LU102374B1 - Method for passivating heavy metal contaminated farmland soil - Google Patents
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Abstract
The present invention relates to a method for passivating heavy metal contaminated farmland soil, which includes the following steps: 1) adding a passivator mainly playing a chemical reaction role into the heavy metal contaminated soil, uniformly stirring same, leaving the same to stand and curing the same; 2) adding a passivator mainly playing an adsorption role into a mixture obtained in step 1), uniformly stirring same, leaving the same to stand and curing the same: and 3) adding water into a mixture obtained in step 2), adjusting a weight water content to 20%-40%. leaving same to stand and curing the same. According to the present invention, ferric oxide, calcium carbonate, hydroxyapatite, plant ash and bentonite are combined and used step by step, advantages of chemically complexing, precipitating and physically adsorbing heavy metal contaminants by different passivation materials are brought into full play, the advantages of all components arc combined together, and an economical, efficient, green and environment-friendly heavy metal passivation agent and a method for remediating heavy metal contaminated farmland are established, so that effective remediation of the heavy metal contaminated farmland is effectively realized.
Description
METHOD FOR PASSIVATING HEAVY METAL CONTAMINATED FARMLAND SOIL Technical Field The present invention belongs to the soil remediation field in the technical field of environment engineering, and particularly relates to a method for passivating heavy metal contaminated farmland soil.
Background Heavy metal contamination in soil has become one of the major environmental pollution problems in China. The discharge of heavy metal pollutants is increasing year by year with the rapid development of mining. metal smelting. chemical industry. battery manufacturing. and other industries involving heavy metals. Worsened by illegal and excessive discharge by some factories, China is faced with a high incidence of heavy metal contamination. In China. the arable land suffering from heavy metal contamination of different degrees is close to 10 million hm’. and it caused more than 10 million tons of food production reduction annually, with as much as 12 million tons contaminated by heavy metals.
The harm of heavy metals in soil on crop production is mainly reflected in two aspects. First, it raises the heavy metal content in agricultural products above the threshold. Second. it poisons the crops. resulting in yield reduction, or even total crop failure. The toxicity of the heavy metal arsenic, even at a low concentration. is detrimental to seedlings of sensitive crops such as rice. chili peppers. red cowpeas. leading to a reduction in biomass by more than 10%. Heavy metals eventually enter the human body [rom the food chain through the soil-plant system and affeet human health. They harm human skin, respiratory. digestive. urinary, cardiovascular, neurological, and hematopoietic systems among others and induce cell chromosomal aberrations. sister chromatid exchange and micronucleus increase and other DNA structure damages of cytological consequences.
At present, main treatment methods for heavy metal contaminated farmland soil in China include soil passivation. agronomic control, phytoremediation, soil washing. and planting structure adjustment. Phytoremediation is the main method adopted, whercas the treatment cycle is relatively long.
Soil passivation minimizes the toxicity of heavy metals by adding chemicat conditioner or passivator to the soil. This approach reduces the mobility of heavy metals through adsorption or co-precipitation to lower the content of effective heavy metals in the soil and reduce the uptake of heavy metals by crops. This is a convenient. effective, economical and practical method for soil remediation of contaminated farmland.
In the prior art. numerous Chinese invention patents CN201711464010. CN201610596960,
CN201710178365. CN201810365538. CN201610079842. cte. disclose a method for passivating soil and passivators for the method. which are mainly used for passivating heavy metal by mixing the passivators of different types with soil to react with the heavy metal, but each type of passivator has a different principle of removing the heavy metal. so actual action and interaction of each type of passivator are diffieult to distinguish, and it is difficult to further improve the heavy metal removal effect. In addition, in the prior art. an adsorption role, chemical action, ete. are conducted at the same time, which may cause restrictive influences among different actions. Chinese invention patent CN201710902422 discloses a technical solution of firstly adding an adsorbent and then adding a chemical reaction reagent to remove heavy metal in soil, but firstly adsorbing the heavy metal may cause local excess of the heavy metal in the soil. which may cause adverse effects on further improvement ol soil passivation. Therefore, deeper research on how 16 improve the technical effect of soil passivation 1s still needed.
