CN117603697A - Resistance-controlled antibiotic resistance gene pollution material composition, resistance-controlled pollution material, preparation method and application thereof - Google Patents

Resistance-controlled antibiotic resistance gene pollution material composition, resistance-controlled pollution material, preparation method and application thereof Download PDF

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Publication number
CN117603697A
CN117603697A CN202311417225.2A CN202311417225A CN117603697A CN 117603697 A CN117603697 A CN 117603697A CN 202311417225 A CN202311417225 A CN 202311417225A CN 117603697 A CN117603697 A CN 117603697A
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resistance
water
component
quaternary ammonium
ammonium salt
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王学江
袁梦
孙振华
陈柳宇
颜常春
赵建夫
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Tongji University
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Tongji University
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    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09KMATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K17/00Soil-conditioning materials or soil-stabilising materials
    • C09K17/40Soil-conditioning materials or soil-stabilising materials containing mixtures of inorganic and organic compounds

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  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Soil Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Agricultural Chemicals And Associated Chemicals (AREA)

Abstract

The invention relates to the technical field of soil pollution treatment and restoration, and particularly discloses a resistance-control antibiotic resistance gene pollution material composition, a resistance-control pollution material, a preparation method and application thereof. The composition comprises a component A, a component B and Portland cement: (I) A component: clay, feSO 4 ·7H 2 O、KMnO 4 The method comprises the steps of carrying out a first treatment on the surface of the (II) component B: water-retaining agent and quaternary ammonium salt; (III) Portland cement. The resistance and control antibiotic resistance gene pollution material provided by the invention has the advantages of simple preparation and convenient use, and can be used for efficiently removing and long-acting resistance and control antibiotic resistance genes in soil.

