CN108772081B - FePO4 heterogeneous visible light Fenton catalyst and method for treating organic wastewater - Google Patents
FePO4 heterogeneous visible light Fenton catalyst and method for treating organic wastewater Download PDFInfo
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- CN108772081B CN108772081B CN201810764585.2A CN201810764585A CN108772081B CN 108772081 B CN108772081 B CN 108772081B CN 201810764585 A CN201810764585 A CN 201810764585A CN 108772081 B CN108772081 B CN 108772081B
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- 229910000399 iron(III) phosphate Inorganic materials 0.000 title claims abstract description 27
- 239000003054 catalyst Substances 0.000 title claims abstract description 21
- 239000002351 wastewater Substances 0.000 title claims abstract description 20
- 238000000034 method Methods 0.000 title claims abstract description 19
- WBJZTOZJJYAKHQ-UHFFFAOYSA-K iron(3+) phosphate Chemical compound [Fe+3].[O-]P([O-])([O-])=O WBJZTOZJJYAKHQ-UHFFFAOYSA-K 0.000 title claims abstract description 11
- 239000000975 dye Substances 0.000 claims abstract description 15
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims abstract description 14
- 238000006731 degradation reaction Methods 0.000 claims abstract description 8
- 230000015556 catabolic process Effects 0.000 claims abstract description 6
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 claims abstract description 3
- 229910000359 iron(II) sulfate Inorganic materials 0.000 claims abstract description 3
- 239000002244 precipitate Substances 0.000 claims abstract description 3
- 239000000243 solution Substances 0.000 claims description 10
- 239000002253 acid Substances 0.000 claims description 6
- 238000002360 preparation method Methods 0.000 claims description 6
- 239000007836 KH2PO4 Substances 0.000 claims description 3
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 claims description 3
- LFVGISIMTYGQHF-UHFFFAOYSA-N ammonium dihydrogen phosphate Chemical compound [NH4+].OP(O)([O-])=O LFVGISIMTYGQHF-UHFFFAOYSA-N 0.000 claims description 3
- MNNHAPBLZZVQHP-UHFFFAOYSA-N diammonium hydrogen phosphate Chemical compound [NH4+].[NH4+].OP([O-])([O-])=O MNNHAPBLZZVQHP-UHFFFAOYSA-N 0.000 claims description 3
- 229910000388 diammonium phosphate Inorganic materials 0.000 claims description 3
- ZPWVASYFFYYZEW-UHFFFAOYSA-L dipotassium hydrogen phosphate Chemical compound [K+].[K+].OP([O-])([O-])=O ZPWVASYFFYYZEW-UHFFFAOYSA-L 0.000 claims description 3
- 229910000396 dipotassium phosphate Inorganic materials 0.000 claims description 3
- 229910000397 disodium phosphate Inorganic materials 0.000 claims description 3
- 229910000402 monopotassium phosphate Inorganic materials 0.000 claims description 3
- GNSKLFRGEWLPPA-UHFFFAOYSA-M potassium dihydrogen phosphate Chemical compound [K+].OP(O)([O-])=O GNSKLFRGEWLPPA-UHFFFAOYSA-M 0.000 claims description 3
- AJPJDKMHJJGVTQ-UHFFFAOYSA-M sodium dihydrogen phosphate Chemical compound [Na+].OP(O)([O-])=O AJPJDKMHJJGVTQ-UHFFFAOYSA-M 0.000 claims description 3
- 229910000162 sodium phosphate Inorganic materials 0.000 claims description 3
- 239000000654 additive Substances 0.000 claims description 2
- 230000000996 additive effect Effects 0.000 claims description 2
- 239000007864 aqueous solution Substances 0.000 claims description 2
- 239000003344 environmental pollutant Substances 0.000 claims description 2
- 231100000719 pollutant Toxicity 0.000 claims description 2
- PYWVYCXTNDRMGF-UHFFFAOYSA-N rhodamine B Chemical group [Cl-].C=12C=CC(=[N+](CC)CC)C=C2OC2=CC(N(CC)CC)=CC=C2C=1C1=CC=CC=C1C(O)=O PYWVYCXTNDRMGF-UHFFFAOYSA-N 0.000 claims description 2
- 229940043267 rhodamine b Drugs 0.000 claims description 2
- 229910052603 melanterite Inorganic materials 0.000 claims 1
- 238000006555 catalytic reaction Methods 0.000 abstract description 5
- 239000002245 particle Substances 0.000 abstract description 5
- 230000009286 beneficial effect Effects 0.000 abstract description 3
- 230000000052 comparative effect Effects 0.000 description 11
- 238000003756 stirring Methods 0.000 description 5
- 238000002441 X-ray diffraction Methods 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 238000001354 calcination Methods 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- 238000012986 modification Methods 0.000 description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- 238000007792 addition Methods 0.000 description 2
- 230000000593 degrading effect Effects 0.000 description 2
- 238000004065 wastewater treatment Methods 0.000 description 2
- 229910017677 NH4H2 Inorganic materials 0.000 description 1
