CN110615501B - A kind of treatment method of landfill leachate - Google Patents
A kind of treatment method of landfill leachate Download PDFInfo
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- CN110615501B CN110615501B CN201910915915.8A CN201910915915A CN110615501B CN 110615501 B CN110615501 B CN 110615501B CN 201910915915 A CN201910915915 A CN 201910915915A CN 110615501 B CN110615501 B CN 110615501B
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- 239000000149 chemical water pollutant Substances 0.000 title claims abstract description 66
- 238000000034 method Methods 0.000 title claims abstract description 42
- 239000002245 particle Substances 0.000 claims abstract description 42
- 239000011790 ferrous sulphate Substances 0.000 claims abstract description 37
- 235000003891 ferrous sulphate Nutrition 0.000 claims abstract description 37
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 claims abstract description 37
- 229910000359 iron(II) sulfate Inorganic materials 0.000 claims abstract description 37
- 239000007788 liquid Substances 0.000 claims abstract description 31
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims abstract description 27
- 238000003756 stirring Methods 0.000 claims abstract description 20
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims abstract description 17
- 238000001556 precipitation Methods 0.000 claims abstract description 8
- 238000005868 electrolysis reaction Methods 0.000 claims abstract 4
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 17
- 238000006243 chemical reaction Methods 0.000 claims description 4
- 238000003672 processing method Methods 0.000 claims 1
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- 229910052725 zinc Inorganic materials 0.000 description 5
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 4
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 description 4
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- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 3
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 3
- 239000001569 carbon dioxide Substances 0.000 description 3
- 229910002092 carbon dioxide Inorganic materials 0.000 description 3
- 238000000354 decomposition reaction Methods 0.000 description 3
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- 230000015556 catabolic process Effects 0.000 description 2
- JOPOVCBBYLSVDA-UHFFFAOYSA-N chromium(6+) Chemical compound [Cr+6] JOPOVCBBYLSVDA-UHFFFAOYSA-N 0.000 description 2
- 238000010276 construction Methods 0.000 description 2
- 238000006731 degradation reaction Methods 0.000 description 2
- 238000006056 electrooxidation reaction Methods 0.000 description 2
- 239000000706 filtrate Substances 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 230000001678 irradiating effect Effects 0.000 description 2
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 2
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- 239000002244 precipitate Substances 0.000 description 2
- YGSDEFSMJLZEOE-UHFFFAOYSA-N salicylic acid Chemical compound OC(=O)C1=CC=CC=C1O YGSDEFSMJLZEOE-UHFFFAOYSA-N 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
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- JPVYNHNXODAKFH-UHFFFAOYSA-N Cu2+ Chemical compound [Cu+2] JPVYNHNXODAKFH-UHFFFAOYSA-N 0.000 description 1
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 1
- VTLYFUHAOXGGBS-UHFFFAOYSA-N Fe3+ Chemical compound [Fe+3] VTLYFUHAOXGGBS-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
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- 229910001431 copper ion Inorganic materials 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- SOCTUWSJJQCPFX-UHFFFAOYSA-N dichromate(2-) Chemical compound [O-][Cr](=O)(=O)O[Cr]([O-])(=O)=O SOCTUWSJJQCPFX-UHFFFAOYSA-N 0.000 description 1
- 229910001882 dioxygen Inorganic materials 0.000 description 1
- 201000010099 disease Diseases 0.000 description 1
- 208000037265 diseases, disorders, signs and symptoms Diseases 0.000 description 1
- 238000004993 emission spectroscopy Methods 0.000 description 1
- 238000000855 fermentation Methods 0.000 description 1
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- 229910001447 ferric ion Inorganic materials 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- TUJKJAMUKRIRHC-UHFFFAOYSA-N hydroxyl Chemical compound [OH] TUJKJAMUKRIRHC-UHFFFAOYSA-N 0.000 description 1
- 238000009616 inductively coupled plasma Methods 0.000 description 1
- 238000005342 ion exchange Methods 0.000 description 1
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 230000002427 irreversible effect Effects 0.000 description 1
- 229910052745 lead Inorganic materials 0.000 description 1
- RVPVRDXYQKGNMQ-UHFFFAOYSA-N lead(2+) Chemical compound [Pb+2] RVPVRDXYQKGNMQ-UHFFFAOYSA-N 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
