CN112429801A - Method for treating high-concentration organic wastewater by ultraviolet light in cooperation with electrochemical oxidation - Google Patents
Method for treating high-concentration organic wastewater by ultraviolet light in cooperation with electrochemical oxidation Download PDFInfo
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- 239000002351 wastewater Substances 0.000 title claims abstract description 58
- 238000006056 electrooxidation reaction Methods 0.000 title claims abstract description 34
- 238000000034 method Methods 0.000 title claims abstract description 20
- 229910003460 diamond Inorganic materials 0.000 claims abstract description 7
- 239000010432 diamond Substances 0.000 claims abstract description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 5
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 5
- 239000010405 anode material Substances 0.000 claims description 10
- 238000006243 chemical reaction Methods 0.000 claims description 10
- 239000003792 electrolyte Substances 0.000 claims description 3
- 229910001410 inorganic ion Inorganic materials 0.000 claims description 3
- 230000035484 reaction time Effects 0.000 claims description 2
- 230000003647 oxidation Effects 0.000 abstract description 8
- 238000007254 oxidation reaction Methods 0.000 abstract description 8
- XKMRRTOUMJRJIA-UHFFFAOYSA-N ammonia nh3 Chemical compound N.N XKMRRTOUMJRJIA-UHFFFAOYSA-N 0.000 abstract description 7
- 239000003344 environmental pollutant Substances 0.000 abstract description 7
- 231100000719 pollutant Toxicity 0.000 abstract description 7
- 230000000694 effects Effects 0.000 abstract description 6
- 230000015556 catabolic process Effects 0.000 abstract description 3
- 238000006731 degradation reaction Methods 0.000 abstract description 3
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 abstract description 3
- 229910052753 mercury Inorganic materials 0.000 abstract description 3
- 239000003153 chemical reaction reagent Substances 0.000 abstract description 2
- 238000005265 energy consumption Methods 0.000 abstract description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 18
- 239000000575 pesticide Substances 0.000 description 13
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 12
- 239000002957 persistent organic pollutant Substances 0.000 description 10
- 230000002195 synergetic effect Effects 0.000 description 10
- 239000000149 chemical water pollutant Substances 0.000 description 9
- 238000005516 engineering process Methods 0.000 description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 5
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 5
- 239000001301 oxygen Substances 0.000 description 5
- 229910052760 oxygen Inorganic materials 0.000 description 5
- 239000010813 municipal solid waste Substances 0.000 description 4
- 231100000357 carcinogen Toxicity 0.000 description 3
- 239000003183 carcinogenic agent Substances 0.000 description 3
- 238000000354 decomposition reaction Methods 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 239000012528 membrane Substances 0.000 description 3
- 238000007086 side reaction Methods 0.000 description 3
- 238000004065 wastewater treatment Methods 0.000 description 3
- 238000010170 biological method Methods 0.000 description 2
- 239000003054 catalyst Substances 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 230000007797 corrosion Effects 0.000 description 2
- 238000005260 corrosion Methods 0.000 description 2
- TUJKJAMUKRIRHC-UHFFFAOYSA-N hydroxyl Chemical compound [OH] TUJKJAMUKRIRHC-UHFFFAOYSA-N 0.000 description 2
- 230000005764 inhibitory process Effects 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 239000007800 oxidant agent Substances 0.000 description 2
- 238000006303 photolysis reaction Methods 0.000 description 2
- 230000015843 photosynthesis, light reaction Effects 0.000 description 2
- 241000282414 Homo sapiens Species 0.000 description 1
- 238000009303 advanced oxidation process reaction Methods 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 239000003242 anti bacterial agent Substances 0.000 description 1
- 229940088710 antibiotic agent Drugs 0.000 description 1
- 150000001491 aromatic compounds Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 229940124307 fluoroquinolone Drugs 0.000 description 1
- 229910001385 heavy metal Inorganic materials 0.000 description 1
- 150000002391 heterocyclic compounds Chemical class 0.000 description 1
- 239000013067 intermediate product Substances 0.000 description 1
- 238000001728 nano-filtration Methods 0.000 description 1
- 239000010815 organic waste Substances 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- YFSUTJLHUFNCNZ-UHFFFAOYSA-N perfluorooctane-1-sulfonic acid Chemical compound OS(=O)(=O)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)F YFSUTJLHUFNCNZ-UHFFFAOYSA-N 0.000 description 1
