Pub Date : 2023-11-22DOI: 10.1021/acsenvironau.3c00035
Dominik van Pinxteren*, Vanessa Engelhardt, Falk Mothes, Laurent Poulain, Khanneh Wadinga Fomba, Gerald Spindler, Andrea Cuesta-Mosquera, Thomas Tuch, Thomas Müller, Alfred Wiedensohler, Gunter Löschau, Susanne Bastian and Hartmut Herrmann*,
Residential wood combustion contributing to airborne particulate matter (PM10) was studied for 1 year at two sites in the village of Melpitz. Significant excess pollution was observed at the Melpitz center compared to that at the TROPOS research station Melpitz reference site, situated only 700 m away. Local concentration increments at the village site for the combustion PM constituents organic carbon, elemental carbon, levoglucosan, and benzo[a]pyrene were determined under appropriate wind directions, and their winter mean values were 0.7 μg m–3, 0.3 μg m–3, 0.1 μg m–3, and 0.4 ng m–3, representing relative increases over the regional background concentration of 24, 70, 61, and 107%, respectively. Yearly, weekly, and diurnal profiles of village increments suggest residential heating as the dominant source of this excess pollution, mainly originating from wood combustion. Receptor modeling using positive matrix factorization quantified 4.5 μg m–3 wood combustion PM at the village site, representing an increment of 1.9 μg m–3 and an increase of ∼75% over the 2.6 μg m–3 regional background wood combustion PM. This increment varied with season, temperature, and boundary layer height and reached daily mean values of 4–6 μg m–3 during unfavorable meteorological conditions. Potential health effects were estimated and resulted in an all-cause mortality from short-term exposure to wood combustion PM of 2.1 cases per 100,000 inhabitants and year for areas with similar wood smoke levels as observed in Melpitz. The excess cancer risk from the concentrations of polycyclic aromatic hydrocarbons was 6.4 per 100,000. For both health metrics, the very local contributions from the village itself were about 40–50%, indicating a strong potential for mitigation through local-scale policies. A compilation of literature data demonstrates wood combustion to represent a major source of PM pollution in Germany, with average winter-time contributions of 10–20%. The present study quantifies the negative impacts of heating with wood in rural residential areas, where the continuous monitoring of air quality is typically lacking. Further regulation of this PM source is warranted in order to protect human health.
{"title":"Residential Wood Combustion in Germany: A Twin-Site Study of Local Village Contributions to Particulate Pollutants and Their Potential Health Effects","authors":"Dominik van Pinxteren*, Vanessa Engelhardt, Falk Mothes, Laurent Poulain, Khanneh Wadinga Fomba, Gerald Spindler, Andrea Cuesta-Mosquera, Thomas Tuch, Thomas Müller, Alfred Wiedensohler, Gunter Löschau, Susanne Bastian and Hartmut Herrmann*, ","doi":"10.1021/acsenvironau.3c00035","DOIUrl":"10.1021/acsenvironau.3c00035","url":null,"abstract":"<p >Residential wood combustion contributing to airborne particulate matter (PM<sub>10</sub>) was studied for 1 year at two sites in the village of Melpitz. Significant excess pollution was observed at the Melpitz center compared to that at the TROPOS research station Melpitz reference site, situated only 700 m away. Local concentration increments at the village site for the combustion PM constituents organic carbon, elemental carbon, levoglucosan, and benzo[a]pyrene were determined under appropriate wind directions, and their winter mean values were 0.7 μg m<sup>–3</sup>, 0.3 μg m<sup>–3</sup>, 0.1 μg m<sup>–3</sup>, and 0.4 ng m<sup>–3</sup>, representing relative increases over the regional background concentration of 24, 70, 61, and 107%, respectively. Yearly, weekly, and diurnal profiles of village increments suggest residential heating as the dominant source of this excess pollution, mainly originating from wood combustion. Receptor modeling using positive matrix factorization quantified 4.5 μg m<sup>–3</sup> wood combustion PM at the village site, representing an increment of 1.9 μg m<sup>–3</sup> and an increase of ∼75% over the 2.6 μg m<sup>–3</sup> regional background wood combustion PM. This increment varied with season, temperature, and boundary layer height and reached daily mean values of 4–6 μg m<sup>–3</sup> during unfavorable meteorological conditions. Potential health effects were estimated and resulted in an all-cause mortality from short-term exposure to wood combustion PM of 2.1 cases per 100,000 inhabitants and year for areas with similar wood smoke levels as observed in Melpitz. The excess cancer risk from the concentrations of polycyclic aromatic hydrocarbons was 6.4 per 100,000. For both health metrics, the very local contributions from the village itself were about 40–50%, indicating a strong potential for mitigation through local-scale policies. A compilation of literature data demonstrates wood combustion to represent a major source of PM pollution in Germany, with average winter-time contributions of 10–20%. The present study quantifies the negative impacts of heating with wood in rural residential areas, where the continuous monitoring of air quality is typically lacking. Further regulation of this PM source is warranted in order to protect human health.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.3c00035","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138507337","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-03DOI: 10.1021/acsenvironau.3c00034
