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Presence of Perfluorohexanoic Acid in Fluoroelastomer Watch Bands
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-18 DOI: 10.1021/acs.estlett.4c0090710.1021/acs.estlett.4c00907
Alyssa Wicks, Heather D. Whitehead and Graham F. Peaslee*, 

Many “smart” and “fitness” watch bands are advertised to contain fluoroelastomers, a type of synthetic rubber designed to be resilient against skin oils and sweat. Fluoroelastomers, which are considered a polymeric form of per- and polyfluoroalkyl substances (PFAS), have historically involved the use of shorter-chain PFAS as surfactants in the polymerization process. In this study, 22 watch bands were analyzed across numerous brands and price points for the presence of PFAS. Products were first screened for total fluorine using particle-induced gamma-ray emission spectroscopy on the surface of these bands, and 15 of the 22 watch bands contained total F concentrations >1% fluorine, suggesting the widespread use of fluoroelastomers in this product category. Watch bands then underwent solvent extraction and targeted LC-MS/MS analysis for 20 PFAS. Perfluorohexanoic acid (PFHxA) was the most frequently detected compound with concentrations from <LoD to 16662 ng/g. A subset of six watch bands also underwent direct total oxidative precursor (dTOP) assay to determine the presence of PFAS precursors. The very high concentrations of PFHxA readily extractable from the surfaces of fluoroelastomer watch bands, together with the current limited knowledge on the dermal absorption of PFHxA, demonstrate the need for more comprehensive exposure studies of PFHxA.

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引用次数: 0
Taming the Unknown: Advancing Non-Targeted Analysis through Collaborative Data Sharing and Standardized Data Repositories
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-18 DOI: 10.1021/acs.estlett.4c0103110.1021/acs.estlett.4c01031
Woo-Young Song, Seungwoo Seo and Tae-Young Kim*, 
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引用次数: 0
Ambient Measurements of Hazardous Air Pollutants in the United States Routinely Exceed Predictions from Screening-Level Exposure Models
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-17 DOI: 10.1021/acs.estlett.4c0091710.1021/acs.estlett.4c00917
Lauren E. Padilla*, Daniel R. Peters, Elizabeth J. Mohr and Ramón A. Alvarez, 

Hazardous air pollutant (HAP) emission regulations in the US often rely on modeled estimates of ambient exposures. Model accuracy compared to real-world measurements of HAPs is crucial for understanding and mitigating exposure and associated health harms. While previous work shows ambient measurements are higher than regulatory model estimates, the implications for health risk assessments are rarely discussed. We provide a comprehensive comparison of the modeled and measured concentrations at 489 US monitoring sites for 79 HAPs. We quantify how model-measurement discrepancies affect the estimation of the exposure and risk of adverse health effects. Measurements were higher than modeled concentrations in 74% of comparisons over all monitors, chemicals, and years assessed, with measurements a median 2 (IQR 1–9) times higher than model estimates. Measurements exceeded noncancer adverse health effect thresholds, while the model did not (model false negatives) for nine pollutants. Adjusting for model bias in two industrial centers, we found the number of people with multipollutant exposure above the US EPA’s acceptable excess lifetime cancer risk increased by a factor of 30 times in Houston, Texas, and 13 times in Baton Rouge, Louisiana. Our results imply that assessments relying exclusively on models like those we evaluated likely underestimate the spatial extent and magnitude of health hazards and risk.

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引用次数: 0
Multiscale Measurements of Greenhouse Gas Emissions at U.S. Natural Gas Liquefaction Terminals
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-16 DOI: 10.1021/acs.estlett.4c0071310.1021/acs.estlett.4c00713
Yuanrui Zhu, Gregory Ross, Olga Khaliukova, Selina A. Roman-White, Fiji C. George, Dorit Hammerling and Arvind P. Ravikumar*, 

Addressing methane emissions across the liquefied natural gas (LNG) supply chain is key to reducing climate impacts of LNG. Actions to address methane emissions have emphasized the importance of the use of measurement-informed emissions inventories given the systematic underestimation in official greenhouse gas (GHG) emission inventories. Despite significant progress in field measurements of GHG emissions across the natural gas supply chain, no detailed measurements at US liquefaction terminals are publicly available. In this work, we conduct multiscale, periodic measurements of methane and carbon dioxide emissions at two US LNG terminals over a 16-month campaign. We find that methane emission intensity varied from 0.007% to 0.045%, normalized to methane in LNG production. Carbon dioxide emissions accounted for over 95% of total GHG emissions using 100-year global warming potential (GWP) for methane. Thus, contrary to observations across other natural gas supply chain segments, we find that reported GHG emissions intensity closely matches measurement informed GHG emissions intensity of 0.24–0.27 kg CO2e/kg CH4. In the context of developing LNG supply chain emissions intensity, we conclude that the use of the Greenhouse Gas Reporting Program emissions intensity provides reasonably accurate estimates of total GHG emissions at LNG terminals.