- SNGREZUHAYWORS-UHFFFAOYSA-N perfluorooctanoic acid Chemical compound OC(=O)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)F SNGREZUHAYWORS-UHFFFAOYSA-N 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 238000010791 quenching Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000001223 reverse osmosis Methods 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 239000002689 soil Substances 0.000 description 1
- 239000002910 solid waste Substances 0.000 description 1
- 150000003568 thioethers Chemical class 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
- 239000003643 water by type Substances 0.000 description 1
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- 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
- C02F1/32—Treatment of water, waste water, or sewage by irradiation with ultraviolet light
-
- 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
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/467—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction
- C02F1/4672—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation
-
- 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
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
-
- 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
- C02F2101/306—Pesticides
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
- C02F2103/06—Contaminated groundwater or leachate
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- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
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- Health & Medical Sciences (AREA)
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Abstract
The invention provides a method for treating high-concentration organic wastewater by ultraviolet light and electrochemical oxidation, which takes boron-doped diamond as an anode and a carbon felt as a cathode, simultaneously utilizes a 10W low-pressure mercury lamp as an ultraviolet light source, and can efficiently degrade and mineralize organic matters in the wastewater and simultaneously remove the content of ammonia nitrogen in the system under the external direct current. The experimental result shows that when the external direct current power supply is 10mA/cm2When the ultraviolet light is cooperated with the electrochemical oxidation system to treat COD in the wastewater, the energy consumption and the degradation effect reach the optimal ratio. By ultraviolet light in conjunction with electrochemistryRealizes the COD of the organic wastewater after the treatment of the oxidation systemCrAnd the advanced treatment of ammonia nitrogen. On the one hand, the invention realizes the efficient removal of COD in the organic wastewaterCrAnd on the other hand, additional chemical reagents are not required to be added, so that secondary pollutants are avoided, and the cost is saved.
Description
Technical Field
The invention belongs to the technical field of organic wastewater treatment, and relates to a method for treating high-concentration organic wastewater by ultraviolet light in cooperation with electrochemical oxidation.
Background
With the continuous development of the urbanization process in China, a large amount of high-concentration organic wastewater is generated in the production and living processes of residents. The high-concentration organic wastewater generated in production and life mainly has the following characteristics: firstly, the concentration of organic matters is high, the COD content is generally about 2000mg/L, and some COD content is even as high as tens of thousands; secondly, the color is high and peculiar smell is generated (for example, landfill leachate). Thirdly, the components are complex, most of organic wastewater contains aromatic and heterocyclic compounds and other refractory organic pollutants, heavy metals, sulfides and the like, and has stronger biological toxicity (such as pesticide wastewater). Fourthly, the water quality fluctuation, the organic pollutants in the wastewater generated in different seasons and different time periods are different in types. These high concentration organic waste waters, if not properly treated, can cause serious pollution to the water, soil and atmospheric environment. In addition, pollutants such as suspicious carcinogens, auxiliary carcinogens, carcinogens and the like contained in the wastewater can cause serious threats to the health of peripheral biological groups and even human beings through the biological enrichment function of a food chain. Therefore, the proper treatment of the wastewater becomes a focus of urgent solution in the current environmental management field.
