title: Removal of ecotoxicity of 17α-ethinylestradiol using TAML/peroxide water treatment.
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.
authors.affiliation: Institute for Green Science and Department of Chemistry, Carnegie Mellon University, 4400 Fifth Avenue, Pittsburgh PA 15213.
authors.forename: Matthew R
authors.initials: MR
authors.lastname: Mills
authors.affiliation: Institute for Green Science and Department of Chemistry, Carnegie Mellon University, 4400 Fifth Avenue, Pittsburgh PA 15213.
authors.forename: Karla
authors.initials: K
authors.lastname: Arias-Salazar
authors.affiliation: Institute of Environment, Health and Societies, Brunel University London, Uxbridge, Middlesex UB83PH, UK.
authors.forename: Alice
authors.initials: A
authors.lastname: Baynes
authors.affiliation: Institute for Green Science and Department of Chemistry, Carnegie Mellon University, 4400 Fifth Avenue, Pittsburgh PA 15213.
authors.forename: Longzhu Q
authors.initials: LQ
authors.lastname: Shen
authors.affiliation: Institute of Environment, Health and Societies, Brunel University London, Uxbridge, Middlesex UB83PH, UK.
authors.forename: John
authors.initials: J
authors.lastname: Churchley
authors.affiliation: Institute of Environment, Health and Societies, Brunel University London, Uxbridge, Middlesex UB83PH, UK.
authors.forename: Nicola
authors.initials: N
authors.lastname: Beresford
authors.affiliation: Institute for Green Science and Department of Chemistry, Carnegie Mellon University, 4400 Fifth Avenue, Pittsburgh PA 15213.
authors.forename: Chakicherla
authors.initials: C
authors.lastname: Gayathri
authors.affiliation: Institute for Green Science and Department of Chemistry, Carnegie Mellon University, 4400 Fifth Avenue, Pittsburgh PA 15213.
authors.forename: Roberto R
authors.initials: RR
authors.lastname: Gil
authors.affiliation: Institute of Environment, Health and Societies, Brunel University London, Uxbridge, Middlesex UB83PH, UK.
authors.forename: Rakesh
authors.initials: R
authors.lastname: Kanda
authors.affiliation: Institute of Environment, Health and Societies, Brunel University London, Uxbridge, Middlesex UB83PH, UK.
authors.forename: Susan
authors.initials: S
authors.lastname: Jobling
authors.affiliation: Institute for Green Science and Department of Chemistry, Carnegie Mellon University, 4400 Fifth Avenue, Pittsburgh PA 15213.
authors.forename: Terrence J
authors.initials: TJ
authors.lastname: Collins
mesh_terms: D002606:Charcoal / Q000737:chemistry; D004997:Ethinyl Estradiol / Q000737:chemistry*; D006861:Hydrogen Peroxide / Q000737:chemistry*; D010126:Ozone / Q000737:chemistry; D062065:Wastewater / Q000737:chemistry*; D014873:Water Pollutants / Q000737:chemistry*; D018508:Water Purification / Q000379:methods*
chemical_list: D002606:Charcoal; D004997:Ethinyl Estradiol; D006861:Hydrogen Peroxide; D010126:Ozone; D062065:Wastewater; D014873:Water Pollutants