CN111704248B - Method for treating arsenic-containing wastewater or arsenic-polluted soil by using autotrophic bacteria - Google Patents
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- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
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Abstract
The invention discloses a method for treating arsenic-containing wastewater or arsenic-polluted soil by using autotrophic bacteria. The method mainly removes arsenic by means of mineralization of acidophilic thiobacillus ferrooxidans, utilizes acidophilic thiobacillus ferrooxidans to oxidize Fe (II) in the wastewater and soil into Fe (III), and fixes As (III) and As (V) in the process of forming Schneider minerals, thereby realizing removal and stabilization of arsenic in water and soil. The method has simple steps, short time and high efficiency; the reaction condition is mild, the process is controllable, and the method is economical and feasible; the application range is wide, and the As (III) and As (V) in polluted water and soil can be treated; and the arsenic removal efficiency is high, the stability of the treated arsenic is strong, and no secondary pollution is caused.
Description
Technical Field
The invention belongs to the technical field of water treatment and soil remediation, and particularly relates to a method for treating arsenic-containing wastewater or arsenic-polluted soil by using acidithiobacillus ferrooxidans.
Background
With the continuous development of industries such as mining, mineral separation, smelting and the like and the continuous use of various arsenic-containing objects, the arsenic pollution of soil and natural water bodies is increasingly serious, the ecological safety is harmed, and the health of people is seriously influenced. The search for a way of effectively degrading and treating arsenic in water and soil becomes the focus of increasing attention of people.
At present, the main technologies for treating arsenic-containing wastewater include a chemical adsorption method, an ion exchange method, a membrane separation method, an iron salt method and the like. The adsorption method mainly utilizes the adsorption material with good adsorption performance to remove and purify arsenic in water, but the adsorption capacity of the adsorption material to arsenic is limited, and the adsorption effect of most adsorption materials to As (V) is superior to that of As (III); the ion exchange method mainly achieves the aim of removing arsenic by ion exchange reaction by means of an ion exchanger, but the method has higher cost and is not suitable for large-scale application; the membrane separation method is used for separating target pollutants such as arsenic and the like from a water body by utilizing the selective permeability of a membrane to treat arsenic-containing wastewater, but the method has the problems of high cost and complex operation and is difficult to popularize on a large scale; the iron salt method utilizes iron ions to form stable substances with arsenate and arsenite so as to achieve the aim of removing arsenic, but the precipitate generated by the method is difficult to treat, and the adsorption effect on As (V) is better than that on As (III). Therefore, there is a need to develop a new technology for treating arsenic-containing wastewater.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a method for treating arsenic-containing wastewater or arsenic-polluted soil by using autotrophic bacteria. The method mainly removes arsenic by mineral formation under the biomineralization of acidophilic thiobacillus ferrooxidans, utilizes acidophilic thiobacillus ferrooxidans to oxidize Fe (II) in the wastewater and soil into Fe (III), and reacts with As (III) and As (V) to form Schneider mineral sediment, can realize the removal and stabilization of arsenic in water and soil, and has simple operation, economy and feasibility.
In order to achieve the purpose, the following technical scheme is adopted:
a method for treating arsenic-containing wastewater and arsenic-contaminated soil by using autotrophic bacteria comprises the following steps: adding ferrous salt into the wastewater to be treated containing As (III) and/or As (V) or soil, and simultaneously adding Acidithiobacillus ferrooxidans (Acidithiobacillus ferrooxidans) for treatment.
In the above method, Acidithiobacillus ferrooxidans is added in an amount of 2.0 × 106-8.0×106The bacteria per ml of arsenic-containing wastewater or per gram of arsenic-contaminated soil is preferably 2.0X 106-7.5×106Each milliliter of arsenic-containing wastewater or each gram of arsenic pollutes the soil.
The bacterial concentration range is important. When the amount is less than this range, the arsenic removing performance is low and the time required is long; when the amount is more than this range, the arsenic removing performance is not improved and the arsenic removing efficiency tends to be stable.
When the arsenic-containing wastewater contains trivalent arsenic and pentavalent arsenic at the same time, the dosage of the ferrous salt in the arsenic-containing wastewater is controlled to control the atomic molar ratio of iron to arsenic to be 10-60: 1, preferably 30 to 60: 1; the Fe/As (III) atomic molar ratio is 30-60:1 when trivalent arsenic is present in the solution alone, and 20-60:1 when pentavalent arsenic is present in the solution alone.
