CN113458127A - Cooperative disposal method for household garbage incineration fly ash and pyrite tailing - Google Patents
Cooperative disposal method for household garbage incineration fly ash and pyrite tailing Download PDFInfo
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- CN113458127A CN113458127A CN202110925064.2A CN202110925064A CN113458127A CN 113458127 A CN113458127 A CN 113458127A CN 202110925064 A CN202110925064 A CN 202110925064A CN 113458127 A CN113458127 A CN 113458127A
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- Prior art keywords
- tailing
- fly ash
- pyrite
- layer
- reaction
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- 239000010881 fly ash Substances 0.000 title claims abstract description 63
- NIFIFKQPDTWWGU-UHFFFAOYSA-N pyrite Chemical compound [Fe+2].[S-][S-] NIFIFKQPDTWWGU-UHFFFAOYSA-N 0.000 title claims abstract description 57
- 229910052683 pyrite Inorganic materials 0.000 title claims abstract description 57
- 239000011028 pyrite Substances 0.000 title claims abstract description 57
- 238000000034 method Methods 0.000 title claims abstract description 25
- 239000010813 municipal solid waste Substances 0.000 title claims abstract description 19
- 239000010410 layer Substances 0.000 claims abstract description 68
- 238000006243 chemical reaction Methods 0.000 claims abstract description 50
- 239000004576 sand Substances 0.000 claims abstract description 47
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 42
- 239000012265 solid product Substances 0.000 claims abstract description 41
- 239000002002 slurry Substances 0.000 claims abstract description 32
- 229910052742 iron Inorganic materials 0.000 claims abstract description 20
- 238000002156 mixing Methods 0.000 claims abstract description 20
- 238000001027 hydrothermal synthesis Methods 0.000 claims abstract description 18
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 17
- 239000001301 oxygen Substances 0.000 claims abstract description 14
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 14
- 239000002344 surface layer Substances 0.000 claims abstract description 14
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 13
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 13
- 239000003895 organic fertilizer Substances 0.000 claims abstract description 12
- 239000007788 liquid Substances 0.000 claims abstract description 11
- SZVJSHCCFOBDDC-UHFFFAOYSA-N iron(II,III) oxide Inorganic materials O=[Fe]O[Fe]O[Fe]=O SZVJSHCCFOBDDC-UHFFFAOYSA-N 0.000 claims abstract description 10
- 238000003860 storage Methods 0.000 claims abstract description 8
- 239000000706 filtrate Substances 0.000 claims abstract description 7
- 238000004537 pulping Methods 0.000 claims abstract description 6
- 238000000926 separation method Methods 0.000 claims abstract description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 38
- 241000196324 Embryophyta Species 0.000 claims description 21
- 239000000203 mixture Substances 0.000 claims description 14
- 238000010438 heat treatment Methods 0.000 claims description 10
- 239000007791 liquid phase Substances 0.000 claims description 8
- 238000000605 extraction Methods 0.000 claims description 7
- 230000035484 reaction time Effects 0.000 claims description 7
- 241000209082 Lolium Species 0.000 claims description 6
- 241000219823 Medicago Species 0.000 claims description 6
- 235000017587 Medicago sativa ssp. sativa Nutrition 0.000 claims description 6
- 235000010086 Setaria viridis var. viridis Nutrition 0.000 claims description 6
- 239000007790 solid phase Substances 0.000 claims description 5
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 claims description 4
- 229910000359 iron(II) sulfate Inorganic materials 0.000 claims description 4
- 230000003472 neutralizing effect Effects 0.000 claims description 4
- MBMLMWLHJBBADN-UHFFFAOYSA-N Ferrous sulfide Chemical compound [Fe]=S MBMLMWLHJBBADN-UHFFFAOYSA-N 0.000 claims description 3
- 239000003054 catalyst Substances 0.000 claims description 3
- 239000011790 ferrous sulphate Substances 0.000 claims description 3
- 235000003891 ferrous sulphate Nutrition 0.000 claims description 3
- 238000000354 decomposition reaction Methods 0.000 claims description 2
- 238000010992 reflux Methods 0.000 claims description 2
- HGUFODBRKLSHSI-UHFFFAOYSA-N 2,3,7,8-tetrachloro-dibenzo-p-dioxin Chemical compound O1C2=CC(Cl)=C(Cl)C=C2OC2=C1C=C(Cl)C(Cl)=C2 HGUFODBRKLSHSI-UHFFFAOYSA-N 0.000 claims 5
- 244000230342 green foxtail Species 0.000 claims 1
- 150000002013 dioxins Chemical class 0.000 abstract description 4
- 230000008569 process Effects 0.000 abstract description 4
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 abstract description 3
- 230000007704 transition Effects 0.000 abstract description 3
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 abstract description 2
- 229910001448 ferrous ion Inorganic materials 0.000 abstract description 2
- 230000001590 oxidative effect Effects 0.000 abstract description 2
- 239000002689 soil Substances 0.000 description 32
- KVGZZAHHUNAVKZ-UHFFFAOYSA-N 1,4-Dioxin Chemical group O1C=COC=C1 KVGZZAHHUNAVKZ-UHFFFAOYSA-N 0.000 description 23
- 238000002386 leaching Methods 0.000 description 20
- 229910001385 heavy metal Inorganic materials 0.000 description 17
- 230000006872 improvement Effects 0.000 description 12
- 238000003914 acid mine drainage Methods 0.000 description 9
- 239000000047 product Substances 0.000 description 9
- 239000002253 acid Substances 0.000 description 8
- 244000025254 Cannabis sativa Species 0.000 description 7
- 239000000463 material Substances 0.000 description 7
- 239000011159 matrix material Substances 0.000 description 7
- 230000003647 oxidation Effects 0.000 description 7
- 238000004056 waste incineration Methods 0.000 description 7
- OSGAYBCDTDRGGQ-UHFFFAOYSA-L calcium sulfate Chemical compound [Ca+2].[O-]S([O-])(=O)=O OSGAYBCDTDRGGQ-UHFFFAOYSA-L 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- 244000304962 green bristle grass Species 0.000 description 6
- 230000004083 survival effect Effects 0.000 description 6
- 231100000419 toxicity Toxicity 0.000 description 6
- 230000001988 toxicity Effects 0.000 description 6
