CN114164004A - Soil zero-valent mercury composite oxidant and method for repairing soil by using same - Google Patents
Soil zero-valent mercury composite oxidant and method for repairing soil by using same Download PDFInfo
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- CN114164004A CN114164004A CN202111424278.8A CN202111424278A CN114164004A CN 114164004 A CN114164004 A CN 114164004A CN 202111424278 A CN202111424278 A CN 202111424278A CN 114164004 A CN114164004 A CN 114164004A
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- valent mercury
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- 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
- C09K17/06—Calcium compounds, e.g. lime
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- 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
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
Abstract
The invention discloses a soil zero-valent mercury composite oxidant and a method for restoring soil by using the same, wherein the soil zero-valent mercury composite oxidant consists of a catalyst, an activator and an oxidant, and the application of the soil zero-valent mercury composite oxidant in restoring soil zero-valent mercury pollution specifically comprises the following steps: (1) naturally drying and crushing the polluted soil; (2) and adding the soil zero-valent mercury composite oxidant into the crushed soil, uniformly mixing, adding water to immerse the soil and the soil zero-valent mercury composite oxidant into the water, and performing semi-closed treatment for 24-72 hours. The method can efficiently oxidize the zero-valent mercury in the soil, effectively oxidize the zero-valent mercury with larger environmental risk in the soil into the divalent mercury with lower environmental risk, and provide conditions for the application of subsequent solidification stabilization and leaching repair technologies.
Description
Technical Field
The invention belongs to the technical field of heavy metal contaminated soil remediation and treatment, and particularly relates to an efficient composite oxidant for zero-valent mercury in soil and a soil remediation method thereof.
Background
Mercury is a heavy metal element with strong toxicity which is widely concerned by the world, and in a natural state, mercury in mercury ore exists mainly in a form of mercuric sulfide (cinnabar), and as the solubility of the mercuric sulfide is extremely low and the chemical property is extremely stable, no ecological and human health risks exist in the mercury ore area which is not exploited by human beings basically.
However, with the economic development of human society, the demand of human beings for mercury increases, and a large amount of original mercury ore is converted into mercury simple substance and divalent mercury salt through smelting and processing processes and is used for production and life of human beings. After the elemental mercury and the divalent mercury salt generated after the secondary processing of the human enter the soil environment, only a small part of the elemental mercury and the divalent mercury salt can form stable mercury sulfide precipitate, and most of the mercury is adsorbed on the surfaces of various mineral and organic matter particles in the soil in a zero-valent and divalent state. Zero-valent mercury in soil can volatilize at normal temperature and enter the atmospheric environment, and then long-distance migration occurs in regional scale and even global scope, which is also the reason why mercury is the only heavy metal pollutant and is also considered as the persistent pollutant.
For contaminated sites, zero-valent mercury in the soil is also a major source of human health risks to the site and its surrounding populations. Generally, mercury in a polluted site is harmful to human health mainly through two ways of oral ingestion and respiratory inhalation, mercury vapor can enter the lung of a human body through the respiratory way, more than 80 percent of mercury vapor can enter the human body through a blood brain barrier to cause serious damage to a human nervous system, and water-soluble divalent mercury ions can enter the internal environment of the human body through a human gastrointestinal digestion and absorption system after being ingested through the oral cavity to cause damage to the human health. As various mineral substances and organic substances in the soil can form various insoluble precipitates with bivalent mercury in the soil and form a strong adsorption effect, the mercury in the soil is difficult to release in the gastrointestinal tract of a human body, and a plurality of gastrointestinal simulation test researches show that the gastrointestinal available state proportion of the mercury in the soil in the human body is below 5%, and the daily oral intake of the soil by people is small. Therefore, the existence of zero-valent mercury in soil is a main source of human health risks caused by the global spread of mercury pollution and mercury pollution sites.
