Ferrate(VI) oxidation of β-lactam antibiotics: reaction kinetics, antibacterial activity changes, and transformation products

Environ Sci Technol. 2014 Sep 2;48(17):10380-9. doi: 10.1021/es5028426. Epub 2014 Aug 18.

Abstract

Oxidation of β-lactam antibiotics by aqueous ferrate(VI) was investigated to determine reaction kinetics, reaction sites, antibacterial activity changes, and transformation products. Apparent second-order rate constants (kapp) were determined in the pH range 6.0-9.5 for the reaction of ferrate(VI) with penicillins (amoxicillin, ampicillin, cloxacillin, and penicillin G), a cephalosporin (cephalexin), and several model compounds. Ferrate(VI) shows an appreciable reactivity toward the selected β-lactams (kapp for pH 7 = 110-770 M(-1) s(-1)). The pH-dependent kapp could be well explained by considering species-specific reactions between ferrate(VI) and the β-lactams (with reactions occurring at thioether, amine, and/or phenol groups). On the basis of the kinetic results, the thioether is the main reaction site for cloxacillin and penicillin G. In addition to the thioether, the amine is a reaction site for ampicillin and cephalexin, and amine and phenol are reaction sites for amoxicillin. HPLC/MS analysis showed that the thioether of β-lactams was transformed to stereoisomeric (R)- and (S)-sulfoxides and then to a sulfone. Quantitative microbiological assay of ferrate(VI)-treated β-lactam solutions indicated that transformation products resulting from the oxidation of cephalexin exhibited diminished, but non-negligible residual activity (i.e., ∼24% as potent as the parent compound). For the other β-lactams, the transformation products showed much lower (<5%) antibacterial potencies compared to the parent compounds. Overall, ferrate(VI) oxidation appears to be effective as a means of lowering the antibacterial activities of β-lactams, although alternative approaches may be necessary to achieve complete elimination of cephalosporin activities.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Anti-Bacterial Agents / chemistry*
  • Anti-Bacterial Agents / pharmacology*
  • Bacillus subtilis / drug effects
  • Biotransformation / drug effects
  • Hydrogen-Ion Concentration
  • Iron / chemistry*
  • Kinetics
  • Microbial Sensitivity Tests
  • Oxidation-Reduction
  • Phenols / chemistry
  • Wastewater / chemistry
  • beta-Lactams / chemistry*
  • beta-Lactams / pharmacology*

Substances

  • Anti-Bacterial Agents
  • Phenols
  • Waste Water
  • beta-Lactams
  • ferrate ion
  • Iron