Removal efficiency and migration characteristics of naphthalene in bioretention facilities: the influences of particulate matter

1. Introduction

With the significant increase area of impervious surfaces in cities, a large amount of pollutants accumulate on the surface of road (Shrestha et al. 2018, Zhang et al. 2020). These pollutants could enter into urban water environment by runoff, which may lead to the degradation of water quality and potential health risks for humans (Esfandiar et al. 2021). Bioretention facilities, one of the most popular stormwater runoff treatment facilities, which can effectively reduce runoff flow and improve runoff quality (Jiang et al. 2019, Mai et al. 2020). Bioretention facilities remove pollutants mainly through such as media adsorption, plant uptake, biodegradation, filtration and volatilization (Davis et al. 2009). Studies have shown that bioretention facilities can effectively remove various pollutants in runoff, such as total nitrogen (32 ~ 61%), total phosphorus (45 ~ 94%), heavy metals (27 ~ 100%) and organic matter (54% ~ 100%) (Biswal et al. 2022).

Polycyclic aromatic hydrocarbons (PAHs), an important kind of pollutants in runoff, mainly originate from asphalt roads and frictional losses by vehicle tires (Leroy et al. 2015). With highly carcinogenic, teratogenic and mutagenic, PAHs could pose a higher environmental risk once accumulated (Sheng et al. 2021). PAHs have been classified as one kind of persistent organic pollutants by the United Nations Environment Programme (UNEP), which should be managed and controlled (Hou et al. 2013, Yang et al. 2021). However, the large amount of particulate matter (PM) generated by rainfall scouring process has a strong adsorption effect on PAHs are strongly adsorbed in the runoff, so PAHs are mainly present in the particulate form (Grant et al. 2015). Therefore, PM is an important carrier for the migration and diffusion of PAHs in runoff (Li et al. 2016). The effective removal of PM in runoff is also the main control method for PAHs elimination. The characteristics of PM (concentration, particle size) affects the removal and distribution of PAHs greatly in runoff (Aryal et al. 2006). Since the small particle size has large specific surface area, which would contain a greater concentration of PAHs (Gunawardana et al. 2015, Zhao et al. 2016). In addition, small particle size particles in runoff are more likely to carry PAHs for migration (Aryal et al. 2009, Yi et al. 2012). Similarly, the correlation between PAHs and PM can occur in bioretention facilities.

However, most of the current studies have focused on the individual removal of PAHs and PM by bioretention facilities. Studies showed that bioretention facility can effectively remove PAHs in runoff, which was mainly accumulated at the top of 10 ~ 40 cm (Hong et al. 2006, Napier et al. 2009, Tedoldi et al. 2016). LeFevre et al. studied the overall naphthalene removal efficacy of 78% ~ 93% for laboratory-scale bioretention facilities (Lefevre et al. 2012). Boving et al. investigated the effect of facilities on PAHs removal under different design conditions in a field experiment, and the results showed that the average removal rate of dissolved-phase PAHs could reach 67%, which was positively correlated with the amount of filter media (Boving et al. 2007). In addition, bioretention facilities are also effective in removing PM and more pronounced interception at the top, with an efficiency of 90% (Vijayaraghavan et al. 2021). The ability of bioretention facilities to remove PM generally increased with particle size decreased (Grant et al. 2015). A growing body of literature has shown that bioretention facilities are effective PAHs treatment devices, with good removal capacities for PM (Shrestha et al. 2018).

However, DiBlasi et al. found that the same correlation between PAHs and PM occurred in bioretention facilities, with a positive correlation for their removal efficiency (Diblasi et al. 2009). Additionally, despite bioretention facilities have been found to have a positive correlation between the removal efficiency of PAHs and PM, but we need more quantitative data to determine the effect of PM on removal efficiency and migration characteristics. Since PM properties significantly affect the amount and migration distance of PAHs in runoff, so it may also affect the removal and migration processes of PAHs at bioretention facilities. However, little is known about the effect of PM on the removal of PAHs from bioretention facilities. Besides, the differences in rainfall intensity may lead to highly variable particulate concentrations and particle sizes in runoff (Wang et al. 2017), so exploring PM properties is important for gaining insight into the input and output loads and migration mechanisms of PAHs at bioretention facilities.

