simulation of multimedia fate of chlorobenzene in ...

Volume 25 – No. 9/2016, pages 3430-3437

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Fresenius Environmental Bulletin

SIMULATION OF MULTIMEDIA FATE OF CHLOROBENZENE IN SHAOKOU SECTION OF THE SONGHUA RIVER, NORTHEASTERN CHINA Meng Fansheng1,2* , Yu Haibin3, Wang Juling1,2, Wang Yeyao2,3, Zhang Lingsong1,2 1

State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing, China 2 Research Center for Water Pollution Control Technology, Chinese Research Academy of Environmental Sciences, Beijing , China 3 China National Environmental Monitoring Center, Beijing, China

reported that the water quality of the Songhua River (SHR) basin has deteriorated, and the toxicity of SHR pollutants provokes ecological concerns [5-8]. However, majority of the reports focusing on halogenated hydrocarbonrelated research are mainly about itsdetection in the section of estuary and the city area [9-10], and very limited research was carried out studying on the migration and fate of halogenated hydrocarbon in large-scale regions [11]. In the past several years, fugacity model has been used to simulate the multi media fate of different types of organic pollutants, such as polycyclic aromatic hydrocarbons, dioxins, nitrobenzene, etc [12-14]. And it has become a good predictor for transportation of contaminants in the environment and the existence of pollutants in various environmental media. Based on the mass balance principle, fugacity model is used to generate quantitative description of the input and output of pollutants in environmental systems, as well as the ransportation and transformationof pollutants between different media. The fugacity model is treated as a simple, straight-forward model, since it only requires the most basic physical and chemical parameters along with the environmental property parameters of the pollutants. Also, a number of parameters can be obtained directly through the thermodynamic calculation, which reduces the burden of the measurement work. Therefore, the fugacity model is a great option for the study on the fate of volatile organic compounds [15-17]. In this study, the fugacity model was used not only to simulate the migration of chlorobenzene in different environmental media after the entrance of chlorobenzene into the natural water environment, but also to mimic the various physical, chemical, biological transformation occurred during the migration process, targeting atobtaining the prediction of possible migration pathways and the existenceforms of chlorobenzene in the environment, as well asthefinal distribution of chlorobenzene in various environmental media. The results of this studyare proposed toprovide the data support for environmental remediation, and to

ABSTRACT A multimedia fugacity model (level III) was used to simulate the concentration distribution of chlorobenzene from Shaokou section to Songhua River Village section of the Second Songhua River based on a steady-state assumption. The concentration distribution was calculated in the air, water, suspended particulate matters (SPMs) and the sediment. The results showed that the model output concentration in the air, water, SPMs and the sediment accounted for 1.448×10-2mg/m3, 9.503×10-5mg/L, 3.043×10-6g/kg(dw), 1.270×105 g/kg respectively, when chlorobenzene was discharged to the water from pollution sources at 20mol/h, of which chlorobenzene in the air was 94.931% in total, indicatingthat after reaching steady-state in the system, chlorobenzene mainly existed in the air. In water environment, chlorobenzene distribution werepresented as 98.362% in water phase, 0.020% in suspended substance phase and 1.618% in sediment phase, respectively, which means that most chlorobenzene in water environment existed in the water phase and little in the suspended substance and the sediment phase.

KEYWORDS: fugacity model Ⅲ; chlorobenzene(CB); Songhua River; multimedia fate

INTRODUCTION Chlorobenzene (CB), as one of thetypical volatile halogenated organic compounds, has been widely used in various industries, such as chemical industry, pharmaceutical industry, pesticide manufacturing, plasticmanufacturing, military industry and organic synthesis, etc [1-2]. With the characteristics of low degradation but easy bioaccumulation in the environment, Chlorobenzene becomes one of the most important environmental pollutants [3-4]. In recent years, it 3430

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Photodegradation

Ai r Advection Output

Ai r bor ne Par t i cl es

Inputting Source

Volatilization

Diffusion

Wat er

Diffusion

Suspended Solids

Resuspension

Advection Output

Dry and Wet Deposition

Adsorption Diffusion

Advection Output

Sediment Deposition

Biodegradation

Biodegradation

Adsorption

Biodegradation

FIGURE 1 The figure of simulation of multimedia fate of chlorobenzene in the Songhua River establish an important scientific basis for the disposal and ecological risk assessment of the environmental emergencies.