Summary of the Invention According to the present invention, ferric oxide, calcium carbonate. hydroxyapatite. plant ash and bentonite are combined and used step by step. advantages of chemically complexing. precipitating and physically adsorbing heavy metal contaminants by different passivation materials are brought into full play, the advantages of all components are combined together. and an economical. efficient, green and environment-friendly heavy metal passivation agent and a method for remediating heavy metal contaminated farmland are established. so that effective remediation of the heavy metal contaminated farmland is effectively realized.
In order to realize the above objective. the present invention provides a method for passivating heavy metal contaminated farmland soil, which specifically includes: 1) adding a passivator mainly playing a chemical reaction role into the heavy metal contaminated soil, unitormly stirring same. leaving the same (lo stand and curing the same; 2) adding a passivator mainly playing an adsorption role into a mixture obtained in step 1). uniformly stirring same. leaving the same to stand and curing the same; and 3) adding water into a mixture obtained in step 2). adjusting a weight water content to 20%-40%. lcaving the same to stand and curing the same.
Preferably. the passivator mainly playing a chemical reaction role is ferric oxide. calcium carbonate and hydroxyapatite. a weight ratio thercof being 0.3-0.7:0.15-0,35:0.15-0.35.
Preferably, the passivator mainly playing an adsorption role is plant ash and bentonite, a weight ratio thercof being 0.23-0.75:0.5-1.5.
Preferably. the weight ratio of the ferric oxide to the calcium carbonate to the hydroxyapatite is 0.5:0.25:0.25. and the weight ratio of the plant ash to the bentonite is 0.5:1.
Preferably. the bentonite is calcium bentonite. à main component thercof being montmorillonite.
Preterably, a weight of the passivator mainly playing a chemical reaction role is 0.6%-1% of a weight of the heavy metal contaminated soil. and a weight of the passivator mainly playing an adsorption role 1s 0.75%-3% of the weight of the heavy metal contaminated soil.
Preferably, curing time of step 1) is 10-30 min. curing time of step 2) is 10-30 min, and curing time of step 3) is 2-5 days.
Preferably. the heavy metal contaminated soil contains As, Cu. Pb. Ni and Zn.
Preferably, the heavy metal contaminated soil is farmland soil, contaminated by heavy metal. around a mining arca.
Compared with an existing farmland soil remediation technology. the present invention has the following advantages: (1) according to the present application, the passivator mainly playing a chemical reaction role is firstly mixed with the heavy metal contaminated soil. so that the passivator and the heavy metal contaminants may be more uniformly distributed in the soil while a chemical reaction is realized. and the passivator and the heavy metal contaminants may make full contact in a soil bulk phase: then the passivator mainly playing an adsorption role is added so as to adsorb part of the passivator mainly playing a chemical reaction role while adsorbing the heavy metal contaminants. and a chemical reaction reagent is distributed around an adsorbent or adsorbed into the adsorbent, so that the physically concentrated heavy metal may be chemically treated in a unified manner better. and a soil passivation effect is realized more cffectively: and as in the prior art, physical adsorption is conducted firstly, which results in a high concentration of the heavy metal contaminants in the adsorbent and à low concentration of the heavy metal contaminants in the soil. and when the chemical reaction reagent is distributed. although the chemical reaction reagent is uniformly distributed in the soil, when the heavy metal contaminants with a low concentration in the soil and a high concentration in the adsorbent are removed by the reagent with a uniform concentration, a situation of local excess or insufficiency of the chemical reaction reagent exists. so that although soil passivation may be realized. the passivation effect hardly reaches a level of the present application, (2) The present application realizes a synergistic effect among the ferric oxide, the calcium carbonate and the hydroxyapatite when using the three substances for removing the heavy metal: the ferric oxide may generate an iron ion reacting with a heavy metal oxyacid radical (such as an arsenate radical) in the presence of the water. so that this type of heavy metal contaminants may be passivated through a chemical reaction: the calcium carbonate is siightly dissolved in the water,
