Role of Design and Operational Factors in the Removal of Pharmaceuticals by Constructed Wetlands
Abstract
:1. Introduction
2. Methods
3. Results and Discussion
3.1. Removal Mechanisms in CWs for PhCs Removal
3.2. Role of Design and Operational Factors of CWs in the Removal of PhCs
3.2.1. Depth
3.2.2. Area
3.2.3. HLR
3.2.4. OLR
3.2.5. HRT
3.3. Role of Physicochemical Parameters of CWs in the Removal of PhCs
3.3.1. pH
3.3.2. Temperature
3.3.3. Effluent DO
3.4. Role of Plants and Support Matrix of CWs in the Removal of PhCs
3.4.1. Role of Plants
3.4.2. Role of Support Matrix
3.5. Effect of Seasonality on the Removal of PhCs
4. Conclusions
- Area, depth, HLR, HRT, and OLR play an important role, although with variable influence, in wetland performance for the removal of PhCs. Depth and OLR showed a significant correlation with the removal efficiency of seven of the studied PhCs, whereas the other three factors, area, HLR, and HRT, were significantly correlated with the removal efficiency of six of the studied PhCs. However, the correlation was not significant with the removal efficiency of the same PhCs, which indicates that the removal of PhCs in CWs might not only relate to one design and operational parameter; all the parameters might directly or indirectly impact their removal. For instance, the removal efficiency of some PhCs showed a significant correlation with three factors such as diclofenac and ketoprofen (depth, area, and HRT), salicylic acid and erythromycin (area, HLR, and OLR), and gemfibrozil (depth, OLR, and HRT). The removal efficiency of some PhCs showed a significant correlation with two of the studied factors such as sulfamethazine (depth and HRT), lincomycin (area and OLR), trimethoprim (HLR and OLR), and oxytetracycline (area and HLR).
- Effluent DO, temperature, and pH play an important role in the removal of PhCs but to different extents. The correlation of these parameters was not significant with the removal efficiency of the same PhCs, which indicates the direct or indirect effect of all the physicochemical parameters on their removal. The significant correlation of effluent DO and temperature with the removal efficiency of most of the studied PhCs (eight and seven, respectively) represents the importance of DO and temperature for the enhancement of microbial processes, which contribute more in their removal. For instance, the removal efficiency of naproxen, diclofenac, ketoprofen, salicylic acid, and lincomycin showed a significant correlation with temperature and effluent DO. The pH can be considered an important parameter because it controls several biotic processes such as plant development, nitrification, and heterotrophic production, as well as abiotic processes such as the attachment of ionizable PhCs to soil/sediment via ion exchange. In CWs, the presence of plants influences the performance by regulating the pH (~7.5), which is the optimal value of pH to control these processes. Nevertheless, the pH directly showed a significant correlation with the removal efficiency of six of the studied PhCs (ketoprofen, erythromycin, lincomycin, ofloxacin, sulfamethazine, and gemfibrozil), which are mainly removed by aerobic biodegradation (erythromycin, lincomycin, sulfamethazine, and gemfibrozil), anaerobic biodegradation (ketoprofen and ofloxacin), adsorption (erythromycin and ofloxacin), and plant uptake (sulfamethazine).
- Plants contribute significantly to the removal of some PhCs by direct uptake (oxytetracycline, sulfamethazine, caffeine, carbamazepine, and venlafaxine). In addition to direct uptake, the other positive effects of plants such as degradation by enzymatic exudates, as well as release of root exudates (such as carbohydrates and amino acids) and oxygen by the plant roots in the rhizosphere, are suitable for aerobic biodegradation, which also enhances the removal efficiency of PhCs in planted CWs compared with unplanted CWs. Aerobic biodegradation was demonstrated as one of the major removal mechanisms of most of the PhCs (15 out of 26).
