CN110813289A - Composite visible-light-driven photocatalyst for degrading organic pollutants - Google Patents
Composite visible-light-driven photocatalyst for degrading organic pollutants Download PDFInfo
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- CN110813289A CN110813289A CN201810901802.8A CN201810901802A CN110813289A CN 110813289 A CN110813289 A CN 110813289A CN 201810901802 A CN201810901802 A CN 201810901802A CN 110813289 A CN110813289 A CN 110813289A
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- aluminum
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- zinc oxide
- solid solution
- doped zinc
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- 239000002131 composite material Substances 0.000 title claims abstract description 37
- 239000011941 photocatalyst Substances 0.000 title claims abstract description 17
- 230000000593 degrading effect Effects 0.000 title claims abstract description 9
- 239000002957 persistent organic pollutant Substances 0.000 title claims abstract description 9
- 239000003054 catalyst Substances 0.000 claims abstract description 16
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 10
- 238000002360 preparation method Methods 0.000 claims abstract description 5
- 238000007540 photo-reduction reaction Methods 0.000 claims abstract description 4
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 70
- 239000011787 zinc oxide Substances 0.000 claims description 35
- 239000006104 solid solution Substances 0.000 claims description 32
- 229910052782 aluminium Inorganic materials 0.000 claims description 14
- 239000004332 silver Substances 0.000 claims description 11
- 229910052709 silver Inorganic materials 0.000 claims description 11
- 239000000243 solution Substances 0.000 claims description 11
- DHMQDGOQFOQNFH-UHFFFAOYSA-N Glycine Chemical compound NCC(O)=O DHMQDGOQFOQNFH-UHFFFAOYSA-N 0.000 claims description 10
- MHLYOTJKDAAHGI-UHFFFAOYSA-N silver molybdate Chemical compound [Ag+].[Ag+].[O-][Mo]([O-])(=O)=O MHLYOTJKDAAHGI-UHFFFAOYSA-N 0.000 claims description 10
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical compound [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 claims description 10
- 238000003756 stirring Methods 0.000 claims description 9
- 238000001035 drying Methods 0.000 claims description 7
- 229920000036 polyvinylpyrrolidone Polymers 0.000 claims description 6
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 claims description 6
- 239000001267 polyvinylpyrrolidone Substances 0.000 claims description 6
- BNGXYYYYKUGPPF-UHFFFAOYSA-M (3-methylphenyl)methyl-triphenylphosphanium;chloride Chemical compound [Cl-].CC1=CC=CC(C[P+](C=2C=CC=CC=2)(C=2C=CC=CC=2)C=2C=CC=CC=2)=C1 BNGXYYYYKUGPPF-UHFFFAOYSA-M 0.000 claims description 5
- 239000004471 Glycine Substances 0.000 claims description 5
- 238000001816 cooling Methods 0.000 claims description 5
- 239000008367 deionised water Substances 0.000 claims description 5
- 229910021641 deionized water Inorganic materials 0.000 claims description 5
- 230000001678 irradiating effect Effects 0.000 claims description 5
- 229910001961 silver nitrate Inorganic materials 0.000 claims description 5
- 239000011684 sodium molybdate Substances 0.000 claims description 5
- 235000015393 sodium molybdate Nutrition 0.000 claims description 5
- TVXXNOYZHKPKGW-UHFFFAOYSA-N sodium molybdate (anhydrous) Chemical compound [Na+].[Na+].[O-][Mo]([O-])(=O)=O TVXXNOYZHKPKGW-UHFFFAOYSA-N 0.000 claims description 5
- 238000005406 washing Methods 0.000 claims description 5
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 4
- 238000001354 calcination Methods 0.000 claims description 2
- 239000006185 dispersion Substances 0.000 claims description 2
- 238000000227 grinding Methods 0.000 claims description 2
- 238000002156 mixing Methods 0.000 claims description 2
- 239000012792 core layer Substances 0.000 claims 3
- 239000010410 layer Substances 0.000 claims 1
- 230000003197 catalytic effect Effects 0.000 abstract description 4
- 239000000126 substance Substances 0.000 abstract description 4
- 239000011248 coating agent Substances 0.000 abstract description 3
- 238000000576 coating method Methods 0.000 abstract description 3
- 230000007613 environmental effect Effects 0.000 abstract description 3
- 238000000034 method Methods 0.000 abstract description 2
- 238000001782 photodegradation Methods 0.000 abstract description 2
- 238000011065 in-situ storage Methods 0.000 abstract 2
- 239000002114 nanocomposite Substances 0.000 abstract 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 11
- ONDPHDOFVYQSGI-UHFFFAOYSA-N zinc nitrate Chemical compound [Zn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ONDPHDOFVYQSGI-UHFFFAOYSA-N 0.000 description 6