- 239000008213 purified water Substances 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- 239000012071 phase Substances 0.000 description 4
- 238000005067 remediation Methods 0.000 description 4
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 3
- 230000015556 catabolic process Effects 0.000 description 3
- 238000006731 degradation reaction Methods 0.000 description 3
- 230000002378 acidificating effect Effects 0.000 description 2
- 239000002956 ash Substances 0.000 description 2
- 230000004888 barrier function Effects 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 239000002734 clay mineral Substances 0.000 description 2
- 238000001514 detection method Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 239000003337 fertilizer Substances 0.000 description 2
- 230000035784 germination Effects 0.000 description 2
- 239000004615 ingredient Substances 0.000 description 2
- 238000005065 mining Methods 0.000 description 2
- 230000020477 pH reduction Effects 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- -1 polytetrafluoroethylene Polymers 0.000 description 2
- 238000003672 processing method Methods 0.000 description 2
- 238000011084 recovery Methods 0.000 description 2
- 239000010865 sewage Substances 0.000 description 2
- 238000002791 soaking Methods 0.000 description 2
- 230000007480 spreading Effects 0.000 description 2
- 238000003892 spreading Methods 0.000 description 2
- 230000006641 stabilisation Effects 0.000 description 2
- 238000011105 stabilization Methods 0.000 description 2
- 231100000331 toxic Toxicity 0.000 description 2
- 230000002588 toxic effect Effects 0.000 description 2
- 238000009966 trimming Methods 0.000 description 2
- 241000894006 Bacteria Species 0.000 description 1
- BHPQYMZQTOCNFJ-UHFFFAOYSA-N Calcium cation Chemical group [Ca+2] BHPQYMZQTOCNFJ-UHFFFAOYSA-N 0.000 description 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 1
- 240000004296 Lolium perenne Species 0.000 description 1
- 240000004658 Medicago sativa Species 0.000 description 1
- 235000010624 Medicago sativa Nutrition 0.000 description 1
- 208000034189 Sclerosis Diseases 0.000 description 1
- 235000002248 Setaria viridis Nutrition 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 1
- 239000005864 Sulphur Substances 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- 230000001133 acceleration Effects 0.000 description 1
- 230000000844 anti-bacterial effect Effects 0.000 description 1
- 239000003899 bactericide agent Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 239000011651 chromium Substances 0.000 description 1
- 238000011278 co-treatment Methods 0.000 description 1
- 230000001276 controlling effect Effects 0.000 description 1
- 230000000185 dioxinlike effect Effects 0.000 description 1
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- 239000010791 domestic waste Substances 0.000 description 1
- 230000002327 eosinophilic effect Effects 0.000 description 1
- 230000007717 exclusion Effects 0.000 description 1
- 239000000284 extract Substances 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- 239000003546 flue gas Substances 0.000 description 1
- 239000002920 hazardous waste Substances 0.000 description 1
- 229910052500 inorganic mineral Inorganic materials 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 238000003973 irrigation Methods 0.000 description 1
- 230000002262 irrigation Effects 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 229910052976 metal sulfide Inorganic materials 0.000 description 1
- 244000005700 microbiome Species 0.000 description 1
- 239000011707 mineral Substances 0.000 description 1
- 235000010755 mineral Nutrition 0.000 description 1
- 239000011268 mixed slurry Substances 0.000 description 1
- 238000010525 oxidative degradation reaction Methods 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 238000002161 passivation Methods 0.000 description 1
- 230000002085 persistent effect Effects 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 238000004382 potting Methods 0.000 description 1
- 230000002265 prevention Effects 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 230000000087 stabilizing effect Effects 0.000 description 1
- 229910052569 sulfide mineral Inorganic materials 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09B—DISPOSAL OF SOLID WASTE NOT OTHERWISE PROVIDED FOR
- B09B3/00—Destroying solid waste or transforming solid waste into something useful or harmless
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09B—DISPOSAL OF SOLID WASTE NOT OTHERWISE PROVIDED FOR
- B09B5/00—Operations not covered by a single other subclass or by a single other group in this subclass
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/54—Improvements relating to the production of bulk chemicals using solvents, e.g. supercritical solvents or ionic liquids
Landscapes
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Processing Of Solid Wastes (AREA)
Abstract
The invention discloses a method for the cooperative disposal of fly ash from incineration of household garbage and pyrite tailing. Firstly, mixing the yellow iron tailing sand and fly ash for pulping. And secondly, placing the slurry in a reaction kettle to sequentially pass through a hydrothermal reaction stage, a transition stage and a supercritical oxidation reaction stage. And thirdly, carrying out solid-liquid separation on the treated slurry to obtain a solid product and a filtrate. Sixthly, excavating surface layer tailing sand of the pyrite tailing pond field; covering a solid product on a pyrite tailing storage site and compacting to form a tailing covering layer; the tailing covering layer is used for preventing oxygen and rainwater from seeping downwards, and the alkalinity of the tailing covering layer is utilized to neutralize the lower yellow iron tailing sand. Paving a vegetation planting layer on the tailing covering layer; and D, mixing the vegetation planting layer with the surface layer tailing sand, the solid product obtained in the step five, a water-retaining agent and an organic fertilizer to obtain the vegetation planting layer. The invention utilizes ferrous ions of the yellow iron tailings to generate magnetite in the hydrothermal reaction process; magnetite is capable of catalytically oxidizing dioxins in the presence of ozone.