Description

Resistance-controlled antibiotic resistance gene pollution material composition, resistance-controlled pollution material, preparation method and application thereof
Technical Field
The invention relates to the technical field of soil pollution treatment and repair, in particular to a resistance-control antibiotic resistance gene pollution material composition, a resistance-control pollution material, a preparation method and application thereof.
Background
Antibiotics are widely used as an antibacterial drug in human medical treatment and livestock and poultry farming, however, excessive use of antibiotics induces the generation of antibiotic resistance genes (antibiotic resistance genes, ARGs) in animals, and causes a certain influence on the ecological environment after the discharge of feces, so that the harm of ARGs is far more than that of the antibiotics per se due to the persistence of ARGs residues, and the ARGs are popular as a novel environmental pollutant in various fields since 2006.
Soil is considered as one of the most important receptors for antibiotic residues, and the antibiotic residues and ARGs enter the soil through fertilization, sludge agriculture, waste water or reclaimed water irrigation and other modes, so that the soil becomes a huge reservoir of the ARGs, and the human health is seriously threatened. In order to reduce the spread of ARGs in soil media, researchers have focused on developing various ARGs abatement technologies, such as aerobic composting, anaerobic fermentation and water treatment processes, to reduce the input and enrichment of antibiotics and exogenous ARGs in soil caused by agricultural production processes such as organic fertilizer, sludge returning, sewage irrigation and the like.
In order to prevent the diffusion of ARGs entering the soil, researchers use a method (CN 202110270919.2) of adding biomass charcoal (CN 202110259591.4), agricultural ferment (CN 202111045142.6) and other materials into the soil and utilizing biomass charcoal-super-enriched plants to repair in situ.
However, the current in-situ repair method still has the problems of long repair period, insufficient resistance to ARGs horizontal transmission, and the like, and is difficult to popularize and apply. Therefore, searching or developing a repair material with excellent performance and economical and practical performance becomes a key for controlling ARGs pollution of soil by primary steric hindrance.
Disclosure of Invention
The invention aims to solve the problems of long repair period, insufficient resistance to ARGs horizontal transmission and control and the like in the in-situ repair method in the prior art.
In order to achieve the above object, a first aspect of the present invention provides a resistance-controlling antibiotic resistance gene pollution material composition comprising an a-component, a B-component and portland cement, wherein the material composition comprises the following components:
(I) And (3) a component A: clay, feSO 4 ·7H 2 O、KMnO 4
(II) component B: water-retaining agent and quaternary ammonium salt;
(III) portland cement;
wherein the clay and the FeSO 4 ·7H 2 O, the KMnO 4 The content weight ratio of the water-retaining agent to the quaternary ammonium salt is 10-50:3-15:2-10:10-30:2-5;
the weight content ratio of the component A, the component B and the Portland cement is 5-10:3-6:0.5-1;
in the component A, the clay is selected from any one of attapulgite, bentonite or diatomite, and the average volume particle diameter is not more than 150 mu m.
In a second aspect, the present invention provides (1) a process for preparing material A: clay, feSO in the presence of water I 4 ·7H 2 O、KMnO 4 After first mixing, regulating the pH value to 7-8, then carrying out first contact reaction, and obtaining a material A after separation, washing and drying;
(2) Preparing a material B: mixing the aqueous solution of the quaternary ammonium salt with a water-retaining agent to perform a second contact reaction, and separating to obtain a material B;
(3) Preparing a resistance and antibiotic resistance gene pollution material: carrying out second mixing on the material A and Portland cement and water III to obtain a mixture I; wherein the amount of water II is controlled such that the water content of the mixture I is 60t%;
rolling and granulating the mixture I and the material B, and drying to obtain the resistance gene pollution material;
wherein the clay and the FeSO 4 ·7H 2 O, the KMnO 4 The weight ratio of the water-retaining agent to the quaternary ammonium salt is 10-50:3-15:2-10:10-30:2-5;
the weight ratio of the material A to the material B to the Portland cement is 5-10:3-6:0.5-1.
In a third aspect, the present invention provides a resistance-controlled antibiotic resistance gene contamination material prepared by the method of the second aspect.
The fourth aspect of the invention provides an application of the resistance-controlled antibiotic resistance gene pollution material in soil pollution control and restoration.
The resistance and control antibiotic resistance gene pollution material provided by the invention has the advantages of simple preparation and convenient use, and can be used for efficiently removing and long-acting resistance and control antibiotic resistance genes in soil.
Detailed Description
The endpoints and any values of the ranges disclosed herein are not limited to the precise range or value, and are understood to encompass values approaching those ranges or values. For numerical ranges, one or more new numerical ranges may be found between the endpoints of each range, between the endpoint of each range and the individual point value, and between the individual point value, in combination with each other, and are to be considered as specifically disclosed herein.