and a calcium ton may also react with the heavy metal oxyacid radical (such as the arsenate radical). so that this type of heavy metal contaminants may be passivated: a carbonate radical and many heavy metal ions may generate carbonate. and a hydroxy radical generated by hydrolysis of the carbonate radical and many heavy metal ions may also generate hydroxide. so that many types of heavy metal contaminants are removed; a calcium ion and a hydroxy radical generated by part. dissolved in the water. of the hydroxyapatite may play a role similar to that of the hydroxy radical generated by hydrolysis of the calcium ton and the carbonate radical in the calcium carbonate, but a generated phosphate radical may also play a role in adjusting and buffering a pll value white reacting with part of the heavy metal ions; for removal of the heavy metal oxyacid radical, the iron ion is usually combined with the heavy metal oxyacid radical to reduce pli of the soil, and the calcium ton is more stably combined with the heavy metal oxyacid radical under a condition that the pl value is neutral and slightly alkaline. so that under pIT buffering action of a polybasic acid radical of the phosphate radical and the carbonate radical. removal of the heavy metal oxyacid radical may be kept under an efficient pH reaction condition; the heavy metal ion. the hydroxy radical. the carbonate radical and the phosphate radical may also efficiently react with the heavy metal ion under the pH buffering action of the phosphate radical and the carbonate radical. so that mutual support of substances of three components, that is the ferric oxide. the calcium carbonate and the hydroxyapatite, is realized. and reaction is conducted under a proper condition all the time. thereby better passivating the soil; the ferric oxide. the calcium carbonate and the hydroxyapatite mainly play a chemical reaction role, but as a solid substance, the ferric oxide. the calcium carbonate and the hydroxyapatite have à certain specific surface arca and also play an adsorption role, but the adsorption role is much smaller than that of the adsorbent; and when the three kinds of reagents are applied. they arc uniformly mixed in a bulk phase of the soil to form a composite passivator to exert the synergistic effect.
(3) The present application uses the plant ash and the bentonite as the passivator mainly playing an adsorption role: the plant ash is a residue obtained after incineration of agricultural herbs and woody plants. has alkalescence, a large specific surface arca and a large pore volume, and has high adsorption capacity and surface complexing capacity for the heavy metal. the alkalescence of the plant ash is conducive to the increase of the pH ol the soil and promotes the heavy metals to form hydroxide precipitates: and the bentonite is a natural clay mineral, which has rich reserves in nature and low price and a main component of which is the montmorillonite having fine particles. a large specific surface area and a high porosity. an interlaver structure includes an exchangeable inorganic cation, part of oxygen atom electrons are exposed on a surface of a crystal. heavy metal elements may be fixed under actions of ion exchange. special adsorbent coprecipitation, ete, in addition, a special structure ol the clay mineral is conducive to formation ol a soil aggregate structure and improvement of lertilizer and water retention capacity of the soil: and having large specific surface areas. the plant ash and the bentonite mainly play an adsorption role and also play a role in pH adjustment and ion exchange. so that the plant ash and the bentonite may exert a synergistic effect with the ferric oxide, the calcium carbonate and the hydroxyapatite which are uniformly distributed in addition to playing an adsorption role, and may further interact with the ferric oxide, the calcium carbonate and the hydroxyapatite by exerting pH adjustment and ion exchange effects. thereby making the soil passivating effect better.
Detailed Description of Embodiments The present invention is further described below with reference to specific embodiments, so that those skilled in the art may better understand the present invention and implement it. but the listed embodiments are not intended to limit the present invention.
In the following embodiments of the present invention. a sample of heavy metal contaminated soil is from farmland soil around a certain mining arca of Fingmen, Hubei. The sample is mainly contaminated by As. Cu, Pb, Ni. Zn. ete., and specific parameters are shown in Table 1.