Inger Odnevall*, Marianne Brookman-Amissah, Franca Stábile, Mikael T. Ekvall, Gunilla Herting, Marie Bermeo Vargas, Maria E. Messing, Joachim Sturve, Lars-Anders Hansson, Christina Isaxon and Jenny Rissler*,
Manual dismantling, shredding, and mechanical grinding of waste from electrical and electronic equipment (WEEE) at recycling facilities inevitably lead to the accidental formation and release of both coarse and fine particle aerosols, primarily into the ambient air. Since diffuse emissions to air of such WEEE particles are not regulated, their dispersion from the recycling plants into the adjacent environment is possible. The aim of this interdisciplinary project was to collect and characterize airborne WEEE particles smaller than 1 μm generated at a Nordic open waste recycling facility from a particle concentration, shape, and bulk and surface composition perspective. Since dispersed airborne particles eventually may reach rivers, lakes, and possibly oceans, the aim was also to assess whether such particles may pose any adverse effects on aquatic organisms. The results show that WEEE particles only exerted a weak tendency toward cytotoxic effects on fish gill cell lines, although the exposure resulted in ROS formation that may induce adverse effects. On the contrary, the WEEE particles were toxic toward the crustacean zooplankter Daphnia magna, showing strong effects on survival of the animals in a concentration-dependent way.
{"title":"Characterization and Toxic Potency of Airborne Particles Formed upon Waste from Electrical and Electronic Equipment Waste Recycling: A Case Study","authors":"Inger Odnevall*, Marianne Brookman-Amissah, Franca Stábile, Mikael T. Ekvall, Gunilla Herting, Marie Bermeo Vargas, Maria E. Messing, Joachim Sturve, Lars-Anders Hansson, Christina Isaxon and Jenny Rissler*, ","doi":"10.1021/acsenvironau.3c00034","DOIUrl":"https://doi.org/10.1021/acsenvironau.3c00034","url":null,"abstract":"<p >Manual dismantling, shredding, and mechanical grinding of waste from electrical and electronic equipment (WEEE) at recycling facilities inevitably lead to the accidental formation and release of both coarse and fine particle aerosols, primarily into the ambient air. Since diffuse emissions to air of such WEEE particles are not regulated, their dispersion from the recycling plants into the adjacent environment is possible. The aim of this interdisciplinary project was to collect and characterize airborne WEEE particles smaller than 1 μm generated at a Nordic open waste recycling facility from a particle concentration, shape, and bulk and surface composition perspective. Since dispersed airborne particles eventually may reach rivers, lakes, and possibly oceans, the aim was also to assess whether such particles may pose any adverse effects on aquatic organisms. The results show that WEEE particles only exerted a weak tendency toward cytotoxic effects on fish gill cell lines, although the exposure resulted in ROS formation that may induce adverse effects. On the contrary, the WEEE particles were toxic toward the crustacean zooplankter <i>Daphnia magna</i>, showing strong effects on survival of the animals in a concentration-dependent way.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.3c00034","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"109143119","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-03DOI: 10.1021/acsenvironau.3c00043
Yuekun Qu, Di Xie and Yingjun Liu*,
Human occupants themselves constitute an important source of volatile organic compounds (VOCs) in indoor environments through breath and dermal emissions. In order to quantify VOC emissions from occupants under real-world settings, previous indoor observational studies often determined emission factors (i.e., average emission rates per person). However, the values obtained across these studies exhibited large variability, and the causes of this variability still need to be understood. Herein we report 10-day real-time VOC measurements in a university student office, using a proton transfer reaction-quadrupole interface-time-of-flight mass spectrometer. A method was developed to identify VOCs of primary human origin and to quantify the corresponding emission factors, accounting for the dynamically changing occupancy level and ventilation rate in the assessed office. We found that the emission factors of many dermally emitted VOCs strongly increased as the ozone concentration increased from <3 to 10–15 ppb. These VOCs include geranyl acetone, 6-methyl-5-hepten-2-one (6-MHO), and C10-C12 saturated aldehydes, which align with characteristic first-generation ozonolysis products of skin oil. The strongest increase occurred for 6-MHO, from 113 to 337 μg/h/p. In comparison, acetone and isoprene, which are primarily emitted from human breath, varied little with the ozone level. In light of this finding, we conducted an integrated analysis of emission factors reported in the literature for two frequently reported species, namely, 6-MHO and decanal. Ozone concentration alone can explain 94–97% of the variation in their emission factors across previous studies, and the best-estimated ozone dependence obtained using the literature data is consistent with those obtained in the current study. These results suggest that the ozone concentration is a key factor regulating emission factors of many dermally emitted VOCs in real indoor environments, which has to be considered when reporting or using the emission factors.
