CN113173631B - Method for promoting ferrous sulfide to remove Sb (III) in polluted water - Google Patents
Method for promoting ferrous sulfide to remove Sb (III) in polluted water Download PDFInfo
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- CN113173631B CN113173631B CN202110482963.XA CN202110482963A CN113173631B CN 113173631 B CN113173631 B CN 113173631B CN 202110482963 A CN202110482963 A CN 202110482963A CN 113173631 B CN113173631 B CN 113173631B
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- MBMLMWLHJBBADN-UHFFFAOYSA-N Ferrous sulfide Chemical compound [Fe]=S MBMLMWLHJBBADN-UHFFFAOYSA-N 0.000 title claims abstract description 36
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims abstract description 27
- 238000000034 method Methods 0.000 title claims abstract description 15
- 230000001737 promoting effect Effects 0.000 title claims abstract description 12
- 229910019142 PO4 Inorganic materials 0.000 claims abstract description 19
- 239000010452 phosphate Substances 0.000 claims abstract description 19
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims abstract description 19
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims abstract description 12
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims abstract description 7
- 239000002244 precipitate Substances 0.000 claims abstract description 7
- 239000007787 solid Substances 0.000 claims abstract description 7
- 230000009471 action Effects 0.000 claims abstract description 5
- 230000002378 acidificating effect Effects 0.000 claims abstract description 4
- 230000007935 neutral effect Effects 0.000 claims abstract description 4
- 239000011734 sodium Substances 0.000 claims abstract description 4
- LWIHDJKSTIGBAC-UHFFFAOYSA-K tripotassium phosphate Chemical compound [K+].[K+].[K+].[O-]P([O-])([O-])=O LWIHDJKSTIGBAC-UHFFFAOYSA-K 0.000 claims description 6
- 239000004254 Ammonium phosphate Substances 0.000 claims description 3
- 229910000148 ammonium phosphate Inorganic materials 0.000 claims description 3
- 235000019289 ammonium phosphates Nutrition 0.000 claims description 3
- MNNHAPBLZZVQHP-UHFFFAOYSA-N diammonium hydrogen phosphate Chemical compound [NH4+].[NH4+].OP([O-])([O-])=O MNNHAPBLZZVQHP-UHFFFAOYSA-N 0.000 claims description 3
- ZPWVASYFFYYZEW-UHFFFAOYSA-L dipotassium hydrogen phosphate Chemical compound [K+].[K+].OP([O-])([O-])=O ZPWVASYFFYYZEW-UHFFFAOYSA-L 0.000 claims description 3
- 235000019797 dipotassium phosphate Nutrition 0.000 claims description 3
- 229910000396 dipotassium phosphate Inorganic materials 0.000 claims description 3
- BNIILDVGGAEEIG-UHFFFAOYSA-L disodium hydrogen phosphate Chemical compound [Na+].[Na+].OP([O-])([O-])=O BNIILDVGGAEEIG-UHFFFAOYSA-L 0.000 claims description 3
- 229910000397 disodium phosphate Inorganic materials 0.000 claims description 3
- 235000019800 disodium phosphate Nutrition 0.000 claims description 3
- 229910000402 monopotassium phosphate Inorganic materials 0.000 claims description 3
- 235000019796 monopotassium phosphate Nutrition 0.000 claims description 3
- PJNZPQUBCPKICU-UHFFFAOYSA-N phosphoric acid;potassium Chemical compound [K].OP(O)(O)=O PJNZPQUBCPKICU-UHFFFAOYSA-N 0.000 claims description 3
- 229910000160 potassium phosphate Inorganic materials 0.000 claims description 3
- 235000011009 potassium phosphates Nutrition 0.000 claims description 3
- 239000001488 sodium phosphate Substances 0.000 claims description 3
- 229910000162 sodium phosphate Inorganic materials 0.000 claims description 3
- 235000011008 sodium phosphates Nutrition 0.000 claims description 3
- RYFMWSXOAZQYPI-UHFFFAOYSA-K trisodium phosphate Chemical compound [Na+].[Na+].[Na+].[O-]P([O-])([O-])=O RYFMWSXOAZQYPI-UHFFFAOYSA-K 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims 1
- 229910052787 antimony Inorganic materials 0.000 description 16
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 description 16
- 229910001608 iron mineral Inorganic materials 0.000 description 5
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 4
- 238000011109 contamination Methods 0.000 description 4
- 229910001385 heavy metal Inorganic materials 0.000 description 4
- 239000013049 sediment Substances 0.000 description 4
- 230000015572 biosynthetic process Effects 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 238000001179 sorption measurement Methods 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 238000003723 Smelting Methods 0.000 description 2
