Pub Date : 2024-07-05DOI: 10.1021/acs.estlett.4c0036610.1021/acs.estlett.4c00366
Anna Kogler, Meili Gong, Kindle S. Williams and William A. Tarpeh*,
Nitrogen in wastewater can be recovered to prevent negative environmental, human health, and economic impacts and to enable distributed chemical manufacturing. We developed novel flexible electrochemical stripping (FECS) for tunable recovery of ammonia/ammonium (total ammonia nitrogen, TAN) from urine as (NH4)2SO4 and aqueous NH3. Batch and continuous experiments demonstrated that product speciation could be readily controlled by modifying electrochemical cell operation frequency, duration, and applied current without affecting TAN removal. During continuous experiments, FECS recovered NH3 solutions with concentrations similar to ready-to-use cleaners (1% and 2% NH3 (w/w) or 8.22 and 16.4 g/L TAN) and cleaner concentrates (5% NH3 (w/w) or 41.1 g/L TAN), as well as (NH4)2SO4 solutions between 5 and 18.4 g/L TAN, approaching commercial fertilizer concentrations (28.4 g/L TAN). Beyond modifying applied current, future process engineering and operating condition optimization should reduce energy consumption, increase recovery efficiency, and enhance economic viability of FECS. Our findings will enable the development and deployment of electrochemical nitrogen recovery in contexts with varying needs for ammonia-based products, paving the way for circular economies that integrate distributed chemical manufacturing with sanitation systems.
{"title":"Flexible Electrochemical Stripping for Wastewater Ammonia Recovery with On-Demand Product Tunability","authors":"Anna Kogler, Meili Gong, Kindle S. Williams and William A. Tarpeh*, ","doi":"10.1021/acs.estlett.4c0036610.1021/acs.estlett.4c00366","DOIUrl":"https://doi.org/10.1021/acs.estlett.4c00366https://doi.org/10.1021/acs.estlett.4c00366","url":null,"abstract":"<p >Nitrogen in wastewater can be recovered to prevent negative environmental, human health, and economic impacts and to enable distributed chemical manufacturing. We developed novel flexible electrochemical stripping (FECS) for tunable recovery of ammonia/ammonium (total ammonia nitrogen, TAN) from urine as (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> and aqueous NH<sub>3</sub>. Batch and continuous experiments demonstrated that product speciation could be readily controlled by modifying electrochemical cell operation frequency, duration, and applied current without affecting TAN removal. During continuous experiments, FECS recovered NH<sub>3</sub> solutions with concentrations similar to ready-to-use cleaners (1% and 2% NH<sub>3</sub> (w/w) or 8.22 and 16.4 g/L TAN) and cleaner concentrates (5% NH<sub>3</sub> (w/w) or 41.1 g/L TAN), as well as (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> solutions between 5 and 18.4 g/L TAN, approaching commercial fertilizer concentrations (28.4 g/L TAN). Beyond modifying applied current, future process engineering and operating condition optimization should reduce energy consumption, increase recovery efficiency, and enhance economic viability of FECS. Our findings will enable the development and deployment of electrochemical nitrogen recovery in contexts with varying needs for ammonia-based products, paving the way for circular economies that integrate distributed chemical manufacturing with sanitation systems.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"11 8","pages":"886–894 886–894"},"PeriodicalIF":8.9,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141972634","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-02DOI: 10.1021/acs.estlett.4c0048510.1021/acs.estlett.4c00485
Bethany Oceguera Johnson, Marlee Shaffer, Devin North, Kien Vu and Kyle Bibby*,
Plasmid pBI143 has recently been identified as being highly abundant in the human gut microbiome, suggesting potential as a fecal water quality indicator and normalization marker in wastewater-based surveillance. We evaluated the relative concentration efficiency and spatial–temporal distribution in raw wastewater to inform its development as a marker. The results showed significantly higher (p < 0.01) enrichment in raw wastewater solids (mean of 9.2 × 107 GC/mL) than in liquid fractions [mean of 2.3 × 106 genome copies (GC)/mL]. The relative concentration efficiencies were 28% for nanotrap particles, 23% for Amicon ultrafiltration, 3.6% for pH drop and filtration, 4% for skim milk flocculation, and 0.04% for poly(ethylene glycol) precipitation compared to direct wastewater extraction. DNase pretreatment reduced pBI143 levels by 90.3%, indicating that it is mainly extracellular in raw wastewater. Over 21 days, pBI143 levels remained stable and were consistently a mean of 1.3 log10 higher than other fecal indicators (Carjivirus, PMMoV, and HF183). In raw wastewater from eight states (n = 16), pBI143 concentrations averaged 2.2 × 106 GC/mL (95% confidence interval of 1.7–2.7 × 106) and pBI143 was detected in all samples. The findings support pBI143’s potential as a fecal indicator and normalization marker, though further validation is needed to confirm its specificity to humans.