In this study, naphthalene was selected as the target pollutant to investigate the removal efficiency and migration characteristics in bioretention facilities under the influences of PM. The removal efficiency and migration characteristics of each layer on naphthalene were investigated and the factor of influent concentrations, rainfall return period and antecedent drying period were selected. In addition, the influences of PM concentration and particle size on the removal behavior of naphthalene in bioretention facilities were investigated. Finally, the occurrence characteristics of naphthalene in each layer of bioretention facility under different particle size was analyzed. This study provided guidelines for runoff pollution control, optimization of stormwater facilities, and risk assessment of PAHs in runoff.

2. Materials And Methods

2.1 Experimental device

The experimental device of bioretention facilities is shown in Fig. 1. The diameter of each facility was 10 cm, the height was 75 cm, and each facility had 50 cm media depth. As shown in Fig. 1(a), the device was consists of a 20 cm overburden layer with sand : oil ratio of 8:2, followed by 20 cm zeolite layer and 10 cm gravel layer at the bottom. Figure 1(b) showed that nine sampling sites were set up along the left side of the bioretention facility, where the media of internal layers were taken out. Figure 1(c) showed that four water intake sites were set up along the right side of the bioretention facility, for taking interstitial water from each layer. According to the climatic conditions of the experimental site, Sedum was selected, which are resistant to drought-tolerance, anti-pollution ability and rich in roots.

2.2 Simulated runoff

According to Beijing's rainfall intensity formula (DB11T 969–2013), a simulated rainfall test was conducted. The rain intensity was calculated as follows.

Where, q represents rainfall intensity (L/s·hm^-2); P represents rainfall return period (a); t represents rainfall duration (min);

The PM used in this study are all from the street dust on the campus of Beijing University of Civil Engineering and Architecture in Daxing District, Beijing. The PM were collected by vacuum sweeper, the impurities such as plant debris are sieved before used.

2.3 Experimental design

A total of 15 bioretention columns were built for this experiment. PM was added to simulated stormwater to investigate the removal efficiency and migration characteristic of naphthalene by bioretention facility. Different stormwater factors were selected, such as initial pollution concentrations (1, 2 and 5 mg/L), rainfall return period (0.5, 1 and 2 a), antecedent drying period (2, 5 and 8 d). In addition, the influences of particulate matter properties such as particle size (0 ~ 45, 45 ~ 75 and 75 ~ 150 µm) and concentration (100, 300 and 500 mg/L) were also investigated. Finally, the occurrence of naphthalene onto media in bioretention facility caused by particle size was examined.

In this experiment, a peristaltic pump was used to add runoff to bioretention facility for 120 min continuously. The water samples were taken out at the different time points at 5, 10, 15, 20, 30, 60 and 120 min on the right side of the bioretention facility. The media was taken out at the different sampling sites with 2, 4, 6, 8, 10, 15, 20, 40 and 50 cm depth along the left side of the bioretention facility. The concentration of naphthalene on the selected media were tested.

2.4 Methods of pretreatment and detection

The water samples were filtered through 0.22 µm membrane. The selected media was firstly freeze-dried by lyophilizer. Then 1 g media and 10 mL 1:1 acetone-hexane solution (V: V) was added into brown bottle. Naphthalene was extracted from the media using hexane sonication for 3 times with 30 min each (Lefevre et al. 2012) ^[22]. Finally, the mixture solution was filtered by 0.22 µm filter membrane and the concentration of naphthalene was examined. The concentration of naphthalene was measured by ultra performance liquid chromatography (UPLC) with the mobile phases of acetonitrile (80%) and water (20%) and the injection volume was 1 µL.