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引用次数: 0
Multiscale Measurements of Greenhouse Gas Emissions at U.S. Natural Gas Liquefaction Terminals. 美国天然气液化终端温室气体排放的多尺度测量。
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-16 eCollection Date: 2025-01-14 DOI: 10.1021/acs.estlett.4c00713
Yuanrui Zhu, Gregory Ross, Olga Khaliukova, Selina A Roman-White, Fiji C George, Dorit Hammerling, Arvind P Ravikumar

Addressing methane emissions across the liquefied natural gas (LNG) supply chain is key to reducing climate impacts of LNG. Actions to address methane emissions have emphasized the importance of the use of measurement-informed emissions inventories given the systematic underestimation in official greenhouse gas (GHG) emission inventories. Despite significant progress in field measurements of GHG emissions across the natural gas supply chain, no detailed measurements at US liquefaction terminals are publicly available. In this work, we conduct multiscale, periodic measurements of methane and carbon dioxide emissions at two US LNG terminals over a 16-month campaign. We find that methane emission intensity varied from 0.007% to 0.045%, normalized to methane in LNG production. Carbon dioxide emissions accounted for over 95% of total GHG emissions using 100-year global warming potential (GWP) for methane. Thus, contrary to observations across other natural gas supply chain segments, we find that reported GHG emissions intensity closely matches measurement informed GHG emissions intensity of 0.24-0.27 kg CO2e/kg CH4. In the context of developing LNG supply chain emissions intensity, we conclude that the use of the Greenhouse Gas Reporting Program emissions intensity provides reasonably accurate estimates of total GHG emissions at LNG terminals.

解决整个液化天然气(LNG)供应链的甲烷排放问题是减少液化天然气对气候影响的关键。鉴于官方温室气体(GHG)排放清单存在系统性低估,解决甲烷排放问题的行动强调了使用基于测量的排放清单的重要性。尽管在天然气供应链的温室气体排放现场测量方面取得了重大进展,但美国液化终端的详细测量数据尚未公开。在这项工作中,我们在为期16个月的活动中对两个美国液化天然气接收站的甲烷和二氧化碳排放量进行了多尺度、定期测量。我们发现甲烷排放强度在0.007% ~ 0.045%之间变化,归一化到LNG生产中的甲烷。使用100年全球变暖潜能值(GWP)计算甲烷,二氧化碳排放量占温室气体总排放量的95%以上。因此,与其他天然气供应链环节的观察结果相反,我们发现报告的温室气体排放强度与测量结果的温室气体排放强度(0.24-0.27 kg CO2e/kg CH4)非常吻合。在开发LNG供应链排放强度的背景下,我们得出结论,使用温室气体报告计划排放强度可以合理准确地估计LNG终端的温室气体排放总量。
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引用次数: 0
Stable Isotopes Reveal the Contribution of Glacier Melting to Mercury Budget in Tibetan Rivers
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-16 DOI: 10.1021/acs.estlett.4c0100810.1021/acs.estlett.4c01008
Sheng He, Hongming Cai*, Ruoyu Sun, Wang Zheng, Shengliu Yuan, Wei Yuan, Yuchun Wang, Ke Zhang, Yuchen An, Jianfeng Liu, Pengfei Chen, Tong Zhang, Shichang Kang and Jiubin Chen*, 

Rapid retreat of glaciers accompanied by the release of mercury (Hg) in the Tibetan Plateau (TP), known as the “Asian water tower”, threatens the water security of billions of people living downstream in China and Southwest Asia. It is thus crucial to identify the sources and transformations of Hg in TP ecosystems. Here we measured Hg isotopes in water samples collected from two adjacent TP rivers, the Upper Mekong River (UMR) and the Upper Salween River (USR), to better constrain Hg geochemistry and its export under climate changes. We found similar δ202Hg and Δ200Hg variations in the two rivers, which reflect a similarly mixed contribution of atmospheric precipitation and catchment input to both rivers. However, in general, USR shows notably higher Δ199Hg than UMR. As the catchment of USR has a larger glacier-covered area than UMR, we propose that the higher Δ199Hg of USR water samples reflects a higher glacier Hg input, which is typically characterized by extremely positive Δ199Hg. Our study indicates that increasing glacier melting, vegetation greening and precipitation induced by climate changes may enhance Hg export from TP, potentially endangering the fragile Tibetan ecosystem and human health.

