CN112684072A - Volatilization flux test and risk assessment of benzene in gas-enclosed zone soil gas - Google Patents
Volatilization flux test and risk assessment of benzene in gas-enclosed zone soil gas Download PDFInfo
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Abstract
The volatilization flux test and risk assessment of benzene in the gas-containing zone soil gas belong to the technical field of risk assessment. The method comprises the steps of simulating the migration of benzene in the aeration zone soil with different soil types, different water contents and different pollution source concentrations at room temperature by utilizing the soil columns, measuring the volatilization flux of the benzene in a passive mode, calculating the respiratory exposure health risk of the benzene based on the actually measured soil gas volatilization flux, selecting different soil types in 7 places across the country, comparing the different soil types with the results calculated by adopting J & E and J & E-DED models based on the soil benzene concentration, and aiming at providing a basis for the selection of the models and the method.
Description
Technical Field
The invention simulates the migration of benzene in an air-covered zone of soil under the room temperature condition by utilizing the soil columns through changing the variables of the water content and the concentration of a pollution source, passively measures the volatilization flux of the benzene, calculates the respiratory exposure health risk of the benzene based on the actually measured volatilization flux of the soil gas, and calculates the respiratory exposure health risk of the benzene based on the concentration (C) of the soil benzenes) By using J&E and J&And comparing the risk results calculated by the E-DED model, evaluating the applicability of the model and the method, and providing a basis for the refined risk evaluation of the benzene in the soil in the aeration zone.
Background
In the evaluation of human health risks of VOCs respiration exposure ways in soil aeration zone areas, the method is based on the concentration (C) of VOCs in soil at homes) Passing model (J)&E and J&E-DED), but many studies demonstrate that assessing risk based on soil concentration may overestimate actual levels, while assessing risk based on measured soil gas VOCs concentration is increasingThe more important it is.
The collection of soil gas mostly adopts an active sampling method of pumping by using a pump at present, and the method needs a power supply, is complex to operate, has higher technical requirements on operators, and is easily limited under the conditions of high water content and low permeability soil.
The volatile flux investigation is a new direction of soil gas investigation, and the current flux acquisition technology comprises three test methods, namely static flux box technology, dynamic flux box technology and passive flux box technology. Static flux methods result in a low measurement result due to the presence of steam accumulation in the flux box; the dynamic flux method continuously performs air blowing and pressure releasing, the operation technology is complex, and pressure loss is easily caused to cause a low measurement result; the passive flux acquisition technology is characterized in that an adsorbent is placed in a flux box, the volatilization flux of pollutants is determined according to the area of the flux bottom and the mass of VOC (volatile organic compounds) captured by the adsorbent in unit time, and the application prospect is good. Compared with the method, the passive flux method has the advantages of lower cost and simple operation for collecting the soil gas, and the collected time-weighted average concentration is more representative of the real level of the soil gas concentration compared with the active pump pumping method. The respiration exposure health risk of benzene is calculated based on the actually measured soil gas volatilization flux, and compared with the results calculated by J & E and J & E-DED models based on the soil benzene concentration, the method is simple, more accurate and efficient, and provides a theoretical basis for risk assessment of the polluted site.
Disclosure of Invention
The method utilizes the soil columns to select different soil types in 7 places across the country, simulates the migration of benzene under different soil conditions in an aeration zone, passively measures the volatilization flux of the benzene, calculates the respiratory exposure health risk of the benzene based on the actually measured soil gas volatilization flux, and compares the respiratory exposure health risk with the results calculated by adopting J & E and J & E-DED models based on the soil benzene concentration.
In order to achieve the purpose, the soil is injected with a pollution source after being prepared, and after the soil is balanced, the soil concentration test and the passive volatilization flux test are carried out to carry out the human health risk assessment of the outdoor respiration exposure way.