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- 238000001728 nano-filtration Methods 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- FJKROLUGYXJWQN-UHFFFAOYSA-N papa-hydroxy-benzoic acid Natural products OC(=O)C1=CC=C(O)C=C1 FJKROLUGYXJWQN-UHFFFAOYSA-N 0.000 description 1
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N phenol group Chemical group C1(=CC=CC=C1)O ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 1
- 238000011112 process operation Methods 0.000 description 1
- 238000006479 redox reaction Methods 0.000 description 1
- 238000001223 reverse osmosis Methods 0.000 description 1
- 229960004889 salicylic acid Drugs 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
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- 239000002689 soil Substances 0.000 description 1
- 238000002798 spectrophotometry method Methods 0.000 description 1
- 230000002269 spontaneous effect Effects 0.000 description 1
- 239000001117 sulphuric acid Substances 0.000 description 1
- 235000011149 sulphuric acid Nutrition 0.000 description 1
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- 238000003786 synthesis reaction Methods 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 238000000108 ultra-filtration Methods 0.000 description 1
Images
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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
-
- 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
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/46109—Electrodes
- C02F1/46114—Electrodes in particulate form or with conductive and/or non conductive particles between them
-
- 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
- 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
- C02F1/4674—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation with halogen or compound of halogens, e.g. chlorine, bromine
-
- 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
-
- 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
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/46109—Electrodes
- C02F2001/46133—Electrodes characterised by the material
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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
- 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
- C02F2101/10—Inorganic compounds
- C02F2101/20—Heavy metals or heavy metal compounds
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- 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
- C02F2101/20—Heavy metals or heavy metal compounds
- C02F2101/22—Chromium or chromium compounds, e.g. chromates
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- 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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- 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
- C02F2305/023—Reactive oxygen species, singlet oxygen, OH radical
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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
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/10—Photocatalysts
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Abstract
本发明公开了一种垃圾渗滤液的处理方法，称取硫酸亚铁溶于垃圾渗滤液中，得硫酸盐掺渗滤液；称取g‑C3N4/PDI@MOF加入硫酸盐掺渗滤液中，搅匀，得颗粒电极混合渗滤液，再用稀硫酸和氢氧化钠调节pH至酸性；将颗粒电极混合渗滤液加入三维电极反应器中，颗粒电极混合渗滤液在边搅拌边可见光照射下进行电解反应，静置沉淀，固液分离，即得处理后的垃圾渗滤液。本发明可实现对垃圾渗滤液中COD、氨氮和多种重金属离子的同步高效去除；本发明的三维光电催化氧化技术对COD、氨氮和重金属离子的去除率明显高于单纯的电催化氧化技术、光催化氧化技术以及两种技术去除率之和；本发明去除工艺简单、成本低。
The invention discloses a method for treating landfill leachate. The ferrous sulfate is weighed and dissolved in the landfill leachate to obtain the sulfate-mixed leachate; g-C 3 N 4 /PDI@MOF is weighed and added to the sulfate-mixed leachate. The mixed leachate of the particle electrode is then adjusted to acidity with dilute sulfuric acid and sodium hydroxide; the mixed leachate of the particle electrode is added to the three-dimensional electrode reactor, and the mixed leachate of the particle electrode is irradiated with visible light while stirring. Carry out electrolysis reaction, stand for precipitation, and separate solid and liquid to obtain the treated landfill leachate. The present invention can realize the simultaneous and efficient removal of COD, ammonia nitrogen and various heavy metal ions in landfill leachate; The photocatalytic oxidation technology and the sum of the removal rates of the two technologies; the invention has a simple removal process and low cost.
Description
Technical Field
The invention relates to a method for treating landfill leachate, in particular to a method for treating landfill leachate by using a three-dimensional photoelectrocatalysis oxidation technology.
Background
The landfill leachate is a filtrate generated by spontaneous fermentation of garbage under anaerobic conditions in the landfill process. Generally, landfill leachate contains high-concentration organic pollutants, ammonia nitrogen, inorganic salts and heavy metals. The landfill leachate can not only spread diseases and directly harm human health, but also pollute surface water and cause irreversible damage to the original ecological environment of surrounding soil.