- 238000002835 absorbance Methods 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 230000001133 acceleration Effects 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000002270 dispersing agent Substances 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 238000007146 photocatalysis Methods 0.000 description 1
- 230000001699 photocatalysis Effects 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 239000011541 reaction mixture Substances 0.000 description 1
- LGZQSRCLLIPAEE-UHFFFAOYSA-M sodium 1-[(4-sulfonaphthalen-1-yl)diazenyl]naphthalen-2-olate Chemical compound [Na+].C1=CC=C2C(N=NC3=C4C=CC=CC4=CC=C3O)=CC=C(S([O-])(=O)=O)C2=C1 LGZQSRCLLIPAEE-UHFFFAOYSA-M 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
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- 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
- B01J27/14—Phosphorus; Compounds thereof
- B01J27/185—Phosphorus; Compounds thereof with iron group metals or platinum group metals
- B01J27/1853—Phosphorus; Compounds thereof with iron group metals or platinum group metals with iron, cobalt or nickel
-
- 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
-
- 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
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
-
- 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
- C02F1/722—Oxidation by peroxides
-
- 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
- C02F2101/308—Dyes; Colorants; Fluorescent agents
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
- C02F2305/026—Fenton's reagent
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Materials Engineering (AREA)
- Health & Medical Sciences (AREA)
- Toxicology (AREA)
- Catalysts (AREA)
Abstract
The invention discloses a FePO4 heterogeneous visible light Fenton catalyst and a method for treating organic wastewater. The invention relates to FePO4The heterogeneous visible light Fenton catalyst comprises the following components in a dosage ratio of 2.5-10 mg: 1mmol of organic dye component, FePO4. A method for treating organic wastewater, comprising the steps of: the method comprises the following steps: (1) XPO with the dosage ratio of 1:14With FeSO4•7H2O is mixed in the organic dye solution; (2) addition of H2O2In the degradation of organic dyes to form FePO4(ii) a (3) The obtained FePO4And putting the precipitate and hydrogen peroxide into the organic wastewater to be treated. FePO of the invention4The heterogeneous visible light Fenton catalyst is introduced into RhB to increase the prepared FePO on the one hand4Thereby increasing the active sites of the catalytic reaction; on the other hand, the FePO prepared4The dispersibility of (A) is better, and the particle size is smaller, which is also beneficial to the catalytic reaction.
Description
Technical Field
The invention relates to the technical field of wastewater treatment, in particular to FePO4A heterogeneous visible light Fenton catalyst and a method for treating organic wastewater.
Background
With the acceleration of urbanization and industrialization in China, the discharge amount of wastewater in China also increases year by year, so that the water environment and water ecology are continuously deteriorated. The Fenton oxidation technology is an environment-friendly novel environment-friendly technology, and is widely applied to treatment of various waste water due to the characteristics of strong oxidation capacity, small occupied space in practical application, environmental friendliness and the like. However, in recent years, Fenton oxidation technology has some bottlenecks in the actual wastewater treatment process, for example, the reaction process is accompanied by the generation of a large amount of iron mud, the treatment cost is increased, organic matters can not be removed any more after reaching a certain removal rate in the organic pollutant treatment process, and H is easily caused2O2Consumption of the amount. Therefore, it is very important to solve these bottlenecks for the wide application of the Fenton oxidation technology. The novel FePO prepared by the invention4The heterogeneous visible light Fenton catalyst can well solve the bottleneck.
Disclosure of Invention
Aiming at the defects in the prior art, the invention provides FePO with simple and convenient operation and high degradation efficiency4A heterogeneous visible light Fenton catalyst and a method for treating organic wastewater.
The invention relates to FePO4The heterogeneous visible light Fenton catalyst comprises the following components in a dosage ratio of 2.5-10 mg: 1mmol of organic dye component, FePO4。
Preferably, the organic dye component is rhodamine B or acid red.