{"title":"Assessing the Relative Concentration Efficiency and Spatial–Temporal Distribution of Plasmid pBI143 in Raw Wastewater","authors":"Bethany Oceguera Johnson, Marlee Shaffer, Devin North, Kien Vu and Kyle Bibby*, ","doi":"10.1021/acs.estlett.4c0048510.1021/acs.estlett.4c00485","DOIUrl":"https://doi.org/10.1021/acs.estlett.4c00485https://doi.org/10.1021/acs.estlett.4c00485","url":null,"abstract":"<p >Plasmid pBI143 has recently been identified as being highly abundant in the human gut microbiome, suggesting potential as a fecal water quality indicator and normalization marker in wastewater-based surveillance. We evaluated the relative concentration efficiency and spatial–temporal distribution in raw wastewater to inform its development as a marker. The results showed significantly higher (<i>p</i> < 0.01) enrichment in raw wastewater solids (mean of 9.2 × 10<sup>7</sup> GC/mL) than in liquid fractions [mean of 2.3 × 10<sup>6</sup> genome copies (GC)/mL]. The relative concentration efficiencies were 28% for nanotrap particles, 23% for Amicon ultrafiltration, 3.6% for pH drop and filtration, 4% for skim milk flocculation, and 0.04% for poly(ethylene glycol) precipitation compared to direct wastewater extraction. DNase pretreatment reduced pBI143 levels by 90.3%, indicating that it is mainly extracellular in raw wastewater. Over 21 days, pBI143 levels remained stable and were consistently a mean of 1.3 log<sub>10</sub> higher than other fecal indicators (<i>Carjivirus</i>, PMMoV, and HF183). In raw wastewater from eight states (<i>n</i> = 16), pBI143 concentrations averaged 2.2 × 10<sup>6</sup> GC/mL (95% confidence interval of 1.7–2.7 × 10<sup>6</sup>) and pBI143 was detected in all samples. The findings support pBI143’s potential as a fecal indicator and normalization marker, though further validation is needed to confirm its specificity to humans.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"11 8","pages":"812–817 812–817"},"PeriodicalIF":8.9,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141973096","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-30DOI: 10.1021/acs.estlett.4c0039910.1021/acs.estlett.4c00399
Luis Guanter*, Javier Roger, Shubham Sharma, Adriana Valverde, Itziar Irakulis-Loitxate, Javier Gorroño, Xin Zhang, Berend J. Schuit, Joannes D. Maasakkers, Ilse Aben, Alexis Groshenry, Antoine Benoit, Quentin Peyle and Daniel Zavala-Araiza,
Accidental blowouts in oil and gas wells can result in large and prolonged methane emissions, which are often unreported when happening in remote places. The rapid advancement of space-based methods for detecting and quantifying methane plumes provides an essential tool for uncovering these superemission events. We use a number of methane-sensitive satellite missions, including the Sentinel-5P/TROPOMI global mapper and several high-resolution instruments, to document a methane leak from a well blowout happening in Kazakhstan’s Karaturun East oil field in 2023. A dense time series of plume detections from those satellites shows that the leak was active during 205 days and that most of the emissions were in the range 20–50 t/h. Using 48 high-quality emission rate estimates, we calculate that a total of 131 ± 34 kt of methane was released to the atmosphere during this leak, which exceeds the total emissions from all previously documented accidents. Our study characterizes the evolution and magnitude of the 2023 Karaturun East methane leak and showcases how different types of satellite instruments can be combined to document and quantify methane leaks active during long time periods.
