On-line measurement of oxidative degradation kinetics for trace gasoline contaminants in aqueous solutions and natural water by membrane introduction tandem mass spectrometry

J Environ Sci Health A Tox Hazard Subst Environ Eng. 2010 Nov;45(13):1720-31. doi: 10.1080/10934529.2010.513250.

Abstract

Membrane introduction mass spectrometry (MIMS) was used to directly monitor the loss of trace gasoline contaminants (benzene, toluene, 2-methylthiophene and methylcyclohexane) in nanomolar (ppb) aqueous solutions under a variety of UV-induced advanced oxidation processes (AOP). The decay kinetics of these contaminants were followed simultaneously in "real-time" via tandem mass spectrometric techniques by re-circulating the reaction mixture in a closed loop over a semi-permeable membrane interface. The photocatalyzed degradations were observed to follow pseudo-first-order kinetics with rate constants ranging from 0.006 to 0.2 min⁻¹ depending on the reaction conditions. We report rate enhancements for several UV-based advanced oxidative processes using physiosorbed titanium dioxide (TiO₂/UV, TiO₂/UV/O₂, TiO₂/UV/H₂O₂) and compare these to the direct photolysis of H₂O₂ under otherwise identical conditions. The relative degradation rates of 4 trace contaminants are reported for reactions carried out in the same solution. The degradation kinetics were also monitored directly in a natural surface water spiked with the same contaminant suite. The observed decay kinetics in the presence of TiO₂ in air-saturated natural water were similar to those carried out in deionized water. However, when the photo-oxidation was enhanced by the addition of H₂O₂, the degradation was markedly slower in natural water relative to deionized water due to competition for photons by dissolved organic matter. This work further demonstrates the use of MIMS as a sensitive on-line measurement technique for "in-situ" reaction monitoring of organic contaminants at environmentally relevant concentrations in complex solutions and reactive media.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Gasoline*
  • Kinetics
  • Oxidation-Reduction
  • Tandem Mass Spectrometry / methods*
  • Water Pollutants, Chemical / chemistry*

Substances

  • Gasoline
  • Water Pollutants, Chemical