3. Results And Discussion

3.1 Effect of different stormwater factors

3.1.1 Effect of influent naphthalene concentration

With the influences of PM, the effect of influent concentrations on the removal of naphthalene by each layer in bioretention facilities were investigated, and the results were shown in Fig. 2. As shown in Fig. 2 (a), when the influent concentration was 1 mg/L, 2 mg/L and 5 mg/L, the average removal efficiency of naphthalene by the bioretention facility was 78%, 83% and 91%, respectively. The bioretention facility can effectively remove naphthalene from runoff, which may be attributed to high affinity between naphthalene and media in bioretention facility. This result was similar to the adsorption of PAHs onto biochar, where the greater influent concentration, the more effective removal of PAHs (Wang et al. 2017). The mainly removal mechanism of naphthalene in bioretention facilities was adsorption (Mehmood et al. 2021). With a large adsorption capacity, the internal media could show high removal efficiency for naphthalene. When the influent concentration was 1 mg/L, the average removal efficiency of naphthalene at 10 cm, 20 cm, 40 cm and 50 cm depth was 66%, 72%, 74% and 78%, respectively. Besides, the naphthalene removal efficiency at the first 20 cm media was about 90% for overall bioretention facility, indicating that the sandy layer was the main removal layer. The phenomenon was similar to the results of Wang's (Wang et al. 2016). Compared with zeolite and gravel, the top layer showed stronger effect on naphthalene removal, which due to the smaller particle size and more adsorption sites. However, when the influent concentration increased to 5 mg/L, the average removal efficiency increased to 73%, 80%, 88% and 91% at 10 cm, 20 cm, 40 cm and 50 cm depth, respectively. Compared with 1 mg/L influent concentration of naphthalene, the removal efficiency of each layer increased about 7%, 8%, 14% and 13%, respectively. With the higher influent concentration, the adsorption of naphthalene in zeolite and gravel layers increased, which lead to the more effective removal and adaptable for various concentration of naphthalene in bioretention facility.

As shown in Fig. 2(b), the naphthalene concentration of bottom layer in bioretention facility increased significantly with the contact time increased. When the influent concentration of naphthalene was 1 mg/L, with the contact time increased from 5 min to 120 min, the effluent concentration of naphthalene at bottom increased from 0.16 mg/L to 0.29 mg/L. With the adsorption of naphthalene gradually saturated, the migration of naphthalene in bioretention facility was significantly enhanced. In addition, the naphthalene concentration in the effluent gradually decreased with the depth increased was shown in Fig. 2(a). When the influent concentration of naphthalene was 1 mg/L, the contact time was 120 min, the average effluent concentrations were 0.41 mg/L, 0.39 mg/L, 0.32 mg/L and 0.29 mg/L at 10 cm, 20 cm, 40 cm and 50 cm depth in bioretention facility, respectively. Similarly, the influent concentration of naphthalene increased to 5 mg/L, the effluent concentration became 1.72 mg/L, 1.50 mg/L, 1.06 mg/L and 0.83 mg/L, respectively. All the results indicated that the different layers had certain removal efficiency for naphthalene, which may be attributed the hydrophobic characteristics (Sheng et al. 2021). As the influent concentration increased, the effluent naphthalene concentration also increased significantly with the same layer, indicating the more migratory in bioretention facility.

3.1.2 Effect of rainfall return periods

Figure 3 showed the effect of rainfall return periods on the removal of naphthalene by each layer in bioretention facilities under the influences of PM. As shown in Fig. 3. (a), the variation of rainfall return period had a great influences on the removal efficiency and migration of naphthalene in bioretention facilities. When the rainfall return period was 0.5 a, the average effluent concentration of naphthalene was 0.62 mg/L, 0.37 mg/L, 0.23 mg/L and 0.18 mg/L at 10 cm, 20 cm, 40 cm and 50 cm depth in bioretention facility, and the corresponding removal efficiency was 69%, 82%, 89% and 91%, respectively. When the rainfall return period increased to 2 a, the corresponding removal efficiency was 59%, 65%, 71% and 74% and reduced by 10%, 15%, 19% and 18%, respectively. The greater the rainfall return period, the higher flow rate and the flushing effect of water flow on the media, with lower removal efficiency of each layer (Luo et al. 2013). Yang et al simulated artificial rainfall experiments, showing that the bioretention facilities were less effective in treating pollutants under high-intensity rainfall conditions (Yang et al. 2021). As shown in Fig. 4. (b), with the contact time of 120min, the bottom effluent concentration increased from 0.28 mg/L to 0.70 mg/L when the rainfall return period increased from 0.5to 2 a. The results showed that the increase in rainfall return period clearly enhanced the migration of naphthalene in bioretention facility. Due to the greater rainfall return period, the greater the inflow naphthalene pollution load. As a result, the media approached saturation easier and the mobility was greatly enhanced.