- The use of substrate material of high adsorption capacity and rich in organic matter enhances the removal efficiency of PhCs by adsorption onto the substrate and sorption by organic surfaces, as these are the major removal mechanisms of most of the examined PhCs (codeine, clarithromycin, erythromycin, ofloxacin, oxytetracycline, carbamazepine, and atenolol) in CWs owing to their physicochemical properties. Additionally, the use of substrate media that could provide a larger available surface area for microbial growth and higher oxygen to promote the elimination of PhCs, which are mainly removed via aerobic biodegradation pathways, is suggested for the enhanced removal of a variety of PhCs by CWs.
- The removal efficiency of PhCs in CWs was comparatively higher in summer compared with winter due to the difference in external temperature, which directly affects water temperature and oxygen solubility, while playing a major role in the removal processes of PhCs such as biodegradation, plant uptake, and photodegradation at warm temperature, and adsorption/sorption processes at low temperature. Although the removal efficiency of almost all of the studied PhCs showed seasonal differences, statistical significance was established in the removal of naproxen, salicylic acid, caffeine, and sulfadiazine. These PhCs are removed better in summer compared with winter, since the major processes contributing to their removal such as biodegradation (naproxen, salicylic acid, caffeine, and sulfadiazine), plant uptake (caffeine), and photodegradation (naproxen) are enhanced in summer.
Supplementary Materials
Author Contributions
Funding
Conflicts of Interest
References
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Design, Operational, and Physicochemical Parameters | References |
---|---|
Operational Factors | |
Hydraulic loading rate (HLR) | Matamoros et al. [20]; Zhang et al. [21]; Dan et al. [22]; Ávila et al. [23]; Sharif et al. [24] |
Hydraulic retention time (HRT) | Conkle et al. [25]; Matamoros et al. [26]; Zhang et al. [13,27]; Matamoros and Salvadó [14]; Dordio and Carvalho [28]; Verlicchi et al. [29]; Herrera-Cárdenas et al. [30]; Auvinen et al. [31]; Vymazal et al. [19]; Salcedo et al. [32] |
Physicochemical Parameters | |
pH | Hijosa-Valsero et al. [16]; Carvalho et al. [33]; Zhang et al. [34] |
Temperature | Hijosa-Valsero et al. [16]; Ávila et al. [35]; Dan et al. [22]; Verlicchi et al. [29]; Matamoros et al. [36]; Vymazal et al. [19]; Nuel et al. [37]; Zhang et al. [34] |
Dissolved oxygen (DO) | Ávila et al. [35,38]; Chen et al. [17]; Auvinen et al. [31,39]; Kahl et al. [40]; Li et al. [41,42]; Vymazal et al. [19]; Zhang et al. [34]; Nivala et al. [43] |
Planted and Unplanted CWs | Dordio et al. [44]; Hijosa-Valsero et al. [15,16,45,46]; Xian et al. [47]; Zhang et al. [13,27]; Reyes-Contreras et al. [48]; Carvalho et al. [33]; Dan et al. [22]; Dordio and Carvalho [28]; Carranza-Diaz et al. [49]; Macci et al. [50]; Li et al. [41,51]; He et al. [52]; Salcedo et al. [32]; Zhang et al. [34]; Button et al. [53] |