Description
Technical Field
The invention relates to the technical field of waste incineration fly ash treatment and the technical field of environmental remediation, in particular to a method for cooperatively treating household waste incineration fly ash and pyrite tailing.
Background
In recent years, with the acceleration of urbanization and the improvement of living standard, municipal solid waste is rapidly increased, and the realization of harmless, quantitative reduction and resource treatment of municipal solid waste is an urgent problem to be solved, and countries encourage and support the comprehensive resource utilization of waste incineration fly ash, but the waste incineration fly ash has complex surface characteristics, so that high-concentration inorganic and organic pollutants are adsorbed or formed from flue gas, especially the waste incineration fly ash often contains high-concentration heavy metals and trace amount highly toxic dioxin compounds, and is a two-material hazardous waste which has both heavy metal hazard characteristics and environmental persistent organic toxicity hazard characteristics, and the resource utilization of the waste incineration fly ash is restricted by the high-concentration soluble salt substances. In the technical specification (trial) for controlling pollution of the fly ash generated by burning the household garbage (HJ1134-2020), the total amount of dioxin residues in the solid product of the fly ash generated by burning the household garbage is regulated not to exceed 50ng-TEQ/kg (calculated by the dry weight of the fly ash). Therefore, the fly ash disposal and utilization technology is very important for removing dioxin and stabilizing/curing treatment of abundant toxic heavy metals such as lead, cadmium, chromium and the like.
After mining, the pyrite tailing exposes metal sulfide to oxidation conditions, and is very easily oxidized to form mining acid wastewater rich in iron, sulfate radical and heavy metal, namely Acid Mine Drainage (AMD) through weathering and leaching, and the generation of the typical Acid Mine Drainage (AMD) starts from the oxidation of pyrite into ferrous iron and sulfate (FeS)2+7/2O2+H2O＝FeSO4+H2SO4). Since AMD is formed by oxidation of sulphide minerals in the presence of oxygen, water and microorganisms (e.g. eosinophilic iron and sulphur oxidising bacteria), exclusion of any of these three components can limit AMD formation. The existing research of the prevention technology of acid mine drainage can be divided into the following categories: oxygen barrier, utilization of bactericides, co-treatment and blending, passivation of sulfide minerals and the like. However, in practical engineering applications, the method adopted is to cut off the acidification condition of ore sand by oxygen barrier through simple surface soil covering or vegetation planting, and the ore sand can be treated in such a wayThe effect of (2) is not good, the covering soil can not neutralize the acidity of the ore sand matrix at the lower layer, and can not completely isolate oxygen, the time of less than one year after the covering soil of the ore sand which is not improved is planted, the soil is found to be seriously re-acidified, the pH value is obviously reduced, and the vegetation re-greening effect is poor. Therefore, for the treatment of the pyrite tailing, the improvement treatment needs to be carried out by combining a chemical means, and then the source removal needs to be carried out by combining a physical means, so that the mine restoration is fundamentally realized.
Disclosure of Invention
The invention aims to provide a method for cooperatively treating waste incineration fly ash and pyrite tailing.
The purpose of the invention can be realized by the following technical scheme: a co-processing method of household garbage incineration fly ash and pyrite tailing comprises the following steps:
step one, mixing the pyrite tailing sand and the fly ash to obtain a fly ash mixture, and pulping by using the fly ash mixture to obtain slurry.
Step two, placing the slurry in a reaction kettle, heating to hydrothermal reaction conditions, starting hydrothermal reaction and introducing O3. Iron sulfide in the pyrite tailing generates ferroferric oxide under hydrothermal reaction, the ferroferric oxide and ferrous sulfate contained in the pyrite tailing are used as catalysts, and solid-phase dioxin adsorbed on the surface of fly ash is catalyzed and oxidized in a hydrothermal environment.