Model framework. Based on the multimedia fugacity model built by Mackay [18], with the combination of environmental characteristics of the Songhua River, the fugacity model Ⅲ was established. Under this model, the environment of the Songhua River is divided into four phases, which are air, water, suspended solidsand sediment. Also, the following assumption should be followed: the chlorobenzene are discharged into the water stably and continuously; all of the degradation reactions of chlorobenzene in various environmental media are first-order reaction; atmosphere is constituted by gaseous phase and aerosol that are in equilibrium; after a certain period of time, the distribution of chlorobenzene in water system becomes stable, and the fugacity within each medium does not change over time. According to the mass balance principle, the process of migration and transformation of chlorobenzene in various environmental media can be simulated. The simulation is shown in Figure 1. According to the basic structure of fugacity model Ⅲ and the mass balance of chlorobenzene in water environmental systems, the expression of the reduction of chlorobenzene under the fugacity model can be generated as follows:

MATERIALS AND METHODS Study area. The Songhua River is located in northeast part of China, with the geographical coordination of 119.52 ° E ~ 129.30 ° E and 41.42 ° N ~ 51.38 ° N. Due to its location in the north temperate monsoon climate zone, the Songhua River basin indicates continental climate characterized by significantly large temperature difference during the year, withannual average temperature between 3 ~ 5 ℃ and wet period average temperature of 20 ~ 25 ℃ , and annual average precipitation of about 500 mm. In this study, it was chosen the river section from Shaokou section to Songhua River Village section of the Second Songhua River as the subject, which covers the river length of 120 km, with an average water depth of 8m, a flowrate of 800m3 / s and the average velocity of 0.5 m/s.

Air：

E A  G AI Z A f AI  DW  A fW  f A DRA  D AW  D A SS  G AO Z A   0

E  G Z fWI  D A W f A  D S W fS  D SS W fSS  fW D RW  DW  A  DW  S  DW  SS  GWO Z W   0

WI W Water： W Suspended solids：

ESS  GSSI Z SS f SSI  DW  SS fW  DA SS f A  DS  SS f S  f SS DRSS  DSS W  DSS  S  GSSO Z SS   0

Sediment：

E S  GSI Z S f SI  DW  S fW  DSS  S f SS  f S DRS  DS  SS  GSO Z S   0

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a44  (GSO Z S  DS  SS  DRS )

Where: A, W, SS, S represent air, water, suspended solids and sediments, respectively; Ei (i = A, W, SS, S) is the emission rate of pollutants in the medium i,mol / h; GiI is the fluid advection input rate in the medium i, m3 / h; GiO is the fluid advection output rate in medium i, m3/h; Zi isthe fugacity capacity of chlorobenzene in a medium i, mol / (m3 • Pa); fi is the fugacity of chlorobenzene in the medium of i, Pa; fiI is the fugacity of chlorobenzene inadvection in putting medium i, Pa; Di-jis the interphase migration rate coefficient ofchlorobenzene from the media i to the media j, mol / (h • Pa); DRiis the degradation reaction rate coefficientof chlorobenzene in the medium i, mol / (h • Pa). The above equation can be represented by a matrix equation as:

Where: U is the increased amount of chlorobenzene caused by the pollutant emissions and the upstream inputper time unit, mol / h; the elements in the main diagonal of matrix F indicate the amount of migration pollutantoutputting toother environmental media per unit time, per unit volume, mol / (h • Pa); the elements in other locations represent theamount of migration pollutantfrom other environmental media inputtingto the corresponding media that is indicated on that row.