It should be noted that, in the aspects of the present invention, the present invention is described only once in one aspect thereof without repeated description with respect to the same components or terms in the aspects, and those skilled in the art should not understand the limitation of the present invention.
As described above, the first aspect of the present invention provides a resistance-controlling antibiotic resistance gene pollution material composition comprising a component a, a component B and portland cement, wherein the material composition comprises the following components:
(I) And (3) a component A: clay, feSO 4 ·7H 2 O、KMnO 4
(II) component B: water-retaining agent and quaternary ammonium salt;
(III) portland cement;
wherein the clay and the FeSO 4 ·7H 2 O, the KMnO 4 The content weight ratio of the water-retaining agent to the quaternary ammonium salt is 10-50:3-15:2-10:10-30:2-5;
the weight content ratio of the component A, the component B and the Portland cement is 5-10:3-6:0.5-1;
in the component A, the clay is selected from any one of attapulgite, bentonite or diatomite, and the average volume particle diameter is not more than 150 mu m.
Preferably, in the component B, the water-retaining agent is at least one selected from cationic polyacrylamide and starch graft cross-linked matter thereof, sodium polyacrylate and starch graft cross-linked matter thereof, potassium polyacrylate and starch graft cross-linked matter thereof.
More preferably, in the component B, the water-retaining agent is sodium polyacrylate and/or potassium polyacrylate. The inventors found that in this preferred case, the control effect of the material against contamination with the antibiotic resistance gene can be made better.
Preferably, in the component B, the quaternary ammonium salt is at least one selected from dodecyl dimethyl benzyl ammonium chloride, dodecyl trimethyl ammonium chloride, dodecyl dimethyl benzyl ammonium bromide, tetradecyl dimethyl benzyl ammonium chloride, cyano quaternary ammonium salt, bis C8 alkyl quaternary ammonium bromide, polyazacyclic quaternary ammonium salt, pyridine derivative, polyquaternary ammonium salt, and bis quaternary ammonium salt.
More preferably, in the component B, the quaternary ammonium salt is at least one selected from dodecyl trimethyl ammonium chloride, tetradecyl dimethyl benzyl ammonium chloride, and dodecyl dimethyl benzyl ammonium chloride.
Preferably, the Portland cement is at least one selected from early strength Portland cements having a strength of PO32.5R to PO42.5R.
According to a preferred embodiment, the composition further comprises water.
As previously mentioned, the second aspect of the present invention provides a method for preparing a material for resistance to controlled antibiotic resistance gene contamination using the substance of the composition of the first aspect, comprising:
(1) Preparing a material A: clay, feSO in the presence of water I 4 ·7H 2 O、KMnO 4 After first mixing, regulating the pH value to 7-8, then carrying out first contact reaction, and obtaining a material A after separation, washing and drying;
(2) Preparing a material B: mixing the aqueous solution of the quaternary ammonium salt with a water-retaining agent to perform a second contact reaction, and separating to obtain a material B;
(3) Preparing a resistance and antibiotic resistance gene pollution material: carrying out second mixing on the material A and Portland cement and water III to obtain a mixture I; wherein the amount of water II is controlled such that the water content of the mixture I is 60t%;
rolling and granulating the mixture I and the material B, and drying to obtain the resistance gene pollution material;
wherein the clay and the FeSO 4 ·7H 2 O, the KMnO 4 The weight ratio of the water-retaining agent to the quaternary ammonium salt is 10-50:3-15:2-10:10-30:2-5;
the weight ratio of the material A to the material B to the Portland cement is 5-10:3-6:0.5-1.
Preferably, in step (1), the pH is adjusted using a NaOH solution having a concentration of 3M.
Preferably, in step (2), the concentration of the quaternary ammonium salt in the aqueous solution of the quaternary ammonium salt is 2 to 5wt%. The inventors found that in this preferred case, the removal rate of the resistance gene is more favorable.
Preferably, in step (1), the conditions of the first mixing at least satisfy: the stirring is carried out under the condition of 300-400rpm for 10-15min.
Preferably, in step (1), the conditions of the first contact reaction at least satisfy: the stirring is carried out under the condition that the temperature is 22-28 ℃, the rotating speed is 300-400rpm, and the time is 6-12h.
Preferably, in step (1), the washing is rinsing with deionized water.
Preferably, in step (1), the drying conditions at least satisfy: the temperature is 100-120 ℃ and the time is 4-6h.
According to a preferred embodiment, in step (2), the conditions of the second contact reaction at least satisfy: the stirring is carried out under the condition that the temperature is 22-28 ℃, the rotating speed is 300-400rpm, and the time is 4-8h.
Preferably, in step (3), the conditions of the second mixing at least satisfy: the stirring is carried out under the condition of 300-400rpm for 0.5-1h.
Preferably, in step (3), the temperature of the drying is 100-110 ℃.
In the present invention, the water I, the water II, and the water III are all water, and the weight of the water II, the weight of the water III, and the weight of the water in the aqueous solution of the quaternary ammonium salt together constitute the weight of the water I.
It should also be noted that the apparatus and conditions for the rolling granulation are not particularly limited by the present invention and may be carried out using conventional means in the art.
As previously described, a third aspect of the present invention provides a resistance-controlling antibiotic resistance gene contamination material prepared by the method of the second aspect described above.