The current treatment technology for landfill leachate mainly comprises the following steps: physical chemical treatment technology, biological treatment technology and membrane treatment technology. The physical and chemical treatment technology mainly comprises the following steps: leachate concentration, stripping, activated carbon adsorption, ion exchange, advanced oxidation and the like, but the physicochemical treatment technology has the problems of single treatment target, high treatment cost, complex treatment process and the like. Although the methods can achieve high removal rate of a certain index in the leachate in a short time, the method is difficult to ensure that the indexes of ammonia nitrogen, organic pollutants, heavy metals and the like are efficiently removed at the same time. Moreover, the application of the physical and chemical treatment technology to treat the landfill leachate also causes other problems to be solved, for example, the concentrated solution generated by the leachate concentration technology still needs to be deeply treated; the stripping and activated carbon adsorption technology only transfers ammonia nitrogen from leachate to activated carbon, so that not only the treated waste liquid needs to be treated, but also the newly generated activated carbon waste needs to be treated; because the oxidant used in the advanced oxidation technology is generally toxic to human bodies, needs supporting safety guarantee and has high dependence on the dosage and performance of the oxidant, the problem of secondary pollution is easily caused in the disposal process, and serious safety accidents can be caused by misoperation of workers. The biological treatment technology is divided into an aerobic process, an anaerobic process and an anaerobic and aerobic combined process according to different process principles, and for the biological treatment technology, the problems of large process floor area, long process operation period, poor process removal effect, high process environment sensitivity and the like exist no matter which process is applied to treat the landfill leachate. The membrane treatment technology is divided into 4 types of microfiltration, ultrafiltration, nanofiltration and reverse osmosis according to the pore size of the material. The treatment of the landfill leachate by using the membrane method treatment technology has the problems of easy blockage of membrane pores, easy loss of membrane materials, unstable treatment working conditions and the like, and the residual waste membrane materials and leachate concentrated solution after the treatment of the leachate still need to be further treated.
Therefore, the existing treatment technology generally has the problems of complex treatment process, high treatment cost, single treatment target, further advanced treatment of the treated percolate and the like.
Disclosure of Invention
The purpose of the invention is as follows: aiming at the problems, the invention provides a method for treating landfill leachate by using a three-dimensional photoelectrocatalysis technology, which has simple treatment process and can realize the high-efficiency synchronous removal of organic pollutants, ammonia nitrogen and various heavy metal ions in the leachate.
The technical scheme is as follows: the invention relates to a method for treating landfill leachate, which comprises the steps of weighing ferrous sulfate, dissolving the ferrous sulfate in the landfill leachate to obtain sulfate-doped leachate; weighing g-C3N4adding/PDI @ MOF into the sulfate doped leachate, uniformly stirring to obtain a particle electrode mixed leachate, and adjusting the pH value to acidity by using dilute sulfuric acid and sodium hydroxide; adding the particle electrode mixed leachate into a three-dimensional electrode reactor, carrying out an electrolytic reaction on the particle electrode mixed leachate under the irradiation of visible light while stirring, standing for precipitation, and carrying out solid-liquid separation to obtain the treated landfill leachate.
Furthermore, the concentration of ferrous sulfate in the sulfate-doped leachate is 0.045-0.175 mol/L, the comprehensive removal effect and cost are further preferably 0.05-0.15 mol/L, and the concentration can be 0.05mol/L, 0.1mol/L or 0.15 mol/L.
Further, said g-C3N4The solid-liquid ratio of the/PDI @ MOF to the sulfate doped leachate is 0.0018-0.02: 1, the comprehensive removal effect and the cost are further preferably 0.002-0.01: 1, and the ratio can be 0.002:1, 0.006:1 or 0.01: 1.
Further, the voltage gradient of the electrolytic reaction is 0.35-1.75V/cm, the comprehensive removal effect and the cost are further preferably 0.5-1.5V/cm, and the comprehensive removal effect and the cost can be 0.5V/cm, 1V/cm or 1.5V/cm.
Further, the pH value of the particle electrode mixed leachate is adjusted to 2-4.
Furthermore, the time of the electrolytic reaction is 2-6 h, and the stirring speed is 30-120 rpm.
