Development of a Water-Soluble Filter for Potential Use in the Toxicity Evaluation of Ambient Particulate Matter

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Abstract Assessment of the toxicity of insoluble particulate matter (PM) in the atmosphere is crucially important. However, because of challenges associated with extracting insoluble PM from filters, the toxicity of insoluble PM remains largely uncharacterized. For this study, the water-soluble filter made of poly (vinyl alcohol) (PVA) was developed with high particle collection efficiency, durability, and weather resistance, which are necessary for ambient PM sampling. The PVA filter is water-soluble under certain conditions, allowing for the recovery of insoluble PM, which can be exposed directly to cells or animals for toxicological studies. The PVA filter was made from PVA nanofibers using the electrospinning (ES) method. Its durability and weather resistance were comparable to those of polytetrafluoroethylene (PTFE) and quartz fiber (QF) filters, and were superior to those of commercially available gelatin filters. The PVA filter particle collection efficiency was evaluated by comparing concentrations of inorganic elements (Mg, Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu and Zn) and water-soluble ionic components (Na + , NH 4 + , K + , Mg 2+ , Ca 2+ , Cl − , NO 3 − , and SO 4 2− ) in the PVA filter-collected ambient PM with those in the PTFE filter-collected PM. The concentrations of almost all measured components in the PVA filter-collected PM were comparable to those in the PTFE filter-collected PM. When the PVA filter dissolved in cell culture medium was exposed to cells, no significant difference was found in cell viability compared to a blank solution containing only culture medium, suggesting that the PVA filter has potential use for cell exposure experiments. Graphical Abstract

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  • Peer Review Report
  • 10.5194/acp-2021-979-rc3
Comment on acp-2021-979
  • Mar 15, 2022

Particulate matter (PM) is the air pollutant which causes the greatest deleterious heath effects across the world and PM is routinely monitored within air quality networks where PM mass according to its size, and sometimes number are reported. However, such measurements do not provide information on the biological toxicity of PM. Oxidative potential (OP) is a complementary metric which aims to classify PM in respect to its oxidising ability in lungs and is being increasingly reported due to its assumed relevance concerning human health. Between June, 2018 and May, 2019, an intensive filter-based PM sampling campaign was conducted across Switzerland in five locations which involved the quantification of a large number of PM constituents and OP for both PM10 and PM2.5. OP was quantified by three assays: ascorbic acid (AA), dithiothreitol (DTT), and dichlorofluorescein (DCFH). OPv (OP by air volume) was found to be variable in time and space with Bern-Bollwerk, an urban-traffic sampling site having the greatest levels of OPv among the Swiss sites (especially when considering ), with more rural locations such as Payerne experiencing lower OPv. However, urban-background and suburban sites did experience significant OPv enhancement, as did the rural Magadino-Cadenazzo site during wintertime because of high levels of wood smoke. The mean OP ranges for the sampling period were: 0.4–4.1, 0.6–3.0, and 0.3–0.7 nmol min−1 m−3 for the , , and respectively. A source allocation method using positive matrix factorisation (PMF) models indicated that although all PM10 and PM2.5 sources which were identified contributed to OPv on average, the anthropogenic road traffic and wood combustion sources had the greatest OPm potency (OP per PM mass). A dimensionality reduction procedure coupled to multiple linear regression modelling consistently identified a handful of metals usually associated with non-exhaust emissions, namely: copper, zinc, iron, tin, antimony and somewhat manganese and cadmium as well as three specific wood burning-sourced organic tracers – levoglucosan, mannosan, and galactosan (or their metal substitutes: rubidium and potassium) were the most important PM components to explain and predict OPv. The combination of a metal and a wood burning specific tracer led to the best performing linear models to explain OPv. Interestingly, within the non-exhaust and wood combustion emission groups, the exact choice of component was not critical, the models simply required a variable to be present to represent the emission source or process. The modelling process also showed that may be a more specific metric for OP than the other assays employed in this work. This analysis strongly suggests that the anthropogenic and locally emitted road traffic and wood burning sources should be prioritised, targeted, and controlled to gain the most efficacious decrease in OPv, and presumably biological harm reductions in Switzerland.

