CN107032485B - Method for effectively controlling arsenic volatilization in arsenic-containing aquaculture wastewater anaerobic treatment process - Google Patents
Method for effectively controlling arsenic volatilization in arsenic-containing aquaculture wastewater anaerobic treatment process Download PDFInfo
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Abstract
The invention discloses a method for effectively controlling arsenic volatilization in an anaerobic treatment process of arsenic-containing aquaculture wastewater, which can control the volatilization of arsenic in the anaerobic treatment process of arsenic-containing aquaculture wastewater by three modes of reducing the arsenic content of anaerobic sludge, reducing the concentration of organic matters in the wastewater and adding sulfur and iron elements to fix soluble inorganic arsenic in situ in the wastewater.
Description
One, the technical field
The invention relates to a method for effectively controlling arsenic volatilization in an arsenic-containing aquaculture wastewater anaerobic treatment process, and belongs to the fields of sewage treatment technology and secondary pollution control.
Second, background Art
In the 40 s of the 20 th century, organic arsenic preparations were beginning to be used as additives for livestock and poultry feeds in large quantities because of their disease-preventing and growth-promoting effects. Loxarsine (ROX) is used as a typical organic arsenic feed additive, and the addition amount of the Roxarsine is 20-50 mg.kg-1. Most ROX will follow the animal waste into the environment or aquaculture wastewater.
The culture wastewater has the characteristics of high COD, SS and ammonia nitrogen concentration. Aiming at the characteristics of the wastewater, the anaerobic treatment process is generally applied to treat the aquaculture wastewater at present. With the use of organic arsenic feed additives in large quantities, the problem of heavy metal residue such as arsenic in aquaculture wastewater is receiving much attention. However, current treatment of aquaculture wastewater is more focused on the removal of conventional contaminants and ignores the problem of heavy metal contamination such as arsenic that may be present therein. Research shows that organic arsenic is rapidly converted into 3-amino-4-hydroxyphenylarsonic acid (HAPA) under anaerobic conditions, and inorganic arsenic (As (III) and As (V)) with higher toxicity is released. Under the action of microorganisms, inorganic arsenic forms volatile arsenic through methylation. Therefore, in the process of anaerobic treatment of the arsenic-containing aquaculture wastewater, part of arsenic enters the atmospheric environment from the wastewater to cause secondary environmental pollution. In addition, volatile arsenic can be taken directly by the human body through respiration. Therefore, in order to ensure the environmental safety and human health, how to solve the volatilization of arsenic in the anaerobic treatment process of arsenic-containing aquaculture wastewater becomes a key problem to be solved urgently at present.
Third, the invention
The invention aims to overcome the defect that arsenic is volatile in the anaerobic treatment process of arsenic-containing aquaculture wastewater, and provides a method for effectively controlling the volatilization of arsenic in the anaerobic treatment process of arsenic-containing aquaculture wastewater.
Research shows that the volatilization of arsenic is possibly closely related to the arsenic content of anaerobic sludge, the concentration of organic matters in wastewater and the concentration of soluble inorganic arsenic in wastewater, so that the volatilization of arsenic in the anaerobic treatment process of arsenic-containing aquaculture wastewater can be controlled by the following three ways:
the first method is as follows: in the anaerobic treatment process of the arsenic-containing culture wastewater, the arsenic content in the anaerobic sludge is controlled to be 1000-1500 mg-As.kg-1In the process, the volatilization of 20-50% of arsenic can be effectively controlled; controlling the arsenic content in the anaerobic sludge to be lower than 50 mg-As.kg-1When in use, 85-90% of arsenic can be effectively controlled to volatilize. Can timely replace the high-arsenic sludge (the high-arsenic sludge refers to the arsenic concentration in the sludge) by monitoring the arsenic concentration of the activated sludge in the anaerobic reactor>1000mg-As·kg-1) The arsenic content of the sludge is maintained at a low level so as to effectively control the generation of volatile arsenic.
Secondly, in the anaerobic treatment process of the arsenic-containing aquaculture wastewater, the concentration of organic matters in the wastewater is controlled to be 500-1200 mg-L-1The volatile content of As can be reduced by 60-70%, and the concentration of organic substances in waste water can be controlled to be lower than 500 mg-L-1In addition, the volatilization amount of arsenic can be reduced by 85-96%. Partial organic pollutants can be reduced by adopting a pretreatment mode on the wastewater before the wastewater enters the anaerobic process treatment, and the control of the volatilization of arsenic in the anaerobic process is facilitated. The organic matter is represented by volatile fatty acid, and comprises acetic acid, propionic acid, isobutyric acid, n-butyric acid and valeric acid.