Adding the granular electrode mixed leachate into an electrolytic cell sample area of a three-dimensional electrode reactor, and after switching on direct current, mixing g-C in the leachate3N4the/PDI @ MO particles are polarized and converted to particle electrodes. Water molecules are hydrolyzed at the cathode of the particle electrode to generate hydroxide ions and hydrogen gas, and are hydrolyzed at the anode of the particle electrode to generate hydrogen ions and oxygen gas. At the same time, under the irradiation of visible light, g-C3N4the/PDI @ MOF particle electrode generates photocatalysis to generate a photoproduction hole and a photoproduction electron. The photo-generated electrons react with oxygen on the surface of the particle electrode and oxygen in the leachate to generate oxygen radicals, and the oxygen radicals further react with hydrogen ions to generate hydrogen peroxide molecules. The hydrogen peroxide molecules react with ferrous ions on the surface of the particle electrode and ferrous ions doped in the leachate to generate hydroxyl radicals. Meanwhile, the photoproduction cavity can directly oxidize water molecules to generate hydroxyl radicals; photogenerated holes can also directly oxidize and decompose part of the organic pollutants. The hydroxyl radicals can effectively degrade organic matters in the leachate to generate hydroxyl ions, carbon dioxide and water. Meanwhile, the hydroxyl radical can react with chloride ions in the leachate to generate a chloride ion radical, and the chloride ion radical can react with ammonia nitrogen to generate chloride ions and nitrogen. The generated ferric ions can obtain electrons at the particle electrode and the cathode of the main electrode of the electrolytic cell and are reduced into ferrous ions again. Hydroxyl ions generated on the surfaces of the particle electrode and the cathode of the main electrode of the electrolytic cell and hydroxyl ions generated by the redox reaction in the leachate react with divalent heavy metal ions in the leachate to generate hydroxyl precipitates. And the hexavalent chromium ions firstly react with carbon dioxide free radicals generated in the indirect process of the organic pollutants to generate trivalent chromium. The trivalent chromium reacts with the hydroxide ions to produce hydroxide precipitate. Meanwhile, due to the electromigration effect and the electroosmotic flow effect, part of the divalent heavy metal ions and trivalent chromium ions are transferred to the electrolytic bath Main electrode the cathode electrode surface and subsequently reacts with hydroxide ions at the electrode surface. Part of ammonia nitrogen is transferred to the surface of the main electrode anode by electromigration and is oxidized into nitrogen. Organic pollutants with different polarities are migrated to the surface of a main electrode (including an anode and a cathode) through electroosmotic flow, and pre-oxidation and pre-reduction decomposition are realized. The pre-decomposition step is beneficial to improving the degradation efficiency of hydroxyl radicals to organic matters.
Has the advantages that: compared with the prior art, the invention has the following remarkable advantages: (1) the invention can realize the synchronous and high-efficiency removal of COD, ammonia nitrogen and various heavy metal ions of zinc, copper, cadmium and chromium in the landfill leachate, and the removal rates of the COD, the ammonia nitrogen and the zinc, the copper, the cadmium and the chromium are respectively as high as 98%, 92% and 95%; (2) the removal rate of COD, ammonia nitrogen and heavy metal ions by the three-dimensional photoelectrocatalysis oxidation technology is obviously higher than the sum of the removal rates of the pure electrocatalysis oxidation technology, the photocatalysis oxidation technology and the two technologies; (3) the invention has simple removal process and low cost, and can not generate other problems to be further solved after treatment.
Drawings
FIG. 1 is a flow chart of the present invention.
Detailed Description
The invention is further described below with reference to the figures and examples.
It should be noted that the landfill leachate of the present invention is obtained from sanitary landfill of domestic garbage in Qingcheng mountain of Haizhou area, Lingyun harbor. The mass concentration of COD in the landfill leachate is 1205mg/L, the concentration of ammonia nitrogen is 757mg/L, and the heavy metal ions (Zn) contained in the landfill leachate are 34mg/L zinc ions2+) 15mg/L of copper ion (Cu)2+) 7mg/L of lead ion (Pb)2+) 21mg/L cadmium ion (Cd)2+) And 58mg/L total chromium (including hexavalent chromium and trivalent chromium ions).
g-C3N4Synthesis of/PDI @ MOF reference Construction of g-C3N4[ the term "/PDI @ MOF heterojunctions for the high effective light-driven definition of pharmaceutical and phenolic micropollutants", which is not described herein in detail.
For the construction of the three-dimensional electrode reactor, reference is made to "Operating optimization for the maintenance metal removal from the mechanical solid contacting flash in the three-dimensional electrochemical devices", which is not described herein again.