{"title":"Multisatellite Data Depicts a Record-Breaking Methane Leak from a Well Blowout","authors":"Luis Guanter*, Javier Roger, Shubham Sharma, Adriana Valverde, Itziar Irakulis-Loitxate, Javier Gorroño, Xin Zhang, Berend J. Schuit, Joannes D. Maasakkers, Ilse Aben, Alexis Groshenry, Antoine Benoit, Quentin Peyle and Daniel Zavala-Araiza, ","doi":"10.1021/acs.estlett.4c0039910.1021/acs.estlett.4c00399","DOIUrl":"https://doi.org/10.1021/acs.estlett.4c00399https://doi.org/10.1021/acs.estlett.4c00399","url":null,"abstract":"<p >Accidental blowouts in oil and gas wells can result in large and prolonged methane emissions, which are often unreported when happening in remote places. The rapid advancement of space-based methods for detecting and quantifying methane plumes provides an essential tool for uncovering these superemission events. We use a number of methane-sensitive satellite missions, including the Sentinel-5P/TROPOMI global mapper and several high-resolution instruments, to document a methane leak from a well blowout happening in Kazakhstan’s Karaturun East oil field in 2023. A dense time series of plume detections from those satellites shows that the leak was active during 205 days and that most of the emissions were in the range 20–50 t/h. Using 48 high-quality emission rate estimates, we calculate that a total of 131 ± 34 kt of methane was released to the atmosphere during this leak, which exceeds the total emissions from all previously documented accidents. Our study characterizes the evolution and magnitude of the 2023 Karaturun East methane leak and showcases how different types of satellite instruments can be combined to document and quantify methane leaks active during long time periods.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"11 8","pages":"825–830 825–830"},"PeriodicalIF":8.9,"publicationDate":"2024-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.estlett.4c00399","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141973382","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-28DOI: 10.1021/acs.estlett.4c0026410.1021/acs.estlett.4c00264
Jenifer Shantha Kumar, Arijit Jana, Jayathraa Raman, Hema Madhuri Veera, Amoghavarsha Ramachandra Kini, Jayoti Roy, Saurav Kanti Jana, Tiju Thomas and Thalappil Pradeep*,
Rapid and naked-eye detection of water-borne contaminants using molecularly precise nanomaterials has emerged as a promising strategy to reduce the impact of chemical pollution. This study presents a luminescence-based arsenic (As) sensor, eliminating the need for sample preparation. Incorporating red-emitting spheroidal cluster-assembled superstructures (CASs), comprised of Cu17 nanoclusters (Cu17NCs), coprotected by l-cysteine (l-Cys) and 1,2-bis(diphenylphosphino) ethane (DPPE) ligands, the sensor exhibits notable sensitivity toward arsenite (As3+) and (As5+) ions. A detection limit of 1 ppb in tap water was achieved through luminescence-based quenching. Remarkably, it demonstrates selective detection of As amidst common interfering metal ions such as Cd2+, Hg2+, Fe3+, Pb2+, Cu2+, and Cr3+. A sensor disc made of CASs coated on nonwoven polypropylene (PP) mats has been devised for practical field applications. Electron microscopy reveals disrupted morphology of the spheroids due to As interaction. Moreover, the CASs exhibit significant antibacterial efficacy against Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus and antibiofilm properties against Bacillus subtilis. This research highlights the effectiveness of atomically precise clusters for a practical application with direct societal relevance.