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  • Peer Review Report
  • 10.5194/acp-2021-979-ac1
Comment on acp-2021-979
  • Apr 20, 2022
  • Stuart Grange

<strong class="journal-contentHeaderColor">Abstract.</strong> Particulate matter (PM) is the air pollutant that causes the greatest deleterious health effects across the world, so PM is routinely monitored within air quality networks, usually in respect to PM mass or number in different size fractions. However, such measurements do not provide information on the biological toxicity of PM. Oxidative potential (OP) is a complementary metric that aims to classify PM in respect to its oxidising ability in the lungs and is being increasingly reported due to its assumed relevance concerning human health. Between June 2018 and May 2019, an intensive filter-based PM sampling campaign was conducted across Switzerland in five locations, which involved the quantification of a large number of PM constituents and the OP for both PM<span class="inline-formula"><sub>10</sub></span> and PM<span class="inline-formula"><sub>2.5</sub></span>. OP was quantified by three assays: ascorbic acid (AA), dithiothreitol (DTT), and dichlorofluorescein (DCFH). OP<span class="inline-formula"><sub>v</sub></span> (OP by air volume) was found to be variable over time and space: Bern-Bollwerk, an urban-traffic sampling site, had the greatest levels of OP<span class="inline-formula"><sub>v</sub></span> among the Swiss sites (especially when considering <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M9" display="inline" overflow="scroll" dspmath="mathml"><mrow><msubsup><mtext>OP</mtext><mi mathvariant="normal">v</mi><mi mathvariant="normal">AA</mi></msubsup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="29pt" height="16pt" class="svg-formula" dspmath="mathimg" md5hash="6ea9d0c9d405312dc379a6b81df0cdc4"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-7029-2022-ie00001.svg" width="29pt" height="16pt" src="acp-22-7029-2022-ie00001.png"/></svg:svg></span></span>), with more rural locations such as Payerne experiencing a lower OP<span class="inline-formula"><sub>v</sub></span>. However, urban-background and suburban sites experienced a significant OP<span class="inline-formula"><sub>v</sub></span> enhancement, as did the rural Magadino-Cadenazzo site during wintertime because of high levels of wood smoke. The mean OP ranges for the sampling period were 0.4–4.1 <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M12" display="inline" overflow="scroll" dspmath="mathml"><mrow class="unit"><mi mathvariant="normal">nmol</mi><mspace linebreak="nobreak" width="0.125em"/><msup><mi mathvariant="normal">min</mi><mrow><mo>-</mo><mn mathvariant="normal">1</mn></mrow></msup><mspace width="0.125em" linebreak="nobreak"/><msup><mi mathvariant="normal">m</mi><mrow><mo>-</mo><mn mathvariant="normal">3</mn></mrow></msup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="76pt" height="13pt" class="svg-formula" dspmath="mathimg" md5hash="57b4bf826357bed61feddce78770afc1"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-7029-2022-ie00002.svg" width="76pt" height="13pt" src="acp-22-7029-2022-ie00002.png"/></svg:svg></span></span>, 0.6–3.0 <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M13" display="inline" overflow="scroll" dspmath="mathml"><mrow class="unit"><mi mathvariant="normal">nmol</mi><mspace width="0.125em" linebreak="nobreak"/><msup><mi mathvariant="normal">min</mi><mrow><mo>-</mo><mn mathvariant="normal">1</mn></mrow></msup><mspace width="0.125em" linebreak="nobreak"/><msup><mi mathvariant="normal">m</mi><mrow><mo>-</mo><mn