Role of Support Matrix | Dordio et al. [44]; Dan et al. [22]; Dordio and Carvalho [28]; Ávila et al. [38]; Chen et al. [54]; Auvinen et al. [31]; Huang et al. [55]; Salcedo et al. [32]; Park et al. [56]; Nivala et al. [43] |
Effect of Seasonality (Summer/Winter) | Matamoros et al. [26,36]; Dordio et al. [44]; Hijosa-Valsero et al. [15,16]; Reyes-Contreras et al. [48]; Dan et al. [22]; Liu et al. [57]; Rühmland et al. [58]; Zhang et al. [34] |
Design, Operational, and Physicochemical Parameters | FWSCW | HFCW | VFCW | HCW |
---|---|---|---|---|
Number of CWs | 47 | 110 | 48 | 37 |
Number of studies | 17 | 32 | 17 | 20 |
Scale of application | Lab, pilot, full | Lab, pilot, full | Lab, pilot | Lab, pilot, full |
Type of treatment | Primary, secondary, tertiary | Primary, secondary, tertiary | Primary, secondary, tertiary | Secondary, tertiary |
Depth (m) | 0.7 ± 0.8 | 0.6 ± 0.2 | 0.7 ± 0.2 | 1.0 ± 0.7 |
Area (m2∙PE−1) | 10 ± 8 | 7.7 ± 5.3 | 4.3 ± 3.8 | 9.2 ± 6.2 |
HLR (m3∙m−2∙day−1) | 0.1 ± 0.1 | 0.4 ± 1.0 | 0.2 ± 0.1 | 0.1 ± 0.2 |
OLR (g COD∙m−2∙day−1) | 17 ± 25 | 25 ± 28 | 62 ± 102 | 21 ± 30 |
HRT (days) | 5.4 ± 7.1 | 4. 3 ± 4.7 | 5.7 ± 5.1 | 8 ± 14 |
pH | 7.1 ± 0.6 | 7.5 ± 0.6 | 7.2 ± 0.4 | 7.4 ± 0.4 |
Temperature (°C) | 16 ± 7 | 17 ± 7 | 19 ± 8 | 14 ± 6 |
Effluent DO (mg∙L−1) | 1.3 ± 2.2 | 1.8 ± 2.0 | 3.4 ± 3.0 | 2.4 ± 2.5 |
Therapeutic Class/Pharmaceutical | Possible Removal Mechanism | References | Most Dominant Removal Mechanism * |
---|---|---|---|
Analgesic/Anti-Inflammatory | |||
Diclofenac | Biodegradation (anaerobic) | Ávila et al. [38,59]; Hijosa-Valsero et al. [60]; Chen et al. [17]; Kahl et al. [40]; He et al. [52]; Zhang et al. [34]; Nivala et al. [43] | Photodegradation; biodegradation (aerobic) ** |
Biodegradation (aerobic) | Hijosa-Valsero et al. [15,16,60]; Ávila et al. [35,38]; Kahl et al. [40] | ||
Photodegradation | Matamoros et al. [26]; Matamoros and Salvadó [14]; Ávila et al. [23,61]; Rühmland et al. [58]; Chen et al. [17]; Francini et al. [62]; Zhang et al. [34] | ||
Plant uptake | Hijosa-Valsero et al. [15]; Zhang et al. [13,63] | ||
Ibuprofen | Biodegradation (aerobic) | Matamoros et al. [20,64]; Hijosa-Valsero et al. [15,65]; Ávila et al. [23,35,38,59,61]; Matamoros and Salvadó [14]; Li et al. [8]; Zhu and Chen [66]; Chen et al. [17]; Vymazal et al. [19]; Březinova et al. [67]; Zhang et al. [34]; Nivala et al. [43] | Biodegradation (aerobic) |
Sorption | Dordio et al. [44]; Dordio and Carvalho [28] | ||
Adsorption | Auvinen et al. [31] | ||
Photodegradation | Reyes-Contreras et al. [48]; Zhang et al. [10] | ||
Plant uptake | Hijosa-Valsero et al. [15]; Li et al. [51] | ||
Ketoprofen | Biodegradation | Hijosa-Valsero et al. [15]; Zhang et al. [27]; Chen et al. [17]; Francini et al. [62]; Zhang et al. [34] | Photodegradation |
Photodegradation | Matamoros et al. [26]; Matamoros and Salvadó [14]; Reyes-Contreras et al. [48]; Francini et al. [62]; Zhang et al. [34] | ||
