CN111889499A - Super-stable mineralizer and application thereof in remediation of heavy metal contaminated soil - Google Patents
Super-stable mineralizer and application thereof in remediation of heavy metal contaminated soil Download PDFInfo
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- CN111889499A CN111889499A CN202010538366.XA CN202010538366A CN111889499A CN 111889499 A CN111889499 A CN 111889499A CN 202010538366 A CN202010538366 A CN 202010538366A CN 111889499 A CN111889499 A CN 111889499A
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- Prior art keywords
- mineralizer
- hyperstable
- soil
- stable
- calcium
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- 239000002689 soil Substances 0.000 title claims abstract description 44
- 229910001385 heavy metal Inorganic materials 0.000 title claims abstract description 42
- 238000005067 remediation Methods 0.000 title claims abstract description 13
- 238000000034 method Methods 0.000 claims abstract description 16
- 239000002002 slurry Substances 0.000 claims abstract description 14
- 239000007788 liquid Substances 0.000 claims abstract description 13
- 238000005507 spraying Methods 0.000 claims abstract description 7
- 230000008569 process Effects 0.000 claims abstract description 5
- 239000000243 solution Substances 0.000 claims description 34
- 229910052751 metal Inorganic materials 0.000 claims description 32
- 239000002184 metal Substances 0.000 claims description 31
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 22
- 150000003839 salts Chemical class 0.000 claims description 16
- 239000003513 alkali Substances 0.000 claims description 14
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 12
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 12
- 239000008367 deionised water Substances 0.000 claims description 12
- 229910021641 deionized water Inorganic materials 0.000 claims description 12
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims description 10
- 239000006185 dispersion Substances 0.000 claims description 10
- 239000012266 salt solution Substances 0.000 claims description 10
- 239000011734 sodium Substances 0.000 claims description 10
- 229910052708 sodium Inorganic materials 0.000 claims description 10
- 229910002651 NO3 Inorganic materials 0.000 claims description 7
- 238000002360 preparation method Methods 0.000 claims description 7
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 claims description 6
- 238000001035 drying Methods 0.000 claims description 5
- 238000005406 washing Methods 0.000 claims description 5
- TWRXJAOTZQYOKJ-UHFFFAOYSA-L Magnesium chloride Chemical compound [Mg+2].[Cl-].[Cl-] TWRXJAOTZQYOKJ-UHFFFAOYSA-L 0.000 claims description 4
- CSNNHWWHGAXBCP-UHFFFAOYSA-L Magnesium sulfate Chemical compound [Mg+2].[O-][S+2]([O-])([O-])[O-] CSNNHWWHGAXBCP-UHFFFAOYSA-L 0.000 claims description 4
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 4
- 239000001110 calcium chloride Substances 0.000 claims description 4
- 229910001628 calcium chloride Inorganic materials 0.000 claims description 4
- ZCCIPPOKBCJFDN-UHFFFAOYSA-N calcium nitrate Chemical compound [Ca+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ZCCIPPOKBCJFDN-UHFFFAOYSA-N 0.000 claims description 4
- 159000000007 calcium salts Chemical class 0.000 claims description 4
- OSGAYBCDTDRGGQ-UHFFFAOYSA-L calcium sulfate Chemical compound [Ca+2].[O-]S([O-])(=O)=O OSGAYBCDTDRGGQ-UHFFFAOYSA-L 0.000 claims description 4
- 238000002425 crystallisation Methods 0.000 claims description 4
- 230000008025 crystallization Effects 0.000 claims description 4
- 229960004887 ferric hydroxide Drugs 0.000 claims description 4
- IEECXTSVVFWGSE-UHFFFAOYSA-M iron(3+);oxygen(2-);hydroxide Chemical compound [OH-].[O-2].[Fe+3] IEECXTSVVFWGSE-UHFFFAOYSA-M 0.000 claims description 4
- VCJMYUPGQJHHFU-UHFFFAOYSA-N iron(3+);trinitrate Chemical compound [Fe+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VCJMYUPGQJHHFU-UHFFFAOYSA-N 0.000 claims description 4
- YIXJRHPUWRPCBB-UHFFFAOYSA-N magnesium nitrate Chemical compound [Mg+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O YIXJRHPUWRPCBB-UHFFFAOYSA-N 0.000 claims description 4
- 159000000003 magnesium salts Chemical class 0.000 claims description 4
- 239000002244 precipitate Substances 0.000 claims description 4
- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 claims description 3
- AXCZMVOFGPJBDE-UHFFFAOYSA-L calcium dihydroxide Chemical compound [OH-].[OH-].[Ca+2] AXCZMVOFGPJBDE-UHFFFAOYSA-L 0.000 claims description 3
- 239000000920 calcium hydroxide Substances 0.000 claims description 3
- 229910001861 calcium hydroxide Inorganic materials 0.000 claims description 3
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 claims description 2
- 229910021578 Iron(III) chloride Inorganic materials 0.000 claims description 2
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 claims description 2
- 239000000292 calcium oxide Substances 0.000 claims description 2
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 claims description 2
- PASHVRUKOFIRIK-UHFFFAOYSA-L calcium sulfate dihydrate Chemical compound O.O.[Ca+2].[O-]S([O-])(=O)=O PASHVRUKOFIRIK-UHFFFAOYSA-L 0.000 claims description 2
- 238000005119 centrifugation Methods 0.000 claims description 2