mathvariant="normal">3</mn></mrow></msup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="76pt" height="13pt" class="svg-formula" dspmath="mathimg" md5hash="78d33a315fc5d2665ea20bfb0fec7a33"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-7029-2022-ie00003.svg" width="76pt" height="13pt" src="acp-22-7029-2022-ie00003.png"/></svg:svg></span></span>, and 0.3–0.7 <span class="inline-formula">nmol H<sub>2</sub>O<sub>2</sub> m<sup>−3</sup></span> for <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M15" display="inline" overflow="scroll" dspmath="mathml"><mrow><msubsup><mtext>OP</mtext><mi mathvariant="normal">v</mi><mi mathvariant="normal">AA</mi></msubsup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="29pt" height="16pt" class="svg-formula" dspmath="mathimg" md5hash="02c202363905e826f456402c89d2d969"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-7029-2022-ie00004.svg" width="29pt" height="16pt" src="acp-22-7029-2022-ie00004.png"/></svg:svg></span></span>, <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M16" display="inline" overflow="scroll" dspmath="mathml"><mrow><msubsup><mtext>OP</mtext><mi mathvariant="normal">v</mi><mi mathvariant="normal">DTT</mi></msubsup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="34pt" height="16pt" class="svg-formula" dspmath="mathimg" md5hash="e357dd246127c04aa854f41c88b6fc26"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-7029-2022-ie00005.svg" width="34pt" height="16pt" src="acp-22-7029-2022-ie00005.png"/></svg:svg></span></span>, and <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M17" display="inline" overflow="scroll" dspmath="mathml"><mrow><msubsup><mtext>OP</mtext><mi mathvariant="normal">v</mi><mi mathvariant="normal">DCFH</mi></msubsup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="40pt" height="16pt" class="svg-formula" dspmath="mathimg" md5hash="2801194684c343fc94ca7869fea69c10"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-7029-2022-ie00006.svg" width="40pt" height="16pt" src="acp-22-7029-2022-ie00006.png"/></svg:svg></span></span>, respectively. A source allocation method using positive matrix factorisation (PMF) models indicated that although all PM<span class="inline-formula"><sub>10</sub></span> and PM<span class="inline-formula"><sub>2.5</sub></span> sources that were identified contributed to OP<span class="inline-formula"><sub>v</sub></span>, the anthropogenic road traffic and wood combustion sources had the greatest OP<span class="inline-formula"><sub>m</sub></span> potency (OP per PM mass) on average. A dimensionality reduction procedure coupled to multiple linear regression modelling consistently identified a handful of metals usually associated with non-exhaust emissions, namely copper, zinc, iron, tin, antimony, manganese, and cadmium, as well as three specific wood-burning-sourced organic tracers – levoglucosan, mannosan, and galactosan (or their metal substitutes: rubidium and potassium), as the most important PM components to explain and predict OP<span class="inline-formula"><sub>v</sub></span>. The combination of a metal and a wood-burning-specific tracer led to the best-performing linear models to explain OP<span class="inline-formula"><sub>v</sub></span>. Interestingly, within the non-exhaust and wood combustion emission groups, the exact choice of component was not critical; the models simply required a variable representing the emission source or process to be present. This analysis strongly suggests that anthropogenic and locally emitting road traffic and wood burning sources should be prioritised, targeted, and controlled to gain the most efficacious decrease in OP<span class="inline-formula"><sub>v</sub></span> and presumably biological harm reductions in Switzerland.