Table 1 Soil sample parameters | Indicator | Parameter Detection method _ | | N NYA 1121.2-2006 part 2 of soil detection: pli 6.24 I electrode method for measuring pH of soil PS © a ‘ GBT 22105.2-2008 soil quality: atomic As content 294 mg/kg fluorescence spectrometry for measuring total contents of Hg. As and Pb Cocoment | 560 make | OBIT 17138:1997 soil quality: flame atomic . - absorption spectrophotometry for measuring Zn content 219 mg/kg Cu and /n © — GB/T 17141-1997 soil quality: graphite Pb content 508 mg/kg furnace atomic absorption spectrophotometry for measuring Pb and Cd a GB/T 17139-1997 soil quality: flame atomic Ni content 161 mg/kg absorption spectrophotometry for measuring Ni Available As ) HJ 700-2014 water quality: inductively
1.77 mg/kg | content coupled plasma mass spectrometry for
LL LU102374 Indicator Parameter Detection method Available Cu | 1° “measuring 65 elements
3.21 mg/kg content 10-1. part 1 of Technical Specification of Soil Available Pb | 0 Sample Analysis and Test Method for Detailed
2.63 mg/kg | content Investigation of National Soil Contamination = a a Condition: extractable element calcium 2,16 mg/kg . content chloride extraction method © Available Ni a
0.65 mg/kg content Embodiment 1 a N a a 1) 4 g of ferric oxide. 2 g of calcium carbonate and 2 g of hydroxyapatite are added into 1 kg of heavy metal contaminated soil. and same are uniformly stirred, and left to stand and cured for min: 2) 5 g of plant ash and 10 g of calcium bentonite are added into a mixture obtained in step 1). and same are uniformly stirred. and left to stand and cured for 20 min: and 3) tap water is sprayed to a mixture obtained in step 2). a weight water content is adjusted to 30%, and same are uniformly stirred. and then left to stand and cured for 3 days. Embodiment 2 1) 3 g of ferric oxide. 3.5 g of calcium carbonate and 1.5 p of hydroxyapatite are added into 1 ke of heavy metal contaminated soil. and same are uniformly stirred. and lett 1o stand and cured for 30 min: 2) 2 g of plant ash and 13 g of calcium bentonite are added into a mixture obtained in step 1), and same are uniformly stirred. and leit to stand and cured for 10 min: and 3) tap water is sprayed to a mixture obtained in step 2). a weight water content is adjusted to 30%. and same are uniformly stirred. and then left to stand and cured for 3 days. Embodiment 3 1) 4.5 g of ferric oxide, 1 g of calcium carbonate and 2.5 ÿ of hydroxyapatite are added into 1 kg of heavy metal contaminated soil, and same are uniformly stirred. and left to stand and cured for 10 min: 2) 9 g of plant ash and 6 ¢ of calcium bentonite are added into a mixture obtained in step 1). and same are uniformly stirred. and left to stand and cured for 30 min: and 3) tap walter is sprayed to a mixture obtained in step 2), a weight water content is adjusted 10 30%. and same are unitormly stirred. and then left to stand and cured for 3 days. Comparative embodiment 1
1) 4 g of ferric oxide. 2 g of calcium carbonate, 2 g of hydroxyapatite. 5 g of plant ash and 10 g of calcium bentonite are added into | kg of heavy metal contaminated soil, and same are uniformly stirred. and left to stand and cured for 40 min: 2) tap water is sprayed to a mixture obtained tn step 1). à weight water content is adjusted to 30%. and same are uniformly stirred. and then left to stand and cured for 3 days.
Comparative embodiment 2 1) 5 g of plant ash and 10 g of calcium bentonite are added into ! kg of heavy metal contaminated soil. and same are uniformly stirred. and left to stand and cured for 20 min: 2) 4 g of ferric oxide. 2 g of calcium carbonate and 2 g of hydroxyapatite are added into a mixture obtained in step 1). and same are uniformly stirred. and lelt 10 stand and cured for 20 min: and 3) tap water is sprayed to a mixture obtained in step 2). a weight water content is adjusted to 30%. and same are uniformly stirred. and then left to stand and cured for 3 days.
Comparative embodiment 3 1) 5 g of ferric oxide and 3 g of calcium carbonate are added into 1 kg of heavy metal contaminated soil. and same are unilormly stirred. and lett to stand and cured for 20 min: 2) 5 g of plant ash and 10 g of calcium bentonite are added into a mixture obtained in step 1). and same are uniformly stirred. and left to stand and cured lor 20 min: and 3) tap water 1s sprayed to a mixture obtained in step 2). a weight water content is adjusted to 30%. and same are uniformly stirred. and then left to stand and cured Tor 3 days.