- 231100000956 nontoxicity Toxicity 0.000 description 3
- 239000011701 zinc Substances 0.000 description 3
- 230000001699 photocatalysis Effects 0.000 description 2
- 238000003915 air pollution Methods 0.000 description 1
- 239000003242 anti bacterial agent Substances 0.000 description 1
- 229940088710 antibiotic agent Drugs 0.000 description 1
- UDSAIICHUKSCKT-UHFFFAOYSA-N bromophenol blue Chemical compound C1=C(Br)C(O)=C(Br)C=C1C1(C=2C=C(Br)C(O)=C(Br)C=2)C2=CC=CC=C2S(=O)(=O)O1 UDSAIICHUKSCKT-UHFFFAOYSA-N 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- MCPLVIGCWWTHFH-UHFFFAOYSA-L methyl blue Chemical compound [Na+].[Na+].C1=CC(S(=O)(=O)[O-])=CC=C1NC1=CC=C(C(=C2C=CC(C=C2)=[NH+]C=2C=CC(=CC=2)S([O-])(=O)=O)C=2C=CC(NC=3C=CC(=CC=3)S([O-])(=O)=O)=CC=2)C=C1 MCPLVIGCWWTHFH-UHFFFAOYSA-L 0.000 description 1
- STZCRXQWRGQSJD-GEEYTBSJSA-M methyl orange Chemical compound [Na+].C1=CC(N(C)C)=CC=C1\N=N\C1=CC=C(S([O-])(=O)=O)C=C1 STZCRXQWRGQSJD-GEEYTBSJSA-M 0.000 description 1
- 229940012189 methyl orange Drugs 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 150000003378 silver Chemical class 0.000 description 1
- 239000007787 solid 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/66—Silver or gold
- B01J23/68—Silver or gold with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/683—Silver or gold with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium with chromium, molybdenum or tungsten
- B01J23/686—Silver or gold with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium with chromium, molybdenum or tungsten with molybdenum
-
- 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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/39—Photocatalytic properties
-
- 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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
- B01J35/51—Spheres
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Catalysts (AREA)
Abstract
The invention belongs to the technical field of environmental chemistry, and particularly relates to a composite visible-light-driven photocatalyst for degrading organic pollutants and a preparation method thereof. The invention obtains a composite visible light catalyst for degrading organic pollutants by utilizing an in-situ coating technology and an in-situ photoreduction method. The nano composite catalyst has high catalytic activity and good chemical stability, and can be widely applied to photodegradation treatment of various organic pollutants in water.
Description
Technical Field
The invention belongs to the technical field of environmental chemistry, and particularly relates to a composite visible-light-driven photocatalyst for degrading organic pollutants, a preparation method and application thereof in the environmental field.
Background
The water body pollution, air pollution and the like in life threaten the health of people all the time, how to reduce the pollution and protect the environment become increasingly concerned problems, and the preparation of the photocatalyst for degrading harmful organic matters becomes one of scientific research hotspots in the field of material chemistry. The zinc oxide-based composite catalyst and the nano silver deposited silver molybdate catalyst are paid much attention to due to their safety, non-toxicity and outstanding photocatalytic performance.
According to the invention, the silver/silver molybdate @ aluminum-doped zinc oxide solid solution composite visible-light-driven photocatalyst is prepared by coating the silver molybdate deposited nano silver molybdate catalyst on the aluminum-doped zinc oxide solid solution. Silver, silver molybdate and aluminum-doped zinc oxide have the advantages of safety, no toxicity, stable physical and chemical properties, excellent mechanical properties and the like, and are paid more and more attention by scientific researchers. The invention creatively designs a novel composite visible-light-driven photocatalyst in order to fully exert the performance advantages of the three substances. The composite visible-light-driven photocatalyst aims at improving the catalytic efficiency and the visible-light utilization rate and greatly improves the recovery rate of the composite catalyst.
Disclosure of Invention
The invention aims to provide a composite visible-light-driven photocatalyst for degrading organic pollutants, which is a novel composite visible-light-driven photocatalyst with excellent catalytic performance and convenient recycling, remarkably improves the catalytic effect and the utilization rate of visible light of the catalyst, and also solves the problem that the existing catalyst is difficult to recycle.