The method for testing the volatilization flux of benzene in the soil gas in the aeration zone is characterized by comprising the following steps of:
1) testing the water content of the soil to be tested, then configuring and filling the soil columns, respectively filling the soil to be tested into the hollow cylinders to form the soil columns, screwing the column covers, sealing the devices, and carrying out aging balance; a reserved space is arranged above the soil column in the cavity cylinder;
2) a soil sampling port is arranged on the side surface of the upper part of the soil column corresponding to the side surface of the cavity cylinder, a pollution source sample inlet is arranged on the side surface of the lower part of the soil column, a pollution source such as pure benzene is injected from the pollution source sample inlet, and the soil column is kept stand for a period of time until the pollutants on the top of the soil column are balanced, namely the pollution concentration in the soil corresponding to the top of the soil column is not changed;
3) testing of passive volatilization flux: putting a badge type passive sampler filled with a certain amount of active carbon into the soil column, immediately screwing a column cover, unscrewing the column cover after adsorbing for a period of time, quickly taking out the SKC sampler, putting the SKC sampler into a refrigerator at 4 ℃ for storage, and waiting for detection;
4) determination of pollution sources such as benzene series in activated carbon: using carbon disulfide desorption-gas chromatography to determine the mass concentration of target pollutants in the active carbon, taking the active carbon out of a badge-type passive sampler, transferring the active carbon into a brown extraction bottle with a polytetrafluoroethylene lining, adding a certain amount of carbon disulfide, sealing, oscillating at constant temperature for a period of time, standing at room temperature for desorption, taking the supernatant, and storing to be determined;
5) testing the sample in the step 4): agilent 7890A-5795C GC/MS was used. The column was of DB-5MS type (30 m.times.0.25 mm.times.0.25 μm), the carrier gas was high purity helium (99.9999%), the scanning mode was selective ion detection (SIM), the temperatures of the transport line and the ion source were 280 ℃ and 230 ℃ respectively, and the ion source was EI. The energy of an electron bombardment source is 70eV, the temperature of a sample inlet is 120 ℃, the temperature of a chromatographic column is 40-50 ℃, the sample injection amount is 1ul, and the split ratio is 10:1-5: 1;
the method for calculating the volatilization flux is as follows:
flux-volatile Flux mg/(m)2·s)。
M-mass of contaminant adsorbed during the test, mg
A-Passive flux acquisition floor area, m2
T-duration of the flux test, s.
6) Then further risk assessment is performed:
the carcinogenic risk prediction model of the outdoor respiration exposure path of VOCs in soil is as follows:
wherein: RI (Ri)HHealth risks based on volatile flux; caIs the outdoor exposure concentration of VOCs, mg/m3。
Preferably, the column cover in step (1) is a threaded cap with a polytetrafluoroethylene lining.
The method utilizes the soil columns to select different soil types in 7 places across the country, simulates the migration of benzene under different soil conditions in aeration zones, passively tests the volatilization flux of the benzene, calculates the respiratory exposure health risk of the benzene based on the actually measured volatilization flux of the soil gas, and compares the respiratory exposure health risk with the results calculated by adopting J & E and J & E-DED models based on the concentration of the soil benzene. Has the following advantages:
(1) and (3) simulating the volatilization of benzene in the aeration zone area by using the soil column, and passively testing the volatilization flux of the concerned pollutant. The method for passively measuring volatilization flux and collecting soil gas does not need external force, is simple to operate, is suitable for soil gas investigation of various soil types, can collect time-weighted concentration, and can reflect the real level of the soil gas concentration. The column cover adopts a thread column cover with a polytetrafluoroethylene lining and a vacuum cup cover type, so that the column cover is convenient to disassemble and assemble and has lower error influence on pollutant testing.
(2) The laboratory soil column simulation method is used for testing volatilization flux, so that variables such as different soil types, different water contents, different pollution source concentrations and the like can be conveniently controlled for testing, the physical and chemical property range of a sample is expanded, the number of data samples is increased, and persuasion is enhanced for researching the risk level of different soil types concerning pollutants.
(3) According to the method, the respiratory exposure health risk of benzene is calculated for different soil types based on actually measured soil gas volatilization flux, and compared with the results calculated by adopting J & E and J & E-DED models based on soil benzene concentration, the difference caused by model calculation is more accurately compared, and a theoretical basis is provided for selection of the models in risk assessment.
Drawings
FIG. 1 is a schematic view of a soil column structure;
FIG. 2 shows the benzene concentration at the sampling port of the black dragon soil during the determination of the equilibration time.
FIG. 3 is a graph of the migration of benzene simulated in 7 soils with water content of 3 and different concentrations of pollution sources, and the risk calculated based on the volatilization flux and the J & E model and the J & E-DED model.
Fig. 4 is a summary of the 7 soil types of fig. 3.
Detailed Description
The present invention will be further illustrated with reference to the following examples, but the present invention is not limited to the following examples.