Example 1
Influence of ferrous sulfate concentration on removal rate of COD, ammonia nitrogen and heavy metal ions in landfill leachate
And (3) treating the landfill leachate: as shown in fig. 1, ferrous sulfate is weighed and dissolved in the landfill leachate to obtain sulfate-doped leachate, wherein the concentrations of the ferrous sulfate are respectively 0.025mol/L, 0.035mol/L, 0.045mol/L, 0.05mol/L, 0.1mol/L, 0.15mol/L, 0.155mol/L, 0.165mol/L and 0.175 mol/L; g-C is weighed according to the solid-to-liquid ratio of 0.002:1(g: mL) 3N4Mixing the/PDI @ MOF powder into the sulfate doped leachate, and uniformly stirring to obtain a granular electrode mixed leachate; adjusting the pH of the particle electrode mixed leachate by using dilute sulfuric acid and sodium hydroxide to ensure that the pH of the particle electrode mixed leachate is equal to 2; then pouring the granular electrode mixed leachate into an electrolytic cell sample area of a three-dimensional electrode reactor, and switching on a direct current power supply, wherein the voltage gradient is 0.5V/cm; and in the electrifying process, turning on a xenon lamp to carry out visible light irradiation on the particle electrode mixed leachate in the sample area, continuously stirring the particle electrode mixed leachate at the stirring speed of 30rpm for 2 hours, standing for precipitation, and carrying out solid-liquid separation to obtain the treated landfill leachate.
COD concentration detection and COD removal rate calculation: the concentration of Chemical Oxygen Demand (COD) in the landfill leachate is measured according to the national standard bichromate method for measuring water quality chemical oxygen demand (GB 11914-; the COD removal rate was calculated according to the formula (1), wherein RCODAs the removal rate of COD, c0And ctThe COD concentration (mg/L) of the landfill leachate before and after treatment is respectively shown.
Detecting the ammonia nitrogen concentration and calculating the ammonia nitrogen removal rate: the concentration of ammonia nitrogen in landfill leachate is measured according to the specification of ammonia nitrogen in water quality Measuring by quantitative salicylic acid spectrophotometry (HJ 536-2009); the ammonia nitrogen removal rate is calculated according to the formula (2), wherein RNFor ammonia nitrogen removal, cN0The initial concentration (mg/L) of ammonia nitrogen in the landfill leachate before treatment, cNtThe residual ammonia nitrogen concentration (mg/L) in the treated landfill leachate is adopted.
Detecting the concentration of the heavy metal ions and calculating the removal rate: the concentration of four heavy metal ions of zinc, copper, lead and cadmium in the landfill leachate is measured according to the method for measuring 32 elements in water quality by inductively coupled plasma emission spectrometry (HJ 776-2015), and the concentration of total chromium is measured according to the method for measuring flame atomic absorption spectrophotometry (HJ 757-2015) for water quality chromium; the removal rate of heavy metal M ions (M: Zn, Cu, Pb, Cd, Cr) is calculated according to the formula (3), wherein RMFor heavy metal ion removal rate, cM0Is the initial concentration (mg/L), c of heavy metal M ions in the landfill leachate before treatmentMtThe concentration (mg/L) of heavy metal M ions in the treated landfill leachate is shown.
The test results of the removal rate of COD, ammonia nitrogen and heavy metal ions in the landfill leachate are shown in table 1.
TABLE 1 influence of ferrous sulfate concentration on removal rate of COD, ammonia nitrogen and heavy metal ions in landfill leachate
As can be seen from Table 1, the removal rate of heavy metal ions is greater than 85%, and the change of the concentration of ferrous sulfate has no significant influence on the removal rate of heavy metal ions in the leachate. For the removal rate of COD and ammonia nitrogen in leachate, when the concentration of ferrous sulfate is less than 0.05mol/L (as in table 1, when the concentration of ferrous sulfate is 0.045, 0.035, 0.025mol/L and lower values not listed in table 1), the divalent iron ions react with hydrogen peroxide molecules to generate less hydroxyl radicals, so that the degradation of organic pollutants is insufficient and the oxidation efficiency of ammonia nitrogen is reduced, resulting in that the removal rate of COD is less than 79% and is significantly reduced with the reduction of the concentration of ferrous sulfate, resulting in that the removal rate of ammonia nitrogen is less than 72% and is significantly reduced with the reduction of the concentration of ferrous sulfate. When the concentration of the ferrous sulfate is equal to 0.05-0.15 mol/L (as shown in Table 1, when the concentration of the externally-doped ferrous sulfate is equal to 0.05, 0.10 and 0.15 mol/L), the externally-doped ferrous ions in the filtrate fully react with hydrogen peroxide molecules to generate a large amount of hydroxyl radicals, the hydroxyl radicals can effectively degrade organic matters in the leachate to generate hydroxyl ions, carbon dioxide and water, meanwhile, the hydroxyl ions can react with chloride ions in the leachate to generate chloride ion radicals, the chloride ion radicals can react with ammonia nitrogen to generate chloride ions and nitrogen, finally, the removal rate of COD is larger than 84%, and the removal rate of ammonia nitrogen is larger than 76%. When the ferrous sulfate concentration is greater than 0.15mol/L (as in table 1, the doped ferrous sulfate concentration is 0.155, 0.165, 0.175mol/L and higher values not listed in table 1), the change in ferrous sulfate concentration has no significant effect on COD removal rate and ammonia nitrogen removal rate. Therefore, in a comprehensive aspect, the benefit and the cost are combined, and when the concentration of the ferrous sulfate is equal to 0.05-0.15 mol/L, the removal rate of COD, ammonia nitrogen and heavy metal ions in the landfill leachate is improved most favorably.
