ORCID Profile
0000-0002-6937-4671
Current Organisations
University of Western Australia
,
CSIRO Waterford
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Organometallic Chemistry | Organic Chemistry | Natural Products Chemistry | Organic Chemical Synthesis
Expanding Knowledge in the Environmental Sciences | Expanding Knowledge in the Chemical Sciences | Expanding Knowledge in the Biological Sciences |
Publisher: American Chemical Society (ACS)
Date: 29-10-2018
Abstract: Chlorine dioxide (ClO
Publisher: American Chemical Society (ACS)
Date: 06-2018
Abstract: Oxidative treatment of iodide-containing waters can form toxic iodinated disinfection byproducts (I-DBPs). To better understand the fate of iodine, kinetics, products, and stoichiometries for the reactions of ferrate(VI) with iodide (I
Publisher: Wiley
Date: 30-03-2022
DOI: 10.5694/MJA2.51481
Publisher: Elsevier BV
Date: 04-2021
Publisher: Elsevier BV
Date: 07-2018
DOI: 10.1016/J.WATRES.2018.03.026
Abstract: Silver impregnated activated carbon (SIAC) has been found to be effective in mitigating the formation of brominated-disinfection by products during drinking water treatment. However, there are still uncertainties regarding its silver leaching properties, and strategies for the prevention of silver leaching have remained elusive. This study focused on the evaluation of one type of commercially available SIAC for its ability to remove bromide while minimising silver leaching from the material. Both synthetic and real water matrices were tested. Depending on solution pH, it was found that changing the surface charge properties of SIAC, as measured by the point of zero charge pH, can result in additional bromide removal while minimising the extent of silver leaching. To better understand the mechanism of silver leaching from the SIAC, eight preconditioning environments, i.e. variable pH and ionic strength were tested for a fixed amount of SIAC and two preconditioning environments were selected for a more detailed investigation. Experiments carried out in synthetic water showed that preconditioning at pH 10.4 did not deteriorate the capacity of SIAC to remove bromide, but significantly decreased the release of silver in the form of ionic silver (Ag
Publisher: Wiley
Date: 23-03-2022
DOI: 10.5694/MJA2.51461
Publisher: Elsevier BV
Date: 10-2013
DOI: 10.1016/J.SCITOTENV.2013.05.079
Abstract: Methyl iodide is a well-known volatile halogenated organic compound that contributes to the iodine content in the troposphere, potentially resulting in damage to the ozone layer. Most methyl iodide sources derive from biological activity in oceans and soils with very few abiotic mechanisms proposed in the literature. In this study we report that synthetic manganese oxide (birnessite δ-MnO2) can catalyze the formation of methyl iodide in the presence of natural organic matter (NOM) and iodide. Methyl iodide formation was only observed at acidic pH (4-5) where iodide is oxidized to iodine and NOM is adsorbed on δ-MnO2. The effect of δ-MnO2, iodide and NOM concentrations, nature of NOM and ionic strength was investigated. High concentrations of methyl iodide were formed in experiments conducted with the model compound pyruvate. The Lewis acid property of δ-MnO2 leads to a polarization of the iodine molecule, and catalyzes the reaction with natural organic matter. As manganese oxides are strong oxidants and are ubiquitous in the environment, this mechanism could significantly contribute to the global atmospheric input of iodine.
Publisher: Elsevier BV
Date: 04-2013
DOI: 10.1016/J.WATRES.2012.12.002
Abstract: The presence of iodinated disinfection by-products (I-DBPs) in drinking water poses a potential health concern since it has been shown that I-DBPs are generally more genotoxic and cytotoxic than their chlorinated and brominated analogs. I-DBPs are formed during oxidation/disinfection of iodide-containing waters by reaction of the transient hypoiodous acid (HOI) with natural organic matter (NOM). In this study, we demonstrate that ozone pre-treatment selectively oxidizes iodide to iodate and avoids the formation of I-DBPs. Iodate is non-toxic and is therefore a desired sink of iodine in drinking water. Complete conversion of iodide to iodate while minimizing the bromate formation to below the guideline value of 10 μg L⁻¹ was achieved for a wide range of ozone doses in five raw waters with DOC and bromide concentrations of 1.1-20 mg L⁻¹ and 170-940 μg L⁻¹, respectively. Lowering the pH effectively further reduced bromate formation but had no impact on the extent of iodate and bromoform formation (the main trihalomethane (THM) formed during ozonation). Experiments carried out with pre-chlorinated ost-clarified s les already containing I-DBPs, showed that ozonation effectively oxidized I-THMs. Therefore, in iodide-containing waters, in which I-DBPs can be produced upon chlorination or especially chloramination, a pre-ozonation step to oxidize iodide to iodate is an efficient process to mitigate I-DBP formation.