At present, high-concentration organic wastewater treatment technologies and methods are continuously proposed and applied. The biological method becomes the leading process for treating the high-concentration organic wastewater due to the advantages of stable removal efficiency, low operation cost and the like, but the application of the biological method is severely restricted by factors such as complex components, poor biodegradability and the like of the high-concentration organic wastewater; although the membrane technology (nanofiltration and reverse osmosis) for treating the high-concentration organic wastewater can realize the standard discharge, the membrane technology has the problems of high energy consumption, large investment, unstable operation and the like,the separation effect of the membrane technology is only to separate pollutants which are difficult to degrade from high-concentration organic wastewater, the pollutants are not thoroughly degraded and mineralized, the obtained concentrated solution is high-risk wastewater, and serious harm can still be caused to the water environment due to improper treatment; the conventional advanced oxidation technology (AOPs) generates strong oxidizing free radicals (e.g.: OH, E) by adding catalysts, oxidants and the like02.80V) can effectively degrade organic pollutants in the water body, but the process is easy to generate a large amount of solid wastes in the treatment process, thereby causing secondary pollution. In addition, advanced oxidation technology requires additional oxidants, catalysts, and certainly increases operating costs.
Disclosure of Invention
Electrochemical oxidation is a novel high-efficiency and green water treatment technology, and in an electrochemical system, water molecules are oxidized into hydroxyl radicals on the surface of an anode, so that organic pollutants in a water body are degraded and mineralized. The non-active anode material represented by boron-doped diamond (BDD) has the advantages of high oxidation potential, wide potential window, low background current and good corrosion resistance, and is widely applied to degradation of organic pollutants. For example, Linyan Zhu et al found that an electrochemical system with BDD as the anode was able to degrade fluoroquinolone antibiotics. Junfeng Niu et al found that BDD as the anode of the electrochemical system can remove perfluorooctanoic acid (PFOS). Recently, researches have found that in the electrochemical system reaction process, surface hydroxyl radicals generated by anodic oxidation water can generate self-quenching reaction to generate hydrogen peroxide, and then oxygen evolution side reaction (formula 1 and formula 2) occurs, so that the utilization rate of the hydroxyl radicals is low, and the electrochemical oxidation efficiency is reduced. Notably, hydrogen peroxide is a major intermediate product for oxygen evolution side reactions. On the other hand, Sharpless, Charels M and the like found that ultraviolet light can efficiently photolyze hydrogen peroxide to generate hydroxyl radicals (formula 3).
BDD+H2O–e-＝BDD(·OH)+H+(formula 1)
2BDD(·OH)＝BDD(H2O2) (formula 2)
H2O2+ UV (λ 254nm) → 2. OH (formula 3)
Based on the analysis, the invention develops a novel process of ultraviolet light synergistic electrochemical oxidation, UV is introduced into an electrochemical system, and H generated by water generated by electrochemical oxidation is photolyzed by UV2O2The method effectively inhibits the occurrence of oxygen evolution side reaction, increases the effective utilization rate of hydroxyl free radicals, and aims to realize the high-efficiency and deep treatment of the high-concentration organic wastewater, further realize the standard-reaching discharge of the high-concentration organic wastewater, and provides a new scheme for solving the problem of the treatment of the current high-concentration organic wastewater, wherein the specific technical scheme is as follows:
a method for treating high-concentration organic wastewater by ultraviolet light in cooperation with electrochemical oxidation is characterized by comprising the following steps: inorganic ions in the high-concentration organic wastewater are used as electrolyte to construct an electrochemical oxidation system; degrading organic pollutants and ammonia nitrogen by active species such as hydroxyl radicals and hydrogen peroxide generated by anodic oxidation of water; decomposition of H on the surface of the anode by UV light2O2Generation of hydroxyl radical, inhibition of H2O2Self-decomposition is carried out to generate oxygen and water, and meanwhile, hydroxyl free radicals adsorbed on the surface of the electrode are promoted to be released into a solution system in a free state, so that the utilization efficiency of the hydroxyl free radicals is improved, and the organic pollutants difficult to degrade in the high-concentration organic wastewater are efficiently and thoroughly mineralized into CO2And H2O, adopting carbon felt as a cathode, boron-doped diamond as an anode and adding 5-16mA/cm2And the direct-current power supply is used for adding high-concentration organic wastewater into the electrochemical reactor and carrying out a photoelectrocatalysis reaction on the high-concentration organic wastewater under the irradiation of an ultraviolet light source.