Example 2
C3N4Influence of solid-liquid ratio of/PDI @ MOF and sulfate doped leachate on removal rate of COD, ammonia nitrogen and heavy metal ions in landfill leachate
And (3) treating the landfill leachate: weighing ferrous sulfate, and dissolving the ferrous sulfate into the landfill leachate to obtain sulfate-doped leachate, wherein the concentration of the ferrous sulfate is 0.15 mol/L; g-C is weighed according to the solid-to-liquid ratio of 0.001:1, 0.0015:1, 0.0018:1, 0.002:1, 0.006:1, 0.01:1, 0.012:1, 0.015:1 and 0.02:1(g: mL)3N4Mixing the/PDI @ MOF powder into the sulfate doped leachate, and uniformly stirring to obtain a granular electrode mixed leachate; the pH value of the mixed leachate of the particle electrode is adjusted by using dilute sulphuric acid and sodium hydroxide to ensure that the particles are chargedThe pH of the extremely mixed percolate is equal to 3; then pouring the granular electrode mixed leachate into an electrolytic cell sample area, and switching on a direct current power supply, wherein the voltage gradient is 1V/cm; and in the electrifying process, turning on a xenon lamp to carry out visible light irradiation on the particle electrode mixed leachate in the sample area, continuously stirring the particle electrode mixed leachate at the stirring speed of 75rpm for 4 hours, standing for precipitation, and carrying out solid-liquid separation to obtain the treated landfill leachate.
The COD concentration detection and the calculation of the COD removal rate, the ammonia nitrogen concentration detection and the calculation of the ammonia nitrogen removal rate, the heavy metal ion concentration detection and the calculation of the removal rate are the same as those in the example 1, and the test results are shown in the table 2.
TABLE 2C3N4Influence of solid-liquid ratio of/PDI @ MOF and sulfate doped leachate on removal rate of COD, ammonia nitrogen and heavy metal ions in landfill leachate
As can be seen from Table 2, when C is3N4The solid-to-liquid ratio of/PDI @ MOF to sulfate-doped leachate was less than 0.002:1(g: mL) (see Table 2, C3N4(PDI) @ MOF to sulfate-doped leachate at solid-to-liquid ratios of 0.0015, 0.0018, 0.001:1(g: mL) and lower ratios not listed in table 2), g-C under visible light irradiation3N4the/PDI @ MOF particle electrode generates less photoproduction holes and photoproduction electrons through photocatalysis, and then the generation amount of hydroxyl radicals and hydroxyl ions is reduced, so that the COD removal rate is less than 85%, and the COD removal rate is increased along with C3N4The solid-to-liquid ratio of the/PDI @ MOF to the sulfate doped leachate is reduced and remarkably reduced, so that the ammonia nitrogen removal rate is lower than 76 percent and the ammonia nitrogen removal rate is changed along with the C3N4The solid-liquid ratio of the/PDI @ MOF to the sulfate doped leachate is reduced and obviously reduced, so that the removal rate of heavy metal ions is lower than 83 percent and is along with C3N4The solid-to-liquid ratio of the/PDI @ MOF to the sulfate doped leachate is reduced and remarkably reduced. When C is present3N4The solid-to-liquid ratio of the/PDI @ MOF to the sulfate-doped leachate is equal to 0.002-0.01: 1(g: mL) (as shown in Table 2, C3N4(PDI) @ MOF to sulfate-doped leachate at a solid-to-liquid ratio of 0.002:1, 0.006:1, 0.01:1(g: mL), under irradiation with visible light g-C 3N4the/PDI @ MOF particle electrode generates a large amount of photo-generated holes and photo-generated electrons through photocatalysis, so that the generation amount of hydroxyl radicals and hydroxyl ions is sufficient, the COD removal rate is higher than 90%, the ammonia nitrogen removal rate is higher than 81%, and the heavy metal ion removal rate is higher than 86%. When C is present3N4The solid-to-liquid ratio of/PDI @ MOF to sulfate-doped leachate was greater than 0.01:1(g: mL) (see Table 2, C3N4(ii) solid to liquid ratio of/PDI @ MOF to sulfate-doped leachate-0.012: 1, 0.015:1, 0.02:1(g: mL) and higher ratios not listed in Table 2), C3N4The solid-liquid ratio change of the/PDI @ MOF and the sulfate doped leachate has no obvious influence on the removal rate of COD, ammonia nitrogen and heavy metal ions. Thus, in summary, combining benefits and costs, when C3N4When the solid-to-liquid ratio of the/PDI @ MOF to the sulfate doped leachate is equal to 0.002-0.01: 1(g: mL), the removal rate of COD, ammonia nitrogen and heavy metal ions in the landfill leachate is improved.