Publisher: Elsevier BV
Date: 2016
DOI: 10.1016/J.SCITOTENV.2015.10.043
Abstract: The impact of elevated bromide concentrations (399 to 750 μg/L) on the formation of halogenated disinfection by-products (DBPs), namely trihalomethanes, haloacetic acids, haloacetonitriles, and adsorbable organic halogen (AOX), in two drinking water systems was investigated. Bromine was the main halogen incorporated into all of the DBP classes and into organic carbon, even though chlorine was present in large excess to maintain a disinfectant residual. Due to the higher reactivity of bromine compared to chlorine, brominated DBPs were rapidly formed, followed by a slower increase in chlorinated DBPs. Higher bromine substitution and incorporation factors for in idual DBP classes were observed for the chlorinated water from the groundwater source (lower concentration of dissolved organic carbon (DOC)), which contained a higher concentration of bromide, than for the surface water source (higher DOC). The molar distribution of adsorbable organic bromine to chlorine (AOBr/AOCl) for AOX in the groundwater distribution system was 1.5:1 and almost 1:1 for the surface water system. The measured (regulated) DBPs only accounted for 16 to 33% of the total organic halogen, demonstrating that AOX measurements are essential to provide a full understanding of the formation of halogenated DBPs in drinking waters. In addition, the study demonstrated that a significant proportion (up to 94%) of the bromide in source waters can be converted AOBr. An evaluation of AOBr and AOCl through a second groundwater treatment plant that uses conventional treatment processes for DOC removal produced 70% of AOX as AOBr, with 69% of the initial source water bromide converted to AOBr. Exposure to organobromine compounds is suspected to result in greater adverse health consequences than their chlorinated analogues. Therefore, this study highlights the need for improved methods to selectively reduce the bromide content in source waters.
Publisher: Copernicus GmbH
Date: 25-10-2023
DOI: 10.5194/AR-1-17-2023
Publisher: Elsevier BV
Date: 05-2012
DOI: 10.1016/J.CHROMA.2012.03.020
Abstract: Trihalomethanes are predominantly formed during disinfection of water via reactions of the oxidant with natural organic matter. Even though chlorinated and brominated trihalomethanes are the most widespread organic contaminants in drinking water, when iodide is present in raw water iodinated trihalomethanes can also be formed. The formation of iodinated trihalomethanes can lead to taste and odor problems and is a potential health concern since they have been reported to be more toxic than their brominated or chlorinated analogs. Currently, there is no published standard analytical method for I-THMs in water. The analysis of 10 trihalomethanes in water s les in a single run is challenging because the iodinated trihalomethanes are found at very low concentrations (ng/L range), while the regulated chlorinated and brominated trihalomethanes are present at much higher concentrations (above μg/L). An automated headspace solid-phase microextraction technique, with a programmed temperature vaporizer inlet coupled with gas chromatography-mass spectrometry, was developed for routine analysis of 10 trihalomethanes i.e. bromo-, chloro- and iodo-trihalomethanes in water s les. The carboxen olydimethylsiloxane/ inylbenzene fiber was found to be the most suitable. The optimization, linearity range, accuracy and precision of the method are discussed. The limits of detection range from 1 ng/L to 20 ng/L for iodoform and chloroform, respectively. Matrix effects in treated groundwater, surfacewater, seawater, and secondary wastewater were investigated and it was shown that the method is suitable for the analysis of trace levels of iodinated trihalomethanes in a wide range of waters. The method developed in the present study has the advantage of being rapid, simple and sensitive. A survey conducted throughout various process stages in an advanced water recycling plant showed the presence of iodinated trihalomethanes at ng/L levels.
Publisher: Elsevier BV
Date: 08-2009
DOI: 10.1016/J.WATRES.2009.05.018
Abstract: The oxidation of iodide by synthetic birnessite (delta-MnO(2)) was studied in perchlorate media in the pH range 4-8. Iodine (I(2)) was detected as an oxidation product that was subsequently further oxidized to iodate (IO(3)(-)). The third order rate constants, second order on iodide and first order on manganese oxide, determined by extraction of iodine in benzene decreased with increasing pH (6.3-7.5) from 1790 to 3.1M(-2) s(-1). Both iodine and iodate were found to adsorb significantly on birnessite with an adsorption capacity of 12.7 microM/g for iodate at pH 5.7. The rate of iodine oxidation by birnessite decreased with increasing ionic strength, which resulted in a lower rate of iodate formation. The production of iodine in iodide-containing waters in contact with manganese oxides may result in the formation of undesired iodinated organic compounds (taste and odor, toxicity) in natural and technical systems. The probability of the formation of such compounds is highest in the pH range 5-7.5. For pH 7.5, iodide is not oxidized to a significant extent.
