TY - JOUR
T1 - Effects of common groundwater ions on the transformation and reactivity of sulfidized nanoscale zerovalent iron
AU - Mangayayam, Marco C.
AU - Alonso-de-Linaje, Virginia
AU - Dideriksen, Knud
AU - Tobler, Dominique J.
N1 - Funding Information:
This research was funded by Metal-Aid Innovative Training Network ( ITN ), supported by a grant from the European Commission ’s Marie Skɫowdowska Curie Actions program under project number 675219 . The authors thank Olaf Borkiewicz, Leighanne Gallington, and Kevin A. Beyer for support with X-ray total scattering measurements at APS beamline 11 ID-B, Argonne, USA. We also thank Theis Brock-Nannestad for support with GC-MS measurements. We acknowledge Eric Querat (Consorci del Parc Agrari del Baix Llobregat), Shikhar Nilabh (Amphos 21), Markus Reischer (Niras, Denmark) and Niels Døssing Overheu (Capital Region of Denmark) for their help with groundwater collection and for providing us part of the groundwater composition data. Part of the data was acquired at Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357. Support for travel to the synchrotron facility came from the Danish Council for Independent Research (via DANSCATT).
Funding Information:
This research was funded by Metal-Aid Innovative Training Network (ITN), supported by a grant from the European Commission's Marie Sk?owdowska Curie Actions program under project number 675219. The authors thank Olaf Borkiewicz, Leighanne Gallington, and Kevin A. Beyer for support with X-ray total scattering measurements at APS beamline 11 ID-B, Argonne, USA. We also thank Theis Brock-Nannestad for support with GC-MS measurements. We acknowledge Eric Querat (Consorci del Parc Agrari del Baix Llobregat), Shikhar Nilabh (Amphos 21), Markus Reischer (Niras, Denmark) and Niels D?ssing Overheu (Capital Region of Denmark) for their help with groundwater collection and for providing us part of the groundwater composition data. Part of the data was acquired at Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357. Support for travel to the synchrotron facility came from the Danish Council for Independent Research (via DANSCATT).
Publisher Copyright:
© 2020 The Authors
PY - 2020/6
Y1 - 2020/6
N2 - Sulfidized nanoscale zerovalent iron (S-nZVI) is an Fe-based reactant widely studied for its potential use for groundwater remediation. S-nZVI reactivity has been widely investigated testing various contaminants in various water matrices, but studies on S-nZVI corrosion behaviour and reactivity upon exposure to complex groundwater chemistries are limited. Here, we show that anoxic aging of S-nZVI for 7 days in the absence and presence of key groundwater solutes (i.e., Cl−, SO42−, Mg2+, Ca2+, HCO3−, CO32−, NO3−, or HPO42−) impacts Fe0 corrosion extent, corrosion product and reduction rates with trichloroethene (TCE). White rust was the dominant corrosion product in ultrapure water and in SO42−, Cl−, Mg2+ or Ca2+ solutions; green rust and/or chukanovite formed in HCO3− and CO32− solutions; magnetite, formed in NO3− solutions and vivianite in HPO42− solutions. The aged S-nZVI materials expectedly showed lower reactivities with TCE compared to unaged S-nZVI, with reaction rates mainly controlled by ion concentration, Fe0 corrosion extent, type(s) of corrosion product, and solution pH. Comparison of these results to observations in two types of groundwaters, one from a carbonate-rich aquifer and one from a marine intruded aquifer, showed that S-nZVI corrosion products are likely controlled by the dominant GW solutes, while reactivity with TCE is generally lower than expected, due to the multitude of ion effects. Overall, these results highlight that S-nZVI corrosion behaviour in GW can be manifold, with varied impact on its reactivity. Thus, testing of S-nZVI stability and reactivity under expected field conditions is key to understand its longevity in remediation applications.
AB - Sulfidized nanoscale zerovalent iron (S-nZVI) is an Fe-based reactant widely studied for its potential use for groundwater remediation. S-nZVI reactivity has been widely investigated testing various contaminants in various water matrices, but studies on S-nZVI corrosion behaviour and reactivity upon exposure to complex groundwater chemistries are limited. Here, we show that anoxic aging of S-nZVI for 7 days in the absence and presence of key groundwater solutes (i.e., Cl−, SO42−, Mg2+, Ca2+, HCO3−, CO32−, NO3−, or HPO42−) impacts Fe0 corrosion extent, corrosion product and reduction rates with trichloroethene (TCE). White rust was the dominant corrosion product in ultrapure water and in SO42−, Cl−, Mg2+ or Ca2+ solutions; green rust and/or chukanovite formed in HCO3− and CO32− solutions; magnetite, formed in NO3− solutions and vivianite in HPO42− solutions. The aged S-nZVI materials expectedly showed lower reactivities with TCE compared to unaged S-nZVI, with reaction rates mainly controlled by ion concentration, Fe0 corrosion extent, type(s) of corrosion product, and solution pH. Comparison of these results to observations in two types of groundwaters, one from a carbonate-rich aquifer and one from a marine intruded aquifer, showed that S-nZVI corrosion products are likely controlled by the dominant GW solutes, while reactivity with TCE is generally lower than expected, due to the multitude of ion effects. Overall, these results highlight that S-nZVI corrosion behaviour in GW can be manifold, with varied impact on its reactivity. Thus, testing of S-nZVI stability and reactivity under expected field conditions is key to understand its longevity in remediation applications.
KW - Aging
KW - Corrosion
KW - Metallic iron
KW - Remediation
KW - Sulfide
KW - Trichloroethene
UR - http://www.scopus.com/inward/record.url?scp=85079148784&partnerID=8YFLogxK
U2 - 10.1016/j.chemosphere.2020.126137
DO - 10.1016/j.chemosphere.2020.126137
M3 - Article
C2 - 32058137
AN - SCOPUS:85079148784
SN - 0045-6535
VL - 249
JO - Chemosphere
JF - Chemosphere
M1 - 126137
ER -