Preferably, inorganic ions in the organic wastewater are used as the electrolyte.
Preferably, characterized in that: the volume consumption of the high-concentration organic wastewater is 100-200mL, and the photoelectrocatalysis reaction time is 10-13 hours.
Preferably, the anode material is an inactive anode material; the wavelength range of the ultraviolet light source is lambda less than 280nm, and the power is 5-20W.
The invention provides a method for treating high-concentration organic wastewater by ultraviolet light synergistic electrochemical oxidation, which is applied to the field of advanced treatment of organic wastewater.
The invention has the advantages that: (1) the ultraviolet synergetic electrochemical oxidation system has simple process flow and high cost performance, and can be used for laboratory operation and industrial application. (2) The anode material used in the invention has good stability and corrosion resistance, and can effectively degrade pollutants and remove ammonia nitrogen. (3) The ultraviolet lamp source used in the invention is a low-pressure mercury lamp of 10W, the equipment is simple, and the cost is low. (4) The ultraviolet synergetic electrochemical oxidation system does not need to additionally add chemical reagents, and saves the operation cost. (5) The ultraviolet light is cooperated with the electrochemical oxidation system, and the anode material is oxidized into H generated by water through the photolysis of ultraviolet light2O2The hydroxyl free radicals are decomposed into free hydroxyl free radicals, so that the electrochemical oxidation efficiency is improved, the high-efficiency degradation of organic pollutants which are difficult to degrade in the high-concentration organic wastewater is realized, and a new method is provided for the advanced treatment of the high-concentration organic wastewater.
Drawings
FIG. 1 shows COD before and after 12 hours reaction of ultraviolet light (λ 254nm) cooperating with electrochemical oxidation system, electrochemical system and ultraviolet light system for treating landfill leachateCrA change in (c).
Fig. 2 is a water sample effect diagram before and after 12-hour reaction of garbage leachate treatment by ultraviolet light (lambda is 254nm) cooperated with an electrochemical oxidation system.
FIG. 3 shows COD before and after the UV light (lambda ═ 254nm) synergistic electrochemical oxidation system, electrochemical system, and UV light system respectively treat the pesticide wastewater for 12 hours reactionCrA change in (c).
Fig. 4 is a water sample effect diagram before and after the pesticide wastewater is treated by the ultraviolet light (lambda is 254nm) cooperated with the electrochemical oxidation system for 12 hours reaction.
Detailed Description
In order to make the technical problems, technical schemes and beneficial effects to be solved by the invention more clear and clear, the invention is further explained in detail by taking the garbage leachate and the pesticide wastewater as the embodiment of the high-concentration organic wastewater. The specific embodiments described herein are merely illustrative of the invention and are not intended to be limiting.
Example 1:
the ultraviolet light is cooperated with the electrochemical oxidation system to treat the landfill leachate, the COD of the landfill leachate is 3000-4000mg/L, and the ammonia nitrogen is 300-500 mg/L.
Firstly, placing 200mL landfill leachate in a photoelectrocatalysis reactor, placing BDD (boron-doped diamond) as an anode and a carbon felt as a cathode in high-concentration organic wastewater, and adjusting the applied current to be 10mA/cm2The method comprises the steps of treating the garbage leachate by using the original garbage leachate as the initial concentration of reaction under the irradiation of an ultraviolet light source with the wavelength of 254nm, and treating high-concentration organic wastewater by using ultraviolet light irradiation alone and an electrochemical oxidation system alone as a control test.
