Ngoc Han Tran

Insight into metabolic and cometabolic activities of autotrophic and heterotrophic microorganisms in the biodegradation of emerging trace organic contaminants

Many efforts have been made to understand the biodegradation of emerging trace organic contaminants (EOCs) in the natural and engineered systems. This review summarizes the current knowledge on the biodegradation of EOCs while having in-depth discussion on metabolism and cometabolism of EOCs. Biodegradation of EOCs is mainly attributed to cometabolic activities of both heterotrophic and autotrophic microorganisms. Metabolism of EOCs can only be observed by heterotrophic microbes. Autotrophic ammonia oxidizing bacteria (AOB) and ammonia oxidizing archaeal (AOA) cometabolize a variety of EOCs via the non-specific enzymes, such as ammonia monooxygenase (AMO). Higher biodegradation of EOCs is often noted under nitrification at high ammonia loading rate. The presence of a growth substrate promotes cometabolic biodegradation of EOCs. Potential strategies for enhancing the biodegradation of EOCs were also proposed in this review.

The characteristics of enriched nitrifier culture in the degradation of selected pharmaceutically active compounds

The biodegradation of 10 selected pharmaceuticals by enriched nitrifier cultures with ammonia oxidizing activity of 30mg NH(4)-N/gMLVSSh was investigated under various initial operating conditions such as in the presence of different growth substrates and inhibitors. The enriched nitrifier culture showed higher degradation of the target pharmaceuticals than the conventional activated sludge. The degradation efficiency of persistent pharmaceuticals such as clofibric acid (CA), diclofenac (DCF), carbamazepine (CBZ), and propyphenazone (PPZ) was increased with the increase in the ammonium concentration. A higher removal efficiency of CA, DCF, CBZ and PPZ was obtained when organic substrates were added. The contribution of autotrophs and heterotrophs in the biotransformation of the pharmaceuticals by the enriched nitrifier culture was successfully estimated by the addition of inhibitors. Experimental results showed that the high degradation of IBP and partial degradation of other selected pharmaceuticals were observed in the presence of allylthiourea (ATU), an ammonia monooxygenase inhibitor, reflecting the activity of heterotrophic bacteria, while the results with and without ATU addition showed that the contribution of the nitrification in the degradation of most pharmaceuticals was also dominant. The results suggest that nitrification can enhance the biotransformation of pharmaceutical substances.

Simultaneous determination of PPCPs, EDCs, and artificial sweeteners in environmental water samples using a single-step SPE coupled with HPLC-MS/MS and isotope dilution.

A high-throughput method for the simultaneous determination of 24 pharmaceuticals and personal care products (PPCPs), endocrine disrupting chemicals (EDCs) and artificial sweeteners (ASs) was developed. The method was based on a single-step solid phase extraction (SPE) coupled with high performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS) and isotope dilution. In this study, a single-step SPE procedure was optimized for simultaneous extraction of all target analytes. Good recoveries (≥ 70%) were observed for all target analytes when extraction was performed using Chromabond(®) HR-X (500 mg, 6 mL) cartridges under acidic condition (pH 2). HPLC-MS/MS parameters were optimized for the simultaneous analysis of 24 PPCPs, EDCs and ASs in a single injection. Quantification was performed by using 13 isotopically labeled internal standards (ILIS), which allows correcting efficiently the loss of the analytes during SPE procedure, matrix effects during HPLC-MS/MS and fluctuation in MS/MS signal intensity due to instrument. Method quantification limit (MQL) for most of the target analytes was below 10 ng/L in all water samples. The method was successfully applied for the simultaneous determination of PPCPs, EDCs and ASs in raw wastewater, surface water and groundwater samples collected in a local catchment area in Singapore. In conclusion, the developed method provided a valuable tool for investigating the occurrence, behavior, transport, and the fate of PPCPs, EDCs and ASs in the aquatic environment.

Suitability of artificial sweeteners as indicators of raw wastewater contamination in surface water and groundwater.