{"title":"Emissions of Volatile Organic Compounds from Human Occupants in a Student Office: Dependence on Ozone Concentration","authors":"Yuekun Qu, Di Xie and Yingjun Liu*, ","doi":"10.1021/acsenvironau.3c00043","DOIUrl":"10.1021/acsenvironau.3c00043","url":null,"abstract":"<p >Human occupants themselves constitute an important source of volatile organic compounds (VOCs) in indoor environments through breath and dermal emissions. In order to quantify VOC emissions from occupants under real-world settings, previous indoor observational studies often determined emission factors (i.e., average emission rates per person). However, the values obtained across these studies exhibited large variability, and the causes of this variability still need to be understood. Herein we report 10-day real-time VOC measurements in a university student office, using a proton transfer reaction-quadrupole interface-time-of-flight mass spectrometer. A method was developed to identify VOCs of primary human origin and to quantify the corresponding emission factors, accounting for the dynamically changing occupancy level and ventilation rate in the assessed office. We found that the emission factors of many dermally emitted VOCs strongly increased as the ozone concentration increased from <3 to 10–15 ppb. These VOCs include geranyl acetone, 6-methyl-5-hepten-2-one (6-MHO), and C<sub>10</sub>-C<sub>12</sub> saturated aldehydes, which align with characteristic first-generation ozonolysis products of skin oil. The strongest increase occurred for 6-MHO, from 113 to 337 μg/h/p. In comparison, acetone and isoprene, which are primarily emitted from human breath, varied little with the ozone level. In light of this finding, we conducted an integrated analysis of emission factors reported in the literature for two frequently reported species, namely, 6-MHO and decanal. Ozone concentration alone can explain 94–97% of the variation in their emission factors across previous studies, and the best-estimated ozone dependence obtained using the literature data is consistent with those obtained in the current study. These results suggest that the ozone concentration is a key factor regulating emission factors of many dermally emitted VOCs in real indoor environments, which has to be considered when reporting or using the emission factors.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.3c00043","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135818484","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-01DOI: 10.1021/acsenvironau.3c00036
Karla Diviesti, Glory A. Russell-Parks, Brian G. Trewyn* and Richard C. Holz*,
Triazine hydrolase fromArthrobacter aurescens TC1 (TrzN) was successfully immobilized on mesoporous silica nanomaterials (MSNs) for the first time. For both nonfunctionalized MSNs and MSNs functionalized with Zn(II), three pore sizes were evaluated for their ability to immobilize wild-type TrzN: Mobile composition of matter no. 41 (small, 3 nm pores), mesoporous silica nanoparticle material with 10 nm pore diameter (MSN-10) (medium, 6–12 nm pores), and pore-expanded MSN-10 (large, 15–30 nm pores). Of these six TrzN:MSN biomaterials, it was shown that TrzN:MSN-10 was the most active (3.8 ± 0.4 × 10–5 U/mg) toward the hydrolysis of a 50 μM atrazine solution at 25 °C. The TrzN:MSN-10 biomaterial was then coated in chitosan (TrzN:MSN-10:Chit) as chitosan has been shown to increase stability in extreme conditions such as low/high pH, heat shock, and the presence of organic solvents. TrzN:MSN-10:Chit was shown to be a superior TrzN biomaterial to TrzN:MSN-10 as it exhibited higher activity under all storage conditions, in the presence of 20% MeOH, at low and high pH values, and at elevated temperatures up to 80 °C. Finally, the TrzN:MSN-10:Chit biomaterial was shown to be fully active in river water, which establishes it as a functional biomaterial under actual field conditions. A combination of these data indicate that the TrzN:MSN-10:Chit biomaterial exhibited the best overall catalytic profile making it a promising biocatalyst for the bioremediation of atrazine.