Simulation and parameter identification. The input process of the Chlorobenzene in the study area was the stabledischarge of thewastewater, while the output process constitutes the degradation F  f  E U  0 of the chlorobenzene in the environmental phases, (1) and the advection output to the air, water and Among which, suspended solids, and the adsorption of 0   a11 DW  A 0 chlorobenzene in the sediments, etc. Theexchange D  process between different environmental phases a D D 22 SS W S W  includes the following aspects:air - water (wet and F   AW  D ASS DW SS a33 DS SS  dry deposition and diffusion process), water - air   (volatilization process), sediment - water  0 DW S DSS S a44  (adsorption process), water - sediment (desorption (2) process), water - suspended solids (adsorption  fA  process), suspended solids - water (desorption f  process), sediments and suspended solids deposition/resuspension, chlorobenzene f  W (3)  f SS  photodegradation and biodegradation processes, etc.   Because the model simulation starting section  fS  –Shaokou is located at thedownstream of Jilin City, the main sources of toxicorganic pollutants were the industrial wastewater dischargedfrom the 1 0 0 0 factorieswith business oforganic synthesis, 0 1 0 0  petroleum refining and other industrial  (4) E productions.Also, there is no obvious inputting 0 0 1 0  source in the upper reaches of the Songhua River   and the surrounding areas.Base on the survey for 0 0 0 1  the pollution sources and existing level of the pollutants in the water environment [19], the initial  E A  GAI Z A f AI  condition of the model was assumed thatthe  E G Z f  discharging speed of chlorobenzene into the WI W WI  Songhua River was20 mol/h;the initial ρ U  W  ESS  GSSI Z SS f SSI  (chlorobenzene) were 0 mg / L or below the   detection limit in the water environment of the  ES  GSI Z S f SI  Songhua River. The environmental parameters in (5) the river sections of the study area are shown in Table 1. a11  (G AO Z A  D AW  D A SS  DRA ) The fugacity capacity (Z) and related parameters of air, water, suspended solidsand a22  (GWO ZW  DW  A  DW  SS  DW  S  DRW ) sediments are defined as follows: Air：ZA=1/RT Water：ZW=1/H Suspended particulate matters ： a33  (GSSO Z SS  DSS W  DSS  S  DRSS ) ZSS=ZW×ρSS×KOC×φSS logKOC=0.989logKOW-0.346 Sediments：ZS=ZW×ρS×KOC×φS[25] 3432

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TABLE 1 The environmental parameters in study region Parameters

Values

Air area（AS）/m2

2.4×107

Height of the air（HA）/m

1.0×103

Average wind speed（Vwind） /m/s Lengh of the water body（L） /km Area of the water body （AW）/m2 Depth of the water body （H）/m

1 120 2.4×107 8

Parameters Influx flow（Q1）/(m3/s) Outflow（Q2）/(m3/s) Average flow rate （Vriver）/m/s Density of the sediment （ρS）/kg/m3 Density of the suspended solids（ρSS）/kg/m3 Volume rate of the suspended solids

Values 800 719.8

Precipitation rate/m/h

1.6×10-5

0.5 2.4×103 2.4×103 7×10-3

TABLE 2 Environmental transport parameters Migration media air-water air-suspended solids water-air water-suspended solids water-sediments suspended solids-water suspendedsolids-sediment sediment-water sediment-suspended solids

Process Diffusion Precipitation dissolution

Migration coefficient and equation DA-W=1/(1/KVAAWZA+1/KVWAWZW) DR=KRAWZW

Dry and wet deposition

DA-SS=KQSAWZA

volatilization Adsorption Diffusion Deposition

DW-A=1/(1/KVAAWZA+1/KVWAWZW) DW-SS=0.693VSSZSS/tWSS DW-SS=KWBSAWZW DW-S=KSASZS

Diffusion Deposition Diffusion

DSS-W=KWBSAWZW DSS-S=KSASZS DS-W=KWBSAWZW

Resuspension

DSR=KSRASZS

Resuspension

DSR=KSRASZS

Where: R is the gas constant, 8.314 J/(mol·K); T is the absolute temperature, K; H is the Henry constant, Pa·m3/mol ; ρSS is the density of the suspended solids, kg/m3; φSS is the contentof organic carbon of the suspended solids; KOC is the organic carbon partition coefficient; KOW is the organic partition coefficient of octanol/water; φS of is the content of organic carbon of the sediment, kg/L. The migration coefficient of the environmental media constitutes of the following aspects: migration of contaminants in various media, degradation of pollutants in various media, and the input and output of pollutants along withthe environmental media [1]. The calculation of the migration coefficient between the media in themodel are illustrated in Table 2.Rainfall dissolved Dry and wet deposition Volatilize Adsorption Spread Settlement Spread Settlement Spread Resuspension Resuspension Note:KVA:air side mass transfer coefficienton air-water interface, m / h; KVW: water side mass