There is no quantitative data on the occurrence of artificial sweeteners in the aquatic environment in Southeast Asian countries, particularly no information on their suitability as indicators of raw wastewater contamination on surface water and groundwater. This study provided the first quantitative information on the occurrence of artificial sweeteners in raw wastewater, surface water and groundwater in the urban catchment area in Singapore. Acesulfame, cyclamate, saccharin, and sucralose were ubiquitous in raw wastewater samples at concentrations in the range of ng/L-μg/L, while other sweeteners were not found or found only in a few of the raw wastewater samples. Residential and commercial effluents were demonstrated to be the two main sources of artificial sweeteners entering the municipal sewer systems. Relatively higher concentrations of the detected sweeteners were frequently found in surface waters at the sampling sites located in the residential/commercial areas. No significant difference in the concentrations of the detected sweeteners in surface water or groundwater was noted between wet and dry weather conditions (unpaired T-test, p> 0.05). Relatively higher concentrations and detection frequencies of acesulfame, cyclamate and saccharin in surface water samples were observed at the potentially impacted sampling sites, while these sweeteners were absent in most of the background surface water samples. Similarly, acesulfame, cyclamate, and saccharin were found in most groundwater samples at the monitoring well (GW6), which is located close to known leaking sewer segment; whereas these were absent in the background monitoring well, which is located in the catchment with no known wastewater sources. Taken together, the results suggest that acesulfame, cyclamate, and saccharin can be used as potential indicators of raw wastewater contamination in surface water and groundwater.

Fecal pollution source tracking toolbox for identification, evaluation and characterization of fecal contamination in receiving urban surface waters and groundwater

The quality of surface waters/groundwater of a geographical region can be affected by anthropogenic activities, land use patterns and fecal pollution sources from humans and animals. Therefore, the development of an efficient fecal pollution source tracking toolbox for identifying the origin of the fecal pollution sources in surface waters/groundwater is especially helpful for improving management efforts and remediation actions of water resources in a more cost-effective and efficient manner. This review summarizes the updated knowledge on the use of fecal pollution source tracking markers for detecting, evaluating and characterizing fecal pollution sources in receiving surface waters and groundwater. The suitability of using chemical markers (i.e. fecal sterols, fluorescent whitening agents, pharmaceuticals and personal care products, and artificial sweeteners) and/or microbial markers (e.g. F+RNA coliphages, enteric viruses, and host-specific anaerobic bacterial 16S rDNA genetic markers) for tracking fecal pollution sources in receiving water bodies is discussed. In addition, this review also provides a comprehensive approach, which is based on the detection ratios (DR), detection frequencies (DF), and fate of potential microbial and chemical markers. DR and DF are considered as the key criteria for selecting appropriate markers for identifying and evaluating the impacts of fecal contamination in surface waters/groundwater.

A critical review on characterization strategies of organic matter for wastewater and water treatment processes

The presence of organic matter (OM) in raw wastewater, treated wastewater effluents, and natural water samples has been known to cause many problems in wastewater treatment and water reclamation processes, such as treatability, membrane fouling, and the formation of potentially toxic by-products during wastewater treatment. This paper summarizes the current knowledge on the methods for characterization and quantification of OM in water samples in relation to wastewater and water treatment processes including: (i) characterization based on the biodegradability; (ii) characterization based on particle size distribution; (iii) fractionation based on the hydrophilic/hydrophobic properties; (iv) characterization based on the molecular weight (MW) size distribution; and (v) characterization based on fluorescence excitation emission matrix. In addition, the advantages, disadvantages and applications of these methods are discussed in detail. The establishment of correlations among biodegradability, hydrophobic/hydrophilic fractions, MW size distribution of OM, membrane fouling and formation of toxic by-products potential is highly recommended for further studies.

Occurrence and fate of emerging contaminants in municipal wastewater treatment plants from different geographical regions-a review

Emerging contaminants, such as antibiotics, pharmaceuticals, personal care products, hormones, and artificial sweeteners, are recognized as new classes of water contaminants due to their proven or potential adverse effects on aquatic ecosystems and human health. This review provides comprehensive data on the occurrence of 60 emerging contaminants (ECs) in influent, treated effluent, sludge, and biosolids in wastewater treatment plants (WWTPs). In particular, data on the occurrence of ECs in the influents and effluents of WWTPs are systematically summarized and categorized according to geographical regions (Asia, Europe, and North America). The occurrence patterns of ECs in raw influent and treated effluents of WWTPs between geographical regions were compared and evaluated. Concentrations of most ECs in raw influent in Asian region tend to be higher than those in European and North American countries. Many antibiotics were detected in the influents and effluents of WWTPs at concentrations close to or exceeding the predicted no-effect concentrations (PNECs) for resistance selection. The efficacy of EC removal by sorption and biodegradation during wastewater treatment processes are discussed in light of kinetics and parameters, such as sorption coefficients (Kd) and biodegradation constants (kbiol), and physicochemical properties (i.e. log Kow and pKa). Commonly used sampling and monitoring strategies are critically reviewed. Analytical research needs are identified, and novel investigative approaches for future monitoring studies are proposed.