At present, the main remediation methods of the mercury polluted site comprise in-situ/ex-situ thermal desorption, soil leaching, solidification and stabilization, biological extraction and the like. The thermal desorption method is considered as the most potential restoration method, and can effectively eliminate mercury in various forms in soil, but the method has overlarge energy consumption and related construction cost consumption, is not suitable for soil with overlarge pollution area and lighter pollution degree; the leaching, solidification and stabilization of soil, biological extraction and the like can only remove mercury in free state and weak combination state in soil or carry out stabilization operation. The ecological environment risk of zero-valent mercury in soil cannot be effectively controlled.
The zero-valent mercury has stable chemical properties and is difficult to be directly oxidized by oxygen in the air, and the reaction rate of mercury in a gas phase state and other strong oxidants is low; the result of research on the oxidation of the zero-valent mercury in the water phase is optimistic, but current research shows that only hydroxyl radicals and ozone can rapidly oxidize the zero-valent mercury in the water phase, and hydrogen peroxide and ferric ions which are commonly used as organic pollutant oxidants have slow oxidation rate to the zero-valent mercury in the liquid phase, and the rate constant is less than 10. The oxidation research on zero-valent mercury in soil is relatively less at present, and CN107457258B discloses a mercury polluted soil remediation method by persulfate oxidation and leaching. But researches show that the purpose of effectively and efficiently oxidizing zero-valent mercury in soil cannot be achieved by simply using persulfate.
Disclosure of Invention
The invention aims to provide a soil zero-valent mercury composite oxidant and a method for restoring soil by using the same.
In order to achieve the purpose, the invention adopts the following technical scheme:
a soil zero-valent mercury composite oxidant consists of a catalyst, an activator and an oxidant.
Preferably, the molar ratio of the catalyst, activator and oxidant is from 0.05 to 0.1: 0.5-1: 1.
preferably, the catalyst is at least one of manganese oxide, manganese dioxide and manganese trioxide.
Preferably, the activator is at least one of calcium peroxide and sodium percarbonate.
Preferably, the oxidizing agent is at least one of sodium persulfate and potassium persulfate.
The invention also provides a preparation method of the soil zero-valent mercury composite oxidant, which is characterized in that the catalyst, the activating agent and the oxidant in the formula amount are uniformly mixed to obtain the soil zero-valent mercury composite oxidant.
The invention also provides application of the soil zero-valent mercury composite oxidant in remediation of soil zero-valent mercury pollution.
Preferably, the soil zero-valent mercury composite oxidant can oxidize zero-valent mercury into divalent mercury.
The invention also provides a soil remediation method for oxidizing zero-valent mercury into divalent mercury, which comprises the following steps:
(1) naturally drying and crushing the polluted soil;
(2) adding the soil zero-valent mercury composite oxidant into the crushed soil, uniformly mixing, adding water to immerse the soil and the soil zero-valent mercury composite oxidant into the water, and performing semi-closed treatment for 24-72 hours.
Preferably, the mass ratio of the soil to the soil zero-valent mercury composite oxidant is 5-10: 1, the specific addition ratio of the composite oxidant is higher than the sum of the contents of organic matters and zero-valent mercury in soil.
The invention has the beneficial effects that:
the soil zero-valent mercury composite oxidant consists of a catalyst, an activating agent and an oxidant, wherein the catalyst is a manganese oxide, and can play a role in adsorbing zero-valent mercury and increasing the total surface area of mercury so as to accelerate the oxidation process of the soil; it is also possible to accelerate the oxidation process of mercury by reducing the reaction activation energy of mercury oxidation; the activators calcium peroxide and sodium percarbonate can slowly generate hydrogen peroxide in water, so that the utilization efficiency of the hydrogen peroxide is improved, and the generated hydrogen peroxide is used as an activator and reacts with sodium persulfate to produce hydroxyl radicals with strong oxidizing property; the oxidant persulfate can be ionized in water to generate persulfuric acid ions with strong oxidability, but the persulfate is stable at normal temperature and has slow reaction rate, so that other oxidants are often needed as activating factors. Compared with the prior art, the soil zero-valent mercury composite oxidant disclosed by the invention is matched with each other, so that zero-valent mercury in soil can be efficiently oxidized, the zero-valent mercury with a large environmental risk in the soil is effectively oxidized into divalent mercury with a low environmental risk, and conditions are provided for the application of subsequent solidification stabilization and leaching restoration technologies.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions of the present invention are further described below. When numerical ranges are given in the examples, it is understood that both endpoints of each of the numerical ranges and any value therebetween can be selected unless the invention otherwise indicated. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.