The method for testing the volatilization flux and evaluating the risk of benzene in the soil gas in the aeration zone comprises the following steps:
1) preparing different water contents and filling soil columns for 7 soil types: assembling the soil columns, respectively filling 7 soils with different water contents into 7 soil columns, uniformly filling the soil columns with the height of 37cm, screwing column covers, sealing the device, and carrying out aging balance; 2) the method comprises the following steps of (1) exploring the equilibrium time of the benzene concentration of soil at a sampling port: and selecting the Heilongjiang black soil with the finest particles and the highest organic matter content, and preparing the highest water content and the lowest pollution source amount for testing. The pure benzene reagent was injected from the contamination source inlet and a soil sample was taken from the sampling port approximately once every one day. Detecting the concentration until the concentration reaches an equilibrium; 3) injecting a pollution source and collecting a soil sample: injecting a certain amount of analytically pure benzene reagent into the bottoms of 7 soil columns through a pollution source sample inlet by using a 1ml gas-phase sample inlet needle, sealing the sample inlet, and standing for a period of time to wait for the pollutants on the tops of the soil columns to reach balance. After balancing, rapidly collecting a benzene soil sample from a sampling port by using a non-disturbance sampler; 4) testing of passive volatilization flux: then putting a passive sampler filled with a certain amount of activated carbon (purchased from SKC company in America) into the earth column, immediately screwing a column cover, unscrewing the column cover after adsorbing for a certain time, quickly taking out the SKC sampler, putting the SKC sampler into a refrigerator at 4 ℃ for storage, and testing; 5) determination of benzene series in activated carbon: the mass concentration of the target pollutant in the activated carbon was determined using carbon disulfide desorption-gas chromatography. Taking out the activated carbon from the badge-type passive sampler, transferring the activated carbon into an 8mL brown extraction bottle with a polytetrafluoroethylene lining, adding a certain amount of carbon disulfide, sealing, oscillating at constant temperature for a certain time, standing at room temperature for desorption for a certain time, and taking the supernatant for storage to be tested; 6) testing the sample in the step 5): agilent 7890A-5795C GC/MS was used. The column was of DB-5MS type (30 m.times.0.25 mm.times.0.25 μm), the carrier gas was high purity helium (99.9999%), the scanning mode was selective ion detection (SIM), the temperatures of the transport line and the ion source were 280 ℃ and 230 ℃ respectively, and the ion source was EI. The energy of the electron bombardment source is 70 eV. The sample inlet temperature is 120 ℃, the chromatographic column temperature is 50 ℃, the sample injection amount is 1ul, and the split ratio is 10: 1; 7) and (4) risk assessment, namely calculating the health risk of the outdoor human body in the respiration exposure path by analyzing the mass concentration of benzene in the material, and performing risk assessment by analyzing the concentration of benzene in soil at a sampling port.
Example 1: soil sample and test device
A. The soil samples for the test are respectively collected from clean soil of 7 provinces of Ningxia, Gansu, Beijing, Shandong, Yunnan, Jilin and Heilongjiang, and are naturally dried in the air, and the serial numbers are sequentially from Z1 to Z7. The basic physicochemical properties of the soil are shown in Table 1.
Table 1: basic physicochemical properties of soil
B. The material of test device is organic glass, and diameter 50mm, height 450mm are apart from bottom 55mm, 305mm department and are pollution source introduction port and soil sample connection respectively, and introduction port and sample connection are sealed with supporting bolt respectively, and internal diameter 36 mm. The top of the soil column is provided with a threaded cap with a polytetrafluoroethylene lining. The left and right sides of the central point of the inner side of the cover are hung with small sticky hooks for hanging the passive sampler. Before the test, the test soil columns are assembled, water is injected, standing is carried out, and the tightness is tested.
Soil pretreatment
And (3) airing and grinding the 7 soil, sieving the ground soil by a 20-mesh sieve, preparing the target water content in a No. 8 self-sealing bag, sealing the self-sealing bag, and standing the self-sealing bag for 24 hours in a dark place to ensure that the water content is sufficiently and uniformly.
Filling of soil column
And (3) assembling the soil columns, respectively filling 7 soils with different water contents into the 7 soil columns, uniformly filling the soils with the height of 37cm, screwing down the threaded covers and sealing the devices.
Preparation of pollution sources
A certain amount of analytically pure benzene reagent is respectively injected into the bottoms of 7 soil columns through pollution source inlets by using 1ml of gas-phase sampling needles (Shanghai 'an's spectrum), the sampling inlets are sealed, and standing is carried out for a period of time so as to enable the concentration of pollutants on the tops of the soil columns to reach balance.
Soil sample collection and sampler insertion
A. After the soil concentration of a soil sample sampling port in the soil column reaches balance, a non-disturbance sampler is used for quickly collecting a benzene soil sample from the sampling port, the benzene soil sample is transferred into a brown blowing bottle added with 10mL of methanol, the brown blowing bottle is placed into a refrigerator at 4 ℃ for storage, and the test is carried out within 7 days.
B. A passive sampler containing 350mg of activated carbon (purchased from SKC, USA) was then placed on top of the column and the column cover was immediately screwed down.