If the molar ratio of the atoms of iron and arsenic is too low, the iron and arsenic cannot be formed into ore, and the arsenic removal efficiency is low; when the concentration is too high, the arsenic removal performance cannot be improved, and the arsenic removal efficiency tends to be stable.
In the method, the ratio of the arsenic-polluted soil to the ferrous salt solution is 0.5-3:1(g/mL), preferably 0.5-2:1 (g/mL); the atomic molar ratio of iron to arsenic added to the soil is 50-150:1, preferably 80-130: 1.
Compared with water, the soil system is more complex, so the molar ratio of iron to arsenic atoms is different.
In the above method, it is preferable to add Acidithiobacillus ferrooxidans in the logarithmic phase of growth.
The acidophilic thiobacillus ferrooxidans in the logarithmic phase of growth has the best activity, the fastest growth rate, the highest oxidation efficiency on ferrous iron and better arsenic-bearing performance; if the added acidithiobacillus ferrooxidans which is not in the logarithmic phase of growth, the reaction time is prolonged, and the arsenic removal effect is reduced.
In the above method, the ferrous salt comprises one or more of ferrous sulfate, ferrous chloride and ferrous nitrate, and is preferably ferrous sulfate.
In the above method, the reaction temperature and pH are adjusted to 25 to 32 ℃ and 1.5 to 3.5, preferably 26 to 30 ℃ and 2.0 to 3.0, respectively.
The shaking table rotation speed of the reaction is 150-190rpm, preferably 160-180 rpm.
The reaction time is 1-5d, preferably 2-4 d.
In the method, the content of arsenic in the wastewater or soil to be treated is 5-100mg/L, preferably 20-80mg/L calculated by arsenic.
The invention relates to a method for treating arsenic-containing wastewater or arsenic-polluted soil by using autotrophic bacteria, which comprises the following steps: adding ferrous salt into the wastewater to be treated respectively containing As (III) and As (V) and the wastewater to be treated simultaneously containing As (III) and As (V), simultaneously adding acidophilic thiobacillus ferrooxidans centrifugal bacterial liquid in a logarithmic phase of growth, and treating the arsenic-containing wastewater by adjusting conditions such as temperature, pH and the like; the method is used for treating and restoring the arsenic-polluted soil according to a certain liquid-soil ratio and treatment conditions in the water body.
The preferable culture mode of the acidithiobacillus ferrooxidans is as follows:
(1) culturing was carried out using 9k medium (medium composition: ammonium sulfate (NH))4)2SO40.5 g; dipotassium hydrogen phosphate K2HPO40.5 g; magnesium sulfate heptahydrate (MgSO)4·7H2O, 0.5 g; calcium nitrate Ca (NO)3)20.01 g; 0.1g of potassium chloride (KCL); deionized water H2O, 1L). The pH of the medium was adjusted to 2.0, and the medium was sterilized at 121 ℃ for 20 minutes. In volume ratio VBacteria：VCulture medium1: 10 while adding FeSO in an amount of 44.7g per liter of the medium solution4·7H2And O, culturing in a constant-temperature culture oscillator at 25-32 ℃ for 2-3d to obtain the thiobacillus acidophilus in the logarithmic phase.
(2) Centrifugation of Acidithiobacillus ferrooxidans: filtering cultured acidophilic thiobacillus ferrooxidans in logarithmic phase, centrifuging the bacterial filtrate in a centrifuge at 10000rpm and 4 ℃, washing for 2 times by using deionized water with pH of 1.5, placing the obtained centrifugal thallus in deionized water with pH of 2.5, and storing in a refrigerator at 4 ℃.
(3) And (3) adding the obtained acidophilic iron protoxide thiobacillus centrifugal bacterial liquid into arsenic-containing wastewater or arsenic-polluted soil, adding a certain amount of ferrous salt, adjusting the temperature, the pH value, the rotating speed and the like, reacting for a certain time to treat the arsenic-containing wastewater or arsenic-polluted soil, and drying the obtained precipitate at the temperature of 50 ℃.