3.1.3 Effect of antecedent drying period

The effect of antecedent drying periods on the removal of naphthalene by each layer in bioretention facilities under the influences of PM were found as Fig. 4 shown. As shown in Fig. 4. (a), antecedent drying periods influenced the removal efficiency and effluent concentration of naphthalene in bioretention facilities greatly. When the antecedent drying periods were 2, 5 and 8 d, the average effluent concentrations were 0.42 mg/L, 0.34 mg/L and 0.29 mg/L, the corresponding removal efficiency was 79%, 83% and 86%, respectively. With the relatively dryer of internal layers, bioretention facilities showed higher removal efficiency for naphthalene. Furthermore, some studies have shown that the hydrophobic microorganisms grew better in proper drying and had a good removal efficiency on hydrophobic organic matter (Liu et al. 2020). Besides, with the antecedent drying period increased from 2 d to 8 d, the removal efficiency at 10 cm, 20 cm and 40 cm accounted for the total removal efficiency changed from 81%, 90% and 97–87%, 91% and 95%. The removal efficiency of naphthalene significantly increased at the top 10 cm, which may be attributed to the relatively drier condition caused by easier connected with outside environment. Besides, as shown in Fig. 4. (b), when the antecedent drying period was 2, 5 and 8 d, the contact time increased from 5 min to 120 min, the effluent concentrations of naphthalene increased from 0.29 mg/L, 0.25 mg/L and 0.18 mg/L to 0.50 mg/L, 0.44 mg/L and 0.37 mg/L, with an increase of 0.21 mg/L, 0.19mg/L and 0.19 mg/L, respectively. With the shorter the drying period, the higher the water content inside the bioretention facility and the easier it is for naphthalene to migrate.

3.2 Effect of particulate properties

3.2.1 Effect of particle size

The removal efficiency and effluent concentration of naphthalene under different particle sizes were shown in Fig. 5. As shown in Fig. 5. (a), the addition of PM with different particle sizes can improve the removal efficiency of naphthalene in bioretention facility. With the particle size of 0, 0 ~ 45, 45 ~ 75 and 75 ~ 150 µm at 50 cm depth, the average removal efficiencies for naphthalene were 81%, 92%, 84% and 87%, respectively. On the one hand, most of PM were trapped in bioretention facility, the adsorbed naphthalene onto PM was removed at the same time. On the other hand, the trapped PM can act as media for naphthalene adsorption and improving the removal efficiency further. Besides, when the particle size was 0 ~ 45 and 75 ~ 150 µm, the average removal efficiency decreased from 74%, 81%, 90% and 92–66%, 74%, 82% and 85% at 10 cm, 20 cm, 40 cm and 50 cm depth in bioretention facility. The similar decreasing phenomenon on removal efficiency with the increase of particle size was also found in Shen's study (Shen et al. 2021). In addition, the removal efficiency of naphthalene in the top 10cm reached a satisfactory level under the influences of 0 ~ 45µm particles. Small particle size with high specific surface area could carry more naphthalene and promote the adsorption of naphthalene by the media at the same time, showing a high removal efficiency (Li et al. 2006, Yi et al. 2012).

Besides, as indicated in the Fig. 5. (a), the average removal efficiency of naphthalene gradually increased with the increase on depth. The removal efficiency of naphthalene at 10 cm depth accounted for 73%, 81%, 78%, and 77% of the overall removal efficiency when the particle sizes was 0, 0 ~ 45, 45 ~ 75, and 75 ~ 150 µm. Therefore, the main removal layer of naphthalene in bioretention facilities was the top layer. Xiong et al. also obtained that the removal of heavy metals by bioretention facility mainly occurred at upper layers (Xiong et al. 2021).Compared with zeolite and gravel at bottom, the sandy layer at top would offer lower porosity and resulted in a large amount of PM and naphthalene retained (Hatt et al. 2009). In addition, due to the trapped PM at top, the removal efficiency of naphthalene at 10 cm depth further improved which may be attributed to the decreased porosity and increased residence time.