Step three, heating the slurry to extraction reaction conditions to enable water to be in a subcritical state, and introducing O3Carrying out reaction; and (3) carrying out homogeneous reaction on the water and the dioxin, so that the solid-phase dioxin adsorbed in the micropores inside the fly ash is extracted and dissolved into a liquid phase.
Step four, heating the slurry to the supercritical oxidation reaction condition, and introducing O3Carrying out reaction; in the course of the reaction, O3Decomposition into O2And active oxygen free radicals which react with the dioxin in the liquid phase to completely oxidize and decompose the dioxin in the liquid phase.
And step five, carrying out solid-liquid separation on the slurry treated in the step four to obtain a solid product and a filtrate.
Step six, digging surface layer tailing sand of the pyrite tailing pond field; covering a solid product on a pyrite tailing storage site and compacting to form a tailing covering layer; the tailing covering layer is used for preventing oxygen and rainwater from seeping downwards, and the alkalinity of the tailing covering layer is utilized to neutralize the lower yellow iron tailing sand. Paving a vegetation planting layer on the tailing covering layer; and D, mixing the vegetation planting layer with the surface layer tailing sand, the solid product obtained in the step five, a water-retaining agent and an organic fertilizer to obtain the vegetation planting layer.
Preferably, the mass fraction of the water-retaining agent in the vegetation planting layer is 0.3-1%, the mass fraction of the organic fertilizer is 3-10%, and the mass fraction of the solid product is 15-25%.
Preferably, in the fly ash mixture obtained in the first step, the mass fraction of the pyrite tailing sand is 25-40%.
Preferably, the slurry in the first step is prepared by mixing the fly ash mixture and water in a solid-to-liquid ratio of 1: 2-1: 8, mixing uniformly to obtain the product. The pH value of the obtained slurry is 11-12.
Preferably, the hydrothermal reaction in the second step is carried out at the temperature of 150-230 ℃ and the pressure of 2-10 Mpa, and the reaction time is 5-15 min; o is3The flow rate of the water is 10-100 mL/min;
preferably, the extraction reaction conditions in the third step are that the temperature is 250-325 ℃, the pressure is 2-10 Mpa, the reaction time is 15-30 min, and O is3The flow rate of (A) is 10 to 100 mL/min.
Preferably, the supercritical oxidation reaction conditions in the fourth step are 375-475 ℃, 22.5-27.5 Mpa, 1-10 min of reaction time and O3The flow rate of the water is 10-100 mL/min;
preferably, the filtrate obtained in the fifth step is refluxed to the first step for pulping.
Preferably, in the sixth step, the vegetation planting layer is covered with black gauze and planted with one or more of ryegrass, green bristlegrass and alfalfa. And removing the black gauze after the plants in the vegetation planting layer germinate.
The invention has the beneficial effects that:
1. the invention mixes the yellow iron tailing sand and the fly ash to prepare the slurry, ferrous ions of the yellow iron tailing sand exist in the form of ferrous sulfate in the mixed slurry, and magnetite (Fe) can be generated in the hydrothermal reaction process3O4) (ii) a Magnetite can catalytically oxidize dioxin in the presence of ozone; in addition, the present invention extracts dioxin in the micropores of the fly ash into a liquid phase in a subcritical state, and water molecules in the supercritical state move at a high speed in a supercritical oxidation reaction stage, and when nonpolar dioxin substances are in supercritical water, the water molecules repeatedly collide with the dioxin molecules, thereby rapidly and efficiently decomposing and oxidizing the dioxin.
2. The method comprises the steps of mixing the pyrite tailing sand and the solid product obtained by treatment, adding an organic fertilizer and a water-retaining agent to obtain a vegetation planting layer, and planting after the vegetation planting layer is laid on a tailing covering layer; the effective and long-term greening of the pyrite tailing can be realized without introducing high-quality soil from the outside.
3. According to the method, a large amount of sulfate ions in the pyrite tailing sand and fly ash rich in calcium ions form a calcium sulfate crystalline phase, and the treated product is used as a covering layer of the ore sand in a tailing pond to isolate the contact of oxygen and pyrite. In addition, calcium sulfate component can form the porosity that the sclerosis layer reduces the material after contacting rainwater for hydraulic conductivity and oxygen diffusivity reduce, prevent the tailing sand from continuing to oxidize reacidify, thereby restrain the formation of acid mine drainage, realize making useless (the yellow iron tailing) with useless (flying ash), "the municipal refuse incineration flying ash innocent treatment has also solved the problem of yellow iron tailing storehouse restoration simultaneously.
4. According to the invention, the heavy metal in the fly ash is stabilized by using a hydrothermal reaction, so that the heavy metal is converted from an acid-soluble state and an oxidizable state to a reducible state and a residue state, the leachability of the heavy metal in the fly ash is further reduced, the alkalinity in the fly ash can neutralize the pyrite tailing, but the pH value of the formed slurry is still larger than 11 due to the strong alkalinity of the fly ash, the zeolite and zeolite-like substances formed by hydrothermal reaction under an alkaline condition can effectively solidify the heavy metal to prevent the heavy metal from being percolated into the residue in the hydrothermal process, and meanwhile, the stabilized product has acid resistance and can be used as a neutralizer for acid mine restoration.