- 230000003247 decreasing effect Effects 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 239000003673 groundwater Substances 0.000 description 2
- 229910052500 inorganic mineral Inorganic materials 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 239000011707 mineral Substances 0.000 description 2
- 238000005065 mining Methods 0.000 description 2
- 230000001376 precipitating effect Effects 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000002352 surface water Substances 0.000 description 2
- 231100000331 toxic Toxicity 0.000 description 2
- 230000002588 toxic effect Effects 0.000 description 2
- 238000003911 water pollution Methods 0.000 description 2
- 241000894006 Bacteria Species 0.000 description 1
- 206010028980 Neoplasm Diseases 0.000 description 1
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 229940026189 antimony potassium tartrate Drugs 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 201000011510 cancer Diseases 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 230000001276 controlling effect Effects 0.000 description 1
- WBTCZEPSIIFINA-MSFWTACDSA-J dipotassium;antimony(3+);(2r,3r)-2,3-dioxidobutanedioate;trihydrate Chemical compound O.O.O.[K+].[K+].[Sb+3].[Sb+3].[O-]C(=O)[C@H]([O-])[C@@H]([O-])C([O-])=O.[O-]C(=O)[C@H]([O-])[C@@H]([O-])C([O-])=O WBTCZEPSIIFINA-MSFWTACDSA-J 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000003063 flame retardant Substances 0.000 description 1
- 229910052598 goethite Inorganic materials 0.000 description 1
- 229910052595 hematite Inorganic materials 0.000 description 1
- 239000011019 hematite Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- AEIXRCIKZIZYPM-UHFFFAOYSA-M hydroxy(oxo)iron Chemical compound [O][Fe]O AEIXRCIKZIZYPM-UHFFFAOYSA-M 0.000 description 1
- 230000036039 immunity Effects 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- LIKBJVNGSGBSGK-UHFFFAOYSA-N iron(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Fe+3].[Fe+3] LIKBJVNGSGBSGK-UHFFFAOYSA-N 0.000 description 1
- 229910000403 monosodium phosphate Inorganic materials 0.000 description 1
- 235000019799 monosodium phosphate Nutrition 0.000 description 1
- 210000000653 nervous system Anatomy 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 238000005325 percolation Methods 0.000 description 1
- 239000004033 plastic Substances 0.000 description 1
- 229920003023 plastic Polymers 0.000 description 1
- 239000002574 poison Substances 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 229910052683 pyrite Inorganic materials 0.000 description 1
- 239000011028 pyrite Substances 0.000 description 1
- NIFIFKQPDTWWGU-UHFFFAOYSA-N pyrite Chemical compound [Fe+2].[S-][S-] NIFIFKQPDTWWGU-UHFFFAOYSA-N 0.000 description 1
- 229910052952 pyrrhotite Inorganic materials 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 238000005067 remediation Methods 0.000 description 1
- AJPJDKMHJJGVTQ-UHFFFAOYSA-M sodium dihydrogen phosphate Chemical compound [Na+].OP(O)([O-])=O AJPJDKMHJJGVTQ-UHFFFAOYSA-M 0.000 description 1
- 239000002689 soil Substances 0.000 description 1
- 239000007790 solid phase Substances 0.000 description 1
- 239000002910 solid waste Substances 0.000 description 1
- 238000010301 surface-oxidation reaction Methods 0.000 description 1
Classifications
-
- 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
- C02F1/58—Treatment of water, waste water, or sewage by removing specified dissolved compounds
-
- 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
Landscapes
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Removal Of Specific Substances (AREA)
Abstract
The invention discloses a method for promoting ferrous sulfide to remove Sb (III) in polluted water, which is characterized by comprising the following steps: (1) anaerobic reactionAdding FeS solid into Sb (III) -polluted water in the state, or adding FeSO into the Sb (III) -polluted water respectively 4 Solution and Na 2 Adding soluble phosphate into the S solution to form a fresh FeS precipitate, uniformly mixing, adjusting the pH value of the system, and adjusting the system to be acidic or neutral by using a hydrochloric acid/sodium hydroxide solution, wherein the pH value is 5-7, and the system action time is 12-24 h.