transfer coefficient on air-water interface, m / h; AW:amount of contacting area between water and air, m2; KR: the mass transfer coefficient during the rain dissolution process, setting at1.6×10-5m/h; KQS: the deposition rate coefficients of dry and wet matter, setting at6.0×10-10m/h[1]; VSS ： volume of the suspension, m3; tWSS: half diffusion time of the water-suspension, h; KWBS: mass transfer coefficient between the sediment and water, m/h; KS: coefficient of sedimentation suspension rate, setting at5.0×10-7m/h [20]; AS: amount of contacting area betweensediment and water, m2; KSR: coefficient of suspension resuspending rate, setting at 2.0 × 107m / h [21].

RESULTS Results generated by the model. According to equation (1), the concentration of chlorobenzene after reaching the balance in air, water, suspended solids and sediments were 1.448×103433

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mg/m3(calculated by dry mass, the same below), 9.503×10-5 mg/L, 3.043×10-6g/kg and 1.270×10-5 g/kg, respectively. By calculating the total mass of chlorobenzene in air, water, suspended solids and sediments, the percentage of the chlorobenzene in eachphase were obtained as follows: the amount of chlorobenzene in the air took 94.931% of the total amount, while there was only 5.069% of the total amount takenby other environmental phases.Thus, it can be explained that majority of the chlorobenzene was evaporated into the air, and only a small amount of it was left in the water. Meanwhile,the amount of chlorobenzenein the aqueous phase was distributed as follows:98.362% in water, 0.020% insuspended solids and 1.618% in sediment, indicating that vast majority of the chlorobenzene in the aqueous phase existed in water, very little amount was left in the sediment and suspended solids.


2

Concentration/(mg· L-1)

simulation test, the surface sediments atthe bottom of the device were sampled to test the w(chlorobenzene).The changes of ρ (chlorophenyl)along withthe time are shown in Figure 3.

Model Validation. The simulation test device is shown in Figure 2.The device is an annular container witheffective volume of 16 L, equipped with a stirrer in the apparatus, and water in the container can circulate at certain speed.A125W high pressure mercury lampand a fixed speed fanare mounted above the device.Also, at the bottom of the device, there isnatural dried sediment (the sediments sampled from Shaokou Section and Songhuajiangcun Section, naturally dried, and mixed with the mass ratio of 1:1), being evenly added, and then the configured chlorobenzene-river water solution was added. After all the parts being set up, the analog of the dismiss process of chlorobenzene in the water of the Songhua River was carried out.

0

20

40

60

80

100

120

Time/h FIGURE 3 The distributionof chlorobenzene concentration in water environmentduring simulation process

R170 mm 100 mm R70 mm 310 mm 340 mm

6.0 5.5 5.0 4.5 4.0 3.5 3.0 2.5 2.0 1.5 1.0 0.5 0.0 -0.5

140 mm

FIGURE 2 The simulator of chlorobenzene subtractive process

Figure 3 shows that ρ(chlorobenzene) in the water decreased with the increase of simulation time.After 104h, the ρ(chlorobenzene) in water decreased from 4.956 mg / L to 7.1 × 10-3mg / L, and the w (chlorobenzene ) in sediment was 1.1 mg / kg (counted by dry mass). At the same time, the mass of chlorobenzene in water accounted for1.433% of the total mass of that added into the device, whereas the amount of chlorobenzene in sediments accounted for 0.028% of the total mass of that added into the device.So, the results basicallymatched with the predicted results generated by the fugacity model(4.986% in water, 0.082% in sediment). Therefore, both the simulation experiments and model predictions show that the chlorobenzene that entered in watercould quickly migrate or convert, and there are very small amount of residual left in water and sediment, causinglimited its impact on the water environment. Parameter Sensitivity Analysis. In order to improve the stability and accuracy of the model, the qualitative analysis of the sensitivity of the parameters in the model were carried out in this study. The Sensitivity of the model (S) was calculated by using the equation below [22-23].