- 229960002089 ferrous chloride Drugs 0.000 claims description 2
- 229960001781 ferrous sulfate Drugs 0.000 claims description 2
- 239000011790 ferrous sulphate Substances 0.000 claims description 2
- 235000003891 ferrous sulphate Nutrition 0.000 claims description 2
- 229910052602 gypsum Inorganic materials 0.000 claims description 2
- 239000010440 gypsum Substances 0.000 claims description 2
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims description 2
- NMCUIPGRVMDVDB-UHFFFAOYSA-L iron dichloride Chemical compound Cl[Fe]Cl NMCUIPGRVMDVDB-UHFFFAOYSA-L 0.000 claims description 2
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 claims description 2
- RUTXIHLAWFEWGM-UHFFFAOYSA-H iron(3+) sulfate Chemical compound [Fe+3].[Fe+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O RUTXIHLAWFEWGM-UHFFFAOYSA-H 0.000 claims description 2
- 229910000359 iron(II) sulfate Inorganic materials 0.000 claims description 2
- 229910000360 iron(III) sulfate Inorganic materials 0.000 claims description 2
- 229910001629 magnesium chloride Inorganic materials 0.000 claims description 2
- VTHJTEIRLNZDEV-UHFFFAOYSA-L magnesium dihydroxide Chemical compound [OH-].[OH-].[Mg+2] VTHJTEIRLNZDEV-UHFFFAOYSA-L 0.000 claims description 2
- 239000000347 magnesium hydroxide Substances 0.000 claims description 2
- 229910001862 magnesium hydroxide Inorganic materials 0.000 claims description 2
- 229910052943 magnesium sulfate Inorganic materials 0.000 claims description 2
- 235000019341 magnesium sulphate Nutrition 0.000 claims description 2
- 238000002156 mixing Methods 0.000 claims description 2
- 239000012670 alkaline solution Substances 0.000 claims 1
- 150000002500 ions Chemical class 0.000 abstract description 20
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 abstract description 15
- 229910052793 cadmium Inorganic materials 0.000 abstract description 14
- 230000000694 effects Effects 0.000 abstract description 10
- 238000003900 soil pollution Methods 0.000 abstract description 7
- GDVKFRBCXAPAQJ-UHFFFAOYSA-A dialuminum;hexamagnesium;carbonate;hexadecahydroxide Chemical compound [OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Al+3].[Al+3].[O-]C([O-])=O GDVKFRBCXAPAQJ-UHFFFAOYSA-A 0.000 abstract description 6
- 229910001701 hydrotalcite Inorganic materials 0.000 abstract description 6
- 229960001545 hydrotalcite Drugs 0.000 abstract description 6
- 239000012528 membrane Substances 0.000 abstract description 6
- 239000013078 crystal Substances 0.000 abstract description 5
- 238000011065 in-situ storage Methods 0.000 abstract description 5
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 abstract description 3
- 239000011572 manganese Substances 0.000 abstract description 3
- 238000006467 substitution reaction Methods 0.000 abstract description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 abstract description 2
- 239000003463 adsorbent Substances 0.000 abstract description 2
- 229910052802 copper Inorganic materials 0.000 abstract description 2
- 239000010949 copper Substances 0.000 abstract description 2
- 229910052748 manganese Inorganic materials 0.000 abstract description 2
- 229910021645 metal ion Inorganic materials 0.000 abstract description 2
- 230000020477 pH reduction Effects 0.000 abstract description 2
- 239000012716 precipitator Substances 0.000 abstract description 2
- 238000009331 sowing Methods 0.000 abstract description 2
- 239000011575 calcium Substances 0.000 description 28
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 26
- 229910052791 calcium Inorganic materials 0.000 description 26
- WLZRMCYVCSSEQC-UHFFFAOYSA-N cadmium(2+) Chemical compound [Cd+2] WLZRMCYVCSSEQC-UHFFFAOYSA-N 0.000 description 16
- 239000000463 material Substances 0.000 description 16
- 239000000047 product Substances 0.000 description 10
- 238000002441 X-ray diffraction Methods 0.000 description 6
- 230000033558 biomineral tissue development Effects 0.000 description 6
- 239000003795 chemical substances by application Substances 0.000 description 6
- 238000002161 passivation Methods 0.000 description 6
- 238000001179 sorption measurement Methods 0.000 description 5
- 238000005303 weighing Methods 0.000 description 5
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 4
- JPVYNHNXODAKFH-UHFFFAOYSA-N Cu2+ Chemical compound [Cu+2] JPVYNHNXODAKFH-UHFFFAOYSA-N 0.000 description 4
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 4
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 4
- 229910001431 copper ion Inorganic materials 0.000 description 4
- 239000011777 magnesium Substances 0.000 description 4
- 229910052749 magnesium Inorganic materials 0.000 description 4
- 229910001437 manganese ion Inorganic materials 0.000 description 4
- -1 nitrate ions Chemical class 0.000 description 4
- 239000011591 potassium Substances 0.000 description 4
- 229910052700 potassium Inorganic materials 0.000 description 4
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 3
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 230000008859 change Effects 0.000 description 3
- 239000002131 composite material Substances 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 239000000017 hydrogel Substances 0.000 description 3
- 229910001388 sodium aluminate Inorganic materials 0.000 description 3