Naproxen | Biodegradation (aerobic) | Matamoros et al. [20,68]; Hijosa-Valsero et al. [15]; Matamoros and Salvadó [14]; Zhang et al. [21]; Chen et al. [17]; He et al. [52]; Zhang et al. [34]; Nivala et al. [43] | Biodegradation (aerobic) **; photodegradation |
Biodegradation (anaerobic) | Matamoros et al. [68]; Ávila et al. [59]; Li et al. [8]; He et al. [52]; Nivala et al. [43] | ||
Photodegradation | Matamoros et al. [26]; Reyes-Contreras et al. [48]; Hijosa-Valsero et al. [46]; Zhang et al. [34] | ||
Plant uptake | Hijosa-Valsero et al. [15]; Zhang et al. [69]; He et al. [52] | ||
Salicylic acid | Biodegradation | Hijosa-Valsero et al. [15,16]; Reyes-Contreras et al. [48]; Zhang et al. [27] | Biodegradation (aerobic) ** |
Plant uptake | Hijosa-Valsero et al. [46] | ||
Analgesic | |||
Acetaminophen | Biodegradation (aerobic) | Ávila et al. [35,61]; Koottatep et al. [70]; Li et al. [42]; Vystavna et al. [71] | Biodegradation (aerobic) ** |
Biodegradation (anaerobic) | Chen et al. [17] | ||
Photodegradation | Ávila et al. [61]; Li et al. [42] | ||
Adsorption | Ávila et al. [61]; Koottatep et al. [70] | ||
Sorption | Chen et al. [17] | ||
Plant uptake | Li et al. [42] | ||
Codeine | Biodegradation (aerobic) | Rühmland et al. [58]; Petrie et al. [72] | Sorption; biodegradation (aerobic) |
Sorption | Petrie et al. [72] | ||
Tramadol | Biological transformation | Rühmland et al. [58]; Chen et al. [17]; Petrie et al. [72] | Biological transformation |
Antibiotic | |||
Clarithromycin | Biodegradation | Hijosa-Valsero et al. [45]; Berglund et al. [73] | Photodegradation; sorption |
Sorption | Hijosa-Valsero et al. [45]; Berglund et al. [73] | ||
Photodegradation | Hijosa-Valsero et al. [45]; Berglund et al. [73] | ||
Erythromycin | Biodegradation (aerobic) | Rühmland et al. [58]; Chen et al. [54] | Biodegradation (aerobic); adsorption |
Adsorption | Chen et al. [54] | ||
Plant uptake | Hijosa-Valsero et al. [45] | ||
Lincomycin | Biodegradation | Chen et al. [54] | Biodegradation (aerobic) ** |
Sorption | Chen et al. [54] | ||
Ofloxacin | Adsorption | Chen et al. [54] | Biodegradation (anaerobic) **; adsorption |
Biodegradation | Chen et al. [54]; Yan et al. [74] | ||
Oxytetracycline | Adsorption | Dordio and Carvalho [28]; Berglund et al. [73]; Huang et al. [55] | Adsorption; plant uptake |
Plant uptake | Dordio and Carvalho [28]; Huang et al. [55] | ||
Biodegradation (aerobic) | Dordio and Carvalho [28]; Huang et al. [55] | ||
Sulfadiazine | Biodegradation | Xian et al. [47] | Biodegradation (anaerobic) ** |
Fermentation | Dan et al. [22] | ||
Sulfamethazine | Adsorption | Liu et al. [57]; Chen et al. [54]; Choi et al. [75] | Biodegradation (aerobic) **; plant uptake |
Biodegradation | Xian et al. [47]; Liu et al. [57]; Chen et al. [54]; Choi et al. [75] | ||
Fermentation | Dan et al. [22] | ||
Plant uptake | Xian et al. [47] | ||
Sulfamethoxazole | Adsorption | Choi et al. [75]; Liang et al. [76] | Biodegradation (aerobic; anaerobic) ** |
