N-nitrosamine rejection by reverse osmosis membranes: a full-scale study.

This study aims to provide longitudinal and spatial insights to the rejection of N-nitrosamines by reverse osmosis (RO) membranes during sampling campaigns at three full-scale water recycling plants. Samples were collected at all individual filtration stages as well as at a cool and a warm weather period to elucidate the impact of recovery and feed temperature on the rejection of N-nitrosamines. N-nitrosodimethylamine (NDMA) was detected in all RO feed samples varying between 7 and 32 ng/L. Concentrations of most other N-nitrosamines in the feed solutions were determined to be lower than their detection limits (3-5 ng/L) but higher concentrations were detected in the feed after each filtration stage. As a notable exception, in one plant, N-nitrosomorpholine (NMOR) was observed at high concentrations in RO feed (177-475 ng/L) and permeate (34-76 ng/L). Overall rejection of NDMA among the three RO systems varied widely from 4 to 47%. Data presented here suggest that the feed temperature can influence rejection of NDMA. A considerable variation in NDMA rejection across the three RO stages (14-78%) was also observed. Overall NMOR rejections were consistently high ranging from 81 to 84%. On the other hand, overall rejection of N-nitrosodiethylamine (NDEA) varied from negligible to 53%, which was considerably lower than values reported in previous laboratory-scale studies. A comparison between results reported here and the literature indicates that there can be some discrepancy in N-nitrosamine rejection data between laboratory- and full-scale studies probably due to differences in water recoveries and operating conditions (e.g. temperature, membrane fouling, and hydraulic conditions).

Boron as a surrogate for N-nitrosodimethylamine rejection by reverse osmosis membranes in potable water reuse applications.

The results of this study reveal a strong linear correlation (R(2) = 0.95) between the rejections of boron and N-nitrosodimethylamine (NDMA) by six different reverse osmosis (RO) membranes, suggesting that boron can be used as a surrogate for NDMA rejection. This proposal is based on the premise that the rejection of both boric acid and NDMA is governed by steric hindrance and that they have similar molecular dimensions. The concept proposed here is shown to be valid at pH 8 or below where boron exists as the neutral boric acid species and NDMA is also a neutral solute. Observed changes in the rejections of these two species, as a function of permeate fluxes and feed solution temperatures, were also almost identical. Boron rejection increased from 21 to 79%, and the correlation coefficient of the linear regression between boron and NDMA rejections was 0.99 as the permeate flux increased from 5 to 60 L m(-2)h(-1). Similarly, a linear correlation between boron and NDMA rejections was observed as the feed solution temperature increased from 10 to 40 °C. This linear correlation was also validated in a tertiary treated effluent matrix.

Evaluating a strategy for maintaining nitrifier activity during long-term starvation in a moving bed biofilm reactor (MBBR) treating reverse osmosis concentrate.

A two-stage moving bed biofilm reactor (MBBR) was applied at the Bundamba advanced water treatment plant (AWTP) (Queensland, Australia) to treat the reverse osmosis concentrate (ROC) for inorganic nutrient removal. One of the operational challenges for the system was to cope with the large fluctuations of the ROC flow. This study investigated the decay rates of ammonia-oxidizing bacteria (AOB) and nitrite-oxidizing bacteria (NOB) and biofilm detachment in MBBR during starvation for up to one month. An intermittent aeration strategy of 15 min aeration every 6 h was applied. This study also evaluated the activity recovery of both AOB and NOB after normal operation was resumed. The results showed that the activity loss of AOB and NOB was relatively minor (<20%) within 10 days of starvation, which ensured relatively quick recovery of ammonium removal when normal operation resumed. In contrast, the AOB and NOB activity loss reached 60-80% when the starvation time was longer than 20 days, resulting in slower recovery of ammonium removal after starvation. Starvation for less than 20 days didn't result in an apparent biomass detachment from carriers.

Evaluation of contaminant removal of reverse osmosis and advanced oxidation in full-scale operation by combining passive sampling with chemical analysis and bioanalytical tools.