The chemical formula of the Schwerer mineral is Fe8O8(OH)8-2x(SO4)x(1<x<1.75) containing sulfate radicals per se; therefore, if the object to be treated contains a large amount of sulfate, ferrous chloride or ferrous nitrate can be selected as an iron source; otherwise, ferrous sulfate should be preferably selected to prevent that schneiderian minerals cannot be generated due to too little sulfate radicals to influence the removal of arsenic.
The method utilizes the biomineralization of acidithiobacillus ferrooxidans to oxidize Fe (II) in the wastewater and the soil into Fe (III), and the Fe (II) reacts with As (III) and As (V) in the process of forming Schneider minerals to fix arsenic in the structure of the Schneider minerals, thereby realizing the removal and stabilization of arsenic in water and soil.
Compared with the prior art, the invention has the following advantages:
(1) the method directly removes and purifies trivalent arsenic and pentavalent arsenic in the wastewater in the process of forming the Schneider minerals, and the formation of the Schneider minerals and the purification of the arsenic are synchronous, so that the method is simple, short in time and high in efficiency.
(2) During the reaction, arsenic is fixed inside the schwertmannite structure; compared with the addition of biogenic Schneider minerals for arsenic removal, the stability of arsenic is better and can be enhanced by about 1-3 times, because arsenite and arsenate existing in the form of anions, particularly arsenate, are easy to replace sulfate radicals in the Schneider mineral structure and exist in the mineral structure in the process of forming the Schneider minerals, so that the arsenic is difficult to release after being fixed. According to the infrared spectrogram, comparing the infrared spectrogram of a reactant after arsenic removal by directly adding biogenic Schlemm mineral, and finding that the infrared characteristic peak related to arsenic is not found in the infrared spectrogram after arsenic removal by directly adding biogenic Schlemm mineral; and arsenic is removed in the process of forming the Schneider mineral by adding acidophilic iron protoxide thiobacillus, and As (III) -O bond and As (V) -O bond appear on an infrared spectrogram, which indicates that arsenic is already present in the structure of the Schneider mineral and is not adsorbed on the surface. The schwann mineral has a tubular lattice structure along the C-axis direction, and the diameter of the lattice structure coincides with the diameter of the oxyanion of heavy (metal-like) metals such as arsenite, arsenate and chromate, indicating that arsenic is likely to enter the schwann mineral structure instead of sulfate ions. See figure 1 for details.
(3) The method has the advantages of mild and controllable reaction conditions, easy operation, cheap and easily obtained raw materials and low treatment cost.
(4) The invention can fix As (III) and As (V) at the same time, can treat arsenic-containing wastewater and arsenic-polluted soil, and has wider application range and no secondary pollution.
Drawings
FIG. 1 is a comparison graph of infrared spectra of arsenic removal by adding Shih mineral and arsenic removal by adding Thiobacillus ferrooxidans.
FIG. 2 is a graph showing the effect of different amounts of Acidithiobacillus ferrooxidans on the treatment of wastewater containing As (III) and As (V), respectively, in example 1 of the present invention.
FIG. 3 is an XRD pattern of precipitates obtained from 50mg/L of wastewater containing As (III) treated with Acidithiobacillus ferrooxidans under different Fe/As atomic molar ratios in example 2 of the present invention.
FIG. 4 is an XRD pattern of precipitates obtained from 50mg/L of wastewater containing As (V) treated with Acidithiobacillus ferrooxidans under different Fe/As atomic molar ratios in example 2 of the present invention.
FIG. 5 is a graph showing the effect of different Fe/As atomic molar ratios on the treatment of wastewater containing As (III) and As (V), respectively, in example 2 of the present invention.
FIG. 6 is an XRD pattern of precipitates obtained by treating As-containing wastewater containing As (III) and As (V) at various concentrations by Acidithiobacillus ferrooxidans in example 5 of the present invention.
Detailed Description
The present invention will be described in further detail below with reference to the accompanying drawings and specific embodiments. It should be noted that the following examples are only for illustrating the present invention and are not intended to limit the scope of the present invention.
Acidithiobacillus ferrooxidans (ATCC 23270) in the examples of the present invention was purchased from American type culture Collection.