{"title":"Cysteine-Protected Antibacterial Spheroids of Atomically Precise Copper Clusters for Direct and Affordable Arsenic Detection from Drinking Water","authors":"Jenifer Shantha Kumar, Arijit Jana, Jayathraa Raman, Hema Madhuri Veera, Amoghavarsha Ramachandra Kini, Jayoti Roy, Saurav Kanti Jana, Tiju Thomas and Thalappil Pradeep*, ","doi":"10.1021/acs.estlett.4c0026410.1021/acs.estlett.4c00264","DOIUrl":"https://doi.org/10.1021/acs.estlett.4c00264https://doi.org/10.1021/acs.estlett.4c00264","url":null,"abstract":"<p >Rapid and naked-eye detection of water-borne contaminants using molecularly precise nanomaterials has emerged as a promising strategy to reduce the impact of chemical pollution. This study presents a luminescence-based arsenic (<i>As</i>) sensor, eliminating the need for sample preparation. Incorporating red-emitting spheroidal cluster-assembled superstructures (CASs), comprised of Cu<sub>17</sub> nanoclusters (Cu<sub>17</sub>NCs), coprotected by <span>l</span>-cysteine (<span>l</span>-Cys) and 1,2-bis(diphenylphosphino) ethane (DPPE) ligands, the sensor exhibits notable sensitivity toward arsenite (<i>As</i><sup>3+</sup>) and (<i>As</i><sup>5+</sup>) ions. A detection limit of 1 ppb in tap water was achieved through luminescence-based quenching. Remarkably, it demonstrates selective detection of <i>As</i> amidst common interfering metal ions such as Cd<sup>2+</sup>, Hg<sup>2+</sup>, Fe<sup>3+</sup>, Pb<sup>2+</sup>, Cu<sup>2+</sup>, and Cr<sup>3+</sup>. A sensor disc made of CASs coated on nonwoven polypropylene (PP) mats has been devised for practical field applications. Electron microscopy reveals disrupted morphology of the spheroids due to <i>As</i> interaction. Moreover, the CASs exhibit significant antibacterial efficacy against Gram-negative <i>Escherichia coli</i> and Gram-positive <i>Staphylococcus aureus</i> and antibiofilm properties against <i>Bacillus subtilis</i>. This research highlights the effectiveness of atomically precise clusters for a practical application with direct societal relevance.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"11 8","pages":"831–837 831–837"},"PeriodicalIF":8.9,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141973503","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The UV/sulfite process shows great potential for reductively degrading or eliminating pollutants. While its mechanism in neutral and alkaline environments has been well-elucidated, the reaction pathway under acidic conditions remains unclear. Herein, we report the novel findings of the formation of reductive SO2•– radicals and their derivatives in the UV/sulfite process at pH levels below 4. Mechanistic investigation revealed that H• radicals and SO3•– radicals formed by the photolysis of sulfite under acidic conditions, with the H• radicals being scavenged by sulfite to produce SO2•– radicals. Subsequently, these SO2•– radicals are transformed into dithionite, thiosulfate, hydrogen sulfide, and elemental sulfur through a series of intricate reactions. This study is expected to expand the potential application of the UV/sulfite process under acid conditions.