A method for treating organic wastewater, comprising the steps of: the method comprises the following steps: (1) XPO with the dosage ratio of 1:14With FeSO4•7H2O is mixed in the organic dye solution; (2) addition of H2O2In the degradation of organic dyes to form FePO4(ii) a (3) The obtained FePO4And putting the precipitate and hydrogen peroxide into the organic wastewater to be treated.
Preferably, the XPO4Is NH4H2PO4、（NH4）2HPO4、KH2PO4、K2HPO4、H3PO4、Na2HPO4Or NaH2PO4。
Preferably, the FePO4The amount of the additive (B) is 0.5-2 g/L.
Preferably, the adding amount of the hydrogen peroxide is 5-20 mmol/L.
Preferably, the content of the pollutants in the organic wastewater to be treated is 0-20 mg/L.
Preferably, the hydrogen peroxide is an aqueous solution with the mass fraction of 30%.
Preferably, the treatment time is 10-150 min.
FePO of the invention4The heterogeneous visible light Fenton catalyst is introduced into RhB to increase the prepared FePO on the one hand4Thereby increasing the active sites of the catalytic reaction; on the other hand, the FePO prepared4The dispersibility of (A) is better, and the particle size is smaller, which is also beneficial to the catalytic reaction.
Drawings
FIG. 1 is FePO of comparative example 14And FePO of example 14XRD pattern after calcination at 800 deg.C (inset is FePO of comparative example 1)4And FePO of example 14XRD pattern without calcination);
FIG. 2 is FePO of comparative example 14And FePO of example 14The aperture profile of (a).
Detailed Description
The following are specific embodiments of the present invention and are further described with reference to the drawings, but the present invention is not limited to these embodiments.
Example 1
FePO4Preparation of
(1) Preparing 100 mL of RhB solution with the concentration of 500 mg/L;
(2) 0.02 mol of FeSO was added thereto4·7H2O and 0.02 mol NH4H2PO4Stirring for 15 min;
(3) to this was slowly added 20 mL of 30wt% H2O2Stirring until RhB is completely degraded;
(4) adjusting pH =2.0, stirring for 1 h, and aging for 8 h;
(5) washing with water, centrifuging, and drying at 105 deg.C to obtain FePO4A catalyst.
An LED lamp of 500W is used as a simulated visible light source, 100 mL of 10 mg/L acid red G (AGR) solution is measured and placed in a beaker in the experiment, and 0.1g of FePO is added in the stirring state without light4Continuously stirring the catalyst for 20 min to uniformly disperse the catalyst in the solution; the beaker was then transferred to a preheated reactor with stable light intensity and 1mmol of H was added rapidly to the beaker2O2The solution was timed and samples were taken at intervals and the absorbance of the solution was measured at the wavelength of maximum absorption using a spectrophotometer.
Examples 2, 3, 4, 5 modification of FePO4The other operating conditions of the reaction mixture of (1) were the same as those of example 1.
Comparative examples 1, 2, 3, 4, 5 FePO4The RhB solution in the preparation step (1) of (1) was replaced with distilled water, and the other operation conditions were the same as in example 1.
Table 1 example, comparative example FePO4Degradation effect on acid red
Table 2 FePO in comparative example 1 and example 14Specific surface area and particle size
As can be seen from Table 1, in FePO4The degradation rate of the acid red by adding the RhB in the preparation process of the catalyst is far higher than that of FePO prepared by not adding the RhB in the reaction process4Degradation rate of the catalyst to acid red. Thus illustrating the novel FePO prepared by the process4The catalyst has strong capacity of degrading acid red by photocatalysis. This is because RhB introduced during the preparation process can act as a dispersant and template.
FePO of comparative example 14And FePO of example 14The XRD pattern of (A) is shown as the interpolated graph in FIG. 1. As can be seen, FePO of comparative example 1 was prepared4And FePO of example 14All amorphous, FePO of comparative example 1 calcined at 800 deg.C4And FePO of example 14XRD pattern of (shown in figure 2) and FePO4(JCPDS: 84-876) one-to-one, which also indicates that the sample without calcination is a pure phase and that the introduction of the dye during the preparation process does not affect FePO4And (4) synthesizing.
The molecular size of RhB is 1.59X 1.18X 0.56 nm, which results in FePO formation4Has more mesopores, as can be seen from FIG. 2, FePO in comparative example 14Mainly at 3-4, 6-7 and 60 nm, compared to FePO in example 14The pore diameter distribution of the catalyst is all at 3-4nm, and the mesoporous structure is beneficial to the catalytic reaction; on the other hand, as can be seen from Table 2, FePO in comparative example 14And FePO of example 14Respectively, are 17.6 m2G and 24.5 m2The particle sizes are 341.4 nm and 245.1 nm, respectively. The introduction of RhB leads to FePO generated4Better dispersivity, larger specific surface area and smaller particle size, thereby increasing the active sites for catalyzing reaction. So that the FePO of the present invention4The catalyst has strong energy for degrading organic dye by photocatalysisForce.