Publisher: American Chemical Society (ACS)
Date: 21-06-2012
DOI: 10.1021/ES301301G
Abstract: The kinetics of iodate formation is a critical factor in mitigation of the formation of potentially toxic and off flavor causing iodoorganic compounds during chlorination. This study demonstrates that the formation of bromine through the oxidation of bromide by chlorine significantly enhances the oxidation of iodide to iodate in a bromide-catalyzed process. The pH-dependent kinetics revealed species specific rate constants of k(HOBr + IO(-)) = 1.9 × 10(6) M(-1) s(-1), k(BrO(-) + IO(-)) = 1.8 × 10(3) M(-1) s(-1), and k(HOBr + HOI) < 1 M(-1) s(-1). The kinetics and the yield of iodate formation in natural waters depend mainly on the naturally occurring bromide and the type and concentration of dissolved organic matter (DOM). The process of free chlorine exposure followed by ammonia addition revealed that the formation of iodo-trihalomethanes (I-THMs), especially iodoform, was greatly reduced by an increase of free chlorine exposure and an increase of the Br(-)/I(-) ratio. In water from the Great Southern River (with a bromide concentration of 200 μg/L), the relative I-incorporation in I-THMs decreased from 18 to 2% when the free chlorine contact time was increased from 2 to 20 min (chlorine dose of 1 mg Cl(2)/L). This observation is inversely correlated with the conversion of iodide to iodate, which increased from 10 to nearly 90%. Increasing bromide concentration also increased the conversion of iodide to iodate: from 45 to nearly 90% with a bromide concentration of 40 and 200 μg/L, respectively, and a prechlorination time of 20 min, while the I-incorporation in I-THMs decreased from 10 to 2%.
Publisher: American Chemical Society (ACS)
Date: 28-11-2022
Abstract: Ferrate (Fe(VI)) is a novel oxidant that can be used to mitigate disinfection byproduct (DBP) precursors. However, the reaction of Fe(VI) with organic nitrogen, which is a potential precursor of potent nitrogenous DBPs, remains largely unexplored. The present work aimed to identify the kinetics and products for the reaction of Fe(VI) with primary amines, notably amino acids. A new kinetic model involving ionizable intermediates was proposed and can describe the unusual pH effect on the Fe(VI) reactivity toward primary amines and amino acids. The Fe(VI) oxidation of phenylalanine produced a mixture of nitrile, nitrite/nitrate, amide, and ammonia, while nitroalkane was an additional product in the case of glycine. The product distribution for amino acids significantly differed from that of uncarboxylated primary amines that mainly generate nitriles. A general reaction pathway for primary amines and amino acids was proposed and notably involved the formation of imines, the degradation of which was affected by the presence of a carboxylic group. In comparison, ozonation led to higher yields of nitroalkanes that could be readily converted to potent halonitroalkanes during chlor(
Publisher: Elsevier BV
Date: 08-2010
DOI: 10.1016/J.WATRES.2010.06.008
Abstract: This paper demonstrates that manganese oxides can initiate the formation of methyl iodide, a volatile compound that participates to the input of iodine into the atmosphere. The formation of methyl iodide was investigated using a natural manganese oxide in batch experiments for different conditions and concentrations of iodide, natural organic matter (NOM) and manganese oxide. Methyl iodide was formed at concentrations <or=1 microg L(-1) for initial iodide concentrations ranging from 0.8 to 38.0 mg L(-1). The production of methyl iodide increased with increasing initial concentrations of iodide ion and Mn sand and when pH decreased from 7 to 5. The hydrophilic NOM isolate exhibited the lowest yield of methyl iodide whereas hydrophobic NOM isolates such as Suwannee River HPOA fraction produced the highest concentration of methyl iodide. The formation of methyl iodide could take place through the oxidation of NOM on manganese dioxide in the presence of iodide. However, the implication of elemental iodine cannot be excluded at acidic pH. Manganese oxides can then participate with ferric oxides to the formation of methyl iodide in soils and sediments. The formation of methyl iodide is unlikely in technical systems such as drinking water treatment i.e. for ppt levels of iodide and low contact times with manganese oxides.