Sorption and biodegradation of artificial sweeteners in activated sludge processes.

There is limited information on the occurrence and removal of artificial sweeteners (ASs) in biological wastewater treatment plants, and in particular, the contribution of sorption and biodegradation to their removal. This study investigated the fate of ASs in both the aqueous and solid phases in a water reclamation plant (WRP). All the four targeted ASs, i.e. acesulfame (ACE), sucralose (SUC), cyclamate (CYC) and saccharine (SAC), were detected in both the aqueous and solid phases of raw influent and primary effluent samples. The concentrations of CYC and SAC in secondary effluent or MBR permeate were below their method detection limits. ACE and SUC were persistent throughout the WRP, whereas CYC and SAC were completely removed in biological treatment (>99%). Experimental results showed that sorption played a minor role in the elimination of the ASs due to the relatively low sorption coefficients (Kd), where Kd<500L/kg. In particular, the poor removal of ACE and SUC in the WRP may be attributed to their physiochemical properties (i.e. logKow<0 or logD<3.2) and chemical structures containing strong withdrawing electron functional groups in heterocyclic rings (i.e. chloride and sulfonate).

Role of nitrification in the biodegradation of selected artificial sweetening agents in biological wastewater treatment process.

The biodegradation of the six artificial sweetening agents including acesulfame (ACE), aspartame (ASP), cyclamate (CYC), neohesperidindihydrochalcone (NHDC), saccharin (SAC), and sucralose (SUC) by nitrifying activated sludge was first examined. Experimental results showed that ASP and NHDC were the most easily degradable compounds even in the control tests. CYC and SAC were efficiently biodegraded by the nitrifying activated sludge, whereas ACE and SUC were poorly removed. However, the biodegradation efficiencies of the ASs were increased with the increase in initial ammonium concentrations in the bioreactors. The association between nitrification and co-metabolic degradation was investigated and a linear relationship between nitrification rate and co-metabolic biodegradation rate was observed for the target artificial sweeteners (ASs). The contribution of heterotrophic microorganisms and autotrophic ammonia oxidizers in biodegradation of the ASs was elucidated, of which autotrophic ammonia oxidizers played an important role in the biodegradation of the ASs, particularly with regards to ACE and SUC.

Occurrence and removal of pharmaceuticals, hormones, personal care products, and endocrine disrupters in a full-scale water reclamation plant

This study provided the first comprehensive data on the occurrence and removal of twenty-five target emerging contaminants (ECs) in a full-scale water reclamation plant (WRP) in the Southeast Asian region. Nineteen out of the twenty-five ECs were ubiquitously detected in raw influent samples. Concentrations of the detected ECs in raw influent samples ranged substantially from 44.3 to 124,966ng/L, depending upon the compound and sampling date. The elimination of ECs in full-scale conventional activated sludge (CAS) and membrane bioreactor (MBR) systems at a local WRP was evaluated and compared. Several ECs, such as acetaminophen, atenolol, fenoprofen, indomethacin, ibuprofen, and oxybenzone, exhibited excellent removal efficiencies (>90%) in biological wastewater treatment processes, while some of the investigated compounds (carbamazepine, crotamiton, diclofenac, and iopamidol) appeared to be persistent in the both CAS and MBR systems. Field-based monitoring results showed that MBR outperformed CAS in the elimination of most target ECs. The relationship between molecular characteristics of ECs (i.e. physicochemical properties and structural features) and their removal efficiencies during biological wastewater treatment was also elucidated. Excellent removal efficiencies (>90%) were often noted for ECs with the sole presence of electron donating groups (i.e. phenolic [OH], amine [NH2], methoxy [OCH3], phenoxy [OC6H5], or alkyl groups). Conversely, ECs with the absence of electron donating groups or the predominance of strong electron withdrawing groups (e.g. halogenated, carbonyl, carboxyl, and sulfonamide) tended to show poor removal efficiencies (<30%) in biological wastewater treatment processes.