{"title":"Atrazine Degradation Using Immobilized Triazine Hydrolase from Arthrobacter aurescens TC1 in Mesoporous Silica Nanomaterials","authors":"Karla Diviesti, Glory A. Russell-Parks, Brian G. Trewyn* and Richard C. Holz*, ","doi":"10.1021/acsenvironau.3c00036","DOIUrl":"https://doi.org/10.1021/acsenvironau.3c00036","url":null,"abstract":"<p >Triazine hydrolase from<i>Arthrobacter aurescens</i> TC1 (TrzN) was successfully immobilized on mesoporous silica nanomaterials (MSNs) for the first time. For both nonfunctionalized MSNs and MSNs functionalized with Zn(II), three pore sizes were evaluated for their ability to immobilize wild-type TrzN: Mobile composition of matter no. 41 (small, 3 nm pores), mesoporous silica nanoparticle material with 10 nm pore diameter (MSN-10) (medium, 6–12 nm pores), and pore-expanded MSN-10 (large, 15–30 nm pores). Of these six TrzN:MSN biomaterials, it was shown that TrzN:MSN-10 was the most active (3.8 ± 0.4 × 10<sup>–5</sup> U/mg) toward the hydrolysis of a 50 μM atrazine solution at 25 °C. The TrzN:MSN-10 biomaterial was then coated in chitosan (TrzN:MSN-10:Chit) as chitosan has been shown to increase stability in extreme conditions such as low/high pH, heat shock, and the presence of organic solvents. TrzN:MSN-10:Chit was shown to be a superior TrzN biomaterial to TrzN:MSN-10 as it exhibited higher activity under all storage conditions, in the presence of 20% MeOH, at low and high pH values, and at elevated temperatures up to 80 °C. Finally, the TrzN:MSN-10:Chit biomaterial was shown to be fully active in river water, which establishes it as a functional biomaterial under actual field conditions. A combination of these data indicate that the TrzN:MSN-10:Chit biomaterial exhibited the best overall catalytic profile making it a promising biocatalyst for the bioremediation of atrazine.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.3c00036","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"109142904","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-10-02DOI: 10.1021/acsenvironau.3c00040
Antonia Garratt, Klaudia Nguyen, Alexander Brooke, Martin J. Taylor and Maria Grazia Francesconi*,
Plastic waste is a critical global issue, yet current strategies to avoid committing plastic waste to landfills include incineration, gasification, or pyrolysis high carbon emitting and energy consuming approaches. However, plastic waste can become a resource instead of a problem if high value products, such as fine chemicals and liquid fuel molecules, can be liberated from controlled its decomposition. This letter presents proof of concept on a low-cost, low energy approach to controlled decomposition of plastic, photocatalytic hydrolysis. This approach integrates photolysis and hydrolysis, both slow natural decomposition processes, with a photocatalytic process. The photocatalyst, α-Fe2O3, is embedded into a polylactic acid (PLA) plastic matrix. The photocatalyst/plastic composite is then immersed in water and subjected to low-energy (25 W) UV light for 90 h. The monomer lactide is produced as the major product. α-Fe2O3 (6.9 wt %) was found to accelerate the PLA degradation pathway, achieving 32% solid transformation into liquid phase products, in comparison to PLA on its own, which was found to not decompose, using the same conditions. This highlights a low energy route toward plastic waste upgrade and valorization that is less carbon intensive than pyrolysis and faster than natural degradation. By directly comparing a 25 W (0.025 kWh) UV bulb with a 13 kWh furnace, the photocatalytic reaction would directly consume 520× less energy than a conventional thermochemical pathway. Furthermore, this technology can be extended and applied to other plastics, and other photocatalysts can be used.
{"title":"Photocatalytic Hydrolysis─A Sustainable Option for the Chemical Upcycling of Polylactic Acid","authors":"Antonia Garratt, Klaudia Nguyen, Alexander Brooke, Martin J. Taylor and Maria Grazia Francesconi*, ","doi":"10.1021/acsenvironau.3c00040","DOIUrl":"https://doi.org/10.1021/acsenvironau.3c00040","url":null,"abstract":"<p >Plastic waste is a critical global issue, yet current strategies to avoid committing plastic waste to landfills include incineration, gasification, or pyrolysis high carbon emitting and energy consuming approaches. However, plastic waste can become a resource instead of a problem if high value products, such as fine chemicals and liquid fuel molecules, can be liberated from controlled its decomposition. This letter presents proof of concept on a low-cost, low energy approach to controlled decomposition of plastic, photocatalytic hydrolysis. This approach integrates photolysis and hydrolysis, both slow natural decomposition processes, with a photocatalytic process. The photocatalyst, α-Fe<sub>2</sub>O<sub>3</sub>, is embedded into a polylactic acid (PLA) plastic matrix. The photocatalyst/plastic composite is then immersed in water and subjected to low-energy (25 W) UV light for 90 h. The monomer lactide is produced as the major product. α-Fe<sub>2</sub>O<sub>3</sub> (6.9 wt %) was found to accelerate the PLA degradation pathway, achieving 32% solid transformation into liquid phase products, in comparison to PLA on its own, which was found to not decompose, using the same conditions. This highlights a low energy route toward plastic waste upgrade and valorization that is less carbon intensive than pyrolysis and faster than natural degradation. By directly comparing a 25 W (0.025 kWh) UV bulb with a 13 kWh furnace, the photocatalytic reaction would directly consume 520× less energy than a conventional thermochemical pathway. Furthermore, this technology can be extended and applied to other plastics, and other photocatalysts can be used.