Publisher: Copernicus GmbH
Date: 30-06-2023
DOI: 10.5194/AR-2023-6
Abstract: Abstract. Introduction: Electronic cigarettes (e-cigarettes) lack regulatory status as therapeutic products in all jurisdictions worldwide. They are potentially unsafe consumer products, with significant evidence showing they pose a risk to human health. Therefore, developing rapid, economical test methods to assess the chemical composition of e-liquids in heated and unheated forms and the aerosols produced by e-cigarettes is crucial. Methods: Four different e-liquids were heated using two different methods: 1) “typical” vaping using an e-cigarette device, by cycling “on” for three seconds every minute for two hours (e-liquid obtained from the remainder in the tank and aerosol collected in an impinger) and, 2) “accelerated” heating, using an e-cigarette coil, submerged in e-liquid, and heating in short 20 second bursts “on” then 20 seconds “off” for two minutes only (liquid traps aerosol produced). All e-liquids were then analyzed to test for the presence and quantity of 13 chemicals by gas-chromatography mass-spectrometry and compared to an unheated s le. Results: E-liquids heated with the “accelerated” method showed a comparable trend to the “typical” heating method, of increase or decrease in chemical compound quantity, for greater than two-thirds of the detected compounds analyzed over all e-liquids. Six chemicals were detected as aerosol from the impinger fluid with the “typical” heating method, most at negligible levels. Conclusion: We propose this rapid method could form the basis of a standardized screening tool to test heated e-liquids (and e-cigarette aerosols) for harmful or banned substances to ensure only approved products reach the consumer, and the potential harms of e-cigarette use are reduced.
Publisher: American Chemical Society (ACS)
Date: 12-08-2009
DOI: 10.1021/ES9010338
Abstract: This study shows that iodinated organic compounds can be produced when iodide-containing waters are in contact with manganese oxide birnessite (delta-MnO2) in the pH range of 5-7. In the absence of natural organic matter (NOM), iodide is oxidized to iodate that is also adsorbed onto delta-MnO2. In the presence of iodide and NOM, adsordable organic iodine compounds (AOI) are formed at pH < 7 because of the oxidation of iodide to iodine by delta-MnO2 and the reactions of iodine with NOM. In addition, iodoacetic acid and iodoform have been identified as specific iodinated byproducts. Formation of iodoform is not observed for high NOM/delta-MnO2 ratios due to inhibition of the catalytic effect of delta-MnO2 by NOM poisoning. Experiments with model compounds such as resorcinol and 3,5-heptanedione confirmed that the delta-MnO2/l(-) system is very effective for the formation of iodinated organic compounds. These results suggest that birnessite acts as a catalyst through the oxidation of iodide to iodine and the polarization of the iodine molecule, which then reacts with NOM moieties. Furthermore, our results indicate that during water treatment in the presence of manganese oxide, iodinated organic compounds may be formed, which may lead to taste and odor or toxicological problems.
Publisher: MDPI AG
Date: 08-08-2015
DOI: 10.3390/W9020094
Publisher: American Chemical Society (ACS)
Date: 07-08-2020
Publisher: Wiley
Date: 11-2021
DOI: 10.1002/AWS2.1257
Abstract: Technologies for per‐ and poly‐fluoroalkyl substances (PFAS) removal at a small scale suitable for point‐of‐entry (POE) treatment systems for household or business water supply are not well‐established. In the current study, a POE filter was tested for the removal of PFAS and precursors in groundwater contaminated with aqueous film‐forming foam. Long‐chain PFAS were more effectively removed than short‐chain PFAS. Total oxidizable precursor assays showed that precursors of short‐chain perfluoroalkyl carboxylic acids (PFCAs) broke through the filter earlier than routinely measured PFCAs and perfluoroalkyl sulfonic acids. The dissolved organic carbon removal trend was similar to that of PFAS and precursors. Overall, the POE filter achieved good long‐term removal (up to 7 months household equivalent) of the United States Environmental Protection Agency and Australian Drinking Water Guidelines‐regulated PFAS. This study provides benchmark data for the long‐term removal of precursors and PFAS using POE treatment systems for household or business water supply impacted by PFAS‐contaminated water.