The raw materials used in the present invention are all common commercial products unless otherwise specified.
A soil zero-valent mercury composite oxidant consists of a catalyst, an activator and an oxidant.
Preferably, the molar ratio of the catalyst, activator and oxidant is from 0.05 to 0.1: 0.5-1: 1.
preferably, the catalyst is at least one of manganese oxide, manganese dioxide and manganese trioxide.
Preferably, the activator is at least one of calcium peroxide and sodium percarbonate.
Preferably, the oxidizing agent is at least one of sodium persulfate and potassium persulfate.
The invention also provides a preparation method of the soil zero-valent mercury composite oxidant, which is characterized in that the catalyst, the activating agent and the oxidant in the formula amount are uniformly mixed to obtain the soil zero-valent mercury composite oxidant.
The invention also provides application of the soil zero-valent mercury composite oxidant in remediation of soil zero-valent mercury pollution.
Preferably, the soil zero-valent mercury composite oxidant can oxidize zero-valent mercury into divalent mercury.
The invention also provides a soil remediation method for oxidizing zero-valent mercury into divalent mercury, which comprises the following steps:
(1) naturally drying and crushing the polluted soil;
(2) adding the soil zero-valent mercury composite oxidant into the crushed soil, uniformly mixing, adding water to immerse the soil and the soil zero-valent mercury composite oxidant into the water, and performing semi-closed treatment for 24-72 hours.
Preferably, the mass ratio of the soil to the soil zero-valent mercury composite oxidant is 5-10: 1, the specific addition ratio of the composite oxidant is higher than the sum of the contents of organic matters and zero-valent mercury in soil.
In two chlor-alkali production chemical fields, total four mercury contaminated soil with different concentrations are adopted, and natural air drying treatment is carried out, so that during the natural air drying process, macroscopic zero-valent mercury drops are separated out from the soil. Through the natural air drying treatment and observation of one week, the research shows that although zero-valent mercury in the soil is obviously separated out, the natural volatilization rate is extremely slow. And grinding the air-dried soil, sieving with a 40-mesh sieve, and sealing for storage. And testing the difference value of the total mercury concentration of the soil before and after treatment under the condition that the soil is heated at the constant temperature of 80 ℃ for 3 hours by using a thermal analysis method, wherein the difference value is the zero-valent mercury content in the soil.
TABLE 1 composition and amount of composite oxidant used in soil remediation
According to the table 1, soil and the soil zero-valent mercury composite oxidant are fully mixed in a glass beaker, a proper amount of distilled water is added, the soil mixture is fully immersed, all the glass beakers are simply covered by preservative films, the phenomenon that water is evaporated too fast is avoided, and the oxidation process lasts for 72 hours. After the oxidation treatment, the soil is heated and treated for 3 hours at 80 ℃, and the total mercury content in the oxidized soil is tested. The difference value of the total mercury content of the oxidized soil and the original soil is the zero-valent mercury content of the oxidized soil. The results of the experiment are shown in table 2.
TABLE 2 content of zero-valent mercury after soil remediation
As shown in Table 2, the soil zero-valent mercury composite oxidant for treating 2, 3 and 4 of the invention has good oxidation effect on zero-valent mercury in soil, the oxidation efficiency of the zero-valent mercury in 4 parts of polluted soil can reach 54.8-60.4%, 66.3-71.5%, 87.2-90.9% and 88.2-92.2%, and the oxidation efficiency is obviously increased along with the reduction of the concentration of the zero-valent mercury in the soil. And the zero-valent mercury composite oxidant (only calcium peroxide and sodium persulfate) for treating the soil in the step 1 has the following oxidation efficiencies of the zero-valent mercury in 4 parts of soil: 7.9%, 27.8%, 32.5%, 28.7%, all below 30%. The manganese dioxide serving as a (catalyst/adsorbent) can obviously improve the oxidation effect of the zero-valent mercury, the bismuth ferrite serving as a catalyst in the treatment 5 can also play a better role in promoting the oxidation of the zero-valent mercury in the soil, and the oxidation efficiency of the zero-valent mercury in 4 parts of polluted soil can reach 45.4%, 59.2%, 87.9% and 86.7%. Chinese patent CN105233687B discloses a technical method for converting elemental mercury in coal gas into divalent mercury, wherein the catalyst is one or a mixture of bismuth ferrite, cobalt-doped bismuth ferrite, cobalt/lanthanum-doped bismuth ferrite, cobalt/strontium-doped bismuth ferrite and cobalt/rubidium-doped bismuth ferrite. However, manganese oxides such as manganese dioxide are relatively cheap and easily available, and have less secondary pollution to the soil environment.
