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ABSTRACT: Pharmaceutical compounds are now considered as emerging contaminants of environmental concern. The overall objective of this study was to evaluate the uptake and translocation of clofibric acid (CA) by the macrophyte Scirpus validus growing hydroponically. A set of the three replicates was established for each exposure time and for each CA concentration. Plants were grown in 4 L vessels (four plants per vessel corresponding to the three exposure period studies, i.e., 7, 14, 18, and 21 days) which contained an aerated modified Hoagland nutrient solution that was spiked with CA at concentrations of 0.5, 1.0, and 2.0 mg L(-1). At each exposure period, CA concentration was measured in the nutrient solutions. A sea sand disruption method was employed for the extraction of CA from plant tissues. The determination of the pharmaceutical concentration was carried out using solid phase extraction (SPE) followed by chromatographic analysis. The quantification of CA concentrations in both nutrient solutions (after SPE) and plant tissues (after extraction) was conducted by chromatographic analysis. CA concentrations of 5.4-26.8 μg g(-1) (fresh weight) were detected in the roots and 7.2-34.6 μg g(-1) (fresh weight) in the shoots after 21 days. Mass balance calculations showed that S. validus uptake alone accounted for a significant contribution (6-13 % for the roots and 22-49 % for the shoots) of the total loss of CA. The bioaccumulation factors (BAFs) based on fresh weight for the roots ranged from 6.6 to 23.2, while values for the shoots ranged from 9.5 to 32.1. All the BAFs for the shoots were greater than those in the roots, implying that CA has greater tendency to be translocated to the shoots, rather than the roots of S. validus. All the shoot-to-root concentration ratios were more than 1, denoting that the shoots of S. validus do preferentially accumulate CA. We demonstrated that CA can be actively taken up, subsequently translocated and accumulated by aboveground tissues of S. validus. Since S. validus could account for the removal of 28-62 % of the total mass loss of CA from the system, such phytoremediation technology has great potential for the removal of pharmaceuticals such as CA from inflowing waters.
Environmental Science and Pollution Research 12/2012; · 2.65 Impact Factor
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ABSTRACT: Scirpus validus was grown hydroponically and exposed to the pharmaceuticals, carbamazepine and naproxen at concentrations of 0.5-2.0mgL(-1) for an exposure duration of up to 21d. By the end of experiment, carbamazepine elimination from the nutrient solution reached to 74%, while nearly complete removal (>98%) was observed for naproxen. Photodegradation and biodegradation played only minor roles for carbamazepine elimination, while naproxen showed a high potential for both photodegradation and biodegradation. Levels of carbamazepine ranged from 3.3 to19.0μgg(-1) (fresh weight) in the roots and 0.3-0.7μgg(-1) (fresh weight) in the shoots, while naproxen concentrations were 0.2-2.4μgg(-1) (fresh weight) in the roots and 0.2-2.8μgg(-1) (fresh weight) in the shoots. Bioaccumulation factors (BAFs) for carbamazepine ranged from 5.5 to 13.0 for roots and 0.3-1.0 for shoots, and uptake by S. validus accounted for up to 22% of the total mass loss of carbamazepine in the nutrient solutions. All BAFs for naproxen were less than 4.2 and plant uptake accounted for less than 5% of the total mass loss of naproxen, implying that plant uptake was not significant in naproxen elimination. The rather limited plant uptake of naproxen was not surprising despite the fact that its log K(ow) is close to the optimal range (1.8-3.1) for maximal potential for plant uptake. Apparently, for ionizable compounds such as naproxen, the effects of pK(a) and pH partitioning might be more important than lipophilicity.
