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Elucidating the dechlorination mechanism of hexachloroethane by Pd-doped zerovalent iron microparticles in dissolved lactic acid polymers using chromatography and indirect monitoring of iron corrosion

  • Romain RodriguesEmail author
  • Stéphanie Betelu
  • Stéfan Colombano
  • Guillaume Masselot
  • Theodore Tzedakis
  • Ioannis Ignatiadis
Research Article
  • 95 Downloads

Abstract

The degradation mechanism of the pollutant hexachloroethane (HCA) by a suspension of Pd-doped zerovalent iron microparticles (Pd-mZVI) in dissolved lactic acid polymers and oligomers (referred to as PLA) was investigated using gas chromatography and the indirect monitoring of iron corrosion by continuous measurements of pH, oxidation-reduction potential (ORP), and conductivity. The first experiments took place in the absence of HCA, to understand the evolution of the Pd-mZVI/PLA/H2O system. This showed that the evolution of pH, ORP, and conductivity is related to changes in solution chemistry due to iron corrosion and that the system is initially cathodically controlled by H+ mass transport to Pd surfaces because of the presence of an extensive PLA layer. We then investigated the effects of Pd-mZVI particles, temperature, initial HCA concentration, and PLA content on the Pd-mZVI/PLA/HCA/H2O system, to obtain a better understanding of the degradation mechanism. In all cases, HCA dechlorination first requires the production of atomic hydrogen H*—involving the accumulation of tetrachloroethylene (PCE) as an intermediate—before its subsequent reduction to non-chlorinated C2 and C4 compounds. The ratio between Pd-mZVI dosage, initial HCA concentration, and PLA content affects the rate of H* generation as well as the rate-determining step of the process. A pseudo-first-order equation can be applied when Pd-mZVI dosage is much higher than the theoretical stoichiometry (600 mg for [HCA]0 = 5–20 mg L−1). Our results indicate that the HCA degradation mechanism includes mass transfer, sorption, surface reaction with H*, and desorption of the product.

Keywords

Hexachloroethane Pd/Fe microparticles Iron corrosion Physical and chemical monitoring Dechlorination mechanism Lactic acid polymers 

Notes

Acknowledgements

This work was supported by the French Environment and Energy Management Agency (ADEME) and the French Geological Survey (BRGM) within the framework of the AMI SILPHES project coordinated by David Cazaux (Inovyn Tavaux). The authors acknowledge Benoit Castermans (Biorem Engineering) for providing Pd-mZVI particles and PLA, Nicolas Maubec (BRGM) for performing XRD analyses, and Christian Perruchot and Philippe Decorse (ITODYS laboratory, Université Paris Diderot) for performing XPS analyses. Romain Rodrigues thanks Chérif Morcos for fruitful discussions. The authors thank the anonymous reviewers for their helpful comments and suggestions. H.M. Kluijver edited the English language of the final MS.

Compliance with ethical standards

Conflict of interest

None.

Supplementary material

11356_2019_4128_MOESM1_ESM.docx (10.1 mb)
ESM 1 (DOCX 10373 kb)

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Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

  1. 1.BRGM (French Geological Survey)Orléans Cedex 2France
  2. 2.ADEME (French Environment and Energy Management Agency)Angers Cedex 1France
  3. 3.LGC (Chemical Engineering Laboratory)Toulouse Cedex 9France
  4. 4.Iris InstrumentsOrléansFrance

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