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 2
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 2
- 230000009471 action Effects 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 229910000019 calcium carbonate Inorganic materials 0.000 description 2
- 238000011109 contamination Methods 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 2
- 229910052625 palygorskite Inorganic materials 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 230000002265 prevention Effects 0.000 description 2
- 239000000376 reactant Substances 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 230000008439 repair process Effects 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- 229910052725 zinc Inorganic materials 0.000 description 2
- 239000011701 zinc Substances 0.000 description 2
- 229910052582 BN Inorganic materials 0.000 description 1
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 description 1
- 241000196324 Embryophyta Species 0.000 description 1
- 229910000616 Ferromanganese Inorganic materials 0.000 description 1
- JYTFHRIBVLXWDT-UHFFFAOYSA-M O.[OH-].[N+](=O)([O-])[O-].[O-2].[Al+3].[Ca+2] Chemical compound O.[OH-].[N+](=O)([O-])[O-].[O-2].[Al+3].[Ca+2] JYTFHRIBVLXWDT-UHFFFAOYSA-M 0.000 description 1
- 240000007594 Oryza sativa Species 0.000 description 1
- 235000007164 Oryza sativa Nutrition 0.000 description 1
- 239000004113 Sepiolite Substances 0.000 description 1
- 238000003917 TEM image Methods 0.000 description 1
- 240000008042 Zea mays Species 0.000 description 1
- 235000005824 Zea mays ssp. parviglumis Nutrition 0.000 description 1
- 235000002017 Zea mays subsp mays Nutrition 0.000 description 1
- PTFCDOFLOPIGGS-UHFFFAOYSA-N Zinc dication Chemical compound [Zn+2] PTFCDOFLOPIGGS-UHFFFAOYSA-N 0.000 description 1
- ULGYAEQHFNJYML-UHFFFAOYSA-N [AlH3].[Ca] Chemical compound [AlH3].[Ca] ULGYAEQHFNJYML-UHFFFAOYSA-N 0.000 description 1
- 150000008065 acid anhydrides Chemical class 0.000 description 1
- WNROFYMDJYEPJX-UHFFFAOYSA-K aluminium hydroxide Chemical compound [OH-].[OH-].[OH-].[Al+3] WNROFYMDJYEPJX-UHFFFAOYSA-K 0.000 description 1
- CKMXBZGNNVIXHC-UHFFFAOYSA-L ammonium magnesium phosphate hexahydrate Chemical compound [NH4+].O.O.O.O.O.O.[Mg+2].[O-]P([O-])([O-])=O CKMXBZGNNVIXHC-UHFFFAOYSA-L 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 229960000892 attapulgite Drugs 0.000 description 1
- 239000011324 bead Substances 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000002860 competitive effect Effects 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 235000005822 corn Nutrition 0.000 description 1
- 238000003795 desorption Methods 0.000 description 1
- 238000000635 electron micrograph Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 229910021389 graphene Inorganic materials 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 238000001095 inductively coupled plasma mass spectrometry Methods 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
- 239000011147 inorganic material Substances 0.000 description 1
- DALUDRGQOYMVLD-UHFFFAOYSA-N iron manganese Chemical compound [Mn].[Fe] DALUDRGQOYMVLD-UHFFFAOYSA-N 0.000 description 1
- 230000001788 irregular Effects 0.000 description 1
- CYPPCCJJKNISFK-UHFFFAOYSA-J kaolinite Chemical compound [OH-].[OH-].[OH-].[OH-].[Al+3].[Al+3].[O-][Si](=O)O[Si]([O-])=O CYPPCCJJKNISFK-UHFFFAOYSA-J 0.000 description 1
- 229910052622 kaolinite Inorganic materials 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 238000001000 micrograph Methods 0.000 description 1
- 239000004005 microsphere Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910021392 nanocarbon Inorganic materials 0.000 description 1
- 239000002074 nanoribbon Substances 0.000 description 1
- 239000002071 nanotube Substances 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 230000008635 plant growth Effects 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 235000009566 rice Nutrition 0.000 description 1
- 238000005070 sampling Methods 0.000 description 1
- 238000012216 screening Methods 0.000 description 1
- 229910052624 sepiolite Inorganic materials 0.000 description 1
- 235000019355 sepiolite Nutrition 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 229910052567 struvite Inorganic materials 0.000 description 1
- 239000000725 suspension Substances 0.000 description 1
Images
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C1/00—Reclamation of contaminated soil
- B09C1/08—Reclamation of contaminated soil chemically
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K17/00—Soil-conditioning materials or soil-stabilising materials
- C09K17/02—Soil-conditioning materials or soil-stabilising materials containing inorganic compounds only
- C09K17/08—Aluminium compounds, e.g. aluminium hydroxide
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C2101/00—In situ
Landscapes
- Chemical & Material Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Soil Sciences (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Inorganic Chemistry (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Processing Of Solid Wastes (AREA)
Abstract
