Abstract

17α-ethinylestradiol (EE2), a synthetic oestrogen in oral contraceptives, is one of many pharmaceuticals found in inland waterways worldwide as a result of human consumption and excretion into wastewater treatment systems. At low parts per trillion (ppt), EE2 induces feminisation of male fish, diminishing reproductive success and causing fish population collapse. Intended water quality standards for EE2 set a much needed global precedent. Ozone and activated carbon provide effective wastewater treatments, but their energy intensities and capital/operating costs are formidable barriers to adoption. Here we describe the technical and environmental performance of a fast- developing contender for mitigation of EE2 contamination of wastewater based upon small- molecule, full-functional peroxidase enzyme replicas called “TAML activators”. From neutral to basic pH, TAML activators with H2O2 efficiently degrade EE2 in pure lab water, municipal effluents and EE2-spiked synthetic urine. TAML/H2O2 treatment curtails estrogenicity in vitro and substantially diminishes fish feminization in vivo. Our results provide a starting point for a future process in which tens of thousands of tonnes of wastewater could be treated per kilogram of catalyst. We suggest TAML/H2O2 is a worthy candidate for exploration as an environmentally compatible, versatile, method for removing EE2 and other pharmaceuticals from municipal wastewaters.

Highlights

  • Increasing evidence suggests that the presence of trace levels of pharmaceuticals in the environment can vitiate ecologies[1]

  • Considered one of the biggest public health accomplishments of the 20th century, current wastewater treatment systems are not sustainable options for removing pharmaceuticals: Treatment by Activated Sludge Process (ASP) has proven to be inadequate at removing numerous pharmaceuticals creating the need for advanced treatment options

  • A technically effective, environmentally compatible and cost-effective way to overcome the impracticality of using ozone or activated carbon (AC) for removing pharmaceuticals from wastewater may come from treatment with hydrogen peroxide catalysed by extremely efficient TAML catalysts

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Summary

Introduction

Increasing evidence suggests that the presence of trace levels of pharmaceuticals in the environment can vitiate ecologies[1]. In vivo toxicity tests using embryonic zebrafish suggest TAML is not overtly toxic to fish[23] and in vitro tests show TAML itself does not show inherent endocrine disrupting activity[24] Taken together, these studies set the stage for the current multidisciplinary, cross-sector study to investigate the removal of EE2 from both laboratory waters and real wastewater, under more environmentally appropriate conditions. These studies set the stage for the current multidisciplinary, cross-sector study to investigate the removal of EE2 from both laboratory waters and real wastewater, under more environmentally appropriate conditions These include neutral pH, lower hydrogen peroxide concentrations and estrogen concentrations of more than a million-fold lower than previously tested, which are much more environmentally relevant and still ecotoxic to fish

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