Submitted to: Environmental Science and Technology
Publication Type: Peer Reviewed Journal
Publication Acceptance Date: 12/4/2007
Publication Date: 2/15/2008
Citation: Shappell, N.W., Vrabel, M.A., Madsen, P.J., Harrington, G.E., Billey, L.O., Hakk, H., Larsen, G.L., Beach, E.S., Horwitz, C.P., Ro, K.S., Hunt, P.G., Collins, T.J. 2008. Destruction of estrogens using Fe-TAML/peroxide catalysis. Environmental Science and Technology 42:1296-1300. Interpretive Summary: Endocrine disrupting chemicals (EDCs) impair living organisms by interfering with hormonal processes controlling cellular development. Reducing EDCs by an environmentally friendly method is an important green chemistry goal. The challenge is most pressing for widely used EDCs such as 17alpha-ethinylestradiol (EE2), the active ingredient in the birth control pill, which is excreted by humans to produce a major source of artificial environmental estrogenicity. Worldwide, surface waters are impacted by EE2, which is incompletely removed by current technologies used by sewage treatment plants (STPs) in addition to natural estrogens found in animal waste from concentrated animal feeding operations (CAFOs). Here we show that an Fe-TAML (iron-tetraamidomacrocyclic ligand) activator in trace concentrations activates hydrogen peroxide to rapidly degrade natural and synthetic reproductive hormones in water. The results demonstrate that Fe-TAML/peroxide could remove the major natural and synthetic estrogens from agricultural and municipal waste streams.
Technical 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, 17 alpha-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. Based on liquid chromatography tandem mass spectrometry, apparent half-lives for 17 alpha- and 17 beta-estradiol, estriol, estrone and EE2 in the presence of Fe-TAML and hydrogen peroxide were approximately five minutes, and included a concomitant loss of estrogenic activity as established by E-Screen assay.