The invention discloses an ultra-stable mineralizer and application thereof in repairing heavy metal contaminated soil. The hyperstable mineralizer is prepared by quickly adding an environment-friendly metal ion solution and a precipitator into a micro-liquid membrane reactor; the application process can be implemented by means of sowing or slurry spraying. The weak alkalinity of the hyperstable mineralizer can not cause the acidification of the soil, and the hyperstable mineralizer is very suitable for southern areas with serious soil pollution. Compared with the adsorbent, the super-stable mineralizer prepared by the invention has very high activity, can quickly anchor heavy metal ions such as copper, cadmium, manganese and the like in soil in crystal lattices of the super-stable mineralizer in an isomorphous substitution or dissolution-reconstruction mode, and mineralizes to form hydrotalcite with a more stable structure, and the heavy metal ions are extremely difficult to dissociate from the hydrotalcite and are in a super-stable mineralized state. In addition, due to the matching rule of the ionic radius, the super-stable mineralizer prepared by the invention also shows good selectivity and has very good effect in-situ remediation of heavy metal pollution of soil.
Description
Technical Field
The invention belongs to the field of inorganic material synthesis and soil remediation, and particularly relates to an ultrastable mineralizer and application thereof in remediation of heavy metal contaminated soil.
Background
Soil is one of the basic elements for maintaining the county of China. However, the soil pollution condition in China is severe due to the irregular disposal of pollutants, geological changes and the like. The data published by the country in 2014 shows a nationwide contaminated soil percentage of 16.1%, with an agricultural land contamination percentage of 19.4% (about 4 billion acres), and a portion of typical plot and surrounding land contamination percentages as high as 36.3%. The harm of the polluted soil to the human health is eye striking, such as the cadmium exceeding rice and the like. The soil method of the national headquarter of the people's republic of China, soil pollution prevention and treatment law, published by 31/8/2018, shows that the national high importance on soil pollution prevention and treatment work on one hand and that the soil pollution treatment work is imminent on the other hand.
In the polluted soil, heavy metal pollution is mainly (82.4%), and the existing remediation technologies for heavy metal pollution in soil are more in variety, wherein the in-situ passivation strategy is to change the occurrence form of heavy metal in soil by adding a passivating agent in situ, and convert an active state with high bioavailability into a stable state with low bioavailability, so that the mobility and bioavailability of the heavy metal in the soil are reduced, and the remediation purpose is achieved. The technology is more competitive in the aspects of repair effect, operation flexibility, economy and large-scale application, and is also favored by key recommendations and industries of national governing departments.
The passivating agent is the core of an in-situ passivation technology, common passivating agents in the market at present, such as organic carbon, sepiolite, palygorskite and the like, mainly realize passivation on heavy metal ions by virtue of electrostatic attraction and surface adsorption of materials, and the passivation mode has weak acting force and is easily influenced by external conditions, so that pollutants are desorbed and polluted again. In addition, due to the complexity of soil composition and the diversity of pollution sources, heavy metal ions, a large amount of harmless and even beneficial other ions exist in the polluted soil, and the mutual interference among various ions brings challenges to the targeted implementation of the passivation of the heavy metal ions. Moreover, as the total amount of the soil pollution area is large, economic cost must be considered seriously while the remediation effect is ensured, and the conventional passivator has low unit price, low adsorption quantity, easy desorption, large using amount and frequent use, and high total cost; materials such as MOF, MXene and the like with excellent adsorption effects are complex in preparation process, harsh in conditions, high in cost and difficult to realize large-scale use. Therefore, the construction of a novel passivator with strong binding force, high selectivity, economy and environmental protection becomes an urgent problem to be solved in the current heavy metal pollution remediation work.
The invention content is as follows:
the invention aims to provide an ultra-stable mineralizer and application thereof in repairing heavy metal contaminated soil. The hyperstable state of mineralization is defined as: in the treatment of heavy metal pollution of soil, when heavy metal ions are in a carbonate state, a relatively stable state is shown, the enrichment of heavy metals in plants is inhibited, and when the heavy metal ions are in a hydrotalcite-like structure, the solubility product constant is smaller, the structure is more stable, namely, an ultrastable mineralization state, and the repairing agent capable of realizing the mineralization effect is called an ultrastable mineralizer.