Advanced water treatment of secondary treated effluent requires stringent quality control to achieve a water quality suitable for augmenting drinking water supplies. The removal of micropollutants such as pesticides, industrial chemicals, endocrine disrupting chemicals (EDC), pharmaceuticals, and personal care products (PPCP) is paramount. As the concentrations of individual contaminants are typically low, frequent analytical screening is both laborious and costly. We propose and validate an approach for continuous monitoring by applying passive sampling with Empore disks in vessels that were designed to slow down the water flow, and thus uptake kinetics, and ensure that the uptake is only marginally dependent on the chemicals' physicochemical properties over a relatively narrow molecular size range. This design not only assured integrative sampling over 27 days for a broad range of chemicals but also permitted the use of a suite of bioanalytical tools as sum parameters, representative of mixtures of chemicals with a common mode of toxic action. Bioassays proved to be more sensitive than chemical analysis to assess the removal of organic micropollutants by reverse osmosis, followed by UV/H2O2 treatment, as many individual compounds fell below the quantification limit of chemical analysis, yet still contributed to the observed mixture toxicity. Nonetheless in several cases, the responses in the bioassays were also below their quantification limits and therefore only three bioassays were evaluated here, representing nonspecific toxicity and two specific end points for estrogenicity and photosynthesis inhibition. Chemical analytical techniques were able to quantify 32 pesticides, 62 PCPPs, and 12 EDCs in reverse osmosis concentrate. However, these chemicals could explain only 1% of the nonspecific toxicity in the Microtox assay in the reverse osmosis concentrate and 0.0025% in the treated water. Likewise only 1% of the estrogenic effect in the E-SCREEN could be explained by the quantified EDCs after reverse osmosis. In comparison, >50% of the estrogenic effect can typically be explained in sewage. Herbicidal activity could be fully explained by chemical analysis as the sampling period coincided with an illegal discharge and two herbicides dominated the mixture effect. The mass balance of the reverse osmosis process matched theoretical expectations for both chemical analysis and bioanalytical tools. Overall the investigated treatment train removed >97% estrogenicity, >99% herbicidal activity, and >96% baseline toxicity, confirming the suitability of the treatment train for polishing water for indirect potable reuse. The product water was indistinguishable from local tap water in all three bioassays. This study demonstrates the suitability and robustness of passive sampling linked with bioanalytical tools for semicontinuous monitoring of advanced water treatment with respect to micropollutant removal.

Characterisation and removal of recalcitrants in reverse osmosis concentrates from water reclamation plants.

Water reclamation plants frequently utilise reverse osmosis (RO), generating a concentrated reject stream as a by-product. The concentrate stream contains salts, and dissolved organic compounds, which are recalcitrant to biological treatment, and may have an environmental impact due to colour and embedded nitrogen. In this study, we characterise organic compounds in RO concentrates (ROC) and treated ROC (by coagulation, adsorption, and advanced oxidation) from two full-scale plants, assessing the diversity and treatability of colour and organic compounds containing nitrogen. One of the plants was from a coastal catchment, while the other was inland. Stirred cell membrane fractionation was applied to fractionate the treated ROC, and untreated ROC along with chemical analysis (DOC, DON, COD), colour, and fluorescence excitation-emission matrix (EEM) scans to characterise changes within each fraction. In both streams, the largest fraction contained < 1 kDa molecules which were small humic substances, fulvic acids and soluble microbial products (SMPs), as indicated by EEM. Under optimal treatment conditions, alum preferentially removed > 10 kDa molecules, with 17-34% of organic compounds as COD. Iron coagulation affected a wider size range, with better removal of organics (41-49% as COD) at the same molar dosage. As with iron, adsorption reduced organics of a broader size range, including organic nitrogen (26-47%). Advanced oxidation (UV/H2O2) was superior for complete decolourisation and provided superior organics removal (50-55% as COD).