Example 3
Influence of voltage gradient on removal rate of COD, ammonia nitrogen and heavy metal ions in landfill leachate
And (3) treating the landfill leachate: weighing ferrous sulfate, and dissolving the ferrous sulfate into the landfill leachate to obtain sulfate-doped leachate, wherein the concentration of the ferrous sulfate is 0.15 mol/L; g-C is weighed according to the solid-to-liquid ratio of 0.01:1(g: mL) 3N4Mixing the/PDI @ MOF powder into the sulfate doped leachate, and uniformly stirring to obtain a granular electrode mixed leachate; adjusting the pH of the particle electrode mixed leachate by using dilute sulfuric acid and sodium hydroxide to ensure that the pH of the particle electrode mixed leachate is equal to 4; then pouring the mixed leachate of the particle electrodes into a sample area of an electrolytic cell, and switching on a direct current power supply, wherein the voltage gradients are respectively 0.25V/cm, 0.35V/cm, 0.45V/cm, 0.5V/cm, 1V/cm, 1.5V/cm, 1.55V/cm, 1.65V/cm and 1.75V/cm; in the electrifying process, a xenon lamp is turned on to carry out visible light irradiation on the particle electrode mixed percolate in the sample area, the particle electrode mixed percolate is continuously stirred at the stirring speed of 120rpm for 6 hours, and the mixture is stood for precipitationAnd carrying out solid-liquid separation to obtain the treated landfill leachate.
The COD concentration detection and the calculation of the COD removal rate, the ammonia nitrogen concentration detection and the calculation of the ammonia nitrogen removal rate, the heavy metal ion concentration detection and the calculation of the removal rate are the same as those in the example 1, and the test results are shown in the table 3.
TABLE 3 influence of voltage gradient on removal rate of COD, ammonia nitrogen and heavy metal ions in landfill leachate
As can be seen from table 3, when the voltage gradient is less than 0.5V/cm (as in table 3, when the voltage gradient is 0.45V/cm, 0.35V/cm, 0.25V/cm and lower values not listed in table 3), the electromigration and the electroosmotic flow are weak, so that the deposition yield of heavy metal ions on the surface of the cathode of the main electrode is reduced, the oxidation efficiency of ammonia nitrogen on the surface of the anode of the main electrode is reduced, the pretreatment effect of organic pollutants is deteriorated, and finally, the COD removal rate is less than 91% and is significantly reduced with the reduction of the voltage gradient, the ammonia nitrogen removal rate is less than 82% and is significantly reduced with the reduction of the voltage gradient, and the heavy metal removal rate is less than 89% and is significantly reduced with the reduction of the voltage gradient. When the voltage gradient is equal to 0.5-1.5V/cm (as shown in table 3, the voltage gradient is equal to 0.5V/cm, 1V/cm, and 1.5V/cm), under the action of electromigration and electroosmotic flow, part of divalent heavy metal and trivalent chromium ions are migrated to the surface of a cathode electrode of a main electrode of an electrolytic cell and then react with hydroxyl ions on the surface of the electrode, part of ammonia nitrogen is transferred to the surface of an anode of the main electrode through electromigration and oxidized into nitrogen, organic pollutants with different polarities are migrated to the surface of the main electrode (including the anode and the cathode) through electroosmotic flow, pre-oxidation and pre-reduction decomposition are realized, and finally, the COD removal rate is greater than 95%, the ammonia nitrogen removal rate is greater than 86%, and the heavy metal removal rate is greater than 90%. When the voltage gradient is more than 1.5V/cm (as shown in the table 3, when the voltage gradient is 1.55V/cm, 1.65V/cm and 1.75V/cm and higher values which are not listed in the table 3), the effect of the change of the voltage gradient on the removal rate of COD, ammonia nitrogen and heavy metals is not obvious. Therefore, in comprehensive terms, the benefit and the cost are combined, and when the voltage gradient is equal to 0.5-1.5V/cm, the removal rate of COD, ammonia nitrogen and heavy metal ions in the landfill leachate is improved most beneficially.