The ultra-stable mineralizer is prepared by quickly adding an environment-friendly metal ion solution and a precipitator into a micro-liquid membrane reactor; the application process can be implemented by means of sowing or slurry spraying. The weak alkalinity of the hyperstable mineralizer can not cause the acidification of the soil, and the hyperstable mineralizer is very suitable for southern areas with serious soil pollution. Compared with the adsorbent, the super-stable mineralizer prepared by the invention has very high activity, can quickly anchor heavy metal ions such as copper, cadmium, manganese and the like in soil in crystal lattices of the super-stable mineralizer in an isomorphous substitution or dissolution-reconstruction mode, mineralizes to form hydrotalcite with a more stable structure, has a solubility product constant which is tens of orders of magnitude smaller than that of corresponding hydroxide or carbonate under the action of multiple chemical bonds, and has stability far beyond that of the hydroxide and carbonate, so that the heavy metal ions are extremely difficult to dissociate from the super-stable mineralizer and are in a super-stable mineralized state. In addition, due to the matching rule of the ionic radius, the super-stable mineralizer prepared by the invention also shows good selectivity and has very good effect in-situ remediation of heavy metal pollution of soil.
The preparation method of the hyperstable mineralizer comprises the following steps:
(1) preparing a metal salt solution or a metal salt dispersion liquid; preparing an alkali solution with the concentration of 0.01-1.5 mol/L;
(2) and simultaneously and quickly pouring a metal salt solution or a metal salt dispersion liquid and an alkali solution into a micro-liquid-film reactor, transferring the obtained slurry into a crystallization kettle for crystallization at the temperature of 25-160 ℃ for 0-12 hours, dispersing and washing the precipitate obtained by centrifugation with deionized water, then centrifuging, and drying the precipitate in an oven at the temperature of 25-40 ℃ for 0-12 hours to obtain the ultra-stable mineralizer.
The metal salt is selected from one or more of magnesium salt, ferrous salt, ferric salt and calcium salt.
The magnesium salt is selected from one or more of magnesium nitrate, magnesium chloride, magnesium sulfate and magnesium hydroxide; the ferric salt is selected from one or more of ferric nitrate, ferric sulfate, ferric chloride and ferric hydroxide; the ferrous salt is selected from one or more of ferrous nitrate, ferrous sulfate, ferrous chloride and ferric hydroxide; the calcium salt is selected from one or more of calcium nitrate, calcium chloride, calcium sulfate, calcium oxide, calcium hydroxide, desulfurized gypsum and phosphogypsum.
The alkali solution is prepared from one or more of sodium metaaluminate, sodium hydroxide and potassium hydroxide.
The alkali solution is sodium metaaluminate solution, and the molar ratio of the metal elements in the metal salt solution or the metal salt dispersion liquid to the sodium metaaluminate in the step (2) is 1.5:1-3: 1.
The alkali solution does not contain sodium metaaluminate, and in the step (2), the metal salt solution or the metal element of the metal salt dispersion liquid and OH of the alkali solution-In a molar ratio of 1.2:1 to 2: 1.
The alkali solution contains sodium metaaluminate and sodium hydroxide orAnd potassium hydroxide, OH of the metal salt solution or the metal element of the metal salt dispersion in the step (2) and the alkali solution-In a molar ratio of 1.0:1 to 1.5: 1.
The application of the hyperstable mineralizer prepared by the method in removing heavy metals in water. The use method of the hyperstable mineralizer for removing heavy metals in water comprises the following steps: adding the hyperstable mineralizer into the solution containing the heavy metals, controlling the pH of the solution to be more than 4, and shaking for 5-120 minutes at room temperature to remove the heavy metals in the solution.
The hyperstable mineralizer prepared by the method is applied to remediation of heavy metal contaminated soil. The application method of the hyperstable mineralizer for repairing heavy metal contaminated soil comprises the following steps: preparing 5-10 wt% slurry with hyperstable mineralizer; after ploughing 1-25cm of soil on the surface, spraying slurry according to the use amount of 150-250 kg/mu to ensure that the hyperstable mineralizer is fully contacted with the soil, spraying water according to the drought degree of the soil in the later period to ensure that the water content of the soil is kept 50-70% of the maximum water holding capacity, and normally planting crops after two weeks.
The invention has the beneficial effects that:
(1) the preparation process of the material is simple, efficient and wide in raw materials. The reactants form a micro liquid film with the thickness of micron scale in the micro liquid film reactor to promote the rapid and sufficient reaction of the reactants, the crystal nucleus is rapidly formed, and meanwhile, the product is rapidly separated from the reactor under the action of high tangential force, so that the stable and continuous synthesis of the material can be realized, the foundation is laid for the rapid batch preparation of the material, the crystal phase structure of the prepared hyperstable mineralizer is good, no obvious impurity exists (figure 1), and the performance is well guaranteed.