Detailed Description
The present invention will be further described with reference to the following embodiments.
The embodiment of the invention is realized by the following technical scheme: a co-processing method of household garbage incineration fly ash and pyrite tailing comprises the following steps:
(1) mixing the pyrite tailing sand with fly ash obtained by burning garbage to obtain a fly ash mixture; the mass fraction of the pyrite tailing sand in the fly ash mixture is 25-40%. Mixing the fly ash mixture and water according to a solid-liquid ratio of 1: 2-1: 8, uniformly mixing to form slurry. The pH value of the obtained slurry is 11-12. Placing the slurry in a high-temperature high-pressure reaction kettle; the slurry in the high-temperature high-pressure reaction kettle sequentially passes through a hydrothermal stage, a transition stage and a supercritical oxidation stage in the subsequent steps. The high-temperature high-pressure reaction kettle is an intermittent high-temperature high-pressure reaction kettle, and the lining is made of polytetrafluoroethylene materials.
(2) A hydrothermal stage. After the slurry in the reaction kettle reaches the reaction conditions (the temperature is 150-230 ℃ and the pressure is 2-10 Mpa) of the hydrothermal stage, starting the hydrothermal reaction, and introducing O3Reacting for 5-15 min; o is3The flow rate of the water is 10-100 mL/min; iron sulfide in the pyrite tailing is subjected to hydrothermal reaction to generate ferroferric oxide (magnetite, Fe)3O4) The ferriferrous sulfate contained in the ferriferrous oxide and the pyrite tailing is used as a catalyst to catalyze, oxidize and decompose dioxin in a hydrothermal environment. This stage is mainly to degrade solid dioxin adsorbed on the surface of fly ash.
(3) And (5) a transition stage. The reaction kettle is continuously heated to the reaction condition of the extraction stage (the temperature is 250-325 ℃, the pressure is 2-10 Mpa), so that the water is in a subcritical state, and O is introduced3Reaction for 15-30 min, O3The flow rate of the water is 10-100 mL/min; ion product (K) of water in this temperature rangew) 1000 times higher than room temperature means that protons and hydroxyl ions present in subcritical water under these conditions are 30 times as high as those present in room temperature water, the dielectric constant of water is also reduced to 20 or less, and the water is a nonpolar dioxin-like substance,O3And O decomposed by it2And active oxygen atoms, thereby promoting the efficiency of hydrothermal degradation of dioxins; in addition, water and dioxin are subjected to homogeneous reaction under the subcritical condition, and a large amount of solid-phase dioxin adsorbed in micropores inside the fly ash is extracted and dissolved into a liquid phase in the process, so that the reaction time of a subsequent supercritical oxidation stage is shortened.
(4) A supercritical oxidation stage. The reaction kettle is continuously heated to the reaction condition of the supercritical oxidation stage (the temperature is 375-475 ℃, the pressure is 22.5-27.5 Mpa), and O is introduced3The reaction is 1-10 min, O3The flow rate of the water is 10-100 mL/min; o is3Rapidly decompose into O2And active oxygen free radicals participate in the oxidative degradation of dioxins; when dioxin and O2After being dissolved in supercritical water, the two quickly react in a uniform medium without the limitation of phase to phase, and the reaction rate is high due to the ultrahigh temperature.
(5) Carrying out solid-liquid separation on the slurry treated in the steps (2) to (4) to obtain a solid product and a filtrate; and (4) refluxing the filtrate to the step (1) for pulping. The solid product is used as a covering layer material of the pyrite tailing pond, and oxygen and rainwater are prevented from permeating into lower-layer acidified tailing sand of the pyrite tailing pond by utilizing a calcium sulfate crystalline phase generated in the reaction, so that acid mine drainage is avoided; meanwhile, the covering layer material is alkaline and can be used as an acid neutralizer, so that the condition of soil acidification of the pyrite tailing pond is further avoided.
(6) Finishing a pyrite tailing storage site, and digging surface layer tailing sand to stack nearby; then, covering and compacting a solid product on the yellow iron tailing storage site with the thickness of the surface layer tailing sand removed to be used as a tailing covering layer; and a vegetation planting layer is laid on the tailing covering layer and is used for planting vegetation, and herbaceous plants are taken as main materials. The covering layer material effectively blocks oxygen and rainwater from infiltrating downwards and is alkaline, so that covered soil is not easy to acidify, and a suitable growing environment can be provided for vegetation for a long time. The vegetation is selected from one or more of Lolium perenne, Setaria viridis and Medicago sativa. Every 500m28kg of grass seeds are sown on the vegetation planting layer, covered with black gauze and watered until the surface soil is moist.
As an optional technical scheme, the vegetation planting layer is obtained by directly utilizing solid products and surface layer tailing sand dug from a yellow iron tailing storage field; specifically, the vegetation planting layer comprises the excavated surface layer tailing sand, a solid product, a water-retaining agent and an organic fertilizer. Wherein the mass fraction of the water-retaining agent is 0.5%, the mass fraction of the organic fertilizer is 5%, and the mass fraction of the solid product is 15-25%.