The invention provides a composite visible light catalyst for degrading organic pollutants, which comprises the following components of taking an aluminum-doped zinc oxide solid solution as a nuclear layer, coating a silver molybdate shell layer on the surface of the nuclear layer, and loading silver quantum dots on the surface of the nuclear layer in a photoreduction mode, namely the silver/silver molybdate @ aluminum-doped zinc oxide solid solution composite visible light catalyst, wherein the specific preparation steps are as follows: a: mixing aluminum nitrate and glycine according to a certain mass ratio, fully grinding, drying for several hours at a certain temperature, and finally calcining to obtain an aluminum-doped zinc oxide solid solution; b: adding a certain amount of aluminum-doped zinc oxide solid solution into a sodium molybdate and polyvinyl pyrrolidone water dispersion system, placing the system in an ultrasonic disperser, dropwise adding a silver nitrate solution into the system under the ultrasonic dispersing condition, naturally cooling the system to room temperature after reacting for a period of time, washing the system with deionized water, and drying the system in an oven to obtain a silver molybdate/aluminum-doped zinc oxide solid solution composite material; c: and irradiating the prepared silver molybdate @ aluminum doped zinc oxide solid solution composite material under the condition of stirring for a period of time under the ultraviolet light with the power of 8W to obtain the silver/silver molybdate @ aluminum doped zinc oxide solid solution composite visible-light-driven photocatalyst.
According to the invention, the silver molybdate @ aluminum doped zinc oxide solid solution composite material is irradiated under the condition of stirring for 10 to 60 seconds under the ultraviolet light with the power of 8W, and the content of silver at the outermost layer of the visible light composite catalyst is controlled through the photoreduction time.
The invention has the following advantages:
1. the silver/silver molybdate @ aluminum-doped zinc oxide solid solution composite visible light catalyst is designed and synthesized for the first time, the visible light utilization rate is remarkably improved, and the photodegradation efficiency is greatly improved.
2. The composite visible-light-driven photocatalyst prepared by the invention can degrade a plurality of pollutants in water such as methyl orange, methyl blue, bromophenol blue, antibiotics and the like under the condition of visible light.
3. The invention uses polyvinylpyrrolidone in the process of preparing the catalyst, and has the effect of enabling the combination of different components of the composite catalyst to be more compact.
4. The composite visible-light-driven photocatalyst prepared by the invention has the advantages of safety, no toxicity, good physical and chemical properties, excellent photocatalytic performance and the like, and does not cause secondary pollution to the environment.
Detailed Description
The present invention will be further illustrated by the following specific examples.
Example 1:
0.225 g of aluminum nitrate (Al (NO) was weighed3)3·9H2O，6.0×10-4mol) and 8.91 g of zinc nitrate (Zn (NO)3)2·6H2O, 0.03mol) and glycine 4.50g (0.06mol), thoroughly ground, dried at 140 ℃ for 2 hours, and then calcined at 600 ℃ for 2 hours to obtain an aluminum-doped zinc oxide solid solution. 0.81g of aluminum-doped zinc oxide solid solution was weighed out and added to 100mL of 0.1 mol. L-10.1 g of polyvinylpyrrolidone is added to the sodium molybdate solution, and after sufficient stirring, 100mL of 0.2 mol/L solution is added dropwise in the presence of ultrasonic waves-1Silver nitrate solution, and fully reacting to be complete. After reacting for a period of time, naturally cooling to room temperature, washing with deionized water, and drying in an oven to obtain the silver molybdate/aluminum doped zinc oxide solid solution composite material; the prepared silver molybdate @ aluminum doped zinc oxide is dissolved in solid solutionAnd irradiating the composite material for 30 seconds under the condition of stirring and under the ultraviolet light with the power of 8W to obtain the silver/silver molybdate @ aluminum doped zinc oxide solid solution composite visible-light-driven photocatalyst.
Example 2
0.225 g of aluminum nitrate (Al (NO) was weighed3)3·9H2O，6.0×10-4mol) and 8.91 g of zinc nitrate (Zn (NO)3)2·6H2O, 0.03mol) and glycine 4.50g (0.06mol), thoroughly ground, dried at 140 ℃ for 2 hours, and then calcined at 600 ℃ for 2 hours to obtain an aluminum-doped zinc oxide solid solution. 1.62g of aluminum-doped zinc oxide solid solution was weighed and added to 100mL of 0.1 mol.L-10.1 g of polyvinylpyrrolidone is added to the sodium molybdate solution, and after sufficient stirring, 100mL of 0.2 mol/L solution is added dropwise in the presence of ultrasonic waves-1Silver nitrate solution, and fully reacting to be complete. After reacting for a period of time, naturally cooling to room temperature, washing with deionized water, and drying in an oven to obtain the silver molybdate/aluminum doped zinc oxide solid solution composite material; and irradiating the prepared silver molybdate @ aluminum doped zinc oxide solid solution composite material for 10 seconds under the condition of stirring and under the ultraviolet light with the power of 8W to obtain the silver/silver molybdate @ aluminum doped zinc oxide solid solution composite visible-light-driven photocatalyst.