(2) In the hyperstable mineralizer, different metal atoms are uniformly dispersed in the material, and a closely-arranged octahedral configuration is formed by sharing hydroxyl. When the ion-like hydrotalcite acts with heavy metal cadmium, manganese and copper ions, as the ionic radius of the heavy metal ions is very close to the radius of a divalent metal atom in the hyperstable mineralizer, a certain metal atom in the hyperstable mineralizer can be replaced by isomorphous replacement to form hydrotalcite-like compounds containing heavy metals, so that the mineralization of the heavy metal ions is realized, as shown in fig. 2, 3 and 4. In addition, different from the conventional adsorption material, the super-stable mineralizer plays a role in removing heavy metals by replacing the original metal atoms in the super-stable mineralizer, so that the number of active sites in the super-stable mineralizer is large, and the removal amount of the super-stable mineralizer on heavy metal ions is extremely high, as shown in fig. 5, the removal amount of the prepared calcium-based super-stable mineralizer on cadmium under the normal temperature condition reaches 548mg/g, which is far higher than the removal capability of most of materials reported at present on cadmium.
(3) Because the hyperstable mineralizer mineralizes the heavy metal ions into the hydrotalcite-like structure to remove the heavy metal ions, the hydrotalcite-like structure has high stability and extremely low solubility product constant, and can be formed in a short time, the treatment speed is high, and as shown in figure 6, when the concentration of cadmium ions is respectively 15ppm, 30ppm and 60ppm, the cadmium removal rate of the calcium-based hyperstable mineralizer in 5 minutes reaches more than 99%. In addition, cadmium atoms are anchored in a layered crystal lattice of the hydrotalcite, so that the hydrotalcite has very good stability, is difficult to be separated out to cause secondary pollution, and has good long-term effect.
(4) As the radius of other ions is close to that of divalent ions in the hyperstable mineralizer, isomorphous substitution is possible, the hyperstable mineralizer has very good selectivity in soil remediation, and the magnesium, potassium and other ions which are beneficial to plant growth cannot be passivated mistakenly, and as can be seen from figure 7, under the condition that a large amount of potassium, magnesium and zinc ions coexist, the removal rate of cadmium by the calcium-based hyperstable mineralizer is not obviously reduced, which indicates that the hyperstable mineralizer has good selectivity.
(5) A large amount of nitrate ions, sulfate ions and chloride ions exist in soil, the effect of the conventional repairing agent is greatly influenced by the existence of the nitrate ions, the sulfate ions and the chloride ions, the effect of the super-stable mineralizer prepared by the invention on removing heavy metals is still not influenced under the interference of high-concentration anions, and the mineralization performance of the material is improved when the nitrate ions and the sulfate ions exist (as shown in figure 8).
(6) The super-stable mineralizer can be promoted to rapidly contact with heavy metals in the soil to act by spraying or broadcasting the slurry after ploughing in the soil treatment process, so that the time is saved.
Description of the drawings:
FIG. 1 is an XRD pattern of the calcium-based hyperstable mineralizer prepared in example 1.
FIG. 2 is an XRD pattern of a product obtained by removing cadmium ions using the calcium-based hyperstable mineralizer of example 1.
FIG. 3 is an XRD pattern of the product obtained after removal of copper ions using the calcium-based hyperstable mineralizer of example 1.
FIG. 4 is an XRD pattern of a product obtained after removing manganese ions by using the calcium-based hyperstable mineralizer of example 1.
FIG. 5 is a graph showing the removal rate of 0.1g of the calcium-based hyperstable mineralizer and 120ppm of cadmium ion in application example 1.
FIG. 6 is a graph showing the removal rate of 0.1g of the calcium-based hyperstable mineralizer of application example 1 at initial concentrations of cadmium ions of 15, 30 and 60 ppm.
Fig. 7 is a graph showing the removal rate of cadmium ions by the calcium-based hyperstable mineralizer when potassium, magnesium, zinc and cadmium ions coexist in application example 1.
FIG. 8 is a graph showing the removal rate of cadmium ions by a calcium-based hyperstable mineralizer when nitrate, sulfate, and chloride ions are present in large amounts in application example 1.
FIG. 9 is a TEM image of the calcium-based hyperstable mineralizer prepared in example 2.
FIG. 10 is an electron micrograph of a product obtained by removing cadmium ions using the calcium-based hyperstable mineralizer of example 1.
Detailed Description
The present invention is further illustrated by the following specific examples in order to better understand the operation of the present invention for the relevant persons, but the scope of the present invention is not limited thereto.
Example 1:
23.6g Ca (NO) are weighed out3)2·4H2Dissolving O in 500ml deionized water to obtain solution A, weighing 4.1g NaAlO2Dissolving the solution B in 500ml of deionized water to obtain a solution B, simultaneously and quickly adding the solution A, B into a micro-liquid membrane reactor with the rotating speed of 3000r/min, collecting slurry at a discharge port, centrifugally washing the slurry by the deionized water, and drying the slurry for 12 hours at 40 ℃ to obtain the calcium-based hyperstable mineralizer. FIG. 1 is the XRD pattern of the prepared material, from which it can be seen that the prepared calcium-based hyperstable mineralization material of calcium-aluminum composite materialThe agent presents the structural characteristics of a layered material, does not have diffraction peaks of substances such as calcium carbonate, calcium hydroxide, aluminum hydroxide and the like, and the composite material prepared on the surface is of a single-phase structure.