Sorption | Zhu and Chen [66] | ||
Biodegradation (aerobic) | Conkle et al. [25]; Choi et al. [75]; Sgroi et al. [77]; Button et al. [53] | ||
Biodegradation (anaerobic) | Hijosa-Valsero et al. [45]; Dan et al. [22]; Rühmland et al. [58]; Liang et al. [76]; Sgroi et al. [77] | ||
Photodegradation | Hijosa-Valsero et al. [45] | ||
Plant uptake | Xian et al. [47]; Hijosa-Valsero et al. [45] | ||
Sulfapyridine | Biodegradation (aerobic) | Conkle et al. [25] | Biodegradation (anaerobic) ** |
Biodegradation (anaerobic) | Dan et al. [22] | ||
Trimethoprim | Biodegradation (aerobic) | Hijosa-Valsero et al. [45]; Rühmland et al. [58] | Biodegradation (anaerobic) ** |
Biodegradation (anaerobic) | Dan et al. [22] | ||
Monensin | Biodegradation | Chen et al. [54] | Biodegradation (aerobic) ** |
Stimulants/Psychoactive Drugs | |||
Caffeine | Biodegradation (aerobic) | Matamoros and Bayona [78]; Hijosa-Valsero et al. [60]; Zhang et al. [10]; Chen et al. [17]; Li et al. [42]; Vymazal et al. [19]; Vystavna et al. [71]; He et al. [52] | Biodegradation (aerobic) **; plant uptake |
Biodegradation (anaerobic) | Hijosa-Valsero et al. [15]; Carranza-Diaz et al. [49]; He et al. [52] | ||
Adsorption onto carbon-rich surfaces of the gravel bed | Matamoros and Bayona [78]; Dettenmaier et al. [79]; Wang et al. [80]; Li et al. [42] | ||
Plant uptake | Hijosa-Valsero et al. [15]; Zhang et al. [81]; Zhu and Chen [66]; Chen et al. [17]; Li et al. [42]; Petrie et al. [72] | ||
Psychiatric drugs | |||
Carbamazepine | Adsorption onto the available organic surfaces | Matamoros et al. [64,82]; Hijosa-Valsero et al. [16]; Carranza-Diaz et al. [49]; Sharif et al. [24]; Vystavna et al. [71]; Park et al. [56] | Adsorption; Sorption; plant uptake |
Sorption | Dordio et al. [44]; Dordio and Carvalho [28]; Park et al. [56] | ||
Biodegradation (aerobic) | Hijosa-Valsero et al. [15] | ||
Reductive transformation | Kahl et al. [40]; Nivala et al. [43] | ||
Plant uptake | Hijosa-Valsero et al. [15,46]; Macci et al. [50]; Yan et al. [74]; Petrie et al. [72]; He et al. [52] | ||
Venlafaxine | Precipitation | Breitholtz et al. [83]; Vystavna et al. [71] | Plant uptake; precipitation |
Biological transformation | Rühmland et al. [58]; Petrie et al. [72] | ||
Plant uptake | Petrie et al. [72] | ||
Beta blockers | |||
Atenolol | Biodegradation (aerobic) | Conkle et al. [25]; Rühmland et al. [58] | Sorption |
Biodegradation (anaerobic) | Chen et al. [17] | ||
Adsorption | Auvinen et al. [31]; Park et al. [56] | ||
Sorption | Petrie et al. [72]; Park et al. [56] | ||
Photodegradation | Salgado et al. [84] | ||
Plant uptake | Francini et al. [62] | ||
Metoprolol | Biodegradation (aerobic) | Conkle et al. [25]; Rühmland et al. [58]; Chen et al. [17]; He et al. [52] | Biodegradation (aerobic) |
Lipid regulators | |||
Gemfibrozil | Biodegradation (aerobic) | Conkle et al. [25]; Yi et al. [85]; Zhang et al. [34] | Biodegradation (aerobic) |