The culture process comprises the following steps:
(1) culturing with 9k medium(the medium component is ammonium sulfate (NH)4)2SO40.5 g; dipotassium hydrogen phosphate K2HPO40.5 g; magnesium sulfate heptahydrate (MgSO)4·7H2O, 0.5 g; calcium nitrate Ca (NO)3)20.01 g; 0.1g of potassium chloride (KCL); deionized water H2O, 1L). The pH of the medium was adjusted to 2.0, and the medium was sterilized at 121 ℃ for 20 minutes. In volume ratio VBacteria：VCulture medium1: 10 while adding FeSO in an amount of 44.7g per liter of the medium solution4·7H2And O, culturing in a constant-temperature culture shaker at 28 ℃ for 2-3d to obtain the acidithiobacillus ferrooxidans in the logarithmic phase.
(2) Centrifugation of Acidithiobacillus ferrooxidans: filtering cultured acidophilic thiobacillus ferrooxidans in logarithmic phase, centrifuging the bacterial filtrate in a centrifuge at 10000rpm and 4 ℃, washing for 2 times by using deionized water with pH of 1.5, placing the obtained centrifugal thallus in deionized water with pH of 2.5, and storing in a refrigerator at 4 ℃.
Example 1
The experiments of treating 50mg/L arsenic-containing wastewater by Thiobacillus ferrooxidans according to the Fe/As atomic molar ratio of 30 (treating As (III)) and 20 (treating As (V)), respectively, are respectively carried out according to the proportion of 2.5 multiplied by 10 per milliliter6、5×106、7.5×106The acidophilic thiobacillus ferrooxidans centrifugal liquid is added into arsenic-containing waste water according to the proportion of each bacterium, the pH value is adjusted to be 2.5, and the mixture is placed in a shaking table with the temperature of 30 ℃ and the rotating speed of 165-175rpm for reaction for 3 d. The precipitate and solution were separated and the arsenic concentration was determined by ICP-OES.
As can be seen from FIG. 2, when the amount of viable bacteria added increases, the effect of Acidithiobacillus ferrooxidans on treating As (III) is significantly improved; when the amount of viable bacteria is 5X 10 per ml6When bacteria exist, after the reaction is carried out for 3d, the treatment efficiency of the acidithiobacillus ferrooxidans on the wastewater to be treated containing As (III) gradually tends to be stable and is maintained at about 90%; for the wastewater to be treated containing As (V), when the adding amount of viable bacteria is increased, the treatment effect of the acidophilic thiobacillus ferrooxidans on As (V) is kept stable, and is basically maintained at the state of small fluctuationAbout 95 percent.
Example 2
FeSO is added into the arsenic-containing wastewater with the Fe/As molar ratio of 1, 3, 5, 7, 10, 20, 30, 40 and 50 respectively4·7H2O, 2.5X 10 per ml6The acidophilic thiobacillus ferrooxidans centrifugal liquid is added into arsenic-containing waste water according to the proportion of each bacterium, the pH value is adjusted to be 2.5, and the mixture is placed in a shaking table with the temperature of 30 ℃ and the rotating speed of 165-175rpm for reaction for 3 d. The precipitate and the solution were separated, the precipitate was analyzed for its phase by X-ray diffractometry, and the solution was subjected to determination of arsenic concentration by ICP-OES.
As can be seen from FIG. 3, when the atomic molar ratio of Fe/As (III) is 30 or more, the XRD spectrum of the generated substance is basically stable and consistent with the standard PDF card of Schneider mineral; as can be seen from FIG. 4, when the molar ratio of Fe/As (V) atoms is 20 or more, the XRD spectrum of the resultant material is substantially stabilized and is consistent with the standard PDF card of Schneider mineral.
As can be seen from FIG. 5, for the wastewater to be treated containing As (III), the treatment effect of Thiobacillus acidophilus tends to be stable when the molar ratio of Fe/As (III) atoms is 30 or more; for wastewater to be treated containing As (V), when the molar ratio of Fe/As (V) atoms is 7 or more, the treatment effect of the acidithiobacillus ferrooxidans tends to be stable and is maintained at about 90%, but according to an XRD diagram of figure 4, when the molar ratio of Fe/As (V) atoms is 20 or more, the generated substance mineral phase tends to be stable and is schneiderian mineral; therefore, the optimum Fe/As atomic molar ratio for the Acidithiobacillus ferrooxidans to treat the As (V) -containing wastewater to be treated is 20.