{"title":"New Insights into the Mechanism of the UV/Sulfite Process: Formation of SO2•– Radicals and Their Derivatives under Acidic Conditions","authors":"Linghao Kong, Zhe Jin, Feng Zhu, Mengchang He, Feng Qian and Xianjia Peng*, ","doi":"10.1021/acs.estlett.4c00251","DOIUrl":"10.1021/acs.estlett.4c00251","url":null,"abstract":"<p >The UV/sulfite process shows great potential for reductively degrading or eliminating pollutants. While its mechanism in neutral and alkaline environments has been well-elucidated, the reaction pathway under acidic conditions remains unclear. Herein, we report the novel findings of the formation of reductive SO<sub>2</sub><sup>•–</sup> radicals and their derivatives in the UV/sulfite process at pH levels below 4. Mechanistic investigation revealed that H• radicals and SO<sub>3</sub><sup>•–</sup> radicals formed by the photolysis of sulfite under acidic conditions, with the H• radicals being scavenged by sulfite to produce SO<sub>2</sub><sup>•–</sup> radicals. Subsequently, these SO<sub>2</sub><sup>•–</sup> radicals are transformed into dithionite, thiosulfate, hydrogen sulfide, and elemental sulfur through a series of intricate reactions. This study is expected to expand the potential application of the UV/sulfite process under acid conditions.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"11 7","pages":"752–758"},"PeriodicalIF":8.9,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141522076","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-26DOI: 10.1021/acs.estlett.4c0040910.1021/acs.estlett.4c00409
Matthew S. Savoca*, Anna R. Robuck, Michaela A. Cashman, Mark G. Cantwell, Lindsay C. Agvent, David N. Wiley, Rachel Rice, Sean Todd, Nicole E. Hunter, Jooke Robbins, Jeremy A. Goldbogen and Rainer Lohmann,
Per- and polyfluoroalkyl substances (PFAS) comprise >10 000 synthetic compounds that are globally distributed and highly persistent but remain challenging to monitor. Here we assess the utility of baleen─an accreting, keratinaceous tissue that baleen whales use for filter-feeding─to track PFAS dynamics in marine food webs. In six species investigated, PFAS were detected in all baleen tested (n = 18 plates, 220 samples, ∑10PFAS range of 0.02–60.5 ng/g of dry weight), at levels higher than those of other tissue types besides liver. Three of the species in our data set had not been tested for PFAS contamination previously, and two of those species (blue whale and North Atlantic right whale) are internationally endangered species. Apparent links were observed between PFAS and life-history events by testing successive subsamples along the growth axis of the baleen plates. These results establish baleen as a viable sample matrix for assessing PFAS contamination in marine ecosystems by enabling multiyear time-series analyses through single-tissue sampling with seasonal resolution.
{"title":"Whale Baleen To Monitor Per- and Polyfluoroalkyl Substances (PFAS) in Marine Environments","authors":"Matthew S. Savoca*, Anna R. Robuck, Michaela A. Cashman, Mark G. Cantwell, Lindsay C. Agvent, David N. Wiley, Rachel Rice, Sean Todd, Nicole E. Hunter, Jooke Robbins, Jeremy A. Goldbogen and Rainer Lohmann, ","doi":"10.1021/acs.estlett.4c0040910.1021/acs.estlett.4c00409","DOIUrl":"https://doi.org/10.1021/acs.estlett.4c00409https://doi.org/10.1021/acs.estlett.4c00409","url":null,"abstract":"<p >Per- and polyfluoroalkyl substances (PFAS) comprise >10 000 synthetic compounds that are globally distributed and highly persistent but remain challenging to monitor. Here we assess the utility of baleen─an accreting, keratinaceous tissue that baleen whales use for filter-feeding─to track PFAS dynamics in marine food webs. In six species investigated, PFAS were detected in all baleen tested (<i>n</i> = 18 plates, 220 samples, ∑<sub>10</sub>PFAS range of 0.02–60.5 ng/g of dry weight), at levels higher than those of other tissue types besides liver. Three of the species in our data set had not been tested for PFAS contamination previously, and two of those species (blue whale and North Atlantic right whale) are internationally endangered species. Apparent links were observed between PFAS and life-history events by testing successive subsamples along the growth axis of the baleen plates. These results establish baleen as a viable sample matrix for assessing PFAS contamination in marine ecosystems by enabling multiyear time-series analyses through single-tissue sampling with seasonal resolution.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"11 8","pages":"862–870 862–870"},"PeriodicalIF":8.9,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141973379","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-26DOI: 10.1021/acs.estlett.4c00364