Example 1
Mixing a fly ash mixture doped with 25% of yellow iron tailings and water according to a solid-to-liquid ratio of 1: 3, uniformly mixing to form slurry, wherein the pH value of the slurry is 12, and placing the slurry in a high-temperature high-pressure reaction kettle; heating to 180 deg.C for hydrothermal reaction under 5Mpa, and introducing O3Reaction for 10min, O3The flow rate is 30 mL/min; continuously heating the high-temperature high-pressure reaction kettle to the extraction temperature of 275 ℃, keeping the pressure at 5Mpa to ensure that water is in a subcritical state, and introducing O3Reaction for 20min, O3The flow rate of (2) is 30 mL/min; the high-temperature high-pressure reaction kettle is continuously heated to 390 ℃, the pressure is increased to 23.5Mpa, so that the water reaches a supercritical state, and O is introduced3Reaction for 2min, O3The flow rate of (2) is 30 mL/min; and after the three reaction stages are finished, carrying out solid-liquid separation on the slurry in the reaction kettle to obtain a solid product.
Preparing a leaching solution from the solid product according to the HJ 557 method; the leaching concentration of heavy metals should not exceed the maximum allowable emission concentration limit specified in GB 8978 (maximum allowable emission concentration of pollutants of the second category is performed according to primary standards); the detection results of the heavy metal concentration of the leachate are shown in table 1; it can be seen that the heavy metal stabilization degree of the treated product is high, and the leaching toxicity is far lower than the comprehensive sewage discharge standard. The concentration content of dioxin in the fly ash before reaction is 112036ng/kg, the concentration content of dioxin in the solid product obtained after reaction is 45ng/kg, and the degradation rate reaches 99.9%. It can be seen that the toxicity of the present embodiment is much lower than the requirement of the total amount of dioxin residues in the solid product specified in HJ1134-2020 (which should not exceed 50 ng-TEQ/kg).
Table 1 heavy metal leaching data
The solid product is used for a simulated leaching test of a covering layer of a tailing pond: the effect of the solid product as a neutralizer in the remediation of pyrite tailings was evaluated by performing a potting fill test using pyrite tailings sand and the solid product obtained in this example. Selecting 100cm × 100cm × 80cm planting pots, and arranging two groups, wherein the first group is formed by paving 50cm of yellow iron tailing sand on the lower layer and paving 30cm of solid product on the upper layer as a covering layer; the second group was 80cm thick yellow iron tailings without additional covering. And (3) performing a 120-day simulated leaching test, performing flood irrigation on the two groups of planting pots from top to bottom until the soil layer is completely soaked, adding 500mL of purified water at one time, gradually allowing the purified water to seep downwards, collecting leaching liquor after a period (7 days), and measuring the pH value. The comparison result shows that the pH value of the first group after 120d leaching test is slowly reduced and then increased and then tends to be in a stable state, and the fluctuation range is 8.0-8.5; after 120d of leaching test, the pH value of the second group rises slowly and then tends to be in a stable state, the fluctuation range is 3.0-3.5, and the second group is acidic. The results demonstrate that the use of solid products as neutralizers for overburden and vegetation growing in acid mine remediation processes is successful.
Greenish recovery test of pyrite tailing pond: three plants of ryegrass, green bristlegrass and alfalfa are selected for carrying out planting tests, and soil ingredients such as a water-retaining agent, clay minerals, fertilizers and the like are added for matrix improvement. 0.5 percent of water-retaining agent and 5 percent of organic fertilizer are proportioned to be used as soil improvement components, and solid products are added to be used as a soil improvement neutralizer. Setting three groups of tests, wherein 15%, 20% and 25% of improved neutralizing agents are added to the 1 st group to the 3 rd group respectively; and then mixed with acid tailings sand to form improved soil as a topsoil layer. Selecting a planting pot of 100cm multiplied by 30cm, and paving 25cm of matrix improved tailing sand as a vegetation planting layer. Soaking plant seeds in warm water for 24h, uniformly spreading the seeds on a surface soil layer, covering the surfaces of the grass seeds with improved tailing sand of about 5mm, watering the seeds thoroughly, covering a layer of black gauze above a planting pot for shading and preserving heat so as to promote the germination of the seeds, and removing the gauze covering layer after the grass seeds generally germinate. Watering the plants thoroughly every 7 days during the growth period, recording the growth conditions of the plants, and measuring the pH value of the soil every 30 days. After a growth period of 120 days, the pH value of the soil of the group 1 is stably maintained between 5.5 and 6.0, and the survival rate of the plants is 83.5 percent; the pH value of the soil of the group 2 is stably maintained between 7.0 and 7.5, and the survival rate of the plants is 91.8 percent; the pH value of the soil of the group 3 is stably maintained between 7.5 and 8.0, the survival rate of the plants is 96.5 percent, and the greening effect is obvious.
In conclusion, an optimal tailing sand greening scheme is selected: 1) trimming a pyrite tailing storage site, and digging 25cm of tailing sand on the surface layer to stack nearby; 2) covering the solid product with the thickness of 50cm and compacting to obtain a tailing covering layer; 3) matrix improvement is carried out on the excavated surface layer tailing sand by proportioning 0.5% of water-retaining agent, 5% of organic fertilizer and 25% of solid product, and the obtained product is used as a vegetation planting layer and is laid on the tailing cover layer; 4) selecting strong stress-resistant plants such as ryegrass, green bristlegrass and alfalfa for planting, wherein the stress-resistant plants are planted every 500m28kg of grass seeds were sown, covered with black gauze and watered until the surface soil was moist.
