Identification of transformation products during advanced oxidation of diatrizoate: Effect of water matrix and oxidation process

Sara P. Azerrad; Christian Lütke Eversloh; Maayan Gilboa; Manoj Schulz; Thomas Ternes; Carlos G. Dosoretz

doi:10.1016/j.watres.2016.07.066

Identification of transformation products during advanced oxidation of diatrizoate: Effect of water matrix and oxidation process

Sara P. Azerrad, Christian Lütke Eversloh, Maayan Gilboa, Manoj Schulz, Thomas Ternes, Carlos G. Dosoretz

Research output: Contribution to journal › Article › peer-review

Abstract

Removal of micropollutants from reverse osmosis (RO) brines of wastewater desalination by oxidation processes is influenced by the scavenging capacity of brines components, resulting in the accumulation of transformation products (TPs) rather than complete mineralization. In this work the iodinated contrast media diatrizoate (DTZ) was used as model compound due to its relative resistance to oxidation. Identification of TPs was performed in ultrapure water (UPW) and RO brines applying nonthermal plasma (NTP) and UVA-TiO ₂ as oxidation techniques. The influence of main RO brines components in the formation and accumulation of TPs, such as chloride, bicarbonate alkalinity and humic acid, was also studied during UVA-TiO ₂ . DTZ oxidation pattern in UPW resulted similar in both UVA-TiO ₂ and NTP achieving 66 and 61% transformation, respectively. However, DTZ transformation in RO brines was markedly lower in UVA-TiO ₂ (9%) than in NTP (27%). These differences can be attributed to the synergic effect of RO brines components during NTP. Moreover, reactive species other than hydroxyl radical contributed to DTZ transformation, i.e., direct photolysis in UVA-TiO ₂ and direct photolysis + O ₃ in NTP accounted for 16 and 23%, respectively. DTZ transformation led to iodide formation in both oxidation techniques but it further oxidized to iodate by ozone in NTP. In total 14 transformation products were identified in UPW of which 3 were present only in UVA-TiO ₂ and 2 were present exclusively in NTP; 5 of the 14 TPs were absent in RO brines. Five of them were new and were denoted as TP-474A/B, TP-522, TP-586, TP-602, TP-628. TP-522 (mono-chlorinated) was elucidated only in presence of high chloride titer-synthetic water matrix in NTP, most probably formed by active chlorine species generated in situ. TPs accumulation in RO brines was markedly different in comparison to UPW. This denotes the influence of RO brines components in the formation of reactive species that could further attack DTZ/TPs and/or scavenging performed by these brine components that could limit further TPs degradation. Five plausible degradation pathways are proposed for DTZ transformation in UPW.

Original language	English
Pages (from-to)	424-434
Number of pages	11
Journal	Water Research
Volume	103
DOIs	https://doi.org/10.1016/j.watres.2016.07.066
State	Published - 15 Oct 2016
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2016 Elsevier Ltd

Keywords

Advanced oxidation processes
Desalination brines
Diatrizoate
Nonthermal plasma
Titanium dioxide oxidation
Transformation products

ASJC Scopus subject areas

Environmental Engineering
Civil and Structural Engineering
Ecological Modeling
Water Science and Technology
Waste Management and Disposal
Pollution

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.watres.2016.07.066

Cite this

@article{7cab68421ca34e718975636e28d87733,

title = "Identification of transformation products during advanced oxidation of diatrizoate: Effect of water matrix and oxidation process",

abstract = " Removal of micropollutants from reverse osmosis (RO) brines of wastewater desalination by oxidation processes is influenced by the scavenging capacity of brines components, resulting in the accumulation of transformation products (TPs) rather than complete mineralization. In this work the iodinated contrast media diatrizoate (DTZ) was used as model compound due to its relative resistance to oxidation. Identification of TPs was performed in ultrapure water (UPW) and RO brines applying nonthermal plasma (NTP) and UVA-TiO 2 as oxidation techniques. The influence of main RO brines components in the formation and accumulation of TPs, such as chloride, bicarbonate alkalinity and humic acid, was also studied during UVA-TiO 2 . DTZ oxidation pattern in UPW resulted similar in both UVA-TiO 2 and NTP achieving 66 and 61% transformation, respectively. However, DTZ transformation in RO brines was markedly lower in UVA-TiO 2 (9%) than in NTP (27%). These differences can be attributed to the synergic effect of RO brines components during NTP. Moreover, reactive species other than hydroxyl radical contributed to DTZ transformation, i.e., direct photolysis in UVA-TiO 2 and direct photolysis + O 3 in NTP accounted for 16 and 23%, respectively. DTZ transformation led to iodide formation in both oxidation techniques but it further oxidized to iodate by ozone in NTP. In total 14 transformation products were identified in UPW of which 3 were present only in UVA-TiO 2 and 2 were present exclusively in NTP; 5 of the 14 TPs were absent in RO brines. Five of them were new and were denoted as TP-474A/B, TP-522, TP-586, TP-602, TP-628. TP-522 (mono-chlorinated) was elucidated only in presence of high chloride titer-synthetic water matrix in NTP, most probably formed by active chlorine species generated in situ. TPs accumulation in RO brines was markedly different in comparison to UPW. This denotes the influence of RO brines components in the formation of reactive species that could further attack DTZ/TPs and/or scavenging performed by these brine components that could limit further TPs degradation. Five plausible degradation pathways are proposed for DTZ transformation in UPW.",

keywords = "Advanced oxidation processes, Desalination brines, Diatrizoate, Nonthermal plasma, Titanium dioxide oxidation, Transformation products",

author = "Azerrad, {Sara P.} and {L{\"u}tke Eversloh}, Christian and Maayan Gilboa and Manoj Schulz and Thomas Ternes and Dosoretz, {Carlos G.}",

note = "Publisher Copyright: {\textcopyright} 2016 Elsevier Ltd",

year = "2016",

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day = "15",

doi = "10.1016/j.watres.2016.07.066",

language = "English",

volume = "103",

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T1 - Identification of transformation products during advanced oxidation of diatrizoate

T2 - Effect of water matrix and oxidation process

AU - Azerrad, Sara P.