Comparative embodiment 4 1) 5 g ol ferric oxide and 3g of hydroxyapatite are added into 1 kg of heavy metal contaminated soil, and same are uniformly stirred. and left to stand and cured for 20 min: 2) 5 g of plant ash and 10 g of calcium bentonite are added into a mixture obtained in step 1). and same are uniformly stirred, and left to stand and cured for 20 min: and 3) tap water is sprayed to a mixture obtained in step 2). a weight water content is adjusted to 30%. and same are uniformly stirred, and then left to stand and cured for 3 days.
Comparative embodiment 5 1) 4 ¢ of calcium carbonate and 4 g of hydroxyapatite are added into 1 kg of heavy metal contaminated soil, and same are uniformly stirred. and left to stand and cured for 20 min: 2) 5 g of plant ash and 10 g of calcium bentonite are added into a mixture obtained in step 1). and same are uniformly stirred. and left to stand and cured for 20 min: and 3) tap water is sprayed to a mixture obtained in step 2). a weight water content is adjusted to 30%. and same are uniformly stirred, and then lett to stand and cured for 3 days.
Comparative embodiment 6 1} 4 g of ferric oxide, 2 g of calcium carbonate and 2 g of hydroxyapatite arc added into 1 kg of heavy metal contaminated soil. and same are uniformly stirred. and left to stand and cured for min; 2) 15 g of activated carbon is added into a mixture obtained in step 1). and same are uniformly stirred. and lell to stand and cured for 20 min; and 3) tap water is sprayed to a mixture obtained in step 2), a weight water content is adjusted to 30%. and same are uniformly stirred, and then left to stand and cured for 3 days.
Research results of passivated soil. obtained by sampling detection. of embodiments 1-3 and comparative embodiments F-6 are shown in Table 2. Table 2 Passivation detection results a Available | Available | Available | Available | Available As Cu Pb Zn Ni - mg/kg mg/kg mg/kg _ | mg/kg | _ mg/kg Contaminated 1.77 3.21 2.63 2.16 0.65 soil lmbodiment 1 0.18 023 | 0.19 01 0.17 | Embodiment 2 0.26 “021 025 [| 008 0.14 Embodiment 3 | 013 | 034 | on | 024 | Die Comparative | 046 | 068 057 | 074 — 0.31 embodiment 1 Comparative 0.78 056. 0.33 69 0.24 | embodiment 2 Comparative | 0.34 042 094; 037 | 020 embodiment 3 Comparative | 042 | 0.63 0.45 0.83 0.35 embodiment 4 Comparative | 083 | 038 052 | 08 021 embodiment 5 Comparative - 0.28 0.36 “020 031 019 embodiment 6 Results of the embodiments 1-3 show that the method for passivating of the present application has a good passivation effect. and may passivate available heavy metal in the contaminated farmland soil, thereby having the good passivation effect.
By comparing results of the embodiment 1 and the comparative embodiments | and 2. it may be seen that 1f the passivator mainly playing a chemical reaction role is uniformly distributed in a bulk phase of the soil contaminated by the heavy metal firstly. and then the passivator mainly playing an adsorption role is uniformly distributed in the mixture. the passivator and the heavy metal which are subjected to a chemical reaction may be uniformly mixed in the soil and then are concentrated on a surface or a periphery of an adsorbent, and the chemical reaction may be conducted under a uniform and effective condition, thereby being capable of realizing a better passivation effect.
The comparative embodiment 1 shows that if the passivators mainly playing a chemical reaction role and an adsorption role are added into the soil at the same time, cach reagent acts at the same time. the condition of the chemical reaction is uncertain, and the reagents of the chemical reaction and physical adsorption are different. which may result in that part of the adsorbent adsorbs excessive contaminants but makes contact with an insutficient amount of the passivator while the other part of the adsorbent adsorbs an excessive amount of the passivator without making contact with a proper amount of contaminants.
The comparative embodiment 2 shows that 1f the passivator mainly playing an adsorption role is added firstly. distribution unevenness of the heavy metal contaminants and the passivator mainly playing a chemical reaction role is intensified, a chemical reaction environment in the soil bulk phase is not uniform, and although most heavy metal may be passivated. the passivation effect cannot reach a level of the embodiment 1. By comparing the embodiment ! with the comparative embodiments 3-5, it may be seen that combined use ol the terric oxide. the calcium carbonate. and the hydroxyapatite functionally has mutually supportive effects, resulting in a synergistic effect to passivate the heavy metal through the chemical reaction.