Diuretics | |||
Furosemide | Hydrolysis | Chen et al. [17]; Vymazal et al. [19] | Hydrolysis; biodegradation (aerobic) ** |
Photolysis | Chen et al. [17] |
Parameter | Depth | Area | HLR | OLR | HRT | Temp | pH | Eff. DO |
---|---|---|---|---|---|---|---|---|
Ibuprofen | 0.326 | −0.115 | −0.150 | 0.111 | 0.099 | 0.062 | −0.121 | 0.541 |
Naproxen | 0.199 | −0.002 | −0.251 | 0.055 | 0.140 | 0.350 | −0.169 | 0.348 |
Diclofenac | 0.451 | −0.279 | −0.191 | −0.018 | 0.313 | 0.316 | 0.179 | 0.562 |
Ketoprofen | 0.320 | −0.249 | 0.053 | −0.134 | 0.293 | 0.308 | 0.438 | 0.465 |
Salicylic acid | −0.044 | 0.567 | −0.394 | −0.518 | 0.119 | 0.676 | 0.134 | 0.297 |
Acetaminophen | 0.123 | 0.238 | −0.386 | 0.243 | −0.127 | −0.201 | −0.436 | 0.051 |
Codeine | 0.833 | 0.632 | −0.260 | −0.986 | 0.072 | −0.097 | −0.802 | −0.215 |
Tramadol | 0.231 | −0.132 | −0.487 | −0.224 | −0.116 | 0.135 | −0.787 | −0.413 |
Sulfadiazine | −0.641 | −0.309 | −0.042 | 0.230 | NA | 0.833 | 0.056 | NA |
Sulfamethoxazole | 0.057 | 0.003 | −0.278 | −0.164 | 0.179 | 0.010 | 0.037 | 0.018 |
Clarithromycin | 0.018 | 0.107 | 0.268 | −0.624 | 0.544 | −0.577 | 0.955 | 0.528 |
Erythromycin | −0.050 | 0.628 | −0.601 | −0.592 | 0.412 | −0.149 | 0.554 | −0.445 |
Lincomycin | 0.000 | 0.609 | −0.408 | −0.600 | −0.508 | −0.546 | 0.576 | −0.526 |
Trimethoprim | −0.114 | 0.261 | −0.353 | −0.347 | −0.324 | 0.143 | −0.254 | −0.891 |
Oxytetracycline | −0.068 | −0.995 | −0.779 | NA | 0.372 | NA | −0.520 | NA |
Ofloxacin | 0.053 | −0.353 | 0.167 | 0.467 | −0.713 | NA | 0.784 | 0.506 |
Sulfamethazine | −0.385 | −0.006 | −0.112 | −0.194 | 0.634 | −0.246 | 0.413 | 0.333 |
Sulfapyridine | 0.599 | 0.318 | −0.213 | −0.272 | NA | −0.304 | 0.080 | NA |
Monensin | NA | 0.280 | −0.296 | −0.296 | NA | −0.128 | −0.022 | 0.172 |
Carbamazepine | 0.181 | −0.211 | −0.144 | 0.030 | 0.209 | 0.247 | 0.070 | −0.094 |
Venlafaxine | 1.000 | −0.307 | −0.708 | 0.697 | −0.523 | 0.403 | −0.792 | 0.362 |
Caffeine | 0.158 | 0.147 | −0.154 | 0.038 | 0.095 | 0.465 | −0.002 | 0.187 |
Furosemide | 0.005 | 0.582 | −0.720 | −0.661 | 0.622 | NA | NA | NA |
Atenolol | 0.227 | −0.169 | 0.008 | 0.734 | 0.398 | 0.166 | −0.971 | −0.577 |
Metoprolol | 0.180 | −0.122 | −0.405 | 0.602 | 0.100 | −0.365 | 0.478 | 0.025 |
Gemfibrozil | 0.561 | 0.207 | −0.247 | −0.650 | 0.711 | 0.248 | −0.913 | 0.576 |
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Ilyas, H.; van Hullebusch, E.D. Role of Design and Operational Factors in the Removal of Pharmaceuticals by Constructed Wetlands. Water 2019, 11, 2356. https://doi.org/10.3390/w11112356
Ilyas H, van Hullebusch ED. Role of Design and Operational Factors in the Removal of Pharmaceuticals by Constructed Wetlands. Water. 2019; 11(11):2356. https://doi.org/10.3390/w11112356
Chicago/Turabian StyleIlyas, Huma, and Eric D. van Hullebusch. 2019. "Role of Design and Operational Factors in the Removal of Pharmaceuticals by Constructed Wetlands" Water 11, no. 11: 2356. https://doi.org/10.3390/w11112356