As described above, the fourth aspect of the present invention provides the use of the resistance-controlled antibiotic resistance gene contaminated material according to the third aspect in soil pollution control and remediation.
Preferably, the adding amount of the resistance-controlled antibiotic resistance gene pollution material is 30-80g/m 2
Preferably, the resistance-controlling antibiotic resistance gene contamination material is applied to the soil to be treated, and the water content of the soil to be treated is maintained at 12-20wt%.
The invention will be described in detail below by way of examples. In the following examples, unless otherwise specified, all the raw materials used are commercially available.
Some of the raw materials and sources used in the examples below were as follows:
room temperature in the present invention means 25±2 ℃ unless otherwise specified.
Example 1
This example is for illustrating the method for preparing a resistance-controlled antibiotic resistance gene contamination material according to the present invention, referring to the amounts and parameters shown in Table 1, and is performed according to the procedure comprising the steps of:
(1) Preparing a material A: 10g of clay, feSO, in the presence of water II (deionized water) 4 ·7H 2 O、KMnO 4 After first mixing, regulating the pH to 7 by using a NaOH solution with the concentration of 3M, then carrying out a first contact reaction, eluting by using deionized water after separation, and drying to obtain a material A;
(2) Preparing a material B: mixing an aqueous solution of quaternary ammonium salt (the concentration of the quaternary ammonium salt is 5 wt%) with a water-retaining agent to perform a second contact reaction, and separating to obtain a material B;
(3) Preparing a resistance and antibiotic resistance gene pollution material: carrying out second mixing on the material A and Portland cement and water III to obtain a mixture I; wherein the amount of water III is controlled such that the water content of the mixture I is 60 wt.%;
the weight ratio of the material A to the material B to the silicate cement is 5:3:0.5;
and rolling and granulating the mixture I and the material B, and drying to obtain the resistance-controlled antibiotic resistance gene pollution material which is named as P1.
Example 2
This example uses a formulation and method similar to that of example 1 except that: the preparation conditions, the names of substances and the addition amount are changed, wherein the weight ratio of the material A to the material B to the silicate cement is 5:3.5:0.4;
referring specifically to Table 1, the resistance gene contamination material of the resistance control antibiotic, designated as P2, was finally obtained.
Example 3
This example uses a formulation and method similar to that of example 1 except that: the preparation conditions, the names of substances and the addition amount are changed, wherein the weight ratio of the material A to the material B to the silicate cement is 5:4:1, a step of;
referring specifically to Table 1, the resistance gene contamination material of the resistance control antibiotic, designated as P3, was finally obtained.
Test example 1
The prepared resistance-controlled antibiotic resistance gene contamination materials prepared in examples and comparative examples were prepared at a rate of 50g/m 2 The adding amount of the fertilizer is added into farmland soil with the thickness of 20cm, the farmland soil is uniformly mixed, and water is sprayed to ensure that the water content of the soil is 15%;
when P1 is used, the initial abundance of several major resistance genes tetO, tetQ, tetWsul 2, intI1 in soil is 2.55X10, respectively 6 copies/g、3.73×10 7 copies/g、1.17×10 7 copies/g、4.11×10 7 Copies/g and 3.14X10 7 copies/g;
When P2 is used, the initial abundance of several major resistance genes tetO, tetQ, tetWsul 2, intI1 in soil is 2.55X10, respectively 6 copies/g、3.73×10 7 copies/g、1.17×10 7 copies/g、4.11×10 7 Copies/g and 3.14X10 7 copies/g;
When P3 is used, the initial abundance of several major resistance genes tetO, tetQ, tetWsul 2, intI1 in soil are 3.12X10, respectively 7 copies/g、2.83×10 6 copies/g、2.45×10 7 copies/g、2.97×10 7 Copies/g and 5.11X10 7 copies/g;
After 7 days of stabilization treatment, the removal rates of the resistance genes in the above 5 were recorded, respectively, and the results are shown in Table 2.
Test example 2
The procedure was carried out in a similar manner to test example 1, except that a ferro-manganese oxide modified clay material was used instead of the resistance-controlling antibiotic resistance gene contamination material and was carried out in the same amount as the addition amount, and the removal rate of the resistance gene in the above 5 was recorded, and the results are shown in Table 2.
TABLE 1
TABLE 2
Resistance gene species P1 P2 P3 Iron-manganese oxide modified clay material
tet O removal Rate (%) 77.8 77.7 85.8 20
tet Q removal Rate (%) 83.5 85.3 86.1 25
tet W removal Rate (%) 82.7 85.9 90.5 23
Sul 2 removal (%) 90.4 91.8 92.8 27
intI1 removal (%) 92.8 91.9 90.9 25
The result shows that the resistance gene pollution material for the resistance antibiotic provided by the invention has the advantages of simple preparation, convenient use, and capability of efficiently removing and long-acting resistance control on the resistance gene in the soil.
The preferred embodiments of the present invention have been described in detail above, but the present invention is not limited thereto. Within the scope of the technical idea of the invention, a number of simple variants of the technical solution of the invention are possible, including combinations of the individual technical features in any other suitable way, which simple variants and combinations should likewise be regarded as being disclosed by the invention, all falling within the scope of protection of the invention.