Chemosphere 12/2012; · 3.21 Impact Factor
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ABSTRACT: Uptake, accumulation and translocation of caffeine by Scirpus validus grown in hydroponic condition were investigated. The plants were cultivated in Hoagland's nutrient solution spiked with caffeine at concentrations of 0.5-2.0mgL(-1). The effect of photodegradation on caffeine elimination was determined in dark controls and proved to be negligible. Removal of caffeine in mesocosms without plants showed however that biodegradation could account for about 15-19% of the caffeine lost from solutions after 3 and 7d. Plant uptake played a significant role in caffeine elimination. Caffeine was detected in both roots and shoots of S. validus. Root concentrations of caffeine were 0.1-6.1μgg(-1), while the concentrations for shoots were 6.4-13.7μgg(-1). A significant (p<0.05) positive correlation between the concentration in the root and the initial concentrations in the nutrient solution was observed. The bioaccumulation factors (BAFs) of caffeine for roots ranged from 0.2 to 3.1, while BAFs for shoots ranged from 3.2 to 16.9. Translocation from roots to shoots was the major pathway of shoot accumulation. The fraction of caffeine in the roots as a percentage of the total caffeine mass in solution was limited to 0.2-4.4% throughout the whole experiment, while shoot uptake percentage ranged from 12% to 25% for caffeine at the initial concentration of 2.0mgL(-1) to 50-62% for caffeine at the initial concentration of 0.5mgL(-1). However, a marked decrease in the concentration of caffeine in the shoots between d-14 and d-21 suggests that caffeine may have been catabolized in the plant tissues subsequent to plant uptake and translocation.
Chemosphere 10/2012; · 3.21 Impact Factor
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ABSTRACT: This study evaluated the effect of continuous and batch feeding on the removal of 8 pharmaceuticals (carbamazepine, naproxen, diclofenac, ibuprofen, caffeine, salicylic acid, ketoprofen and clofibric acid) from synthetic wastewater in mesocosm-scale constructed wetlands (CWs). Both loading modes were operated at hydraulic application rates of 5.6 cm day(-1) and 2.8 cm day(-1). Except for carbamazepine, clofibric acid and naproxen, removal in CWs was significantly (p < 0.05) enhanced under the batch versus continuous mode. For all compounds tested except naproxen, values for first-order decay constants (k) for drain and fill operation were higher than that for the continuous mode of operation. Correlation between the distribution coefficient (log D(ow)) and removal efficiencies of pharmaceutical compounds in the CWs, showed that pharmaceutical removal efficiency was significantly (p < 0.1) and inversely correlated with log D(ow) value, but not with log K(ow) value.
Environmental pollution (Barking, Essex: 1987) 05/2012; 167:124-31. · 3.43 Impact Factor
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ABSTRACT: The aim of this investigation was to evaluate the influence of batch versus continuous flow on the removal efficiencies of chemical oxygen demand (COD), nitrogen (N) and total phosphorus (TP) in tropical subsurface flow constructed wetlands (SSF CW). The quantitative role of the higher aquatic plants in nutrient removal in these two operational modes was also investigated. Results indicated no significant difference (p > 0.05) in COD removal between batch and continuous flow modes for either the planted or unplanted treatments. Furthermore, the batch-loaded planted wetlands showed significantly (p < 0.05) higher ammonium removal efficiencies (95.2%) compared with the continuously fed systems (80.4%), most probably because the drain and fill batch mode presented systematically more oxidized environmental conditions. With respect to TP removal, for both planted and unplanted beds, there was significant enhancement (p < 0.05) in batch flow operation (69.6% for planted beds; 39.1% for unplanted beds) as compared to continuous flow operation (46.8% for planted beds; 25.5% for unplanted beds). In addition, at a 4-day hydraulic retention time (HRT), the presence of plants significantly enhanced both ammonia oxidation and TP removal in both batch and continuous modes of operation as compared to that for unplanted beds. An estimation of the quantitative role of aeration from drain and fill operation at a 4-day HRT, as compared to rhizosphere aeration by the higher aquatic plant, indicated that drain and fill operation might account for only less than half of the higher aquatic plant's quantitative contribution of oxygen (1.55 g O2 per m2 per day for batch flow versus 1.13 g O2 per m2 per day for continuous flow).