Publisher: Elsevier BV
Date: 10-2020
Publisher: Elsevier BV
Date: 03-2018
DOI: 10.1016/J.SCITOTENV.2017.09.281
Abstract: In this study, a comprehensive kinetic model was developed and validated to predict the stability of monochloramine (NH
Publisher: Elsevier BV
Date: 2021
Publisher: Elsevier BV
Date: 11-2015
DOI: 10.1016/J.WATRES.2015.08.051
Abstract: Phenolic compounds are known structural moieties of natural organic matter (NOM), and their reactivity is a key parameter for understanding the reactivity of NOM and the disinfection by-product formation during oxidative water treatment. In this study, species-specific and/or apparent second order rate constants and mechanisms for the reactions of bromine and chlorine have been determined for various phenolic compounds (phenol, resorcinol, catechol, hydroquinone, phloroglucinol, bisphenol A, p-hydroxybenzoic acid, gallic acid, hesperetin and tannic acid) and flavone. The reactivity of bromine with phenolic compounds is very high, with apparent second order rate constants at pH 7 in the range of 10(4) to 10(7) M(-1) s(-1). The highest value was recorded for the reaction between HOBr and the fully deprotonated resorcinol (k = 2.1 × 10(9) M(-1) s(-1)). The reactivity of phenolic compounds is enhanced by the activating character of the phenolic substituents, e.g. further hydroxyl groups. With the data set from this study, the ratio between the species-specific rate constants for the reactions of chlorine versus bromine with phenolic compounds was confirmed to be about 3000. Phenolic compounds react with bromine or chlorine either by oxidation (electron transfer, ET) or electrophilic aromatic substitution (EAS) processes. The dominant process mainly depends on the relative position of the hydroxyl substituents and the possibility of quinone formation. While phenol, p-hydroxybenzoic acid and bisphenol A undergo EAS, hydroquinone, catechol, gallic acid and tannic acid, with hydroxyl substituents in ortho or para positions, react with bromine by ET leading to quantitative formation of the corresponding quinones. Some compounds (e.g. phloroglucinol) show both partial oxidation and partial electrophilic aromatic substitution and the ratio observed for the pathways depends on the pH. For the reaction of six NOM extracts with bromine, electrophilic aromatic substitution accounted for only 20% of the reaction, and for one NOM extract (Pony Lake fulvic acid) it accounted for <10%. This shows that for natural organic matter s les, oxidation (ET) is far more important than bromine incorporation (EAS).
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0EW00411A
Abstract: Pre-oxidation is commonly used to mitigate the formation of byproducts during post-disinfection.
Publisher: American Chemical Society (ACS)
Date: 13-04-2017
Abstract: During chlorination of bromide-containing waters, a significant formation of brominated disinfection byproducts is expected. This is of concern because Br-DBPs are generally more toxic than their chlorinated analogues. In this study, synthetic water s les containing dissolved organic matter (DOM) extracts and bromide were treated under various disinfection scenarios to elucidate the mechanisms of Br-DBP formation. The total concentration of Br-DBPs was measured as adsorbable organic bromine (AOBr). A portion of the bromine (HOBr) was found to react with DOM via electrophilic substitution (≤40%), forming AOBr, and the remaining HOBr reacted with DOM via electron transfer with a reduction of HOBr to bromide (≥60%). During chlorination, the released bromide is reoxidized (recycled) by chlorine to HOBr, leading to further electrophilic substitution of unaltered DOM sites and chlorinated DOM moieties. This leads to an almost complete bromine incorporation to DOM (≥87%). The type of DOM (3.06 ≤ SUVA
Publisher: American Chemical Society (ACS)
Date: 14-06-2018
Abstract: During chloramination of bromide-containing waters, the main brominated amine formed is bromochloramine (NHBrCl). To date, there is no analytical method, free of interference, allowing its accurate quantification. The major reason is that it is not possible to produce a pure NHBrCl solution. In this study, we report a method allowing the accurate quantification of NHBrCl with membrane introduction mass spectrometry (MIMS). First, the molar absorption coefficient for NHBrCl was determined by quantifying NHBrCl as 2,4,6-tribromophenol by HPLC-UV and comparing the results with the direct UV response at 320 nm. A molar absorption coefficient of 304 M
Publisher: Springer Science and Business Media LLC
Date: 07-08-2019
DOI: 10.1007/S11356-019-05861-0