Description
Technical Field
The invention relates to a method for promoting ferrous sulfide (FeS) to remove Sb (III) in polluted water under anaerobic conditions by using soluble phosphate, belonging to the field of water pollution control.
Background
There are many ways of producing antimony contamination in the surface environment. Antimony ore mining and dressing smelting generate serious antimony pollution, antimony can be released when coal is combusted, in addition, antimony metal is widely applied to industries such as plastics, alloys, flame retardants, automobiles and the like, the industries can discharge antimony pollution, and the articles can also cause the antimony pollution in the environment in the using process. Antimony is a toxic and harmful element that can poison the human nervous system and cause cancer, and is therefore considered to be a priority for controlling pollutants. At present, in a mining area of a mine and an antimony metal smelting area, soil and surface water have severe antimony pollution. In particular, antimony is converted from the form Sb (V) which is common under oxidizing conditions to Sb (III) which is more toxic than Sb (V) after it has entered the groundwater by percolation or the like, which is a reducing environment. Therefore, remediation of sb (iii) contamination in groundwater is a significant challenge.
Markenoite (FeS) is an important iron mineral in the surface reduction environment. The natural marine sediments and lake sediments are in anaerobic environment, and the underground water is also in anaerobic environment, in which the main iron minerals are reduced iron minerals, mainly including markenoite (FeS) and pyrite (FeS) 2 ) And a small amount of pyrrhotite (Fe) 3 S 4 ). The relationship between the minerals and iron minerals in the surface oxidation environment is that goethite, hematite and the like on the surface are washed into the sediment along with surface water flow and then reduced, wherein FeS is the metastable mineral formed firstly after the reduction of the oxidized iron mineral, has small particles and large specific surface area, and absorbs heavy metalsStrong adhesion, and is an important carrier of heavy metal in the sediment. For example, in contaminated lake deposits in the vicinity of antimony mines or antimony smelters, the antimony bound to FeS can be a significant proportion, and thus FeS is an important substance affecting antimony behavior in a reducing environment.
Due to the characteristics, the FeS can be used for removing heavy metal pollution in water in the field of heavy metal pollution treatment. FeS can be used for adsorbing heavy metals in underground water in permeable reactive barrier technology commonly used in underground water pollution treatment. Research in recent years has shown that FeS can be used to remove sb (iii) contamination in water under anaerobic conditions by way of FeS as a solid phase to adsorb/precipitate sb (iii), as follows.
First, the mode of removing antimony from FeS includes adsorption, and in addition to electrostatic adsorption, Sb (III) can be adsorbed on FeS particles via the Fe terminal and S terminal of the FeS surface in the form of ≡ Fe-OAs (OH) 2 And ≡ S 2 -As (OH). Secondly, the mode of removing Sb (III) by FeS also comprises the formation of Sb 2 S 3 And (4) precipitating. Since FeS has a solubility which increases with decreasing pH, a certain amount of dissolved Fe (II) and S (-II) (comprising H) is present in the FeS-water system in dissolved form 2 S, HS - , S 2- Three forms). When Sb (III) concentration is high, S (-II) will form Sb with Sb (III) 2 S 3 And (4) precipitating.
Li et al (2021) (Li, d., Zhang, g., Wang, q., Liu, s., Ma, c., Chen, j., Liu, f. Interaction of aqueous immunity (III) with synthetic bacteria sulfate. appl. geochem. 2021, 128: 104957.) when this method was used to remove sb (III) contamination in water, the removal of sb (III) was found to be closely related to the pH of the system. The lower the pH of the system, the higher the sb (iii) removal rate. In the experiment, the removal rate of Sb (III) by FeS is 55% when the pH is 7 and 67.5% when the pH is 5.5 in a certain initial system (initial conditions: FeS-44 mg/L, Sb (III) -20 mg/L and action time: 24 h). Therefore, the method has certain disadvantages that the removal rate of Sb (III) is not very high, and a great promotion space is provided. With the increasing requirement of environmental protection, new methods for improving the removal efficiency of Sb (III) are urgently needed to be researched. Therefore, the invention provides that the soluble phosphate can be utilized to promote the removal of Sb (III) by FeS under anaerobic condition, and the removal rate of Sb (III) is improved.