Removal of PFOS, PFOA and other perfluoroalkyl acids at water reclamation plants in South East Queensland Australia.

This paper examines the fate of perfluorinated sulfonates (PFSAs) and carboxylic acids (PFCAs) in two water reclamation plants in Australia. Both facilities take treated water directly from WWTPs and treat it further to produce high quality recycled water. The first plant utilizes adsorption and filtration methods alongside ozonation, whilst the second uses membrane processes and advanced oxidation to produce purified recycled water. At both facilities perfluorooctane sulfonate (PFOS), perfluorohexane sulfonate (PFHxS), perfluorohexanoic acid (PFHxA) and perfluorooctanoic acid (PFOA) were the most frequently detected PFCs. Concentrations of PFOS and PFOA in influent (WWTP effluent) ranged up to 3.7 and 16 ng L⁻¹ respectively, and were reduced to 0.7 and 12 ng L⁻¹ in the finished water of the ozonation plant. Throughout this facility, concentrations of most of the detected perfluoroalkyl compounds (PFCs) remained relatively unchanged with each successive treatment step. PFOS was an exception to this, with some removal following coagulation and dissolved air flotation/sand filtration (DAFF). At the second plant, influent concentrations of PFOS and PFOA ranged up to 39 and 29 ng L⁻¹. All PFCs present were removed from the finished water by reverse osmosis (RO) to concentrations below detection and reporting limits (0.4-1.5 ng L⁻¹). At both plants the observed concentrations were in the low parts per trillion range, well below provisional health based drinking water guidelines suggested for PFOS and PFOA.

Understanding the operational parameters affecting NDMA formation at Advanced Water Treatment Plants.

N-nitrosodimethylamine (NDMA) can be formed when secondary effluents are disinfected by chloramines. By means of bench scale experiments this paper investigates operational parameters than can help Advanced Water Treatment Plants (AWTPs) to reduce the formation of NDMA during the production of high quality recycled water. The formation of NDMA was monitored during a contact time of 24h using dimethylamine as NDMA model precursor and secondary effluent from wastewater treatment plants. The three chloramine disinfection strategies tested were pre-formed and in-line formed monochloramine, and pre-formed dichloramine. Although the latter is not employed on purpose in full-scale applications, it has been suggested as the main contributing chemical generating NDMA during chloramination. After 24h, the NDMA formation decreased in both matrices tested in the order: pre-formed dichloramine>in-line formed monochloramine≫pre-formed monochloramine. The most important parameter to consider for the inhibition of NDMA formation was the length of contact time between disinfectant and wastewater. Formation of NDMA was initially inhibited for up to 6h with concentrations consistently <10 ng/L during these early stages of disinfection, regardless of the disinfection strategy. The reduction of the contact time was implemented in Bundamba AWTP (Queensland, Australia), where NDMA concentrations were reduced by a factor of 20 by optimizing the disinfection strategy.

Removal of magnetic resonance imaging contrast agents through advanced water treatment plants.

Stable gadolinium (Gd) complexes have been used as paramagnetic contrast agents for magnetic resonance imaging (MRI) for over 20 years, and have recently been identified as environmental contaminants. As the rare earth elements (REE), which include Gd, are able to be measured accurately at very low concentrations (e.g. Tb is measured at 7 fmol/kg in this study) using inductively coupled plasma mass spectrometry (ICP-MS), it is possible to determine the fate of this class of compounds during the production of purified recycled water from effluent. Coagulation and microfiltration have negligible removal, with the major removal step occurring across the reverse osmosis membrane where anthropogenic Gd (the amount of Gd attributable to MRI contrast agents) is reduced from 0.39 nmol/kg to 0.59 pmol/kg, a reduction of 99.85%. The RO concentrate has anthropogenic Gd concentrations of 2.6 nmol/kg, an increase in concentration in line with the design characteristics of the plant. The increased concentration in the RO concentrate may allow further development of anthropogenic Gd as a tracer of the fate of the RO concentrate in the environment.