In conclusion, the soil zero-valent mercury composite oxidant consists of the catalyst, the activator and the oxidant, wherein the catalyst is manganese oxide, and can play a role in adsorbing zero-valent mercury and increasing the total surface area of mercury so as to accelerate the oxidation process of the soil; it is also possible to accelerate the oxidation process of mercury by reducing the reaction activation energy of mercury oxidation; the activators calcium peroxide and sodium percarbonate can slowly generate hydrogen peroxide in water, so that the utilization efficiency of the hydrogen peroxide is improved, and the generated hydrogen peroxide is used as an activator and reacts with sodium persulfate to produce hydroxyl radicals with strong oxidizing property; the oxidant persulfate can be ionized in water to generate persulfuric acid ions with strong oxidability, but the persulfate is stable at normal temperature and has slow reaction rate, so that other oxidants are often needed as activating factors. Compared with the prior art, the soil zero-valent mercury composite oxidant disclosed by the invention is matched with each other, so that zero-valent mercury in soil can be efficiently oxidized, the zero-valent mercury with a large environmental risk in the soil is effectively oxidized into divalent mercury with a low environmental risk, and conditions are provided for the application of subsequent solidification stabilization and leaching restoration technologies.
It should be emphasized that the embodiments described herein are illustrative rather than restrictive, and thus the present invention is not limited to the embodiments described in the detailed description, but also includes other embodiments that can be derived from the technical solutions of the present invention by those skilled in the art.
Claims (10)
1. The soil zero-valent mercury composite oxidant is characterized by comprising a catalyst, an activator and an oxidant.
2. The soil zero-valent mercury composite oxidant according to claim 1, wherein the molar ratio of the catalyst, the activator and the oxidant is 0.05-0.1: 0.5-1: 1.
3. the soil zero-valent mercury composite oxidant according to claim 1, wherein the catalyst is at least one of manganese oxide, manganese dioxide and manganese trioxide.
4. The soil zero-valent mercury composite oxidant according to claim 1, wherein the activator is at least one of calcium peroxide and sodium percarbonate.
5. The soil zero-valent mercury complex oxidant according to claim 1, wherein the oxidant is at least one of sodium persulfate and potassium persulfate.
6. The preparation method of the soil zero-valent mercury composite oxidant according to any one of claims 1 to 5, characterized in that the soil zero-valent mercury composite oxidant is obtained by uniformly mixing the catalyst, the activator and the oxidant according to the formula amount.
7. The use of the soil zero-valent mercury complex oxidant according to any one of claims 1 to 5 in remediation of soil zero-valent mercury contamination.
8. The use of claim 7, wherein the soil zero-valent mercury complex oxidant oxidizes zero-valent mercury to divalent mercury.
9. A method for restoring zero-valent mercury in soil comprises the following steps:
(1) naturally drying and crushing the polluted soil;
(2) adding the soil zero-valent mercury composite oxidant according to any one of claims 1 to 5 into crushed soil, uniformly mixing, adding water, immersing the soil and the soil zero-valent mercury composite oxidant into the water, and performing semi-closed treatment for 24 to 72 hours.
10. The remediation method of claim 8 wherein the mass ratio of soil to soil zero-valent mercury complex oxidant is from 5 to 10: 1.
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