Comparative example 1
Weighing ferrous sulfate, and dissolving the ferrous sulfate into the domestic garbage leachate to obtain sulfate doped leachate, wherein the concentration of the ferrous sulfate is 0.15 mol/L; adjusting the pH value of the sulfate-doped percolate by using dilute sulfuric acid and sodium hydroxide to ensure that the pH value of the sulfate-doped percolate is equal to 4; then pouring the sulfate-doped percolate into a sample area of an electrolytic cell, and switching on a direct current power supply, wherein the voltage gradient is 1.5V/cm; and in the electrifying process, continuously stirring the leachate at the stirring speed of 120rpm, electrifying for 6 hours, standing for precipitation, and carrying out solid-liquid separation to obtain the landfill leachate subjected to electrochemical oxidation treatment.
Comparative example 2
Weighing ferrous sulfate, and dissolving the ferrous sulfate into the landfill leachate to obtain sulfate-doped leachate, wherein the concentration of the ferrous sulfate is 0.15 mol/L; g-C is weighed according to the solid-to-liquid ratio of 0.01:1(g: mL)3N4Mixing the/PDI @ MOF powder into the sulfate doped leachate, and uniformly stirring to obtain a granular electrode mixed leachate; adjusting the pH of the particle electrode mixed leachate by using dilute sulfuric acid and sodium hydroxide to ensure that the pH of the particle electrode mixed leachate is equal to 4; and (3) turning on a xenon lamp to carry out visible light irradiation on the particle electrode mixed leachate in the sample area, irradiating for 6 hours, standing for precipitation, and carrying out solid-liquid separation to obtain the landfill leachate subjected to photocatalytic oxidation treatment.
Example 4
Weighing ferrous sulfate, and dissolving the ferrous sulfate into the landfill leachate to obtain sulfate-doped leachate, wherein the concentration of the ferrous sulfate is 0.15 mol/L; g-C is weighed according to the solid-to-liquid ratio of 0.01:1(g: mL)3N4Mixing the/PDI @ MOF powder into the sulfate doped leachate, and uniformly stirring to obtain a granular electrode mixed leachate; adjusting the pH of the particle electrode mixed leachate by using dilute sulfuric acid and sodium hydroxide to ensure that the pH of the particle electrode mixed leachate is equal to 4; then pouring the granular electrode mixed leachate into an electrolytic cell sample area of a three-dimensional electrode reactor, and switching on a direct current power supply, wherein the voltage gradient is 1.5V/cm; in the electrifying process, the xenon lamp is turned on to carry out particle electrode in the sample areaAnd irradiating the mixed leachate with visible light, continuously stirring the particle electrode mixed leachate at the stirring speed of 120rpm, electrifying for 6 hours, standing for precipitation, and performing solid-liquid separation to obtain the landfill leachate subjected to three-dimensional photoelectrocatalysis oxidation treatment.
The landfill leachate treated by the comparative example 1, the comparative example 2 and the example 4 is respectively subjected to COD concentration detection and COD removal rate calculation, ammonia nitrogen concentration detection and ammonia nitrogen removal rate calculation, and heavy metal concentration detection and removal rate calculation, and the test results are shown in Table 4.
TABLE 4 influence of different treatment methods on removal rate of COD, ammonia nitrogen and heavy metal ions in landfill leachate
From the results in table 4, compared with two treatment methods, namely electrochemical oxidation and photocatalytic oxidation, the three-dimensional photoelectrocatalysis oxidation technology adopted by the invention can realize high-efficiency removal of COD, ammonia nitrogen and heavy metal ions in the landfill leachate, and moreover, the removal rate of the invention is higher than the sum of the removal rates of the comparative example 1 and the comparative example 2. The three-dimensional photoelectrocatalysis technology applied by the invention is obviously superior to the method which only applies electric technology, photocatalysis technology and the addition of the electric technology and the photocatalysis technology.
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