Example 2:
weighing 29.4g of CaCl2·2H2Dissolving O in 500ml deionized water to obtain solution A, weighing 8.2g NaAlO2Dissolving in 500ml deionized water to obtain solution B, simultaneously and rapidly adding the solution A, B into a micro-liquid membrane reactor with the rotating speed of 3000r/min, collecting slurry at a discharge port, centrifugally washing with deionized water, and drying at 40 ℃ for 12 hours. The transmission electron microscope image of the prepared material is shown in fig. 9, and the material has a random nano two-dimensional sheet structure.
Example 3:
weighing 37.0g Ca (OH)2Dissolving in 500ml deionized water to obtain suspension A, weighing 20.1g NaAlO2Dissolving in 500ml deionized water to obtain solution B, simultaneously and rapidly adding the solution A, B into a micro-liquid membrane reactor with the rotating speed of 3000r/min, collecting slurry at a discharge port, crystallizing at 120 ℃ for 8 hours, centrifugally washing with deionized water, and drying at 40 ℃ for 12 hours.
Application example 1:
removing cadmium in water by using a calcium-based hyperstable mineralizer: 0.1g of the calcium-based hyperstable mineralizer prepared in example 1 was weighed into a 1L beaker, and 500ml of Cd-containing mineralizer2+In which Cd is2+The concentration of (2) is 60mg/L, after magnetically stirring for 20 minutes at room temperature, taking the upper solution, filtering the upper solution by a filter membrane of 0.22 mu m, and measuring Cd in the upper solution by ICP-MS2+The concentration of (c). The result shows that the cadmium is removed by the calcium-based hyperstable mineralizer within 5 minutes by more than 99 percent, and extremely high efficiency is displayed. And respectively adopting calcium-based hyperstable mineralizers to carry out the same experimental operation for removing cadmium ions on the solutions with the initial concentrations of the cadmium ions of 15ppm, 30ppm, 60ppm and 120 ppm. When Cd2+The maximum removal amount reaches 548mg/g when the initial concentration of the cadmium is 120mg/L, which is far beyond the removal capability of most materials to cadmium reported at present (shown in Table 1). The solution containing cadmium ions and potassium, magnesium and zinc coexisting ions is subjected to the same experimental operation for removing the cadmium ions by adopting a calcium-based hyperstable mineralizer, and the removal rate is highAs shown in fig. 7. The same experimental operation for removing cadmium ions was performed on a cadmium ion solution containing a large amount of nitrate, sulfate and chloride ions by using a calcium-based hyperstable mineralizer, and the removal rate results are shown in fig. 8.
TABLE 1
| Material | Maximum adsorption capacity | Literature reference |
| Poly(b-cyclodextrin)-conjugated magnetic graphene oxide | 92.4mg/g | J.Mater.Chem.A,2019,7,2055-2065 |
| Ferromanganese binary oxide–BC composites(FMBC) | 101.0mg/g | Sci.Total Environ.,2018,615,115-122 |
| Amino-modified nanocarbon(NH2-C) | 102.0mg/g | ACS Appl.Nano Mater.2020,3,1,218-228 |
| Kaolinite nanotubes(KNTs) | 116mg/g | J Hazard.Mater.,2019,374,296-308 |
| Struvite attapulgite(MAP/APT) | 121.14mg/g | J.Hazard.Mater.,2017,329,66-76 |
| Corn stalk(Nitrolotriacetic acid anhydride) | 143.4mg/g | RSC Adv.,2015,5,11475-11484 |
| Hydrogel particles(P(AMPS-co-AA)) | 220mg/g | Chem.Eng.J.,2019,359,1360-1371 |
| Iron-embedded carbon beads | 222.6mg/g | RSC Adv.,2020,10,6277-6286 |
| exfoliate a Ti2AlCsheet | 325.89mg/g | ACS Appl.Mater.Interfaces 2019,11,21,19156-19166 |
| 3D mesoporous nanostructured carbon florets | 402mg/g | ACS Appl.Nano Mater.2020,3,1,468-478 |
| Double network hydrogel(PAA/HS) | 412mg/g | J.Mater.Chem.A,2018,6,20110-20120 |
| porous boron nitride nanoribbons | 530mg/g | New J.Chem.,2019,43,3280-3290 |
| Calcium aluminum oxide nitrate hydroxide hydrate | 548mg/g | The product |
| Hydrogel microspheres(PES/HEMA-VP/PAA) | 640mg/g | ACS Sustainable Chem.Eng.,2018,6,5950-5958 |
| magnetic calcium carbonate | 821mg/g | ACS Appl.Nano Mater.2020,3,2,1272-1281 |
The same experimental procedure as described above was carried out on the solutions containing copper ions and manganese ions, respectively, using the calcium-based hyperstable mineralizer prepared in example 1 to remove copper ions and manganese ions, respectively, and XRD patterns of the resulting products are shown in fig. 3 and 4.