Ashley M. Lin, Jake T. Thompson, Jeremy P. Koelmel, Yalan Liu, John A. Bowden and Timothy G. Townsend*,
The undisclosed and ubiquitous use of perfluoroalkyl and polyfluoroalkyl substances (PFAS) in consumer products has led to a growing issue of environmental pollution, particularly within the solid waste community, where the fate of volatile (neutral) PFAS in landfilled refuse is not well understood. Here, three municipal solid waste landfills in Florida were assessed for neutral PFAS in landfill gas and ionic PFAS in landfill leachate to compare the relative mobility between the two pathways. Landfill gas was directly sampled using a high volume, XAD-2 resin based sampling approach developed for adsorption and analysis of 27 neutral PFAS. Across sites, 13 neutral PFAS were identified from fluorotelomer alcohol (FTOH), fluorotelomer olefin (FTO), secondary FTOH, fluorotelomer acetate (FTOAc), and fluorotelomer methyl acrylate (FTMAc) classes; however, FTOHs dominated concentrations (87–97% total neutral PFAS), with most detections surpassing utilized calibration levels. Even under conservative assumptions, the mass of fluorine leaving in landfill gas (32–76%) was comparable to or greater than the mass leaving in landfill leachate (24–68%). These findings suggest that landfill gas, a less scrutinized byproduct, serves as a major pathway for the mobility of PFAS from landfills.
{"title":"Landfill Gas: A Major Pathway for Neutral Per- and Polyfluoroalkyl Substance (PFAS) Release","authors":"Ashley M. Lin, Jake T. Thompson, Jeremy P. Koelmel, Yalan Liu, John A. Bowden and Timothy G. Townsend*, ","doi":"10.1021/acs.estlett.4c00364","DOIUrl":"10.1021/acs.estlett.4c00364","url":null,"abstract":"<p >The undisclosed and ubiquitous use of perfluoroalkyl and polyfluoroalkyl substances (PFAS) in consumer products has led to a growing issue of environmental pollution, particularly within the solid waste community, where the fate of volatile (neutral) PFAS in landfilled refuse is not well understood. Here, three municipal solid waste landfills in Florida were assessed for neutral PFAS in landfill gas and ionic PFAS in landfill leachate to compare the relative mobility between the two pathways. Landfill gas was directly sampled using a high volume, XAD-2 resin based sampling approach developed for adsorption and analysis of 27 neutral PFAS. Across sites, 13 neutral PFAS were identified from fluorotelomer alcohol (FTOH), fluorotelomer olefin (FTO), secondary FTOH, fluorotelomer acetate (FTOAc), and fluorotelomer methyl acrylate (FTMAc) classes; however, FTOHs dominated concentrations (87–97% total neutral PFAS), with most detections surpassing utilized calibration levels. Even under conservative assumptions, the mass of fluorine leaving in landfill gas (32–76%) was comparable to or greater than the mass leaving in landfill leachate (24–68%). These findings suggest that landfill gas, a less scrutinized byproduct, serves as a major pathway for the mobility of PFAS from landfills.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"11 7","pages":"730–737"},"PeriodicalIF":8.9,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141522074","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-25DOI: 10.1021/acs.estlett.4c00384
Ran Yin*, Xinyi Ruan, Jiadong Peng, Jing Zhao, Yuliang Zhang, Arnaud Heuzard and Chii Shang,
Increasing radical yields to reduce energy consumption for micropollutant degradation would make advanced oxidation processes more sustainable in the context of the United Nations’ Sustainable Development Goals and carbon neutrality. We herein demonstrate that switching the UV radiation source from conventional low-pressure UV (UV254) to far-UVC (UV222) increases the UV fluence-based concentration of hydroxyl radicals (HO•) in the UV/peracetic acid (UV/PAA) process by 4.1-fold and 27.9-fold in deionized water and real surface water, respectively. Acetyloxyl radicals (CH3C(O)O•) are generated in the UV222/PAA process at a steady-state concentration of 2.4 × 10–12 M in deionized water, while they are undetectable in the UV254/PAA process under the comparable conditions. The enhancement to radical production is mainly attributed to the 15.7-fold higher molar absorption coefficients of PAA0 at 222 nm than 254 nm (50 vs 3.5 M–1 cm–1), which suppresses the compromised 1.1-fold lower innate quantum yield at 222 nm than 254 nm (0.78 vs 0.86 mol einstein–1). The enhanced radical generation and direct photolysis promote the fluence-based degradation rate constants of bisphenol A, phenol, and nitrobenzene by 4.1-fold, 3.3-fold, and 2.9-fold in the UV222/PAA process than the UV254/PAA process.