Example 2
Mixing a fly ash mixture doped with 35% of yellow iron tailings and water according to a solid-to-liquid ratio of 1: 5, uniformly mixing to form slurry, wherein the pH value of the slurry is 11.5, and placing the slurry in a high-temperature high-pressure reaction kettle; heating to 200 deg.C for hydrothermal reaction under 5Mpa, and introducing O3Reaction for 10min, O3The flow rate is 50 mL/min; continuously heating the high-temperature high-pressure reaction kettle to the extraction temperature of 300 ℃, keeping the pressure at 5Mpa to ensure that water is in a subcritical state, and introducing O3Reaction for 15min, O3The flow rate of (A) is 50 mL/min; the high-temperature high-pressure reaction kettle is continuously heated to 390 ℃, the pressure is increased to 23.5Mpa, so that the water reaches a supercritical state, and O is introduced3Reaction for 3min, O3The flow rate of (A) is 50 mL/min; and after the three reaction stages are finished, carrying out solid-liquid separation on the slurry in the reaction kettle to obtain a solid product. Preparing a leaching solution from the solid product according to the HJ 557 method, wherein the leaching concentration of the heavy metal does not exceed the maximum allowable discharge concentration limit value specified in GB 8978 (the maximum allowable discharge concentration of the second type of pollutant is implemented according to a first-class standard), and the detection result of the concentration of the heavy metal in the leaching solution is shown in Table 2; as can be seen,the treated product has high heavy metal stabilization degree, and the leaching toxicity is far lower than the comprehensive sewage discharge standard. The concentration content of dioxin in the fly ash before reaction is 112036ng/kg, the concentration content of dioxin in a solid product obtained after reaction is 38ng/kg, and the degradation rate reaches 99.9%, so that the toxicity of the fly ash is far lower than the requirement of the total amount of dioxin residues in the solid product specified in HJ1134-2020 (the toxicity should not exceed 50 ng-TEQ/kg).
Table 2 heavy metal leaching data
The solid product is used for a simulated leaching test of a covering layer of a tailing pond: and (3) performing a pot filling test on the mixed product of the pyrite tailing sand and the treated fly ash and the pyrite tailing to evaluate the effect of the mixed product as a neutralizer for repairing the pyrite tailing. Selecting 100cm × 100cm × 80cm planting pots, and arranging two groups, wherein the first group is formed by paving 50cm of yellow iron tailing sand on the lower layer, and paving 30cm of fly ash and tailing mixed solid product on the upper layer to serve as a covering layer; the second group was 80cm thick yellow iron tailings without additional covering. After 120d of simulated leaching test, the two groups of planting pots are filled with purified water from top to the soil layer completely, 500mL of purified water is added at one time, after the purified water gradually seeps downwards, leaching liquor is collected and the pH value is measured after a period (7 days). The comparison result shows that the pH value of the first group after 120d leaching test is slowly reduced and then increased and then tends to be in a stable state, and the fluctuation range is 8.0-8.5; after 120d of leaching test, the pH values of the two groups slowly rise and then tend to be in a stable state, the fluctuation range is 3.0-3.5, and the two groups are acidic. The results demonstrate that the use of solid products as neutralizers for overburden and vegetation growing in acid mine remediation processes is successful.
Greenish recovery test of pyrite tailing pond: three plants of ryegrass, green bristlegrass and alfalfa are selected for carrying out planting tests, and soil ingredients such as a water-retaining agent, clay minerals, fertilizers and the like are added for matrix improvement. The soil improvement method comprises the following steps of proportioning 0.5% of water-retaining agent and 5% of organic fertilizer as soil improvement components, adding solid products of fly ash and pyrite tailing as soil improvement neutralizing agents, setting three groups of tests, sequentially adding 15%, 20% and 25% of improvement neutralizing agents into 1-3 groups, and mixing with acid tailing sand to form improved soil as a surface soil layer. Selecting a planting pot of 100cm multiplied by 30cm, and paving 25cm of matrix improved tailing sand as a vegetation planting layer. Soaking plant seeds in warm water for 24h, uniformly spreading the seeds on a surface soil layer, covering the surfaces of the grass seeds with improved tailing sand of about 5mm, watering the seeds thoroughly, covering a layer of black gauze above a planting pot for shading and preserving heat so as to promote the germination of the seeds, and removing the gauze covering layer after the grass seeds generally germinate. Watering the plants thoroughly every 7 days during the growth period, recording the growth conditions of the plants, and measuring the pH value of the soil every 30 days. After a growth period of 120 days, the pH value of the soil of the group 1 is stably maintained between 5.5 and 6.0, and the survival rate of the plants is 81.6 percent; the pH value of the soil of the group 2 is stably maintained between 7.0 and 7.5, and the survival rate of the plants is 90.3 percent; the pH value of the soil of the group 3 is stably maintained between 7.5 and 8.0, the survival rate of the plants is 95.0 percent, and the greening effect is obvious.