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.3c00040","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"109142891","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-09-20DOI: 10.1021/acsenvironau.3c00042
Yujun Tao*,
{"title":"We Are All Stars─Collaboration Builds Constellations and Galaxies","authors":"Yujun Tao*, ","doi":"10.1021/acsenvironau.3c00042","DOIUrl":"10.1021/acsenvironau.3c00042","url":null,"abstract":"","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://ftp.ncbi.nlm.nih.gov/pub/pmc/oa_pdf/0d/95/vg3c00042.PMC10515707.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41167879","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-09-20DOI: 10.1021/acsenvironau.3c00051
Peter Vikesland*,
A a field, environmental science and engineering has long focused on improving our collective understanding of the processes dictating the formation, transport, and ultimate disposition of environmental contaminants. While the identities of the contaminants of interest continually change, our focus on these fundamental processes remains the same. The five contributions in this issue address a range of pollutants, including both airborne and waterborne. Yeh et al. describe the development of a “Soft Sensor” that relies upon machine learning algorithms to relate input signals acquired by common in-line sensors to water quality parameter outputs that are challenging to measure in the field. In particular, they are interested in using machine learning to predict chemical oxygen demand (COD), total suspended solids (TSS), or Escherichia coli concentrations, based upon inline turbidity, pH, ammonium ion, nitrate ion, and electrical conductivity measurements. The researchers evaluate the potential of this approach using two years of data collected at an onsite wastewater treatment system operating in a South African informal settlement. Encouragingly, their approach was successful at predicting COD (mean absolute percentage error (MAPE) of 14.5%; R2 = 0.96) and TSS (MAPE 24.8%; R2 = 0.99). However, E. coli (MAPE 71.4%; R2 = 0.22) detection remains a challenge and will require extended experimentation and the collection of larger data sets for model parametrization. In their contribution, Zambrana and Boehm reviewed the occurrence of human viruses on fomites (i.e., inanimate objects that may play a role in disease transmission). Using a systemic review based-approach, they surveyed the literature and, based upon the 134 articles that met their search criteria, found that a variety of different virus families have been detected on fomites and that the Coronaviridae are the most commonly reported. They note, however, that this finding most likely reflects expanded interrogation of fomites for SARS-CoV-2 during the COVID-19 pandemic. This contribution highlights the need to expand the range of viral targets examined on fomite surfaces. Such expansion could result in the development of fomite monitoring as a means to quantify the circulation of infectious diseases within a community. As the authors note, however, such a monitoring approach will require additional development of standardized fomite sampling protocols, standardized reporting units, and sample analysis methods that differentiate infectious viruses from noninfectious viral DNA or RNA. James and de Vos et al. examine the environmental impacts of a highly different type of pollution episode. In 2021, an onboard explosion led the M/V X-Press Pearl to catch fire off the coast of Sri Lanka, prior to its ultimate sinking. This fire resulted in the release of hundreds of tons of high-density polyethylene and low density polyethylene resin pellets, or nurdles. Because of the onboard fire, these nurdles