Disclosure of Invention
The technical problem to be solved by the invention is as follows: a method for promoting FeS to remove Sb (III) in polluted water by using soluble phosphate. In a system for removing harmful substances Sb (III) in polluted water by using FeS, the addition of soluble phosphate can promote Sb 2 S 3 The formation of the precipitate effectively improves the removal rate of Sb (III). Sb (III) in the polluted water is removed, enters the solid of the system, coexists with the FeS solid, and can be treated according to the method of solid waste after being separated from the treated water.
The technical scheme of the invention is as follows: a method for promoting the removal of Sb (III) in polluted water by ferrous sulfide is characterized by adding phosphate.
A method for promoting the removal of Sb (III) in polluted water by ferrous sulfide, (1) adding FeS solid into the polluted water containing Sb (III) in an anaerobic state, or respectively adding FeSO 4 Solution and Na 2 Adding soluble phosphate into the S solution to form a fresh FeS precipitate, uniformly mixing, adjusting the pH value of the system, and adjusting the system to be acidic or neutral by using a hydrochloric acid/sodium hydroxide solution, wherein the pH value is 5-7, and the system action time is 12-24 h.
The phosphate is soluble phosphate, and is one or more of potassium hydrogen phosphate, sodium hydrogen phosphate, potassium dihydrogen phosphate, sodium phosphate, potassium phosphate, and ammonium phosphate.
The concentration of the phosphate is 95 mg/L (as PO) 4 3- Meter) above.
The invention has the beneficial effects that:
(1) the adsorption/precipitation of Sb (III) by FeS is a method for removing Sb (III) pollution in polluted water, and the addition of soluble phosphate can improve the removal rate of Sb (III) in water by FeS.
(2) One feature of the invention is that phosphate is added to the PO 4 3- Sb is promoted only after reaching a certain concentration 2 S 3 Formation of a precipitate, ofThe removal of Sb (III) is promoted. Another feature is that the effect increases with decreasing pH. The removal of Sb (III) is not promoted under alkaline conditions, the promoting effect is obvious under neutral conditions, and the promoting effect is more obvious under acidic conditions.
Detailed Description
The embodiment is as follows: the antimony potassium tartrate is used for preparing polluted water containing Sb (III), and the polluted water is regulated to be under anaerobic condition by nitrogen. Adding a certain amount of FeS particles (or adding FeSO respectively according to the amount) into the polluted water 4 Solution and Na 2 S solution to form FeS precipitate) whereupon a system is formed containing sb (iii) and solid FeS at an initial concentration. Adding soluble phosphate (such as sodium hydrogen phosphate, potassium hydrogen phosphate, sodium dihydrogen phosphate, potassium dihydrogen phosphate, sodium phosphate, potassium phosphate, and ammonium phosphate), mixing, comparing with the experiment without adding phosphate and with phosphate of different concentrations, and adjusting pH with HCl/NaOH.
The conditions of the experimental system are that the initial concentration of Sb (III) is 20 mg/L, the initial concentration of solid FeS is 44 mg/L, and after phosphate is added, the initial PO in the system 4 3- The concentrations are respectively 0, 9.5, 19, 95 and 475 mg/L, the system pH is respectively 7 and 5.5, and the action time of the system is 12-24 h. The specific treatment results are as follows:
example one, the treatment system was adjusted to pH =7. When PO is added 4 3- When the concentration of Sb (III) in the solution is respectively 0, 9.5, 19, 95 and 475 mg/L, the residual Sb (III) in the solution is respectively 9.0, 9.0, 9.0, 6.5 and 2.3 mg/L, and the corresponding Sb (III) removal rates are respectively 55%, 55%, 55%, 67.5% and 88.5%. Visible, PO 4 3- The content is 9.5, and when the content is 19 mg/L, the removal of Sb (III) is not promoted; when PO is present 4 3- When 95 mg/L is reached, the removal of Sb (III) is obviously increased; in particular PO 4 3- When the concentration reaches 475 mg/L, the Sb (III) removal rate reaches 88.5 percent.