AU - Lütke Eversloh, Christian

AU - Gilboa, Maayan

AU - Schulz, Manoj

AU - Ternes, Thomas

AU - Dosoretz, Carlos G.

PY - 2016/10/15

Y1 - 2016/10/15

N2 - Removal of micropollutants from reverse osmosis (RO) brines of wastewater desalination by oxidation processes is influenced by the scavenging capacity of brines components, resulting in the accumulation of transformation products (TPs) rather than complete mineralization. In this work the iodinated contrast media diatrizoate (DTZ) was used as model compound due to its relative resistance to oxidation. Identification of TPs was performed in ultrapure water (UPW) and RO brines applying nonthermal plasma (NTP) and UVA-TiO 2 as oxidation techniques. The influence of main RO brines components in the formation and accumulation of TPs, such as chloride, bicarbonate alkalinity and humic acid, was also studied during UVA-TiO 2 . DTZ oxidation pattern in UPW resulted similar in both UVA-TiO 2 and NTP achieving 66 and 61% transformation, respectively. However, DTZ transformation in RO brines was markedly lower in UVA-TiO 2 (9%) than in NTP (27%). These differences can be attributed to the synergic effect of RO brines components during NTP. Moreover, reactive species other than hydroxyl radical contributed to DTZ transformation, i.e., direct photolysis in UVA-TiO 2 and direct photolysis + O 3 in NTP accounted for 16 and 23%, respectively. DTZ transformation led to iodide formation in both oxidation techniques but it further oxidized to iodate by ozone in NTP. In total 14 transformation products were identified in UPW of which 3 were present only in UVA-TiO 2 and 2 were present exclusively in NTP; 5 of the 14 TPs were absent in RO brines. Five of them were new and were denoted as TP-474A/B, TP-522, TP-586, TP-602, TP-628. TP-522 (mono-chlorinated) was elucidated only in presence of high chloride titer-synthetic water matrix in NTP, most probably formed by active chlorine species generated in situ. TPs accumulation in RO brines was markedly different in comparison to UPW. This denotes the influence of RO brines components in the formation of reactive species that could further attack DTZ/TPs and/or scavenging performed by these brine components that could limit further TPs degradation. Five plausible degradation pathways are proposed for DTZ transformation in UPW.

AB - Removal of micropollutants from reverse osmosis (RO) brines of wastewater desalination by oxidation processes is influenced by the scavenging capacity of brines components, resulting in the accumulation of transformation products (TPs) rather than complete mineralization. In this work the iodinated contrast media diatrizoate (DTZ) was used as model compound due to its relative resistance to oxidation. Identification of TPs was performed in ultrapure water (UPW) and RO brines applying nonthermal plasma (NTP) and UVA-TiO 2 as oxidation techniques. The influence of main RO brines components in the formation and accumulation of TPs, such as chloride, bicarbonate alkalinity and humic acid, was also studied during UVA-TiO 2 . DTZ oxidation pattern in UPW resulted similar in both UVA-TiO 2 and NTP achieving 66 and 61% transformation, respectively. However, DTZ transformation in RO brines was markedly lower in UVA-TiO 2 (9%) than in NTP (27%). These differences can be attributed to the synergic effect of RO brines components during NTP. Moreover, reactive species other than hydroxyl radical contributed to DTZ transformation, i.e., direct photolysis in UVA-TiO 2 and direct photolysis + O 3 in NTP accounted for 16 and 23%, respectively. DTZ transformation led to iodide formation in both oxidation techniques but it further oxidized to iodate by ozone in NTP. In total 14 transformation products were identified in UPW of which 3 were present only in UVA-TiO 2 and 2 were present exclusively in NTP; 5 of the 14 TPs were absent in RO brines. Five of them were new and were denoted as TP-474A/B, TP-522, TP-586, TP-602, TP-628. TP-522 (mono-chlorinated) was elucidated only in presence of high chloride titer-synthetic water matrix in NTP, most probably formed by active chlorine species generated in situ. TPs accumulation in RO brines was markedly different in comparison to UPW. This denotes the influence of RO brines components in the formation of reactive species that could further attack DTZ/TPs and/or scavenging performed by these brine components that could limit further TPs degradation. Five plausible degradation pathways are proposed for DTZ transformation in UPW.

KW - Advanced oxidation processes

KW - Desalination brines

KW - Diatrizoate

KW - Nonthermal plasma

KW - Titanium dioxide oxidation

KW - Transformation products

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Identification of transformation products during advanced oxidation of diatrizoate: Effect of water matrix and oxidation process

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

UN SDGs

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