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  • Peer Review Report
  • 10.5194/acp-2021-979-rc1
Comment on acp-2021-979
  • Feb 26, 2022

Particulate matter (PM) is the air pollutant which causes the greatest deleterious heath effects across the world and PM is routinely monitored within air quality networks where PM mass according to its size, and sometimes number are reported. However, such measurements do not provide information on the biological toxicity of PM. Oxidative potential (OP) is a complementary metric which aims to classify PM in respect to its oxidising ability in lungs and is being increasingly reported due to its assumed relevance concerning human health. Between June, 2018 and May, 2019, an intensive filter-based PM sampling campaign was conducted across Switzerland in five locations which involved the quantification of a large number of PM constituents and OP for both PM10 and PM2.5. OP was quantified by three assays: ascorbic acid (AA), dithiothreitol (DTT), and dichlorofluorescein (DCFH). OPv (OP by air volume) was found to be variable in time and space with Bern-Bollwerk, an urban-traffic sampling site having the greatest levels of OPv among the Swiss sites (especially when considering ), with more rural locations such as Payerne experiencing lower OPv. However, urban-background and suburban sites did experience significant OPv enhancement, as did the rural Magadino-Cadenazzo site during wintertime because of high levels of wood smoke. The mean OP ranges for the sampling period were: 0.4–4.1, 0.6–3.0, and 0.3–0.7 nmol min−1 m−3 for the , , and respectively. A source allocation method using positive matrix factorisation (PMF) models indicated that although all PM10 and PM2.5 sources which were identified contributed to OPv on average, the anthropogenic road traffic and wood combustion sources had the greatest OPm potency (OP per PM mass). A dimensionality reduction procedure coupled to multiple linear regression modelling consistently identified a handful of metals usually associated with non-exhaust emissions, namely: copper, zinc, iron, tin, antimony and somewhat manganese and cadmium as well as three specific wood burning-sourced organic tracers – levoglucosan, mannosan, and galactosan (or their metal substitutes: rubidium and potassium) were the most important PM components to explain and predict OPv. The combination of a metal and a wood burning specific tracer led to the best performing linear models to explain OPv. Interestingly, within the non-exhaust and wood combustion emission groups, the exact choice of component was not critical, the models simply required a variable to be present to represent the emission source or process. The modelling process also showed that may be a more specific metric for OP than the other assays employed in this work. This analysis strongly suggests that the anthropogenic and locally emitted road traffic and wood burning sources should be prioritised, targeted, and controlled to gain the most efficacious decrease in OPv, and presumably biological harm reductions in Switzerland.

  • PDF Download Icon
  • Peer Review Report
  • 10.5194/acp-2021-979-rc2
Comment on acp-2021-979
  • Mar 11, 2022

Particulate matter (PM) is the air pollutant which causes the greatest deleterious heath effects across the world and PM is routinely monitored within air quality networks where PM mass according to its size, and sometimes number are reported. However, such measurements do not provide information on the biological toxicity of PM. Oxidative potential (OP) is a complementary metric which aims to classify PM in respect to its oxidising ability in lungs and is being increasingly reported due to its assumed relevance concerning human health. Between June, 2018 and May, 2019, an intensive filter-based PM sampling campaign was conducted across Switzerland in five locations which involved the quantification of a large number of PM constituents and OP for both PM10 and PM2.5. OP was quantified by three assays: ascorbic acid (AA), dithiothreitol (DTT), and dichlorofluorescein (DCFH). OPv (OP by air volume) was found to be variable in time and space with Bern-Bollwerk, an urban-traffic sampling site having the greatest levels of OPv among the Swiss sites (especially when considering ), with more rural locations such as Payerne experiencing lower OPv. However, urban-background and suburban sites did experience significant OPv enhancement, as did the rural Magadino-Cadenazzo site during wintertime because of high levels of wood smoke. The mean OP ranges for the sampling period were: 0.4–4.1, 0.6–3.0, and 0.3–0.7 nmol min−1 m−3 for the , , and respectively. A source allocation method using positive matrix factorisation (PMF) models indicated that although all PM10 and PM2.5 sources which were identified contributed to OPv on average, the anthropogenic road traffic and wood combustion sources had the greatest OPm potency (OP per PM mass). A dimensionality reduction procedure coupled to multiple linear regression modelling consistently identified a handful of metals usually associated with non-exhaust emissions, namely: copper, zinc, iron, tin, antimony and somewhat manganese and cadmium as well as three specific wood burning-sourced organic tracers – levoglucosan, mannosan, and galactosan (or their metal substitutes: rubidium and potassium) were the most important PM components to explain and predict OPv. The combination of a metal and a wood burning specific tracer led to the best performing linear models to explain OPv. Interestingly, within the non-exhaust and wood combustion emission groups, the exact choice of component was not critical, the models simply required a variable to be present to represent the emission source or process. The modelling process also showed that may be a more specific metric for OP than the other assays employed in this work. This analysis strongly suggests that the anthropogenic and locally emitted road traffic and wood burning sources should be prioritised, targeted, and controlled to gain the most efficacious decrease in OPv, and presumably biological harm reductions in Switzerland.

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