As shown in Fig. 5. (b), the difference of effluent concentration with time at different particle sizes was obvious. When particle sizes of PM were 0, 0 ~ 45, 45 ~ 75, and 75 ~ 150 µm in runoff, with the contact time increased from 5 min to 120 min, the effluent concentration of naphthalene increased from 0.28 mg/L, 0.08 mg/L, 0.16 mg/L and 0.20 mg/L to 0.56 mg/L, 0.29 mg/L, 0.38 mg/L and 0.45 mg/L. With the increase of time, the adsorption sites of naphthalene by the media gradually decreased, so the migration gradually increased. The final effluent concentration of naphthalene was low under the influences of PM, indicating that PM was beneficial to reduce the migration of naphthalene in bioretention facilities. Besides, the effluent concentration of naphthalene increased by 0.28 mg/L, 0.21 mg/L, 0.22 mg/L and 0.25 mg/L when particle sizes of PM were 0, 0 ~ 45, 45 ~ 75, and 75 ~ 150 µm in runoff, respectively. Due to the stronger carrying capacity of PM with small particle size, they could greater share the adsorption pressure of naphthalene by the media, so the migration was worse.

3.2.2. Effect of PM concentration

Figure 6 showed the removal efficiency and migration of naphthalene under the influences of different PM concentrations of each layer in bioretention facilities. As can be seen in Fig. 6. (a), it is possible to note that naphthalene removal performance of each layer under the influences of different PM concentrations was better than without PM in bioretention facility. When PM with concentrations of 0, 100, 300, and 500 mg/L, the average effluent concentrations of naphthalene were 0.37 mg/L, 0.32mg/L, 0.28 mg/L, 0.21 mg/L, and the corresponding removal efficiency was 82%, 84%, 86%, and 90%, respectively. The higher the concentration of PM, the higher the efficiency for naphthalene removal and the worse the mobility in bioretention facility, which is similar to Li's research results (Li et al. 2013). Besides, under four different concentrations of PM, each layer had a satisfactory removal effect on naphthalene, more than 60% removal efficiency could be achieved, especially in the influences of 500 mg/L PM could stably keep above 70% removal efficiency. Due to the strong retention of PM at the top, the higher the concentration of PM in runoff, the greater amount of PM and naphthalene was retained at the top. The porosity decreased and the adsorption of naphthalene onto the media increased, so the removal efficiency increased further.

Besides, when there was no PM in runoff, the removal efficiency of naphthalene was 59%, 67%, 77% and 81% at 10 cm, 20 cm, 40 cm and 50 cm depth, respectively. However, when the PM concentration was 500 mg/L, the removal efficiency increased by 11%, 10%, 7% and 6% at 10 cm, 20 cm, 40 cm and 50 cm depth, respectively. The addition of PM had a decreasing effect on the removal efficiency of each media layer from the top to bottom. Compared to the zeolite and gravel at the bottom, the top media was sandy soil, which had a smaller particle size. Therefore, the adsorption and interception of naphthalene by the media in the biretention facility decreased from top to bottom. Besides, a large number of PM were trapped at the top, leading to a further decrease in porosity, so the removal efficiency of naphthalene from the top media was obviously improved.