Thirdly, in the anaerobic treatment process of the arsenic-containing aquaculture wastewater, adding sulfur and iron elements, and fixing inorganic arsenic in situ in a coprecipitation mode of sulfur, iron and arsenic, thereby controlling the volatilization of arsenic, 5.52 mg. L-1Fe2(SO4)3The addition of the arsenic removal agent can effectively reduce 45-56% of arsenic volatilization.
The invention verifies the control mode of arsenic volatilization in the anaerobic treatment process of arsenic-containing aquaculture wastewater through two aspects of static anaerobic batch test and Upflow Anaerobic Sludge Blanket (UASB) reactor experiment:
(1) study of static anaerobic batch test
The static anaerobic batch experiment is used for determining the possibility of controlling the volatilization of arsenic by adjusting the arsenic content in sludge and the concentration of organic matters in wastewater.
Preparing synthetic wastewater with ROX concentration of 20-50 mg-L-1COD concentration 0-3500 mg. L-1The ammonia nitrogen concentration is 50-150 mg. L-1The total phosphorus concentration is 1-20 mg. L-1The water inlet temperature is 15-40 ℃, the pH value is 6-9, and elements necessary for the growth of microorganisms are added into the water inlet according to the volume ratio of 1:10000-1: 5000. The essential trace elements are composed as follows: MgCl2(0-10g·L-1)，MnSO4(0-5g·L-1)，CaCl2(0-30g·L-1)，ZnCl2(0-1g·L-1)，CuCl2(0-0.5g·L-1)，NiCl2(0-5g·L-1)，CoCl2(0-5g·L-1)。
Anaerobic granular sludge: three kinds of arsenic-containing anaerobic granular sludge (S0: 0-50 mg-As.kg) are adopted-1；S1：1000-1500mg-As·kg-1；S2：3500-4000mg-As·kg-1) To verify the influence of the arsenic content of the sludge on arsenic volatilization, the sludge inoculation amount is 1-5g-VSS L-1。
The operation condition is that the reactor is a serum bottle with the effective volume of 150m L, and the temperature of the reactor is controlled to be 15-40 ℃.
(2) Study of UASB reactor
In the UASB reactor for treating arsenic-containing waste water for a long time, the possibility of sulfur and iron elements for controlling the volatilization of arsenic is clarified by regulating and controlling the arsenic deposition related elements (sulfur and iron) in the inlet water of the UASB reactor. The parameters of the reactor were set as follows:
controlling water inlet parameters that the ROX concentration is 5-50 mg. L-1COD concentration 500--1The ammonia nitrogen concentration is 50-150 mg. L-1The total phosphorus concentration is 1-20 mg. L-1The water inlet temperature is 15-40 ℃, the pH value is 6-9, and elements necessary for the growth of microorganisms are added into the water inlet according to the volume ratio of 1:10000-1: 5000. The essential trace elements are composed as follows: MgCl2(0-10g·L-1)，MnSO4(0-5g·L-1)，CaCl2(0-30g·L-1)，ZnCl2(0-1g·L-1)，CuCl2(0-0.5g·L-1)，NiCl2(0-5g·L-1)，CoCl2(0-5g·L-1). Wherein, Fe2(SO4)3The sulfur and iron elements in the alloy are reported to combine with arsenic to form precipitate or precipitate to realize in-situ fixation of arsenic, and the addition amount is 0.5-10 mg-L-1。
And (3) controlling the operation parameters: the sludge inoculation amount is 10 kg-SS.m-3～30kg-SS·m-3The hydraulic retention time is 5-24h, and the dissolved oxygen concentration is 0-0.5 mg. L-1The temperature of the reactor is controlled at 15-40 ℃, and the rising flow rate is 0.01-0.1 m.h-1. The reactor is used for the research of treating the arsenic-containing wastewater and continuously operates for more than 320 days, wherein Fe is not added into the inlet water during the 205 th and 300 th days2(SO4)3。
The invention has the beneficial effects that:
1. the invention takes three technical strategies for controlling arsenic volatilization in the anaerobic treatment process of the arsenic-containing aquaculture wastewater as the core, can realize effective control of arsenic volatilization, and avoids arsenic pollution transfer and secondary pollution.