Abstract: Many studies of disinfection by-products (DBPs) in pools have focused on haloacetic acids, trihalomethanes, and chloramines, with less studies investigating the occurrence of other DBPs, such as haloketones, haloacetaldehydes, haloacetonitriles, halonitromethanes, and haloacetamides. Furthermore, while many studies have achieved a broadscreen analysis across several pools, fewer studies have followed the water quality of pools over time, with information regarding the production and fate of DBPs in pools over extended periods (e.g. > 1 year) being limited. This study reports the occurrence of 39 DBPs and several general water quality parameters in two newly built and filled swimming pools over 15 months, where investigations began prior to opening. DBP concentrations measured in this study were generally similar to or higher than those previously reported in chlorinated pools, with concentrations of chloroacetic acid, dichloroacetic acid, trichloroacetic acid, and chloral hydrate (trichloroacetaldehyde) in some s les being higher than previously reported maximum concentrations. Considering both pools, lower concentrations of DBPs were measured in the pool where a steady state non-purgeable organic carbon concentration was achieved, highlighting the importance of the establishment of a steady state balance of mineralisation versus addition of organic carbon to reduce precursors for DBP formation in pools. Pools were found to exhibit significantly higher estimated cytotoxicity than their filling water, which reflects the significantly higher concentrations of DBPs measured in the pools in comparison to the filling water. Chloral hydrate accounted for up to 99% the total estimated cytotoxicity and was found to be correlated to the number of pool entries, suggesting that swimmers may be a potential source of chloral hydrate precursors in pools. The presence and subsequent peak of non-purgeable organic carbon and DBPs prior to, and soon after, opening suggest that the building process and/or new pool infrastructure may have had a significant impact on the chemical water quality, particularly on DBP formation. This study includes the first quantification of bromochloroacetaldehyde, bromodichloroacetaldehyde, bromochloronitromethane, and dichloronitromethane in chlorinated swimming pools, and provides important new knowledge on the long-term trends of DBPs in pools.
Publisher: Elsevier BV
Date: 08-2017
DOI: 10.1016/J.JES.2017.06.010
Abstract: Determination of halogen-specific total organic halogen (TOX) is vital for studies of disinfection of waters containing bromide, since total organic bromine (TOBr) is likely to be more problematic than total organic chlorine. Here, we present further halogen-specific TOX method optimisation and validation, focusing on measurement of TOBr. The optimised halogen-specific TOX method was validated based on the recovery of model compounds covering different classes of disinfection by-products (haloacetic acids, haloacetonitriles, halophenols and halogenated benzenes) and the recovery of total bromine (mass balance of TOBr and bromide concentrations) during disinfection of waters containing dissolved organic matter and bromide. The validation of a halogen-specific TOX method based on the mass balance of total bromine has not previously been reported. Very good recoveries of organic halogen from all model compounds were obtained, indicating high or complete conversion of all organic halogen in the model compound solution through to halide in the absorber solution for ion chromatography analysis. The method was also successfully applied to monitor conversion of bromide to TOBr in a groundwater treatment plant. An excellent recovery (101%) of total bromine was observed from the raw water to the post-chlorination stage. Excellent recoveries of total bromine (92%-95%) were also obtained from chlorination of a synthetic water containing dissolved organic matter and bromide, demonstrating the validity of the halogen-specific TOX method for TOBr measurement. The halogen-specific TOX method is an important tool to monitor and better understand the formation of halogenated organic compounds, in particular brominated organic compounds, in drinking water systems.
Publisher: American Chemical Society (ACS)
Date: 16-07-2013
DOI: 10.1021/ES401304R
Abstract: The oxidation of dissolved manganese(II) (Mn(II)) during chlorination is a relatively slow process which may lead to residual Mn(II) in treated drinking waters. Chemical Mn(II) oxidation is autocatalytic and consists of a homogeneous and a heterogeneous process the oxidation of Mn(II) is mainly driven by the latter process. This study demonstrates that Mn(II) oxidation during chlorination is enhanced in bromide-containing waters by the formation of reactive bromine species (e.g., HOBr, BrCl, Br2O) from the oxidation of bromide by chlorine. During oxidation of Mn(II) by chlorine in bromide-containing waters, bromide is recycled and acts as a catalyst. For a chlorine dose of 1 mg/L and a bromide level as low as 10 μg/L, the oxidation of Mn(II) by reactive bromine species becomes the main pathway. It was demonstrated that the kinetics of the reaction are dominated by the adsorbed Mn(OH)2 species for both chlorine and bromine at circumneutral pH. Reactive bromine species such as Br2O and BrCl significantly influence the rate of manganese oxidation and may even outweigh the reactivity of HOBr. Reaction orders in [HOBr]tot were found to be 1.33 (±0.15) at pH 7.8 and increased to 1.97 (±0.17) at pH 8.2 consistent with an important contribution of Br2O which is second order in [HOBr]tot. These findings highlight the need to take bromide, and the subsequent reactive bromine species formed upon chlorination, into account to assess Mn(II) removal during water treatment with chlorine.