Journal of Environmental Management 04/2012; 96(1):1-6. · 3.24 Impact Factor
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ABSTRACT: Determining the fate of emerging organic contaminants in an aquatic ecosystem is important for developing constructed wetlands (CWs) treatment technology. Experiments were carried out in subsurface flow CWs in Singapore to evaluate the fate and transport of eight pharmaceutical compounds. The CW system included three parallel horizontal subsurface flow CWs and three parallel unplanted beds fed continuously with synthetic wastewater at different hydraulic retention times (HRTs). The findings of the tests at 2-6 d HRTs showed that the pharmaceuticals could be categorized as (i) efficiently removed compounds with removal higher than 85% (ketoprofen and salicylic acid); (ii) moderately removed compounds with removal efficiencies between 50% and 85% (naproxen, ibuprofen and caffeine); and (iii) poorly removed compounds with efficiency rate lower than 50% (carbamazepine, diclofenac, and clofibric acid). Except for carbamazepine and salicylic acid, removal efficiencies of the selected pharmaceuticals showed significant (p<0.05) enhancement in planted beds as compared to the unplanted beds. Removal of caffeine, ketoprofen and clofibric acid were found to follow first order decay kinetics with decay constants higher in the planted beds than the unplanted beds. Correlations between pharmaceutical removal efficiencies and log K(ow) were not significant (p>0.05), implying that their removal is not well related to the compound's hydrophobicity.
Chemosphere 04/2012; 87(3):273-7. · 3.21 Impact Factor
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ABSTRACT: The ability of tropical horizontal subsurface constructed wetlands (HSSF CWs) planted with Typha angustifolia to remove four widely used pharmaceutical compounds (carbamazepine, declofenac, ibuprofen and naproxen) at the relatively short hydraulic residence time of 2–4 days was documented. For both ibuprofen and naproxen, pharmaceutical compounds with low Dow values, the planted beds showed significant (p < 0.05) enhancement of removal efficiencies (80% and 91%, respectively, at the 4 day HRT), compared to unplanted beds (60% and 52%, respectively). The presence of plants resulted in the removal of these pharmaceutical compounds from artificial wastewater. The more oxidizing environment in the rhizosphere might have played an important role, but other rhizosphere effects, beside rhizosphere aeration, appeared to be important also. Carbamazepine, considered one of the most recalcitrant pharmaceuticals, and declofenac showed low removal efficiencies in our CW, and this is attributable to their higher hydrophobicity. The fact that the removal of these compounds could be explained by the sorption onto the available organic surfaces, explains why there was no significant difference (p > 0.05) in their removal efficiencies between planted as compared to unplanted beds. No statistical significant differences (p > 0.05) were observed for the removal efficiencies of any of the pharmaceuticals tested for the 2-day HRT as compared to that corresponding to 4-day HRT. The rather efficient removal shown by the wetlands in this study (with HRTs of 2–4 days), indicates that such a CW system may be more practically used (with less land requirements) in tropical regions for removing conventional pollutants and certain pharmaceutical compounds from wastewater effluents.
Ecological Engineering. 37(3):460-464.
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ABSTRACT: This study presents findings on an assessment of the effect of continuous and batch feeding strategies on the removal of selected pharmaceuticals from synthetic wastewater. Six mesocosm-scale constructed wetlands, including three horizontal subsurface flow constructed wetlands and three sand filters, were set up at the campus of Nanyang Technological University, Singapore. The findings showed that ibuprofen and diclofenac removal in the wetlands was significantly ( < 0.05) enhanced in the batch versus continuous mode. In contrast, naproxen and carbamazepine showed no significant differences ( > 0.05) in elimination under either feeding strategy. Our results also clearly showed that the presence of plants exerts a stimulatory effect on pharmaceutical removal for ibuprofen, diclofenac, and naproxen in batch and continuous mode. Estimation of the quantitative role of this stimulatory effect on pharmaceutical elimination of batch operation as compared with the effect of the presence of the higher plant alone showed that batch operation may account for 40 to 87% of the contribution conferred by the aquatic plant. The findings of this study imply that where maximal removal of pharmaceutical compounds is desired, periodic draining and filling might be the preferred operational strategy for full-scale, subsurface flow constructed wetlands.
Journal of Environmental Quality 41(5):1674-80. · 2.32 Impact Factor