The experimental result shows that the COD of the landfill leachate is treated by photoelectrocatalysis oxidation for 12 hours under the irradiation of ultraviolet light with the wavelength of 254nmCrThe concentration is 63mg/L, and the ammonia nitrogen concentration is 37 mg/L. Specific data of water quality before and after the landfill leachate is treated by the ultraviolet light synergistic electrochemical oxidation system are shown in table 1, and figure 1 is a COD removal effect diagram of a comparative test.
The following table shows the change of the pollutant content in the landfill leachate before and after the treatment by adopting the ultraviolet light synergistic electrochemical oxidation system:
example 2:
the ultraviolet light is cooperated with the electrochemical oxidation system to treat the pesticide wastewater, the COD of the pesticide is 8000-10000mg/L, and the ammonia nitrogen is 200-300 mg/L.
Firstly, putting 200mL pesticide wastewater into a photoelectrocatalysis reactor, putting BDD (boron-doped diamond) as an anode and a carbon felt as a cathode into the pesticide wastewater, and adjusting the applied current to be 10mA/cm2Under the irradiation of an ultraviolet light source with the wavelength of 254nm, the pesticide wastewater is subjected to a photoelectrocatalysis reaction for 12 hours, and the high-concentration organic wastewater is treated by singly using ultraviolet irradiation and a singly using electrochemical oxidation system as a control test.
By constructing an ultraviolet light synergistic electrochemical oxidation systemHydroxyl free radicals, hydrogen peroxide and other active species generated by the polar oxidation of water are adsorbed on the surface of the electrode to degrade organic pollutants; h generated by photolysis of anode by ultraviolet2O2Generation of hydroxyl radical, inhibition of H2O2The self-decomposition generates oxygen and water, the effective utilization rate of hydroxyl radicals is improved, and organic pollutants in the pesticide wastewater are effectively removed. Specific data of water quality before and after the pesticide wastewater is treated by the ultraviolet light synergistic electrochemical oxidation system are shown in table 1, and fig. 2 is a COD removal effect graph of a comparative test.
The following table is a table of the change of the pollutant content in the pesticide wastewater before and after the treatment of the ultraviolet light synergistic electrochemical oxidation system:
the foregoing is only a preferred embodiment of the present invention, and the anode material in the present invention is not limited to boron-doped diamond, but is also applicable to any other anode material; the ultraviolet lamp source used in the invention is not limited to a low-pressure mercury lamp with the wavelength of 254nm and the power of 10W, and can be still applicable to ultraviolet light with other wave bands and powers. It will be apparent to those skilled in the art that the anode material, the source of ultraviolet light, and the like can be rearranged and substituted without departing from the scope of the invention. The application field of the invention is not limited to the treatment of landfill leachate and pesticide wastewater, and can also be applied to the treatment of other wastewater without departing from the concept of the invention. The scope of the invention is to be determined by the scope of the appended claims.
Claims (4)
1. A method for treating high-concentration organic wastewater by ultraviolet light in cooperation with electrochemical oxidation is characterized by comprising the following steps: introducing ultraviolet light into electrochemical oxidation system, using carbon felt as cathode, boron-doped diamond as anode, and adding 5-16mA/cm2And the direct-current power supply is used for adding high-concentration organic wastewater into the electrochemical reactor and carrying out a photoelectrocatalysis reaction on the high-concentration organic wastewater under the irradiation of an ultraviolet light source.
2. The method for treating high-concentration organic wastewater by ultraviolet light cooperated with electrochemical oxidation according to claim 1, wherein: inorganic ions in the organic wastewater are used as electrolyte.
3. The method for treating high-concentration organic wastewater by ultraviolet light cooperated with electrochemical oxidation according to claim 1, wherein: the volume consumption of the high-concentration organic wastewater is 100-200mL, and the photoelectrocatalysis reaction time is 10-13 hours.
4. The method for treating high-concentration organic wastewater by ultraviolet light cooperated with electrochemical oxidation according to any one of claims 1-3, wherein: the anode material is an inactive anode material; the wavelength range of the ultraviolet light source is lambda less than 280nm, and the power is 5-20W.
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