Example two, the treatment system was adjusted to pH = 5.5. When PO is added 4 3- When the concentration of Sb (III) in the solution is respectively 0, 9.5, 19, 95 and 475 mg/L, the residual Sb (III) in the solution is respectively 6.5, 6.5, 6.5, 3.2 and 0.1 mg/L, and the corresponding Sb (III) removal rates are respectively 67.5%, 67.5%, 67.5%, 84% and 99.5%. Also visible is PO 4 3- The content is 9.5, and when the content is 19 mg/L, the removal of Sb (III) is not promoted; when 95 mg/L is reached, the Sb (III) removal is obviously increased; in particular PO 4 3- When the concentration reaches 475 mg/L, the removal rate of Sb (III) reaches 99.5 percent.
Specifically, the specific effect of promoting sb (iii) removal: in this system, when PO 4 3- When the concentration reaches 95 mg/L or more, the Sb (III) removal is obviously promoted. Such as:
no PO was added at pH =7.0 4 3- The removal rate of Sb (III) was 51%, PO was added 4 3- At 95 mg/L, the removal rate of Sb (III) increased to 70%. Adding PO 4 3- At 475 mg/L, the Sb (III) removal rate increased to 90%.
At pH =5.5, no PO was added 4 3- When the removal rate of Sb (III) was 67.5%, PO was added 4 3- At 95 mg/L, the Sb (III) removal rate increased to 84%, PO was added 4 3- At 475 mg/L, the Sb (III) removal rate increased to 99.5%.
Claims (2)
1. A method for promoting the removal of Sb (III) in polluted water by ferrous sulfide is characterized in that: (1) adding FeS solid into water polluted by Sb (III) in anaerobic state or respectively adding FeSO 4 Solution and Na 2 S solution to form fresh FeS precipitate, (2) adding soluble phosphate, and adding initial PO in the system after adding phosphate 4 3- The concentration is more than 95 mg/L, the mixture is uniformly mixed, the pH value of the system is adjusted, the system is adjusted to be acidic or neutral by hydrochloric acid or sodium hydroxide solution, the pH value is 5-7, and the system action time is 12-24 h.
2. The method for promoting the removal of Sb (III) in the polluted water by ferrous sulfide as claimed in claim 1, wherein: the soluble phosphate comprises potassium hydrogen phosphate, sodium hydrogen phosphate, potassium dihydrogen phosphate, sodium phosphate, potassium phosphate, and ammonium phosphate.
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Citations (1)
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CN88100262A (en) * | 1987-01-26 | 1988-12-14 | 魁北克水电公司 | From the aqueous solution, remove heavy metal and other ionic method |
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US4177142A (en) * | 1974-04-04 | 1979-12-04 | Ecodyne Corporation | Mixture of oppositely charged filter aid material |
DE2515861A1 (en) * | 1975-04-11 | 1976-10-28 | Norddeutsche Affinerie | PROCEDURE FOR ADSORPTIVE REMOVAL OF ARSENIC, ANTIMONE AND / OR ISMUTH |
JP3513754B2 (en) * | 2000-12-28 | 2004-03-31 | 独立行政法人産業技術総合研究所 | Antimony removal method and remover |
US9379368B2 (en) * | 2011-07-11 | 2016-06-28 | California Institute Of Technology | Electrochemical systems with electronically conductive layers |
CN104845626B (en) * | 2015-05-05 | 2018-05-29 | 长沙华时捷环保科技发展股份有限公司 | For administering the passivator of heavy-metal contaminated soil and its preparation and application |
EP3434391A1 (en) * | 2017-07-28 | 2019-01-30 | Rijksuniversiteit Groningen | A method for producing a metallic structure and a metallic structure obtainable by the method |
CN109382396A (en) * | 2017-08-11 | 2019-02-26 | 上海环境节能工程股份有限公司 | One kind is for handling antimony pollution soil remediation medicament and its application method |
CN107970878B (en) * | 2017-11-09 | 2021-01-05 | 南华大学 | Preparation method of phosphate group functionalized hollow mesoporous silica microspheres |
CN110293126A (en) * | 2019-05-27 | 2019-10-01 | 上海傲江生态环境科技有限公司 | One kind is for arsenic and antimony pollution soil remediation medicament and its application method |
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CN88100262A (en) * | 1987-01-26 | 1988-12-14 | 魁北克水电公司 | From the aqueous solution, remove heavy metal and other ionic method |
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