By combining the obtained data, the optimal Fe/As atomic molar ratio of the As (III) -containing wastewater treated by the acidithiobacillus ferrooxidans is 30, and the optimal Fe/As atomic molar ratio of the As (V) -containing wastewater treated by the acidithiobacillus ferrooxidans is 20.
Example 3
Respectively adding FeSO into 50mg/L wastewater containing As (III) according to the Fe/As atomic molar ratio of 304·7H2O, at 7.5X 10 per ml6The acidophilic thiobacillus ferrooxidans centrifugate is added into the arsenic-containing wastewater according to the proportion of the bacteria to adjust pH is 2.5, the mixture is placed in a shaking table with the temperature of 30 ℃ and the rotation speed of 165-175rpm for reaction for 3d, the precipitate and the solution are separated, and the removal rate of As (III) by the acidophilic thiobacillus ferrooxidans is 90.22 percent according to the measurement of ICP-OES.
Example 4
Respectively adding FeSO into 50mg/L of As (V) -containing wastewater according to the Fe/As atomic molar ratio of 304·7H2O, at 7.5X 10 per ml6The method comprises the steps of adding acidophilic thiobacillus ferrooxidans centrifugal liquid into arsenic-containing wastewater according to the proportion of bacteria, adjusting the pH to be 2.5, placing the centrifugal liquid in a shaking table with the temperature of 30 ℃ and the rotation speed of 165-175rpm for reaction for 3d, separating precipitates and solution, and measuring the solution through ICP-OES, wherein the removal rate of the acidophilic thiobacillus ferrooxidans on As (V) is 95.31%.
Example 5
FeSO is added into 50mg/L arsenic-containing wastewater (containing As (III) and As (V) according to the Fe/As atomic molar ratio of 30 and the content ratio of 1:14·7H2O, 5X 10 per ml6The method comprises the steps of adding acidophilic thiobacillus ferrooxidans centrifugal liquid into arsenic-containing wastewater according to the proportion of bacteria, adjusting the pH to be 2.5, placing the centrifugal liquid in a shaking table with the temperature of 30 ℃, the rotation speed of 165-175rpm for reaction for 3d, separating precipitates and solution, and measuring the solution through ICP-OES, wherein the removal rate of the acidophilic thiobacillus ferrooxidans on arsenic is 92.87%.
Figure 6 is an XRD pattern of the resulting precipitate, schlerian mineral by comparison with a standard schlerian mineral card.
Example 6
Taking 25 g of the soil polluted by the arsenic to be treated, wherein the exchangeable arsenic content in the soil is 52mg/kg, and the arsenic types are sodium arsenate and sodium arsenite (the content ratio is 1: 1). FeSO is added into the arsenic contaminated soil (containing As (III) and As (V)) according to the proportion that the mol ratio of Fe/As atoms is 1004·7H2O solution with a liquid-soil ratio of 1:1 (L/kg); wherein the pH of the solution is 2.5; according to the proportion of 5 multiplied by 10 per gram of soil6The acidophilic thiobacillus ferrooxidans centrifugate is added into arsenic contaminated soil according to the proportion of each bacterium, and is placed in a shaking table with the temperature of 30 ℃ and the rotating speed of 165-175rpm for reaction for 3 d.
Drying and sieving a proper amount of treated soil, adding an extracting agent, and oscillating and centrifuging; the centrifugal liquid is measured by ICP-OES, and the exchangeable arsenic removal rate in the soil is detected to reach 68.05%.
Example 7
Taking 25 g of the soil polluted by the arsenic to be treated, wherein the exchangeable arsenic content in the soil is 52mg/kg, and the arsenic types are sodium arsenate and sodium arsenite (the content ratio is 1: 1). Adding biogenic Schwerner mineral into the arsenic-containing soil to be treated according to the mass percent of 1%, wherein the liquid-soil ratio is 1:1 (L/kg); wherein the pH of the solution is 2.5, and the solution is placed in a shaking table with the temperature of 30 ℃ and the rotation speed of 165-175rpm for reaction for 3 d.
Drying and sieving a proper amount of treated soil, adding an extracting agent, and oscillating and centrifuging; the centrifugal liquid is measured by ICP-OES, and the exchangeable arsenic removal rate in the soil is detected to reach 52.97%.