Publisher: Elsevier BV
Date: 12-2020
Publisher: American Chemical Society (ACS)
Date: 28-08-2015
Abstract: Chlorination followed by chloramination can be used to mitigate the formation of potentially toxic iodinated disinfection byproducts (I-DBPs) while controlling the formation of regulated chloro-bromo-DBPs (Cl-/Br-DBPs). Water s les containing dissolved organic matter (DOM) isolates were subjected to 3 disinfection scenarios: NH2Cl, prechlorination followed by ammonia addition, and HOCl alone. A theoretical cytotoxicity evaluation was carried out based on the trihalomethanes (THMs) formed. This study demonstrates that the presence of bromide not only enhances the yield and rate of iodate formation, it also increases the formation of brominated I-THM precursors. A shift in the speciation from CHCl2I to the more toxic CHBr2I, as well as increased iodine incorporation in THMs, was observed in the presence of bromide. For low bromide concentrations, a decrease in I-THM formation and theoretical cytotoxicity was achieved only for high prechlorination times, while for high bromide concentrations, a short prechlorination time enabled the full conversion of iodide to iodate. For low DOM concentrations or DOM with low reactivity, Br-/I-THMs were preferentially formed for short prechlorination times, inducing high cytotoxicity. However, for high chlorine exposures, the cytotoxicity induced by the formation of regulated THMs might outweigh the benefit of I-THM mitigation. For high DOM concentrations or DOM with higher reactivity, mixed I-THMs were formed together with high concentrations of regulated THMs. In this case, based on the cytotoxicity of the THMs formed, the use of NH2Cl is recommended.
Publisher: MDPI AG
Date: 09-07-2021
DOI: 10.3390/W13141899
Abstract: Hypersaline ecosystems—aquatic environments where concentration of salt exceeds 35 g L−1—host microbial communities that are highly specialised to cope with these extreme conditions. However, our knowledge on the taxonomic ersity and functional metabolisms characterising microbial communities in the water columns of hypersaline ecosystems is still limited, and this may compromise the future preservation of these unique environments. DNA metabarcoding provides a reliable and affordable tool to investigate environmental dynamics of aquatic ecosystems, and its use in brine can be highly informative. Here, we make use of bacterial 16S metabarcoding techniques combined with hydrochemical analyses to investigate the microbial patterns ( ersity and functions) from five hypersaline lakes located at Rottnest Island (WA). Our results indicate lake-driven microbial aquatic assemblages that are characterised by taxonomically and functionally moderately to extremely halophilic groups, with TDS (total dissolved solids) and alkalinity amongst the most influential parameters driving the community patterns. Overall, our findings suggest that DNA metabarcoding allows rapid but reliable ecological assessment of the hypersaline aquatic microbial communities at Rottnest Island. Further studies involving different hypersaline lakes across multiple seasons will help elucidate the full extent of the potential of this tool in brine.
Publisher: Elsevier BV
Date: 04-2017
DOI: 10.1016/J.SCITOTENV.2017.01.120
Abstract: Redox reactions of inorganic and organic contaminants on manganese oxides have been widely studied. However, these reactions are strongly affected by the presence of natural organic matter (NOM) at the surface of the manganese oxide. Interestingly, the mechanism behind NOM adsorption onto manganese oxides remains unclear. Therefore, in this study, the adsorption kinetics and equilibrium of different NOM isolates to synthetic manganese oxide (birnessite) and natural manganese oxide (Mn sand) were investigated. Natural manganese oxide is composed of both amorphous and well-crystallised Mn phases (i.e., lithiophorite, birnessite, and cryptomelane). NOM adsorption on both manganese oxides increased with decreasing pH (from pH7 to 5), in agreement with surface complexation and ligand exchange mechanisms. The presence of calcium enhanced the rate of NOM adsorption by decreasing the electrostatic repulsion between NOM and Mn sand. Also, the adsorption was limited by the diffusion of NOM macromolecules through the Mn sand pores. At equilibrium, a preferential adsorption of high molecular weight molecules enriched in aromatic moieties was observed for both the synthetic and natural manganese oxide. Hydrophobic interactions may explain the adsorption of organic matter on manganese oxides. The formation of low molecular weight UV absorbing molecules was detected with the synthetic birnessite, suggesting oxidation and reduction processes occurring during NOM adsorption. This study provides a deep insight for both environmental and engineered systems to better understand the impact of NOM adsorption on the biogeochemical cycle of manganese.