{"title":"Environmental Contaminants─Today, Tomorrow, and Forever","authors":"Peter Vikesland*, ","doi":"10.1021/acsenvironau.3c00051","DOIUrl":"10.1021/acsenvironau.3c00051","url":null,"abstract":"A a field, environmental science and engineering has long focused on improving our collective understanding of the processes dictating the formation, transport, and ultimate disposition of environmental contaminants. While the identities of the contaminants of interest continually change, our focus on these fundamental processes remains the same. The five contributions in this issue address a range of pollutants, including both airborne and waterborne. Yeh et al. describe the development of a “Soft Sensor” that relies upon machine learning algorithms to relate input signals acquired by common in-line sensors to water quality parameter outputs that are challenging to measure in the field. In particular, they are interested in using machine learning to predict chemical oxygen demand (COD), total suspended solids (TSS), or Escherichia coli concentrations, based upon inline turbidity, pH, ammonium ion, nitrate ion, and electrical conductivity measurements. The researchers evaluate the potential of this approach using two years of data collected at an onsite wastewater treatment system operating in a South African informal settlement. Encouragingly, their approach was successful at predicting COD (mean absolute percentage error (MAPE) of 14.5%; R2 = 0.96) and TSS (MAPE 24.8%; R2 = 0.99). However, E. coli (MAPE 71.4%; R2 = 0.22) detection remains a challenge and will require extended experimentation and the collection of larger data sets for model parametrization. In their contribution, Zambrana and Boehm reviewed the occurrence of human viruses on fomites (i.e., inanimate objects that may play a role in disease transmission). Using a systemic review based-approach, they surveyed the literature and, based upon the 134 articles that met their search criteria, found that a variety of different virus families have been detected on fomites and that the Coronaviridae are the most commonly reported. They note, however, that this finding most likely reflects expanded interrogation of fomites for SARS-CoV-2 during the COVID-19 pandemic. This contribution highlights the need to expand the range of viral targets examined on fomite surfaces. Such expansion could result in the development of fomite monitoring as a means to quantify the circulation of infectious diseases within a community. As the authors note, however, such a monitoring approach will require additional development of standardized fomite sampling protocols, standardized reporting units, and sample analysis methods that differentiate infectious viruses from noninfectious viral DNA or RNA. James and de Vos et al. examine the environmental impacts of a highly different type of pollution episode. In 2021, an onboard explosion led the M/V X-Press Pearl to catch fire off the coast of Sri Lanka, prior to its ultimate sinking. This fire resulted in the release of hundreds of tons of high-density polyethylene and low density polyethylene resin pellets, or nurdles. Because of the onboard fire, these nurdles ","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://ftp.ncbi.nlm.nih.gov/pub/pmc/oa_pdf/e6/64/vg3c00051.PMC10515706.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41170234","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-09-11DOI: 10.1021/acsenvironau.3c00015
Kotiba Malek, Kanishk Gohil, Esther A. Olonimoyo, Nahin Ferdousi-Rokib, Qishen Huang, Kiran R. Pitta, Lucy Nandy, Katelyn A. Voss, Timothy M. Raymond*, Dabrina D Dutcher*, Miriam Arak Freedman* and Akua Asa-Awuku*,
It is well known that atmospheric aerosol size and composition impact air quality, climate, and health. The aerosol composition is typically a mixture and consists of a wide range of organic and inorganic particles that interact with each other. Furthermore, water vapor is ubiquitous in the atmosphere, in indoor air, and within the human body’s respiratory system, and the presence of water can alter the aerosol morphology and propensity to form droplets. Specifically, aerosol mixtures can undergo liquid–liquid phase separation (LLPS) in the presence of water vapor. However, the experimental conditions for which LLPS impacts water uptake and the subsequent prediction of aerosol mixtures are poorly understood. To improve our understanding of aerosol mixtures and droplets, this study explores two ternary systems that undergo LLPS, namely, the 2MGA system (sucrose + ammonium sulfate + 2-methylglutaric acid) and the PEG1000 system (sucrose + ammonium sulfate + polyethylene glycol 1000). In this study, the ratio of species and the O:C ratios are systematically changed, and the hygroscopic properties of the resultant aerosol were investigated. Here, we show that the droplet activation above 100% RH of the 2MGA system was influenced by LLPS, while the droplet activation of the PEG1000 system was observed to be linearly additive regardless of chemical composition, O:C ratio, and LLPS. A theoretical model that accounts for LLPS with O:C ratios was developed and predicts the water uptake of internally mixed systems of different compositions and phase states. Hence, this study provides a computationally efficient algorithm to account for the LLPS and solubility parameterized by the O:C ratio for droplet activation at supersaturated relative humidity conditions and may thus be extended to mixed inorganic–organic aerosol populations with unspeciated organic composition found in the ambient environment.