Compared with the example 6, compared with the method for removing arsenic by directly adding biogenic Shi mineral into arsenic-containing polluted soil, the method has the advantages that the arsenic removal rate by utilizing the mineralization effect of the acidophilic thiobacillus ferrooxidans is improved by 15 percent, and the arsenic removal effect is obviously improved.
Example 8
The soil after the reaction in example 6 and example 7 was dried, ground and sieved for toxicity leaching experiments. Drying and sieving a proper amount of treated soil, and respectively adding deionized water and acidified deionized water (the pH is 4 and is adjusted by using 2M HCl) according to the liquid-soil ratio of 10:1 (L/kg); then placing the mixture in a shaking table, and oscillating the mixture for 8 hours at the room temperature and at the rpm of 110; after the shaking was completed, the mixture was left standing for 16 hours.
Measuring the supernatant by ICP-OES, and detecting that the soil treated by directly adding biogenic Schwerer minerals has arsenic leaching rates of 2.27% and 2.65% after water leaching and acid leaching respectively; the leaching rates of arsenic after water leaching and acid leaching of the soil treated by the acidithiobacillus ferrooxidans are 0.95% and 0.76% respectively, and the stabilizing effect on arsenic is obviously enhanced.
The above description describes some embodiments of the invention, but is only exemplary, not limited to the given embodiments, and should not be used to limit the scope of the invention. Changes may be made in the embodiments given without departing from the principles and spirit of the invention.
Claims (10)
1. A method for treating arsenic-containing wastewater or arsenic-contaminated soil by using autotrophic bacteria, comprising: adding ferrous salt into the wastewater to be treated containing As (III) and/or As (V) or soil, and simultaneously adding acidophilic thiobacillus ferrooxidans for treatment to form a Schneider mineral precipitate; when the arsenic-containing wastewater contains trivalent arsenic and pentavalent arsenic at the same time, the dosage of the ferrous salt in the arsenic-containing wastewater is controlled to control the atomic molar ratio of iron to arsenic to be 10-60: 1; Fe/As (III) atomic molar ratio is 30-60:1 when trivalent arsenic is contained in the solution alone, and 20-60:1 when pentavalent arsenic is contained in the solution alone; the ratio of the arsenic-polluted soil to the ferrous salt solution is 0.5-3:1 (g/mL); adding iron and arsenic into the soil at an atomic molar ratio of 50-150: 1;
adding Acidithiobacillus ferrooxidans in an amount of 2.0 × 106-8.0×106Each milliliter of arsenic-containing wastewater or each gram of arsenic-polluted soil by each bacterium;
adjusting the reaction temperature and pH value to 26-30 deg.C and 2.0-3.0 respectively; the rotating speed of a shaking table for reaction is 150-190 rpm; the reaction time is 2-4 d.
2. The method of claim 1, wherein the amount of added Acidithiobacillus ferrooxidans is 2.0 x 106-7.5×106Each milliliter of arsenic-containing wastewater or each gram of arsenic pollutes the soil.
3. The method of claim 1 or 2, wherein when the arsenic-containing wastewater contains trivalent and pentavalent arsenic simultaneously, the ferrous salt is added to the arsenic-containing wastewater in an amount to control the atomic molar ratio of iron to arsenic to be 30-60: 1.
4. the method of claim 1 or 2, wherein the ratio of arsenic contaminated soil to ferrous salt solution is 0.5-2:1 (g/mL); the atomic molar ratio of iron to arsenic added into the soil is 80-130: 1.
5. The method according to claim 1 or 2, characterized in that Acidithiobacillus ferrooxidans is dosed in logarithmic phase of growth.
6. The method of claim 1 or 2, wherein the ferrous salt comprises one or more of ferrous sulfate, ferrous chloride, and ferrous nitrate.
7. The method of claim 6, wherein the ferrous salt is ferrous sulfate.
8. The method as claimed in claim 1, wherein the shaking table rotation speed of the reaction is 160-180 rpm.
9. The method according to claim 1, wherein the content of arsenic in the wastewater or soil to be treated is 5 to 100mg/L in terms of arsenic.
10. The method according to claim 1, wherein the content of arsenic in the wastewater or soil to be treated is 20 to 80mg/L in terms of arsenic.
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