limiting the scope of the present invention, and although the present invention has been described in detail with reference to the preferred embodiments, it should be understood by those skilled in the art that modifications or equivalent substitutions can be made to the technical solution of the present invention without departing from the spirit and scope of the technical solution of the present invention.
Claims (8)
1. The preparation method of the metal-free carbon-based catalyst is characterized by comprising the following steps of:
(1) Dissolving dicyandiamide and ascorbic acid in methanol, placing the mixture in an oven until the methanol is completely volatilized, and then roasting to obtain a metal-free carbon-based catalyst;
(2) Adding dopamine, a metal-free carbon-based catalyst and quartz sand into a phosphate buffer solution, and stirring in a water bath to obtain a first mixed solution;
(3) Filtering the first mixed solution, removing the liquid part to obtain semi-solidified quartz sand and suspended solids, flushing the semi-solidified quartz sand and suspended solids with deionized water for a plurality of times, and drying the semi-solidified quartz sand and suspended solids to obtain first solids;
(4) Roasting the first solid in a muffle furnace to obtain metal-free carbon-based catalyst-supported quartz sand;
in the step (1), dicyandiamide: ascorbic acid: the molar ratio of methanol is 100:3:750; roasting at 500 ℃ for 4 hours;
in the step (2), the time is 5-15h, and the temperature is 15-35 ℃.
2. The method for preparing a metal-free carbon-based catalyst according to claim 1, wherein in the step (2), the concentration of the phosphate buffer solution is 0.05-0.5mol/L and the pH value is 7.5-8.5.
3. The method for preparing a metal-free carbon-based catalyst according to claim 1, wherein in the step (3), the obtained mixed solid is washed with deionized water and dried before the calcination.
4. The method for preparing the metal-free carbon-based catalyst according to claim 1, wherein in the step (3), the deionized water is washed 3 to 5 times, and the drying temperature is 60 to 100 ℃.
5. The method for preparing a metal-free carbon-based catalyst according to claim 1, wherein in the step (4), the calcination time is 0.5-2 hours and the temperature is 300-400 ℃.
6. The method for preparing metal-free carbon-based catalyst according to claim 1, wherein in the step (4), the first solid obtained after calcination is washed with deionized water to remove suspended solids and dried.
7. The metal-free carbon-based catalyst-supported quartz sand is characterized in that the metal-free carbon-based catalyst-supported quartz sand is prepared by using the metal-free carbon-based catalyst-supported preparation method according to any one of claims 1 to 6.
8. Use of the metal-free carbon-based catalyst-supported quartz sand of claim 7 for degrading organic contaminants in water.
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