Behaviour and fate of nine recycled water trace organics during managed aquifer recharge in an aerobic aquifer

doi:10.1016/j.jconhyd.2010.11.003

Journal of Contaminant Hydrology

Volume 122, Issues 1–4, 25 March 2011, Pages 53-62

https://doi.org/10.1016/j.jconhyd.2010.11.003 Get rights and content

Abstract

The fate of nine trace organic compounds was evaluated during a 12 month large-scale laboratory column experiment. The columns were packed with aquifer sediment and evaluated under natural aerobic and artificial anaerobic geochemical conditions, to assess the potential for natural attenuation of these compounds during aquifer passage associated with managed aquifer recharge (MAR). The nine trace organic compounds were bisphenol A (BPA), 17β-estradiol (E2), 17α-ethynylestradiol (EE2), N-nitrosodimethylamine (NDMA), N-nitrosomorpholine (NMOR), carbamazepine, oxazepam, iohexol and iodipamide. In the low organic carbon content Spearwood sediment, all trace organics were non-retarded with retardation coefficients between 1.0 and 1.2, indicating that these compounds would travel at near groundwater velocities within the aquifer. The natural aerobic geochemical conditions provided a suitable environment for the rapid degradation for BPA, E2, iohexol (half life < 1 day). Lag-times for the start of degradation of these compounds ranged from < 15 to 30 days. While iodipamide was persistent under aerobic conditions, artificial reductive geochemical conditions promoted via the addition of ethanol, resulted in rapid degradation (half life < 1 days). Pharmaceuticals (carbamazepine and oxazepam) and disinfection by-products (NDMA and NMOR) did not degrade under either aerobic or anaerobic aquifer geochemical conditions (half life > 50 days). Field-based validation experiments with carbamazepine and oxazepam also showed no degradation. If persistent trace organics are present in recycled waters at concentrations in excess of their intended use, natural attenuation during aquifer passage alone may not result in extracted water meeting regulatory requirements. Additional pre treatment of the recycled water would therefore be required.

Research Highlights

► The aerobic conditions were suitable for rapid degradation for BPA, E2, iohexol. ► Iodipamide degraded under anaerobic conditions, but not under aerobic conditions. ► Pharmaceuticals and disinfection by-products did not degrade under either condition. ► Field-based experiments with carbamazepine and oxazepam also showed no degradation.

Introduction

One of the major health concerns associated with the use of recycled water is the potential presence of low concentrations of a range of trace organics (Díaz-Cruz and Barceló, 2008). These trace organics include endocrine-disrupting compounds, hormones, pharmaceuticals, pesticides and disinfection by-products. Recycled water can be used in many different ways but one mechanism gaining favour in many countries is recharging the recycled water to aquifers using Managed Aquifer Recharge (MAR) (Dillon et al., 2006). When recycled water is used for MAR, it may undergo biogeochemical changes during aquifer storage or aquifer passage resulting in the natural attenuation of some trace organics. MAR has been shown to reduce nutrient concentrations and microbial pathogen numbers in recharged water (Dillon et al., 2006, Toze and Hanna, 2002) but less is known about the potential removal of trace organics during recharge and storage. As the fate of trace organics are determined by aquifer biological and geochemical conditions (Barber et al., 2009, Carrara et al., 2008), fate assessment results from one aquifer system may not apply to other systems. To assess the transferability of results between different aquifer systems, fate assessment comparative data is required for different aquifer systems where MAR using recycled water is planned.

Knowledge of the fate of trace organic compounds in aquifers is essential to the assessment and design of proposed MAR recycled water treatment strategies. This fate data can be used to provide design criteria for (i) injection/extraction borehole spacing or extraction rate to ensure sufficient aquifer residence time for degrading compounds to be naturally attenuated so that the extraction water meets regulatory requirements, and (ii) identify if additional pre or post MAR treatment options such as reverse osmosis, advanced oxidation or UV radiation are required for persistent trace organic compounds, where sufficient natural attenuation is unlikely to be achieved during aquifer passage and where significant human exposure to the recovered water is considered likely.

This paper describes the findings of a 12 month large-scale column experiment investigating the fate of nine trace organics under natural aerobic aquifer geochemical conditions and under artificial anaerobic reducing conditions via ethanol addition. The fate of each trace organic was assessed based on their chemical retardation coefficient (R) and degradation rate, determined from the experimental data.

Section snippets

Materials and methods

Nine trace organics were investigated. Bisphenol A (BPA), 17β-estradiol (E2), 17α-ethynylestradiol (EE2), carbamazepine (CARB), N-nitrosomorpholine (NMOR) and iohexol (IOX) were all obtained from Sigma-Aldrich (Sydney, Australia). N-nitrosodimethylamine (NDMA) was obtained from Chem Service (Perth, Australia), iodipamide (IDP) was obtained from Fluka (Sydney, Australia) and oxazepam (OXAZ) was obtained from the Chemistry Centre of Western Australia. These trace organics were selected, as all

Retardation coefficients

Sediment analysis by XRD showed the mineral composition was predominantly quartz (75%), with calcite (12%), microcline/orthoclase (11%), and albite/anorthite (2%). All other minerals were below analytical detection (< 1%). Details of the sediment properties are given in Table 1.

Prior to the introduction of the trace organics and bromide, sediment site groundwater was passed through the column at approximately 360 mL d^− 1 for a period of 2 months to stabilize column water chemistry. After the trace

Conclusions

For the Spearwood sediment investigated in this experiment, the low R values of the trace organics for the sediment suggest these compounds will migrate at similar velocities to groundwater flow. The natural aerobic geochemical conditions provided a suitable environment for degradation for the endocrine-disrupting compounds (BPA and E2), and IOH, with bacterial acclimation lag-times ranging from < 15 to 30 days. However, an alternative artificial induced anaerobic geochemical condition would be

Acknowledgements

This research was made possible through funding from the Western Australian Government through the Water Foundation, CSIRO Water for a Healthy Country Flagship Program, and the Water Corporation of Western Australia. The authors wish to acknowledge useful discussions with H. Prommer and P. Blair. This work also contributes to the National Water Commission Raising National Standards project on facilitating recycling of sewerage and stormwater via managed aquifer recharge.

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Behaviour and fate of nine recycled water trace organics during managed aquifer recharge in an aerobic aquifer

Abstract

Research Highlights

Introduction

Section snippets

Materials and methods

Retardation coefficients

Conclusions

Acknowledgements

Journal of Hydrology

Journal of Chromatography A

Water Research

Chemosphere

Desalination

Talanta

Water Research

Hazardous Materials

Toxicology Letters

Water Res.

Journal of Hydrology

Journal of Contaminant Hydrology

Water Research

Journal of Contaminant Hydrology

Water Research

Fate of sulfamethoxazole, 4-nonylphenol, and 17β-estradiol in groundwater contaminated by wastewater treatment plant effluent

Environmental Science & Technology

Improvements in wastewater quality from soil and aquifer passage using infiltration galleries: case study in Western Australia

Biodegradation of N-nitrosodimethylamine in soil from a water reclamation facility

Bioremediation Journal