Taking out and testing sampler
A. After adsorbing for 4-5 days, unscrewing the column cover, quickly taking out the SKC sampler, storing in a refrigerator at 4 ℃, and carrying out desorption test within 24 hours.
B. The activated carbon material was transferred to an 8ml brown glass bottle with a teflon liner cap. Adding 4ml of carbon disulfide, sealing, shaking at room temperature for 1min, desorbing for 30min, and testing.
Determination of the equilibration time
A. Testing of maximum equilibration time: VOCs diffuse and migrate upwards from the bottom of the earth pillar and reach equilibrium after a period of time. The time required for the soil concentration at the top of the soil column to reach balance is determined by 5 factors of the thickness degree of soil particles, the content of organic matters, the water content, the concentration of a pollution source and the environmental temperature. Soil with finer soil particles, higher organic content, higher water content and lower source concentration generally requires longer equilibration times when ambient temperatures are constant. At this time, soil (black soil of Heilongjiang) with the finest particles and the highest organic matter content is selected, and the highest water content (30%) and the lowest pollution source amount (200ul) are prepared for testing so as to explore the longest balance time under all experimental conditions of 7 soil types.
Table 2 shows the water content of 7 different soil types
B. Preparing the 20-mesh-sieve Heilongjiang soil into 30% of water content, placing the Heilongjiang soil in a dark place for standing for 24 hours, filling a soil column, injecting a pure benzene reagent (200ul) from a pollution source sample inlet, taking a soil sample from a sample inlet every day, and detecting the concentration until the concentration reaches the balance.
C. Determination of the equilibration time: since the time required for the soil type to reach equilibrium under this soil condition is greater than the time required for all other soil types to reach equilibrium at room temperature, 7 days were selected as the equilibration time for all experiments this time to ensure that all soils were able to reach equilibrium.
Benzene sample analysis
A. In the case soil samples were tested according to USEPA,8620D rev.4(2017.2) purge trap/gas chromatography mass spectrometry.
B. The samples obtained in the case were diluted to a concentration of about 1ppm and injected into a gas chromatograph for analysis.
GC-MS operating conditions: the column was of DB-5MS type (30 m.times.0.25 mm.times.0.25 μm), the carrier gas was high purity helium (99.9999%), the scanning mode was selective ion detection (SIM), the temperatures of the transport line and the ion source were 280 ℃ and 230 ℃ respectively, and the ion source was EI. The energy of the electron bombardment source is 70 eV. The sample inlet temperature is 120 ℃, the chromatographic column temperature is 50 ℃, the sample injection amount is 1ul, and the split ratio is 10: 1.
Passive sampler flux results:
in the test, the calculation method of the benzene volatilization flux collected by the SKC passive sampler comprises the following steps:
flux mg/(m) of Flux-benzene2·s)。
M-mass of contaminant adsorbed during the test, mg
A-Passive flux acquisition floor area, m2
T-duration of the flux test, s
Risk assessment of benzene in aeration zone soil
(1) Evaluation model based on actually measured soil gas volatilization flux
Exposure of contaminants from soil to humans can go through three processes: firstly, the pollutants diffuse and migrate from deep soil to reach an unsaturated zone, secondly, the pollutants in the unsaturated zone invade the ground through steam, thirdly, the pollutants on the ground are mixed and migrate with the atmosphere, and the volatilization fluxes are equal. Therefore, the prediction model of the carcinogenic risk of the outdoor respiration exposure pathway of VOCs in soil is as follows:
wherein: RI (Ri)HHealth risks based on volatile flux; caIs the outdoor exposure concentration of VOCs, mg/m3. The definition and value of other parameters are shown in the table.
(2) J & E evaluation model
Wherein: RI (Ri)JIs J&Concentration (C) based on VOCs in soil under model Es) A predicted health risk;
is the diffusion coefficient of VOCs in unsaturated zone soil, m2And s. The definitions and values of the remaining parameters are shown in Table 2.
(3) J & E-DED evaluation model
The J & E-DED model for evaluating the health risk of the outdoor respiration path polluted by the soil VOCs comprises the following steps:
coefficients A and F (C)s) And G (C)s) A function of
RIJ-DIs J&Soil-based VOCs concentration (C) under E-DED models) A predicted health risk. Where f is the extent to which the irreversible adsorption of the second fraction proceeds, and the recommended value is 1. The definitions and values of the remaining parameters are shown in Table 3.
The DED model assumes that there are two parts, reversible and irreversible, to the adsorption:
q＝q1st+q2nd
in the formula: q is total adsorption capacity of soil solid-phase particles to VOCs (volatile organic compounds), mg/kg; q. q.s1stAnd q is2ndThe adsorption amounts of the reversible and irreversible fractions, mg/kg, respectively.