The above is not relevant and is applicable to the prior art.
While certain specific embodiments of the present invention have been described in detail by way of illustration, it will be understood by those skilled in the art that the foregoing is illustrative only and is not limiting of the scope of the invention, as various modifications or additions may be made to the specific embodiments described and substituted in a similar manner by those skilled in the art without departing from the scope of the invention as defined in the appending claims. It should be understood by those skilled in the art that any modifications, equivalents, improvements and the like made to the above embodiments in accordance with the technical spirit of the present invention are included in the scope of the present invention.
Claims (8)
1. FePO4Heterogeneous visible light Fenton catalyst, its characterized in that: comprises the following components in a ratio of 2.5-10 mg: 1mmol of organic dye component, FePO4(ii) a The preparation method of the catalyst comprises the following steps: (1) XPO with a molar ratio of 1:14With FeSO4·7H2O is mixed in the organic dye solution; (2) addition of H2O2In the degradation of organic dyes to form FePO4(ii) a Wherein, the XPO4Is NH4H2PO4、(NH4)2HPO4、KH2PO4、K2HPO4、H3PO4、Na2HPO4Or NaH2PO4。
2. A FePO according to claim 14Heterogeneous visible light Fenton catalyst, its characterized in that: the organic dye component is rhodamine B or acid red.
3. A method for treating organic wastewater, which is characterized by comprising the following steps: the method comprises the following steps: (1) XPO with a molar ratio of 1:14With FeSO4•7H2O mixed in organicIn a dye solution; (2) addition of H2O2In the degradation of organic dyes to form FePO4(ii) a (3) Adjusting the pH of the solution and combining the resulting FePO4Putting the precipitate and hydrogen peroxide into the organic wastewater to be treated; wherein, the XPO4Is NH4H2PO4、(NH4)2HPO4、KH2PO4、K2HPO4、H3PO4、Na2HPO4Or NaH2PO4。
4. A method of treating organic wastewater according to claim 3 wherein: the FePO4The amount of the additive (B) is 0.5-2 g/L.
5. A method of treating organic wastewater according to claim 3 wherein: the adding amount of the hydrogen peroxide is 5-20 mmol/L.
6. A method of treating organic wastewater according to claim 3 wherein: the content of pollutants in the organic wastewater to be treated is 0-20 mg/L.
7. A method of treating organic wastewater according to claim 3 wherein: the hydrogen peroxide is an aqueous solution with the mass fraction of 30 wt%.
8. A method of treating organic wastewater according to claim 3 wherein: the treatment time is 10-150 min.
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| CN113244937B (en) * | 2021-04-25 | 2022-05-03 | 中南民族大学 | Fenton oxidation water treatment method of coupling sludge biochar-iron phosphate catalyst |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102513141A (en) * | 2011-12-08 | 2012-06-27 | 中国科学院上海硅酸盐研究所 | Photocatalyst and preparation method and application thereof |
| CN105948216A (en) * | 2016-05-16 | 2016-09-21 | 江苏省环境科学研究院 | Airlift type heterogeneous Fenton reactor |
| CN106492860A (en) * | 2016-10-19 | 2017-03-15 | 常州大学 | A kind of preparation method of iron phosphate/manganese phosphate/yttrium phosphate composite catalyst |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN102513141A (en) * | 2011-12-08 | 2012-06-27 | 中国科学院上海硅酸盐研究所 | Photocatalyst and preparation method and application thereof |
| CN105948216A (en) * | 2016-05-16 | 2016-09-21 | 江苏省环境科学研究院 | Airlift type heterogeneous Fenton reactor |
| CN106492860A (en) * | 2016-10-19 | 2017-03-15 | 常州大学 | A kind of preparation method of iron phosphate/manganese phosphate/yttrium phosphate composite catalyst |
Non-Patent Citations (2)
| Title |
|---|
| Photo-Fenton reaction of dyes with Fe(III)-treated hydroxyapatites as heterogeneous catalysts in water;Moriguchi, T.、Nakagawa, S.;《Phosphorus Research Bulletin》;20121231;第26卷;39-52 * |
| 新型非均相Fenton催化剂的制备及其催化降解有机污染物性能研究;郭盛;《中国博士学位论文全文数据库》;20180115;B027-172 * |
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