{"title":"Control of Micropollutants in Water by Far-UVC Photolysis of Peracetic Acid","authors":"Ran Yin*, Xinyi Ruan, Jiadong Peng, Jing Zhao, Yuliang Zhang, Arnaud Heuzard and Chii Shang, ","doi":"10.1021/acs.estlett.4c00384","DOIUrl":"10.1021/acs.estlett.4c00384","url":null,"abstract":"<p >Increasing radical yields to reduce energy consumption for micropollutant degradation would make advanced oxidation processes more sustainable in the context of the United Nations’ Sustainable Development Goals and carbon neutrality. We herein demonstrate that switching the UV radiation source from conventional low-pressure UV (UV<sub>254</sub>) to far-UVC (UV<sub>222</sub>) increases the UV fluence-based concentration of hydroxyl radicals (HO<sup>•</sup>) in the UV/peracetic acid (UV/PAA) process by 4.1-fold and 27.9-fold in deionized water and real surface water, respectively. Acetyloxyl radicals (CH<sub>3</sub>C(O)O<sup>•</sup>) are generated in the UV<sub>222</sub>/PAA process at a steady-state concentration of 2.4 × 10<sup>–12</sup> M in deionized water, while they are undetectable in the UV<sub>254</sub>/PAA process under the comparable conditions. The enhancement to radical production is mainly attributed to the 15.7-fold higher molar absorption coefficients of PAA<sup>0</sup> at 222 nm than 254 nm (50 vs 3.5 M<sup>–1</sup> cm<sup>–1</sup>), which suppresses the compromised 1.1-fold lower innate quantum yield at 222 nm than 254 nm (0.78 vs 0.86 mol einstein<sup>–1</sup>). The enhanced radical generation and direct photolysis promote the fluence-based degradation rate constants of bisphenol A, phenol, and nitrobenzene by 4.1-fold, 3.3-fold, and 2.9-fold in the UV<sub>222</sub>/PAA process than the UV<sub>254</sub>/PAA process.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"11 7","pages":"759–763"},"PeriodicalIF":8.9,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141522075","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-25DOI: 10.1021/acs.estlett.4c00484
Linsey C. Marr*, Zezhen Cheng, Weinan Leng, Swarup China and Aaron J. Prussin II,
{"title":"Response to Comment on “Size-Resolved Elemental Composition of Respiratory Particles in Three Healthy Subjects”","authors":"Linsey C. Marr*, Zezhen Cheng, Weinan Leng, Swarup China and Aaron J. Prussin II, ","doi":"10.1021/acs.estlett.4c00484","DOIUrl":"10.1021/acs.estlett.4c00484","url":null,"abstract":"","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"11 7","pages":"767–769"},"PeriodicalIF":8.9,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.estlett.4c00484","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141522077","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-25DOI: 10.1021/acs.estlett.4c00243
Steven C. Hill*, and , David C. Doughty*,
{"title":"Comment on “Size-Resolved Elemental Composition of Respiratory Particles in Three Healthy Subjects”","authors":"Steven C. Hill*, and , David C. Doughty*, ","doi":"10.1021/acs.estlett.4c00243","DOIUrl":"10.1021/acs.estlett.4c00243","url":null,"abstract":"","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"11 7","pages":"765–766"},"PeriodicalIF":8.9,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141522073","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}