Publisher: Elsevier BV
Date: 10-2016
DOI: 10.1016/J.WATRES.2016.07.050
Abstract: Large amount of iodinated contrast media (ICM) are found in natural waters (up to μg.L(-)(1) levels) due to their worldwide use in medical imaging and their poor removal by conventional wastewater treatment. Synthetic water s les containing different ICM and natural organic matter (NOM) extracts were subjected to UV254 irradiation followed by the addition of chlorine (HOCl) or chloramine (NH2Cl) to simulate final disinfection. In this study, two new quantum yields were determined for diatrizoic acid (0.071 mol.Einstein(-1)) and iotalamic acid (0.038 mol.Einstein(-1)) while values for iopromide (IOP) (0.039 mol.Einstein(-1)), iopamidol (0.034 mol.Einstein(-1)) and iohexol (0.041 mol.Einstein(-1)) were consistent with published data. The photodegradation of IOP led to an increasing release of iodide with increasing UV doses. Iodide is oxidized to hypoiodous acid (HOI) either by HOCl or NH2Cl. In presence of NOM, the addition of oxidant increased the formation of iodinated disinfection by-products (I-DBPs). On one hand, when the concentration of HOCl was increased, the formation of I-DBPs decreased since HOI was converted to iodate. On the other hand, when NH2Cl was used the formation of I-DBPs was constant for all concentration since HOI reacted only with NOM to form I-DBPs. Increasing the NOM concentration has two effects, it decreased the photodegradation of IOP by screening effect but it increased the number of reactive sites available for reaction with HOI. For experiments carried out with HOCl, increasing the NOM concentration led to a lower formation of I-DBPs since less IOP are photodegraded and iodate are formed. For NH2Cl the lower photodegradation of IOP is compensated by the higher amount of NOM reactive sites, therefore, I-DBPs concentrations were constant for all NOM concentrations. 7 different NOM extracts were tested and almost no differences in IOP degradation and I-DBPs formation was observed. Similar behaviour was observed for the 5 ICM tested. Both oxidant poorly degraded the ICM and a higher formation of I-DBPs was observed for the chloramination experiments compared to the chlorination experiment. Results from toxicity testing showed that the photodegradation products of IOP are toxic and confirmed that the formation of I-DBPs leads to higher toxicity. Therefore, for the experiment with HOCl where iodate are formed the toxicity was lower than for the experiments with NH2Cl where a high formation of I-DBPs was observed.
Publisher: Public Library of Science (PLoS)
Date: 28-08-2020
Publisher: Elsevier BV
Date: 04-2020
DOI: 10.1016/J.WATRES.2019.115463
Abstract: The presence of Dissolved Organic Matter (DOM) can exert a strong influence on the effectiveness of the UV/chlorine process. This study examined the impact of five DOM isolates with different characteristics on the degradation kinetics of model contaminant primidone (PM) during UV/chlorine treatment. The formation of Disinfection By-Products (DBPs) from DOM after 15-min UV/chlorine treatment followed by 24 h chlorination was investigated and compared with chlorination alone. The use of chemical probes and radical scavengers revealed that
Publisher: Elsevier BV
Date: 03-2023
Publisher: Elsevier BV
Date: 2020
DOI: 10.1016/J.JENVMAN.2019.109655
Abstract: The beneficial effect of combining ozone with ceramic membrane filtration (CMF) to enhance membrane flux performances during water treatment (e.g., wastewater and drinking water) could be related to the formation of hydroxyl (HO) radicals from the interaction of ozone with ceramic membrane. To explore this effect, para-chlorobenzoic acid was used to probe HO radical activity during a combined ozone/CMF process using a 0.1 μm pore size membrane supplied by Metawater, Japan. Tests were then extended to explore the impact on bromate formation downstream CMF, a well-known undesirable by-product from ozone use in water treatment. Ozone reduction by the membrane and its module appeared to be more associated with physical degassing, but a noticeable formation of HO radicals was observed during the interaction of ozone with the ceramic membrane. CMF treatment of ozonated potable water containing bromide showed a reduced bromate formation of 50% when the water was recirculated to the filtration module containing the ceramic membrane, compared to the experiment performed with an empty module. Single pass experiments showed bromate mitigation of around 10%. The mitigation of bromate formation was attributed to reduced overall ozone exposure by deagassing effect, but also potentially from suppression of the oxidation of Br
Start Date: 2021
End Date: 06-2023
Amount: $474,000.00
Funder: Australian Research Council
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