{"title":"Liquid–Liquid Phase Separation Can Drive Aerosol Droplet Growth in Supersaturated Regimes","authors":"Kotiba Malek, Kanishk Gohil, Esther A. Olonimoyo, Nahin Ferdousi-Rokib, Qishen Huang, Kiran R. Pitta, Lucy Nandy, Katelyn A. Voss, Timothy M. Raymond*, Dabrina D Dutcher*, Miriam Arak Freedman* and Akua Asa-Awuku*, ","doi":"10.1021/acsenvironau.3c00015","DOIUrl":"https://doi.org/10.1021/acsenvironau.3c00015","url":null,"abstract":"<p >It is well known that atmospheric aerosol size and composition impact air quality, climate, and health. The aerosol composition is typically a mixture and consists of a wide range of organic and inorganic particles that interact with each other. Furthermore, water vapor is ubiquitous in the atmosphere, in indoor air, and within the human body’s respiratory system, and the presence of water can alter the aerosol morphology and propensity to form droplets. Specifically, aerosol mixtures can undergo liquid–liquid phase separation (LLPS) in the presence of water vapor. However, the experimental conditions for which LLPS impacts water uptake and the subsequent prediction of aerosol mixtures are poorly understood. To improve our understanding of aerosol mixtures and droplets, this study explores two ternary systems that undergo LLPS, namely, the 2MGA system (sucrose + ammonium sulfate + 2-methylglutaric acid) and the PEG1000 system (sucrose + ammonium sulfate + polyethylene glycol 1000). In this study, the ratio of species and the O:C ratios are systematically changed, and the hygroscopic properties of the resultant aerosol were investigated. Here, we show that the droplet activation above 100% RH of the 2MGA system was influenced by LLPS, while the droplet activation of the PEG1000 system was observed to be linearly additive regardless of chemical composition, O:C ratio, and LLPS. A theoretical model that accounts for LLPS with O:C ratios was developed and predicts the water uptake of internally mixed systems of different compositions and phase states. Hence, this study provides a computationally efficient algorithm to account for the LLPS and solubility parameterized by the O:C ratio for droplet activation at supersaturated relative humidity conditions and may thus be extended to mixed inorganic–organic aerosol populations with unspeciated organic composition found in the ambient environment.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.3c00015","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"109143021","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-07-26DOI: 10.1021/acsenvironau.3c00023
Srinidhi Lokesh, Siththarththan Arunthavabalan, Elie Hajj, Edgard Hitti and Yu Yang*,
N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine (6PPD)-quinone (6PPD-Q), a transformation byproduct of 6PPD used in tires as an antiozonant and antioxidant, was recently discovered as the chemical primarily responsible for the acute lethal toxicity of urban storm runoff to coho salmon. The asphalt concrete (AC) surface layer is the primary medium to contact 6PPD-Q immediately upon its release from tires, and the addition of recycled tire rubber (RTR) to the asphalt binder and mixture is a widely accepted practice in asphalt production. Therefore, it is urgent to understand the fate of 6PPD-Q at the asphalt concrete surface layer–water interface. This study analyzed the sorption and desorption of 6PPD-Q by compacted and crushed loose (loose particles, ∼5 mm) rubberized asphalt mixtures and their mobilization from compacted asphalt mixtures during simulated rainfall events. It should be noted that the crushed loose asphalt mixtures demonstrated the physicochemical properties of the asphalt materials, while the compacted asphalt mixtures represent in-service AC layers. Sorption of 6PPD-Q by crushed loose and compacted asphalt mixtures reached equilibrium within 12 days, with a sorption coefficient of 151.57–257.51 L/kg for compacted asphalt mixtures. Within 12 days, desorption of 6PPD-Q from crushed loose and compacted rubberized asphalt mixtures (20 g particles/L) to the double deionized (DDI) water and synthetic stormwater was 0.01–0.09 and 0.025–0.05 μg/L, respectively. Through the rainfall simulation experiments, 0.0015–0.0049 μg/L 6PPD-Q was detected in the runoff water, much lower than the lethal concentration (LC50) of 6PPD-Q of 0.095 μg/L and 308.67 μg/L for coho salmon and zebrafish larvae. Our results indicate that, while the release of 6PPD-Q from compacted rubberized asphalt mixtures is minor, the mixtures can serve as sorbents for tire-derived 6PPD-Q and retain this emerging contaminant.
{"title":"Investigation of 6PPD-Quinone in Rubberized Asphalt Concrete Mixtures","authors":"Srinidhi Lokesh, Siththarththan Arunthavabalan, Elie Hajj, Edgard Hitti and Yu Yang*, ","doi":"10.1021/acsenvironau.3c00023","DOIUrl":"10.1021/acsenvironau.3c00023","url":null,"abstract":"<p >N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine (6PPD)-quinone (6PPD-Q), a transformation byproduct of 6PPD used in tires as an antiozonant and antioxidant, was recently discovered as the chemical primarily responsible for the acute lethal toxicity of urban storm runoff to coho salmon. The asphalt concrete (AC) surface layer is the primary medium to contact 6PPD-Q immediately upon its release from tires, and the addition of recycled tire rubber (RTR) to the asphalt binder and mixture is a widely accepted practice in asphalt production. Therefore, it is urgent to understand the fate of 6PPD-Q at the asphalt concrete surface layer–water interface. This study analyzed the sorption and desorption of 6PPD-Q by compacted and crushed loose (loose particles, ∼5 mm) rubberized asphalt mixtures and their mobilization from compacted asphalt mixtures during simulated rainfall events. It should be noted that the crushed loose asphalt mixtures demonstrated the physicochemical properties of the asphalt materials, while the compacted asphalt mixtures represent in-service AC layers. Sorption of 6PPD-Q by crushed loose and compacted asphalt mixtures reached equilibrium within 12 days, with a sorption coefficient of 151.57–257.51 L/kg for compacted asphalt mixtures. Within 12 days, desorption of 6PPD-Q from crushed loose and compacted rubberized asphalt mixtures (20 g particles/L) to the double deionized (DDI) water and synthetic stormwater was 0.01–0.09 and 0.025–0.05 μg/L, respectively. Through the rainfall simulation experiments, 0.0015–0.0049 μg/L 6PPD-Q was detected in the runoff water, much lower than the lethal concentration (LC<sub>50</sub>) of 6PPD-Q of 0.095 μg/L and 308.67 μg/L for coho salmon and zebrafish larvae. Our results indicate that, while the release of 6PPD-Q from compacted rubberized asphalt mixtures is minor, the mixtures can serve as sorbents for tire-derived 6PPD-Q and retain this emerging contaminant.