In conclusion, we can select an optimal tailing sand greening scheme: 1) trimming a pyrite tailing storage site, and digging 25cm of tailing sand on the surface layer to stack nearby; 2) covering the fly ash and the pyrite tailing mixed solid product with the thickness of 50cm and compacting; 3) the excavated surface layer tailing sand is matched with 0.5 percent of water retention agent, 5 percent of organic fertilizer and 25 percent of improved neutralizer (a mixed solid product of fly ash and pyrite tailing) for matrix improvement, and is used as a vegetation planting layer to be paved above a tailing covering layer; 4) selecting strong stress-resistant plants such as ryegrass, green bristlegrass and alfalfa for planting, wherein the stress-resistant plants are planted every 500m28kg of grass seeds were sown, covered with black gauze and watered until the surface soil was moist.
Claims (9)
1. A method for the cooperative disposal of incineration fly ash of household garbage and pyrite tailing is characterized in that: mixing yellow iron tailing sand with fly ash to obtain a fly ash mixture, and pulping by using the fly ash mixture to obtain slurry;
step two, placing the slurry in a reaction kettle, heating to hydrothermal reaction conditions, starting hydrothermal reaction and introducing O3(ii) a Iron sulfide in the pyrite tailing generates ferroferric oxide under hydrothermal reaction, the ferroferric oxide and ferrous sulfate contained in the pyrite tailing are used as catalysts, and solid-phase dioxin adsorbed on the surface of fly ash is catalytically oxidized in a hydrothermal environment;
step three, heating the slurry to extraction reaction conditions to enable water to be in a subcritical state, and introducing O3Carrying out reaction; carrying out homogeneous reaction on water and dioxin to ensure that solid-phase dioxin adsorbed in micropores inside fly ash is extracted and dissolved into a liquid phase;
step four, heating the slurry to the supercritical oxidation reaction condition, and introducing O3Carrying out reaction; in the course of the reaction, O3Decomposition into O2And active oxygen radicals, which react with dioxin in the liquid phase to cause the dioxin in the liquid phase to be oxidized and decomposed;
step five, carrying out solid-liquid separation on the slurry treated in the step four to obtain a solid product and a filtrate;
step six, digging surface layer tailing sand of the pyrite tailing pond field; covering a solid product on a pyrite tailing storage site and compacting to form a tailing covering layer; the tailing covering layer is used for preventing oxygen and rainwater from seeping downwards, and plays a role in neutralizing the lower yellow iron tailing sand by utilizing the alkalinity of the tailing covering layer; paving a vegetation planting layer on the tailing covering layer; and D, mixing the vegetation planting layer with the surface layer tailing sand, the solid product obtained in the step five, a water-retaining agent and an organic fertilizer to obtain the vegetation planting layer.
2. The method for the co-disposal of fly ash from incineration of domestic garbage and pyrite tailing according to claim 1, wherein: the mass fraction of the water-retaining agent in the vegetation planting layer is 0.3-1%, the mass fraction of the organic fertilizer is 3-10%, and the mass fraction of the solid product is 15-25%.
3. The method for the co-disposal of fly ash from incineration of domestic garbage and pyrite tailing according to claim 1, wherein: in the fly ash mixture obtained in the step one, the mass fraction of the pyrite tailing sand is 25-40%.
4. The method for the co-disposal of fly ash from incineration of domestic garbage and pyrite tailing according to claim 1, wherein: the slurry in the first step is prepared by mixing a fly ash mixture and water according to a solid-to-liquid ratio of 1: 2-1: 8, uniformly mixing to obtain the mixture; the pH value of the obtained slurry is 11-12.
5. The method for the co-disposal of fly ash from incineration of domestic garbage and pyrite tailing according to claim 1, wherein: the hydrothermal reaction in the second step is carried out at the temperature of 150-230 ℃ and the pressure of 2-10 Mpa, and the reaction time is 5-15 min; o is3The flow rate of (A) is 10 to 100 mL/min.
6. The method for the co-disposal of fly ash from incineration of domestic garbage and pyrite tailing according to claim 1, wherein: the extraction reaction conditions in the third step are that the temperature is 250-325 ℃, the pressure is 2-10 Mpa, the reaction time is 15-30 min, and O3The flow rate of (A) is 10 to 100 mL/min.
7. The method for the co-disposal of fly ash from incineration of domestic garbage and pyrite tailing according to claim 1, wherein: the supercritical oxidation reaction conditions in the step four are that the temperature is 375-475 ℃, the pressure is 22.5-27.5 Mpa, the reaction time is 1-10 min, and O is3The flow rate of (A) is 10 to 100 mL/min.
8. The method for the co-disposal of fly ash from incineration of domestic garbage and pyrite tailing according to claim 1, wherein: and refluxing the filtrate obtained in the step five to the step one for pulping.
9. The method for the co-disposal of fly ash from incineration of domestic garbage and pyrite tailing according to claim 1, wherein: in the sixth step, covering the vegetation planting layer with black gauze and planting one or more of ryegrass, green bristlegrass and alfalfa; and removing the black gauze after the plants in the vegetation planting layer germinate.
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