An iron ion and a calcium ton are capable of reacting with a heavy metal oxyacid radical under an environmental condition of neutral meta-acid or neutral meta-alkali. a reaction effect of the iron ion and the calcium ion may be exerted together under a butler condition of a phosphate radical and a carbonate radical, and therefore the heavy metal oxyacid radical may be ceffectively passivated under the stable chemical environment condition from weak acid to weak alkali.
À carbonate ion, à hydroxyl ton and a phosphate ion also stably passivate a heavy metal ion under buffer action of the phosphate radical and the carbonate radical.
Therefore. the heavy metal in a wide range may be removed by only using the above three substances, and an effect of using the three substances cannot be exerted by only using two of the three substances. which indicates that the three substances generate the synergistic effect.
By comparing the embodiment 1 and the comparative embodiment 6. it may be seen that when the passivator mainly playing an adsorption role is replaced with the activated carbon. the activated carbon may also realize a better passivation effect compared with the prior art. but if the plant ash and the bentonite which play a role in pli adjustment and ion exchange in addition to an adsorption role are used. adjustment and supplementation to the ferric oxide. the calcium carbonate and the hydroxyapatite in chemical action may be better realized. thereby realizing a better passivation effect on heavy metal substances.
According to the present application. the passivator mainly playing a chemical reaction role is firstly added. and then the passivator mainly playing an adsorption role is added. so that organic combination ol chemical action and physical action is realized. a unified reaction environment is provided for removal of the heavy metal, and a better passivation effect is realized. The present application further researches and develops a way of combining the ferric oxide, the calcium carbonate. the hydroxyapatite. the plant ash and the bentonite and using them step by step. the combined use of the ferric oxide. the calcium carbonate and the hydroxyapatite has the synergistic effect. and the plant ash and the bentonite which are further added may further promote the synergistic effect. thereby obtaining a good passivation effect.
The above-described embodiments are merely preferred embodiments listed to fully illustrate the present invention and are not intended to limit the scope of protection of the present invention. l‘quivalent substitutions or modifications made by those skilled in the art on the basis of the present invention fall within the scope ol protection of the present invention. The scope of protection ol the present invention 1s subject to the claims.
Claims (9)
1. A method for passivating heavy metal contaminated farmland soil. comprising the following steps: 1) adding à passivator mainly playing a chemical reaction role into the heavy metal contaminated soil, uniformly stirring same, leaving the same 10 stand and curing the same: 2) adding a passivator mainly playing an adsorption role into a mixture obtained in step 1). uniformly stirring same, leaving the same to stand and curing the same; and 3) adding waler into a mixture obtained in step 2), adjusting a weight water content to 20%-40%. leaving same to stand and curing the same.
2. The method according to claim 1. characterized in that the passivator mainly playing a chemical reaction role is ferric oxide. calcium carbonate and hydroxyapatite, a weight ratio thereof being 0.3-0.7:0.15-0.35:0.15-0.35.
3. The method according to claim 2. characterized in that the passivator mainly playing an adsorption role is plant ash and bentonite. a weight ratio thercol being 0.25-0.75:0.5-1.5.
4. The method according to claim 3, characterized in that a weight ratio of ferric oxide to calcium carbonate to hydroxyapatite is (1.5:0.25:0.25, and a weight ratio of plant ash to bentonite is 0.5:1.
5. The method according to claim 3, characterized in that the bentonite is calcium bentonite. a main component thereof being montmorillonite.
6, The method according to claim |. characterized in that a weight of the passivator mainly playing a chemical reaction role is 0.6%-1% of a weight of the heavy metal contaminated soil, and a weight of the passivator mainly playing an adsorption role is 0.75%-3% of the weight of the heavy metal contaminated soil.
7. The method according to claim 6, characterized in that curing time of step 1) is 10-30 min, curing time of step 2) 1s 10-30 min. and curing time of step 3) is 2-5 days.
8. The method according to claim 1, characterized in that the heavy metal contaminated soil contains As. Cu. Pb. Ni and Zn.
9. The method according to claim 8. characterized in that the heavy metal contaminated soil is farmland soil. contaminated by heavy metal. around a mining area.
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