2. The arsenic content of the anaerobic sludge is monitored and controlled, so that the volatilization of arsenic can be controlled, and the working condition of an anaerobic system can be fed back.
3. The pretreatment process is utilized to reduce the concentration of organic matters in the wastewater so as to control the volatilization of arsenic, thereby realizing the combination of the sewage treatment process and the secondary pollution prevention and control.
4. The volatilization of arsenic is reduced by adding sulfur and iron elements, and the method is economical and feasible and is simple to operate.
Description of the drawings
FIG. 1 shows the close relationship between arsenic volatilization and arsenic content in anaerobic granular sludge, wherein a is a static experiment (20 mg. L added)-1ROX), and b is a graph of total arsenic content change of each anaerobic granular sludge after a static experiment. As can be seen from fig. 1, the higher the arsenic content in the anaerobic granular sludge, the higher the arsenic volatilization amount, indicating the feasibility of reducing arsenic volatilization by controlling the arsenic content in the sludge.
Fig. 2 shows the effect of adding sulfur and iron elements to the feed water of the UASB reactor on the volatilization of arsenic (indicated by the absence of sulfur and iron elements). As can be seen from fig. 2, the reactor produced significantly more volatile arsenic without the addition of the sulfur and iron elements, indicating the feasibility of controlling arsenic volatilization by adding the sulfur and iron elements.
FIG. 3 is a schematic diagram of three strategies for controlling arsenic volatilization in an anaerobic reactor for treating arsenic-containing aquaculture wastewater according to the invention.
Fifth, detailed description of the invention
Aiming at the key problem of arsenic volatilization in the process of anaerobic treatment of arsenic-containing aquaculture wastewater, the invention provides three technical schemes to realize effective control of volatile arsenic, and the control mode of arsenic volatilization in the process of anaerobic treatment of arsenic-containing aquaculture wastewater is verified through two aspects of a static anaerobic batch test and an up-flow anaerobic sludge blanket (UASB) reactor test:
(1) study of static anaerobic batch test
The static anaerobic batch experiment is used for determining the possibility of controlling the volatilization of arsenic by adjusting the arsenic content in sludge and the concentration of organic matters in wastewater.
Preparing synthetic wastewater with ROX concentration of 20-50 mg-L-1COD concentration 0-3500 mg. L-1The ammonia nitrogen concentration is 50-150 mg. L-1The total phosphorus concentration is 1-20 mg. L-1The water inlet temperature is 15-40 ℃, the pH value is 6-9, and elements necessary for the growth of microorganisms are added into the water inlet according to the volume ratio of 1:10000-1: 5000. Necessary trace amountThe element composition is as follows: MgCl2(0-10g·L-1)，MnSO4(0-5g·L-1)，CaCl2(0-30g·L-1)，ZnCl2(0-1g·L-1)，CuCl2(0-0.5g·L-1)，NiCl2(0-5g·L-1)，CoCl2(0-5g·L-1)。
Anaerobic granular sludge: three kinds of arsenic-containing anaerobic granular sludge (S0: 0-50 mg-As.kg) are adopted-1；S1：1000-1500mg-As·kg-1；S2：3500-4000mg-As·kg-1) To verify the influence of the arsenic content of the sludge on arsenic volatilization, the sludge inoculation amount is 1-5g-VSS L-1。
The operation condition is that the reactor is a serum bottle with the effective volume of 150m L, and the temperature of the reactor is controlled to be 15-40 ℃.