Example 3
0.225 g of aluminum nitrate (Al (NO) was weighed3)3·9H2O，6.0×10-4mol) and 8.91 g of zinc nitrate (Zn (NO)3)2·6H2O, 0.03mol) and glycine 4.50g (0.06mol), thoroughly ground, dried at 140 ℃ for 2 hours, and then calcined at 600 ℃ for 2 hours to obtain an aluminum-doped zinc oxide solid solution. 2.43g of aluminum-doped zinc oxide solid solution was weighed out and added to 100mL of 0.1 mol. L-10.1 g of polyvinylpyrrolidone is added to the sodium molybdate solution, and after sufficient stirring, 100mL of 0.2 mol/L solution is added dropwise in the presence of ultrasonic waves-1Silver nitrate solution, and fully reacting to be complete. After reacting for a period of time, naturally cooling to room temperature, washing with deionized water, and drying in an oven to obtain silver molybdate/aluminum dopeA zinc oxide solid solution composite; and irradiating the prepared silver molybdate @ aluminum doped zinc oxide solid solution composite material under the condition of stirring for 60 seconds under the ultraviolet light with the power of 8W to obtain the silver/silver molybdate @ aluminum doped zinc oxide solid solution composite visible-light-driven photocatalyst.
Claims (1)
1. A composite visible light catalyst for degrading organic pollutants comprises a core layer made of aluminum-doped zinc oxide solid solution, a silver molybdate shell layer coated on the surface of the core layer, and silver quantum dots loaded on the surface of the core layer in a photoreduction mode, namely, the silver/silver molybdate @ aluminum-doped zinc oxide solid solution composite visible light catalyst, and the preparation method specifically comprises the following steps: a: mixing aluminum nitrate and glycine according to a certain mass ratio, fully grinding, drying for several hours at a certain temperature, and finally calcining to obtain an aluminum-doped zinc oxide solid solution; b: adding a certain amount of aluminum-doped zinc oxide solid solution into a sodium molybdate and polyvinyl pyrrolidone water dispersion system, placing the system in an ultrasonic disperser, dropwise adding a silver nitrate solution into the system under the ultrasonic dispersing condition, naturally cooling the system to room temperature after reacting for a period of time, washing the system with deionized water, and drying the system in an oven to obtain a silver molybdate @ aluminum-doped zinc oxide solid solution composite material; c: and irradiating the prepared silver molybdate/aluminum doped zinc oxide solid solution composite material under the condition of stirring for a period of time under the ultraviolet light with the power of 8W to obtain the silver/silver molybdate @ aluminum doped zinc oxide solid solution composite visible-light-driven photocatalyst.
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201810901802.8A CN110813289A (en) | 2018-08-09 | 2018-08-09 | Composite visible-light-driven photocatalyst for degrading organic pollutants |
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| Application Number | Priority Date | Filing Date | Title |
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| CN201810901802.8A CN110813289A (en) | 2018-08-09 | 2018-08-09 | Composite visible-light-driven photocatalyst for degrading organic pollutants |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113181922A (en) * | 2021-05-08 | 2021-07-30 | 南昌航空大学 | Preparation method of Ag quantum dot modified high-entropy oxide photocatalyst |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104607216A (en) * | 2014-12-31 | 2015-05-13 | 华东理工大学 | One-step synthesis method of phosphorus-aluminum co-doped type conductive zinc oxide nanometer catalyst |
-
2018
- 2018-08-09 CN CN201810901802.8A patent/CN110813289A/en active Pending
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104607216A (en) * | 2014-12-31 | 2015-05-13 | 华东理工大学 | One-step synthesis method of phosphorus-aluminum co-doped type conductive zinc oxide nanometer catalyst |
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|---|
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| V. P. DINESH等: "Plasmon-mediated, highly enhanced photocatalytic degradation of industrial textile dyes using hybrid ZnO@Ag core-shell nanorods", 《RSC ADVANCES》, vol. 4, 23 October 2014 (2014-10-23), pages 58930 - 58940 * |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113181922A (en) * | 2021-05-08 | 2021-07-30 | 南昌航空大学 | Preparation method of Ag quantum dot modified high-entropy oxide photocatalyst |
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