Both the ambient temperature and water temperature of the simulation test werecarried out at 20 ~ 30℃. The test on the ρ(chlorobenzene) in the water sampledat certain time intervals was employed, and it was accompanied by thecomplement ofthe reduced water caused byevaporation and other reasons.After 104 h of

S

Y1.01  Y1.0  / Y1.0  X 1.01  X 1.0  / X 1.0

Where: X1.01represents an increase of the input parameters to 101% of the original value;. 3434

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Sensitivity Value Added

14 12

Air Water SPMs Sediment

10 8 6 4 2

φs

ρs

Ks

As

Kp

Q2

L

t

φss

ρss

Vw

H

Ei

logKow

0

Parameter

Note: KOW is the octanol-water partition coefficient; H is water depth; VW is water volume; ρSS is the density ofsuspended solids; φSSis the content of organic carbon in suspended solids; t is the simulation time; L is the water body length; KPis the photolysis rate of chlorobenzene; ASis the amount of water-air contactarea inthe study area; KSis coefficient of suspended mattersedimentation rate; ρSis sediment density; φSisorganic carbon content of the sediment; FIGURE 4 The sensitivity coefficients of main parameters in the model

X1.0represents the original value of the parameter; Y1.01, Y1.0represents theoutput results of the model when the parameter value wereX1.01 and X1.0, respectively. The sensitivity of all the environmental parameters and other input parameters were calculated, and the sensitivities of each parameter corresponding to different environmental phaseswere added up [24]. The results were shown in Figure 3 It can be seen in Figure 3 thata number of parameters has great impact on the sensitivity of the model, such as lgKow, Q1, H, VW, ρSS, φSS, t, L, Q2, KP, AS, KS, ρS, φS, etc. KOW has a major impact on the distribution of chlorobenzenein water and air, mainly displayedin the volatile process of chlorobenzene.In addition, there is big influence on the distribution of chlorobenzene in each environmentalphasecaused by the amount of emissions,H, VW, ρSS and φSS etc. Thus, it is highly important to improve the measuremen taccuracy of these parameters to ensure the accuracy of the simulation results.

water in summer time. By the calculation generated by the model, the chlorobenzenewas discharged into the Songhua River from the sources at the rate of 20 mol / h. After the equilibrium of the system, ρ (chlorine benzene) in the atmospheric phase is 1.448×10-2 mg/m3, ρ (chlorobenzene) in the aqueous phase was 9.503×10-5 mg/L, w (chlorobenzene) in suspended solids was 3.043×106 g/kg, and w (chlorobenzene) in sediment was 1.270×10-5 g/kg. By calculation through the model:the amount of chlorobenzene in the air accounted for94.931% of the total input amount, while there was only 5.069% of the total amount was taken in water phases. Thus, it is conclude that majority of the chlorobenzene was evaporated to the air, and only a small amount of it was left in the water. Meanwhile, the amount of chlorobenzene in the aqueous environment was distributed as follows:98.362% in water, 0.020% insuspended solids and 1.618% in sediment, indicating that the vast majority of the chlorobenzene in the aqueous environment existed in water, very little amount was left in the sediment and suspended solids.Simulation results suggestthat themass of chlorobenzene in water account for 1.433% of the total mass of that added into the device, and the amount of chlorobenzene in sediments account for 0.028% of the total mass of that added into the

DISCUSSION AND CONCLUSIONS This model is customized to the simulation of the high temperature and high flowSonghua River 3435

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device. And the results basically matched with the predicted results generated by the fugacity model. By the sensitivityanalysis on each of the parameters of the model, it can be seen that a couple of parameters could significantly affect the distribution of chlorobenzene in all environmental phases. For instance,the octanol - water partition coefficient parameters, the amount of pollutant emission, water depth etc.hold a great impact on the model as well.


[8]

[9]

ACKNOWLEDGEMENTS The research work was financially supported by National Major Science and Technology Program for Water Pollution Control and Treatment (Grant no. 2014ZX07502-002).

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Received: Accepted:

17.08.2015 10.05.2016

CORRESPONDING AUTHOR Meng Fansheng State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing, China e-mail: [email protected]

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