Table 3 exposure factors and parameters
Note: except actual measurement, other parameters come from HJ 25.3-2019 technical guide for evaluating soil pollution risks of construction land
TABLE 4 soil parameters for each soil type corresponding to 7 soil columns
TABLE 5 Risk of different water content and concentration of pollution source in each soil
As shown in fig. 3: the abscissa is the soil concentration, and the ordinate is the respiratory exposure path outdoor human health risk calculated based on the volatilization flux and the J & E model and the J & E-DED model. The red horizontal dashed line represents the lg value at 1.00E-06 of the human acceptable risk, and the red vertical dashed line represents the soil screening value, i.e., 1.0mg/kg (which is considered the lowest limit at which soil remediation is not required). The 4 pairs of data that the soil detected concentration is lower than the screening value and the risk calculated based on the actually measured soil volatilization flux exceeds the risk acceptable by human bodies are all Beijing, Jilin and Gansu soils, the commonality of the soils is that the soil particles are thicker, and the soils with the main sandy property are coarse sand soil and sandy silty soil according to the domestic soil qualitative standard. It is shown that when the soil is mainly sandy, the pollutants are easy to escape in the sample collection process due to weak occurrence capacity of the pollutants in the soil, so that the detected concentration of the soil is low, and the actual risk level can be underestimated when the risk is calculated based on the soil concentration. This does not occur for soils with a high proportion of fine-grained components such as Shandong, Yunnan, Heilongjiang, etc.
As shown in fig. 4, the evaluation of health risk based on the J & E-DED model underestimates the actual risk level for 7 soils at lower concentrations of pollutants. Overall the J & E model is based on to be closer to calculating risk levels based on volatilization flux. Assessing risk based on the J & E model overestimates the actual risk level.
Claims (2)
1. The method for testing the volatilization flux of benzene in the soil gas in the aeration zone is characterized by comprising the following steps of:
1) testing the water content of the soil to be tested, preparing and filling the soil column, respectively filling the soil into the hollow cavity cylinder to form the soil column, screwing a column cover, sealing the device, and carrying out aging balance; a reserved space is arranged above the soil column in the cavity cylinder;
2) a soil sampling port is arranged on the side surface of the upper part of the soil column corresponding to the side surface of the cavity cylinder, a pollution source sample inlet is arranged on the side surface of the lower part of the soil column, a pollution source such as pure benzene is injected from the pollution source sample inlet, and the soil column is kept stand for a period of time until the pollutants on the top of the soil column are balanced, namely the pollution concentration in the soil corresponding to the top of the soil column is not changed;
3) testing of passive volatilization flux: putting a badge type passive sampler filled with a certain amount of active carbon into the soil column, immediately screwing a column cover, unscrewing the column cover after adsorbing for a period of time, quickly taking out the SKC sampler, putting the SKC sampler into a refrigerator at 4 ℃ for storage, and waiting for detection;
4) determination of pollution sources such as benzene series in activated carbon: using carbon disulfide desorption-gas chromatography to determine the mass concentration of target pollutants in the active carbon, taking the active carbon out of a badge-type passive sampler, transferring the active carbon into a brown extraction bottle with a polytetrafluoroethylene lining, adding a certain amount of carbon disulfide, sealing, oscillating at constant temperature for a period of time, desorbing at room temperature, taking the supernatant, and storing to be determined;
5) testing the sample in the step 4): agilent 7890A-5795C GC/MS was used. The column was of DB-5MS type (30 m.times.0.25 mm.times.0.25 μm), the carrier gas was high purity helium (99.9999%), the scanning mode was selective ion detection (SIM), the temperatures of the transport line and the ion source were 280 ℃ and 230 ℃ respectively, and the ion source was EI. The energy of an electron bombardment source is 70eV, the temperature of a sample inlet is 120 ℃, the temperature of a chromatographic column is 40-50 ℃, the sample injection amount is 1ul, and the split ratio is 10:1-5: 1;
the method for calculating the volatilization flux is as follows:
flux-volatile Flux mg/(m)2·s)。
M-mass of contaminant adsorbed during the test, mg
A-Passive flux acquisition floor area, m2
T-duration of the flux test, s.
2. A risk assessment method for benzene in gas-enclosed zone soil gas is characterized in that a carcinogenic risk prediction model of an outdoor respiration exposure path of VOCs in soil is as follows:
wherein: RI (Ri)HHealth risks based on volatile flux; caIs the outdoor exposure concentration of VOCs, mg/m3。
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