Claims (10)

1. A composition of a material for preventing and controlling antibiotic resistance gene pollution, which is characterized by comprising an A component, a B component and Portland cement, wherein the composition of the material comprises the following components:
(I) And (3) a component A: clay, feSO 4 ·7H 2 O、KMnO 4
(II) component B: water-retaining agent and quaternary ammonium salt;
(III) portland cement;
wherein the clay and the FeSO 4 ·7H 2 O, the KMnO 4 The content weight ratio of the water-retaining agent to the quaternary ammonium salt is 10-50:3-15:2-10:10-30:2-5;
the weight content ratio of the component A, the component B and the Portland cement is 5-10:3-6:0.5-1;
in the component A, the clay is selected from any one of attapulgite, bentonite or diatomite, and the average volume particle diameter is not more than 150 mu m.
2. The composition according to claim 1, wherein in the B component, the water-retaining agent is selected from at least one of cationic polyacrylamide and starch graft type crosslinks thereof, sodium polyacrylate and starch graft type crosslinks thereof, potassium polyacrylate and starch graft type crosslinks thereof; and/or
In the component B, the quaternary ammonium salt is at least one selected from dodecyl dimethyl benzyl ammonium chloride, dodecyl trimethyl ammonium chloride, dodecyl dimethyl benzyl ammonium bromide, tetradecyl dimethyl benzyl ammonium chloride, cyano quaternary ammonium salt, double C8 alkyl quaternary ammonium bromide, polyazacyclic quaternary ammonium salt, pyridine derivatives, polyquaternary ammonium salt and double quaternary ammonium salt.
3. The composition according to claim 1 or 2, wherein the portland cement is selected from at least one of early strength portland cements having a strength of the order PO32.5R-PO42.5R.
4. The composition according to claim 1 or 2, wherein the composition further comprises water.
5. A method for preparing a material for resistance to genetic contamination by a controlled antibiotic, the method being carried out using a substance in a composition according to any one of claims 1 to 4, comprising:
(1) Preparing a material A: clay, feSO in the presence of water I 4 ·7H 2 O、KMnO 4 After first mixing, regulating the pH value to 7-8, then carrying out first contact reaction, and obtaining a material A after separation, washing and drying;
(2) Preparing a material B: mixing the aqueous solution of the quaternary ammonium salt with a water-retaining agent to perform a second contact reaction, and separating to obtain a material B;
(3) Preparing a resistance and antibiotic resistance gene pollution material: carrying out second mixing on the material A and Portland cement and water III to obtain a mixture I; wherein the amount of water II is controlled such that the water content of the mixture I is 60t%;
rolling and granulating the mixture I and the material B, and drying to obtain the resistance gene pollution material;
wherein the clay and the FeSO 4 ·7H 2 O, the KMnO 4 The weight ratio of the water-retaining agent to the quaternary ammonium salt is 10-50:3-15:2-10:10-30:2-5;
the weight ratio of the material A to the material B to the Portland cement is 5-10:3-6:0.5-1.
6. The method according to claim 5, wherein in step (2), the concentration of the quaternary ammonium salt in the aqueous solution of the quaternary ammonium salt is 2 to 5wt%.
7. The method according to claim 5 or 6, wherein in step (1), the conditions of the first mixing at least satisfy: stirring at 300-400rpm for 10-15min; and/or
In step (1), the conditions of the first contact reaction at least satisfy: stirring at 22-28deg.C at 300-400rpm for 6-12 hr; and/or
In step (1), the drying conditions at least satisfy: the temperature is 100-120 ℃ and the time is 4-6h.
8. The method according to claim 5 or 6, wherein in step (2), the conditions of the second contact reaction at least satisfy: stirring at 22-28deg.C at 300-400rpm for 4-8 hr; and/or
In step (3), the conditions of the second mixing at least satisfy: the stirring is carried out under the condition of 300-400rpm for 0.5-1h.
9. A resistance-controlled antibiotic-resistance gene contaminated material prepared by the method of any one of claims 5 to 8.
10. The use of the resistance-controlled antibiotic resistance gene pollution material of claim 9 in soil pollution control and remediation.
CN202311417225.2A 2023-10-30 2023-10-30 Resistance-controlled antibiotic resistance gene pollution material composition, resistance-controlled pollution material, preparation method and application thereof Pending CN117603697A (en)

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