(2) Study of UASB reactor
In the UASB reactor for treating arsenic-containing waste water for a long time, the possibility of sulfur and iron elements for controlling the volatilization of arsenic is clarified by regulating and controlling the arsenic deposition related elements (sulfur and iron) in the inlet water of the UASB reactor. The parameters of the reactor were set as follows:
controlling water inlet parameters that the ROX concentration is 5-50 mg. L-1COD concentration 500--1The ammonia nitrogen concentration is 50-150 mg. L-1The total phosphorus concentration is 1-20 mg. L-1The water inlet temperature is 15-40 ℃, the pH value is 6-9, and elements necessary for the growth of microorganisms are added into the water inlet according to the volume ratio of 1:10000-1: 5000. The essential trace elements are composed as follows: MgCl2(0-10g·L-1)，MnSO4(0-5g·L-1)，CaCl2(0-30g·L-1)，ZnCl2(0-1g·L-1)，CuCl2(0-0.5g·L-1)，NiCl2(0-5g·L-1)，CoCl2(0-5g·L-1). Wherein, Fe2(SO4)3The sulfur and iron elements in the alloy are reported to combine with arsenic to form precipitate or precipitate to realize in-situ fixation of arsenic, and the addition amount is 0.5-10 mg-L-1。
And (3) controlling the operation parameters: the sludge inoculation amount is 10 kg-SS.m-3～30kg-SS·m-3The hydraulic retention time is 5-24h, and the dissolved oxygen is concentratedThe degree is 0-0.5 mg. L-1The temperature of the reactor is controlled at 15-40 ℃, and the rising flow rate is 0.01-0.1 m.h-1. The reactor is used for the research of treating the arsenic-containing wastewater and continuously operates for more than 320 days, wherein Fe is not added into the inlet water during the 205 th and 300 th days2(SO4)3。
Example 1:
referring to fig. 3, the first arsenic volatilization reduction technology invention is described in detail, and the method for effectively controlling arsenic volatilization by monitoring the arsenic content in anaerobic sludge and controlling the formation of high-arsenic sludge in the embodiment is implemented as follows:
preparing synthetic water COD (3500 mg. L)-1)，ROX(20mg·L-1)，NH4 +-N(100mg·L-1)，TP(15mg·L-1)。
Essential trace element composition: MgCl2(4.25mg·L-1)，MnSO4(0.38mg·L-1)，CaCl2(5.20mg·L-1)，ZnCl2(0.24mg·L-1)，CuCl2(0.12mg·L-1)，NiCl2(0.48mg·L-1)，CoCl2(0.24mg·L-1)。
The reactor is an anaerobic reactor with the effective volume of 150m L, and the inoculation amount of the anaerobic granular sludge is 2.5g-VSS L-1The running temperature is controlled at 35 +/-1 ℃.
As shown in Table 1, when the arsenic content in the sludge is reduced by more than 50%, the yield of volatile arsenic is reduced to 20-50% of the original yield; when the arsenic content in the sludge is lower than 50 mg-As.kg-1When in use, 85-90% of arsenic can be effectively controlled to volatilize. Namely, the arsenic content in the sludge is controlled to be lower, thereby effectively inhibiting the volatilization of arsenic and reducing the threat to the surrounding environment and the human health. Therefore, in the treatment process of the arsenic-containing aquaculture wastewater, attention is paid to the detection of the arsenic content in the sludge, and the sludge with high arsenic content formed by long-term operation is replaced.
TABLE 1 Effect of background arsenic content in anaerobic granular sludge on arsenic volatilization
Example 2:
referring to fig. 3, the second arsenic volatilization reduction technology invention is described in detail, and the method for effectively controlling arsenic volatilization by adjusting the content of organic pollutants in wastewater in the embodiment is implemented as follows:
preparing synthetic water COD (3000 mg. L)-1)，ROX(20mg·L-1)，NH4 +-N(100mg·L-1)，TP(15mg·L-1)。
Essential trace element composition: MgCl2(4.25mg·L-1)，MnSO4(0.38mg·L-1)，CaCl2(5.20mg·L-1)，ZnCl2(0.24mg·L-1)，CuCl2(0.12mg·L-1)，NiCl2(0.48mg·L-1)，CoCl2(0.24mg·L-1)。
The reactor is an anaerobic reactor with the effective volume of 150m L, and the inoculation amount of the anaerobic granular sludge is 2.5g-VSS L-1The arsenic content of the sludge is 3.69 g-As.kg-1The running temperature is controlled at 35 +/-1 ℃.
The methyl supply required for arsenic volatilization was derived from the organics in the wastewater, therefore, adjustment of the organic concentration in the wastewater was considered to control arsenic volatilization, as shown in Table 2, when the organic concentration was 1500--1When the arsenic is volatilized, the volatilization amount of the arsenic can reach 2.5-9.0 mu g.d-1When the concentration of organic matter is regulated to 0.3-0.5, the volatilization of arsenic can be reduced by 60-70%, and when the concentration of organic matter is controlled to 500 mg-L-1In the following, the volatilization amount of arsenic can be reduced by 85-96%. Experiments prove that the volatilization of arsenic can be effectively controlled by adjusting the concentration of organic matters in the wastewater. Due to the characteristic of high COD of the aquaculture wastewater, proper pretreatment is carried out on the wastewater before the wastewater enters the anaerobic process treatment, part of organic pollutants are reduced, and the control of the volatilization of arsenic in the anaerobic process is facilitated.