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-07-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.3c00023","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"45868344","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-07-25DOI: 10.1021/acsenvironau.3c00025
Winnie Zambrana, and , Alexandria B. Boehm*,
Documenting the occurrence of viruses on fomites is crucial in determining the significance of fomite-mediated transmission and the potential use of fomites for environmental disease surveillance. We conducted a systematic review and meta-analysis to compile information on the occurrence of human viruses on fomites in the environment; we identified 134 peer-reviewed papers. We compiled sampling and measurement methods, results, quality control information, and whether virus data were compared with community health data from the papers. We conducted univariate and multivariate analyses to investigate if presence of virus on fomites was associated with virus type (enveloped, nonenveloped), sampling location (healthcare setting, nonhealthcare temporary setting, nonhealthcare nontemporary setting), and area of fomite swabbed (<50, 50–100, >100 cm2). Across 275 data sets from the 134 papers, there was the most data available for Coronaviridae and from fomites at hospitals. Positivity rates, defined as the percent positive fomite samples, were low (median = 6%). Data were available on viruses from 16 different viral families, but data on viruses from 9 families had few (n < 5) data sets. Many human virus families were not identified in this review (11 families). Less than 15% of the data sets reported virus concentrations in externally valid units (viruses per area of surface), and 16% provided a quantitative comparison between virus and health data. Virus type and area swabbed were significant predictors of virus presence on fomites, and the positivity rate of data sets collected from healthcare settings and nonhealthcare nontemporary settings (e.g., individual housing) were significantly higher than those collected in nonhealthcare temporary settings (e.g., restaurants). Data from this review indicates that viruses may be present on fomites, that fomite-mediated virus transmission may occur, and that fomites may provide information on circulation of infectious diseases in the community. However, more quantitative data on diverse viruses are needed, and method reporting needs significant improvements.
{"title":"Occurrence of Human Viruses on Fomites in the Environment: A Systematic Review and Meta-analysis","authors":"Winnie Zambrana, and , Alexandria B. Boehm*, ","doi":"10.1021/acsenvironau.3c00025","DOIUrl":"10.1021/acsenvironau.3c00025","url":null,"abstract":"<p >Documenting the occurrence of viruses on fomites is crucial in determining the significance of fomite-mediated transmission and the potential use of fomites for environmental disease surveillance. We conducted a systematic review and meta-analysis to compile information on the occurrence of human viruses on fomites in the environment; we identified 134 peer-reviewed papers. We compiled sampling and measurement methods, results, quality control information, and whether virus data were compared with community health data from the papers. We conducted univariate and multivariate analyses to investigate if presence of virus on fomites was associated with virus type (enveloped, nonenveloped), sampling location (healthcare setting, nonhealthcare temporary setting, nonhealthcare nontemporary setting), and area of fomite swabbed (<50, 50–100, >100 cm<sup>2</sup>). Across 275 data sets from the 134 papers, there was the most data available for Coronaviridae and from fomites at hospitals. Positivity rates, defined as the percent positive fomite samples, were low (median = 6%). Data were available on viruses from 16 different viral families, but data on viruses from 9 families had few (<i>n</i> < 5) data sets. Many human virus families were not identified in this review (11 families). Less than 15% of the data sets reported virus concentrations in externally valid units (viruses per area of surface), and 16% provided a quantitative comparison between virus and health data. Virus type and area swabbed were significant predictors of virus presence on fomites, and the positivity rate of data sets collected from healthcare settings and nonhealthcare nontemporary settings (e.g., individual housing) were significantly higher than those collected in nonhealthcare temporary settings (e.g., restaurants). Data from this review indicates that viruses may be present on fomites, that fomite-mediated virus transmission may occur, and that fomites may provide information on circulation of infectious diseases in the community. However, more quantitative data on diverse viruses are needed, and method reporting needs significant improvements.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://ftp.ncbi.nlm.nih.gov/pub/pmc/oa_pdf/fb/83/vg3c00025.PMC10515712.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41167878","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}