Application example 2:
the calcium-based hyperstable mineralizer is used for repairing cadmium-polluted soil: taking a soil sample polluted by cadmium from a polluted land, detecting that the cadmium in the soil exceeds a risk screening value by 40 times according to the national standard GB-15618 plus 2008, taking 1000g of the pretreated soil sample, fully mixing 20g of the calcium-based hyperstable mineralizer prepared in the embodiment 1 in a 1L beaker, adding 500ml of deionized water, naturally placing, sampling at certain intervals, and then adopting CaCl2The method is used for measuring the biological effective state. Table 2 shows the change values of the effective state content of Cd in different repairing time periods, the data in the table shows that the effective state content of Cd is reduced from 0.482mg/kg to 0.023mg/kg after 7 days of repairing, the reduction amplitude is 95.2%, the effective state content of Cd is reduced from 0.467mg/kg to 0.018mg/kg after 14 days of repairing, the reduction amplitude is 96.1%, and the effective state content of Cd is reduced from 0.473mg/kg to 0.015mg/kg after 28 days, and is reduced by 96.8%. The data show that the calcium-based hyperstable mineralizer can be greatly reduced in a short timeThe effective state content of Cd in the soil basically reaches an equilibrium state in 7 days, and excellent passivation performance is shown.
TABLE 2 different repair periods Cd2+Change in active State concentration (mg/kg)
| 7days | 14days | 28days | |
| Blank space | 0.482 | 0.467 | 0.473 |
| Calcium-based hyperstable mineralizer | 0.023 | 0.018 | 0.015 |
Claims (10)
1. The preparation method of the hyperstable mineralizer is characterized by comprising the following operation steps:
(1) preparing a metal salt solution or a metal salt dispersion liquid; preparing an alkali solution with the concentration of 0.01-1.5 mol/L;
(2) and simultaneously and quickly pouring a metal salt solution or a metal salt dispersion liquid and an alkali solution into a micro-liquid-film reactor, transferring the obtained slurry into a crystallization kettle for crystallization at the temperature of 25-160 ℃ for 0-12 hours, dispersing and washing the precipitate obtained by centrifugation with deionized water, then centrifuging, and drying the precipitate in an oven at the temperature of 25-40 ℃ for 0-12 hours to obtain the ultra-stable mineralizer.
2. The method according to claim 1, wherein the metal salt is selected from one or more of magnesium salt, ferrous salt, ferric salt and calcium salt.
3. The preparation method according to claim 2, wherein the magnesium salt is selected from one or more of magnesium nitrate, magnesium chloride, magnesium sulfate and magnesium hydroxide; the ferric salt is selected from one or more of ferric nitrate, ferric sulfate, ferric chloride and ferric hydroxide; the ferrous salt is selected from one or more of ferrous nitrate, ferrous sulfate, ferrous chloride and ferric hydroxide; the calcium salt is selected from one or more of calcium nitrate, calcium chloride, calcium sulfate, calcium oxide, calcium hydroxide, desulfurized gypsum and phosphogypsum.
4. The preparation method of claim 1, wherein the alkali solution is prepared from one or more of sodium metaaluminate, sodium hydroxide and potassium hydroxide.
5. The process according to claim 4, wherein the alkali solution is a sodium metaaluminate solution, and the molar ratio of the metal element in the metal salt solution or metal salt dispersion to sodium metaaluminate in step (2) is 1.5:1 to 3: 1.
6. The method according to claim 4, wherein the alkali solution does not contain sodium metaaluminate, and the OH groups of the alkali solution and the metal element of the metal salt solution or metal salt dispersion in step (2)-In a molar ratio of 1.2:1 to 2: 1.
7. The process according to claim 4, wherein the alkaline solution comprises sodium metaaluminate and sodium hydroxide and/or potassium hydroxide, and the metal salt solution or metal salt dispersion in step (2) is prepared by mixing the metal element with the alkaline solutionOH-In a molar ratio of 1.0:1 to 1.5: 1.
8. Use of the hyperstable mineralizer prepared according to the method of claim 1 for removing heavy metals from water.
9. The application of the hyperstable mineralizer prepared according to the method of claim 1 to remediation of heavy metal contaminated soil.
10. The application of the hyperstable mineralizer according to claim 9, wherein the hyperstable mineralizer is used for repairing heavy metal contaminated soil by the following method: preparing 5-10 wt% slurry with hyperstable mineralizer; after ploughing 1-25cm of soil on the surface, spraying slurry according to the use amount of 150-250 kg/mu to ensure that the hyperstable mineralizer is fully contacted with the soil, spraying water according to the drought degree of the soil in the later period to ensure that the water content of the soil is kept 50-70% of the maximum water holding capacity, and normally planting crops after two weeks.
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