TABLE 2 Effect of organic concentration (in terms of volatile fatty acids) in wastewater on arsenic volatilization
Example 3:
referring to fig. 3, a detailed description is given below of a third arsenic volatilization reduction technology invention, in this embodiment, a method for effectively controlling arsenic volatilization by adding sulfur and iron elements to fix soluble inorganic arsenic in situ is specifically implemented as follows:
preparing synthetic water COD (3000 mg. L)-1)，ROX(5.0mg·L-1)，NH4 +-N(100mg·L-1)，TP(15mg·L-1)。
Essential trace element composition: MgCl2(4.25mg·L-1)，MnSO4(0.38mg·L-1)，CaCl2(5.20mg·L-1)，ZnCl2(0.24mg·L-1)，CuCl2(0.12mg·L-1)，NiCl2(0.48mg·L-1)，CoCl2(0.24mg·L-1). Wherein Fe is not added between the 275 th and 300 days of reactor operation2(SO4)35.52 mg-L on day 301-350-1Fe2(SO4)3。
The reactor is an up-flow anaerobic sludge bed reactor with the effective volume of 3.0L, and the sludge inoculation amount is 20 kg-SS.m-3The hydraulic retention time is 12h, and the dissolved oxygen concentration is 0-0.5 mg. L-1The temperature of the reactor is controlled to be 35 +/-1 ℃, and the rising flow rate is 0.03 m.h-1。
Based on the previous research results, the formation of volatile arsenic is achieved by the continuous methylation of inorganic arsenic (As (III) and As (V)), and the addition of sulfur and iron elements rapidly reduces the soluble inorganic arsenic in wastewater by in-situ fixing inorganic arsenic in the form of coprecipitation of sulfur, iron and arsenic, thereby controlling the volatilization of arsenic to a certain extent, as shown in Table 3, 5.52 mg-L during the operation of UASB reactor-1Fe2(SO4)3The addition of the arsenic removal agent can effectively reduce 45-56% of arsenic volatilization.
TABLE 3 control of arsenic volatilization by addition of sulfur and iron elements
Claims (1)
1. A method for effectively controlling arsenic volatilization in the process of anaerobic treatment of arsenic-containing aquaculture wastewater is characterized by comprising the following steps:
in the anaerobic treatment process of the arsenic-containing aquaculture wastewater, the concentration of organic matters in the wastewater is controlled to be lower than 500mg ∙ L-1The generation of volatile arsenic can be effectively inhibited, and the volatilization amount of the arsenic can be reduced by 85-96%; part of organic pollutants are reduced by adopting a pretreatment mode on the wastewater before the wastewater enters the anaerobic process treatment, so that the volatilization of arsenic in the anaerobic process is favorably controlled; the organic matter is represented by volatile fatty acid, and comprises acetic acid, propionic acid, isobutyric acid, n-butyric acid and valeric acid; the volatile arsenic is achieved by the continuous methylation of inorganic arsenic, As (III) and As (V).
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| CN102167443A (en) * | 2011-05-23 | 2011-08-31 | 合肥工业大学 | Method for removing organic arsenic in cultivation wastewater by anaerobic granular sludge |
| CN102674547A (en) * | 2012-05-30 | 2012-09-19 | 合肥工业大学 | Method for removing organic arsenic in livestock cultivation waste water by utilizing three-stage anaerobic treatment process |
| CN103663884A (en) * | 2013-12-30 | 2014-03-26 | 合肥工业大学 | Method for enhancing degradation of organic arsenic in waste water of livestock breeding into pentavalent arsenic by utilizing weak potential |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN102167443A (en) * | 2011-05-23 | 2011-08-31 | 合肥工业大学 | Method for removing organic arsenic in cultivation wastewater by anaerobic granular sludge |
| CN102674547A (en) * | 2012-05-30 | 2012-09-19 | 合肥工业大学 | Method for removing organic arsenic in livestock cultivation waste water by utilizing three-stage anaerobic treatment process |
| CN103663884A (en) * | 2013-12-30 | 2014-03-26 | 合肥工业大学 | Method for enhancing degradation of organic arsenic in waste water of livestock breeding into pentavalent arsenic by utilizing weak potential |
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