As can be seen in Fig. 6. (b), unlike the effluent concentration without PM, lower effluent concentration of naphthalene was observed when the PM concentration was 100, 300, and 500 mg/L, respectively. When there was no PM in runoff, the contact time increased from 5 min to 120 min, and effluent concentration of naphthalene increased from 0.28 to 0.56 mg/L. Similarly, when the concentration of PM in runoff was 500mg/L, the effluent concentration of naphthalene increased from 0.07 mg/L to 0.40 mg/L. As can be seen from the final effluent concentration, the migration of naphthalene could be effectively inhibited under the influences of 500 mg/L PM. Besides, the first 30 min of contact increased the effluent concentration by 0.15 mg/L, 0.15 mg/L, 0.14 mg/L and 0.12 mg/L when PM with concentrations of 0, 100, 300 and 500 mg/L, respectively. However, the latter 90 min of contact increased by 0.13 mg/L, 0.12 mg/L, 0.12 mg/L and 0.10 mg/L. The effluent concentration changed relatively faster in the first 30 min, which indicated that the migration of naphthalene was enhanced faster and the migration rate was larger. Some studies have shown that naphthalene with strong hydrophobicity had a higher adsorption affinity with hydrophobic groups on the media surface (Degenkolb et al. 2018). Consequently, the faster the adsorption removal process on the internal media over a shorter period of time, thus the faster migration rate. With the contact time increased, the internal media tend to saturate at a slower rate. In addition, the greater the concentration of PM in runoff, with the lower the migration rate. This is because under the influence of high concentration of PM, the absorption of media enhanced for naphthalene, with a low mobility.

3.3 The occurrence of naphthalene onto the media

The effect of particle size on the amount of naphthalene adsorbed onto the media was investigated, and the results were shown in Fig. 7. With the increase depth of bioretention facility, the adsorption of naphthalene by the media first increased and then gradually decreased. The maximum adsorption occurred at the first 10 cm, which is similar to the results of Degenkolb's study (Degenkolb et al. 2018). Compared with the bottom, bioretention facilities had a great potential to intercept pollution at the top (Tedoldi et al. 2017). However, due to the highly volatile characteristic, the content of naphthalene at the top of bioretention facilities was relative low (Akdeniz et al. 2021). Therefore, the adsorption amount of naphthalene showed the trend of first increasing and then gradually decreasing. In addition, bioretention facilities had plants on the top, which absorbed naphthalene in a natural way, and showed an impact on the adsorption amount of naphthalene at the top media (Mehmood et al. 2021). The addition of PM significantly changed the adsorption behavior of naphthalene in each layer. Due to the strong retention capacity of PM and naphthalene at the top, the adsorption capacity increased at the first 10 cm and decreased at the bottom 40 ~ 50 cm media. Moreover, PM can effectively inhibit the migration of naphthalene in bioretention facilities, which is similar to the results of Schwientek (Schwientek et al. 2013). With the particle sizes were 0, 0 ~ 45, 45 ~ 75 and 75 ~ 150 µm, the maximum adsorption capacity were 0.58 mg/kg, 0.71 mg/kg, 0.69 mg/kg and 0.68 mg/kg, respectively. The corresponding position was 8 cm, 6 cm, 4 cm and 4 cm depth and shifted upward by 2 cm, 4 cm and 4 cm under the influences of different particle sizes, respectively. With the same concentration of PM, the smaller size PM could carry more naphthalene and were more easily retained by the top media of bioretention facilities, which result in the higher adsorption. Besides, compared with sand at top layer, the bottom layer of bioretention facilities was zeolite and gravel layer, which showed a larger particle size and weak retention for naphthalene and PM.

Figure 8 represented the solid-liquid partition coefficient (K) of naphthalene in each layer of bioretention facility under the different particle sizes. The value of K decreased with the increasing depth, indicating that the mobility of naphthalene in bioretention facility gradually increased with depth. As shown in Fig. 8, the addition of PM increased the K values of naphthalene in all layers. It showed that the PM inhibited the migration of naphthalene, reducing the risk of pollution in runoff. The K value of naphthalene was 1.17 and 0.32 at 10 cm and 50 cm depth with the particles size of f 0 ~ 45 µm. Compared to zeolite and gravel layers at 40 cm and 50 cm, sandy layer at 10 cm was the main adsorption and retention layer of naphthalene. Moreover, the K values decreased with increasing particle size in all three selected ranged. The K values were 1.17, 0.87 and 0.79 at 10 cm depth when the particle sizes were 0 ~ 45 µm, 45 ~ 75 µm and 75 ~ 150 µm, respectively. Due to the strong carrying and retention capacity of PM, it would distribute more naphthalene onto the media, especially under the influences of smaller particle size, which had the largest K value.

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