Destruction of Estrogens Using Fe-TAML/Peroxide Catalysis

Nancy W. Shappell*†, Melanie A. Vrabel‡, Peter J. Madsen‡, Grant Harrington†, Lloyd O. Billey†, Heldur Hakk†, Gerald L. Larsen†, Evan S. Beach‡, Colin P. Horwitz‡, Kyoung Ro§, Patrick G. Hunt§ and Terrence J. Collins‡
Animal Metabolism Unit, Biosciences Research Laboratory, United States Department of Agriculture−Agricultural Research Service, 1605 Albrecht Boulevard, Fargo, North Dakota 58105, Institute for Green Oxidation Chemistry, Department of Chemistry, Carnegie Mellon University, 4400 Fifth Avenue, Pittsburgh, Pennsylvania 15213, and Coastal Plains Soil, Water and Plant Research Center, United States Department of Agriculture−Agricultural Research Service, 2611 West Lucas Street, Florence, South Carolina 29501
Environ. Sci. Technol., 2008, 42 (4), pp 1296–1300
DOI: 10.1021/es7022863
Publication Date (Web): January 16, 2008
Copyright © 2008 American Chemical Society
* Corresponding author phone: (701) 239-1233 ; fax: (701) 239-1430; e-mail: nancy.shappell@ars.usda.gov.
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†

Biosciences Research Laboratory, United States Department of Agriculture−Agricultural Research Service.

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‡

Carnegie Mellon University.

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§

Coastal Plains Soil, Water and Plant Research Center, United States Department of Agriculture−Agricultural Research Service.

Abstract

Endocrine disrupting chemicals (EDCs) impair living organisms by interfering with hormonal processes controlling cellular development. Reduction of EDCs in water by an environmentally benign method is an important green chemistry goal. One EDC, 17α-ethinylestradiol (EE2), the active ingredient in the birth control pill, is excreted by humans to produce a major source of artificial environmental estrogenicity, which is incompletely removed by current technologies used by municipal wastewater treatment plants (MWTPs). Natural estrogens found in animal waste from concentrated animal feeding operations (CAFOs) can also increase estrogenic activity of surface waters. An iron-tetraamidomacrocyclic ligand (Fe-TAML) activator in trace concentrations activates hydrogen peroxide and was shown to rapidly degrade these natural and synthetic reproductive hormones found in agricultural and municipal effluent streams. On the basis of liquid chromatography tandem mass spectrometry, apparent half-lives for 17 α- and 17 β-estradiol, estriol, estrone, and EE2 in the presence of Fe-TAML and hydrogen peroxide were approximately 5 min and included a concomitant loss of estrogenic activity as established by E-Screen assay.

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History

  • Published In Issue February 15, 2008
  • Article ASAPJanuary 16, 2008
  • Received: September 11, 2007
    Revised: November 29, 2007
    Accepted: December 4, 2007

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