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引用次数: 0
Infectivity and Persistence of Influenza A Virus in Raw Milk
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-12 DOI: 10.1021/acs.estlett.4c0097110.1021/acs.estlett.4c00971
Alessandro Zulli, Mengyang Zhang, Sehee Jong, Catherine Blish and Alexandria B. Boehm*, 

Influenza A viruses present important public health risks, with recent outbreaks of highly pathogenic avian influenza (HPAI) H5N1 in dairy cattle raising concerns about potential transmission through raw milk consumption. This study investigated the persistence of influenza A virus H1N1 PR8 (IAV PR8) in raw cow milk at 4 °C. We found a first-order decay rate constant of −2.05 day–1 equivalent to a T99 of 2.3 days. Viral RNA remained detectable for at least 57 days with no degradation. Pasteurization (63 °C for 30 min) reduced infectious virus to undetectable levels and reduced viral RNA concentrations, but reduction was less than 1 log10. These findings highlight the potential risk of zoonotic virus transmission through raw milk consumption and underscore the importance of milk pasteurization. The prolonged persistence of viral RNA in both raw and pasteurized milk has implications for food safety assessments and environmental monitoring, particularly in the context of the environmental surveillance of influenza viruses.

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引用次数: 0
Qualitative and Quantitative Analysis of Tire Wear Particles (TWPs) in Road Dust Using a Novel Mode of Operation of TGA-GC/MS. 基于TGA-GC/MS的道路粉尘中轮胎磨损颗粒的定性和定量分析
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-12 eCollection Date: 2025-01-14 DOI: 10.1021/acs.estlett.4c00937
Kieran S Evans, Daniel Baqer, Marc-Krystelle Mafina, Maya Al-Sid-Cheikh

Detecting and quantifying tire wear particles (TWPs) in the environment pose a unique environmental challenge due to their chemical complexity. There are emerging concerns around TWPs due to their potential high numbers of particles released, outnumbering microplastics, as well as the leaching of toxic additives such as 6-PPD which has been linked to the death of salmon even when present at very low levels (<0.1 μg/L). Analytical techniques such as pyrolysis gas chromatography mass spectrometry (Py-GC/MS) and thermal extraction-desorption gas chromatography mass spectrometry (TED-GC/MS) have been used but also demonstrate limitations including low sample mass, low sample throughput, and complex characterization and quantification procedures. This work aims to overcome these challenges by developing a new approach which utilizes a coupling between thermogravimetric analysis (TGA) and gas chromatography-mass spectrometry (GC/MS). This work is the first to harness conventional TGA-GC/MS for the analysis of tire rubber, with the detection of additives such as 6-PPD, while also pioneering a novel mode of operation, PyroTGA-GC/MS, using fast heating to enable robust quantitative analysis of TWPs in road dust. The limits of detection and quantification of 0.08/0.16 μg and 0.20/0.40 μg for SBR and PI, respectively, are lower than those achieved using Py-GC/MS and TED-GC/MS for SBR and align with those achieved for PI. This study reveals a clear link between the ratio of PI to SBR and the proportion of heavy goods vehicles. This work solves key issues in tire particle analysis related to sample size and throughput. By overcoming these limitations, we introduce a technique that provides an economically viable solution for large-scale commercial analysis of tire rubber and particles.

由于其化学成分的复杂性,对环境中轮胎磨损颗粒(twp)的检测和量化构成了一项独特的环境挑战。由于twp可能释放出大量的颗粒,数量超过微塑料,以及6-PPD等有毒添加剂的浸出,人们对twp越来越关注,6-PPD即使含量很低,也与鲑鱼的死亡有关(
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引用次数: 0
Qualitative and Quantitative Analysis of Tire Wear Particles (TWPs) in Road Dust Using a Novel Mode of Operation of TGA-GC/MS
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-11 DOI: 10.1021/acs.estlett.4c0093710.1021/acs.estlett.4c00937
Kieran S. Evans, Daniel Baqer, Marc-Krystelle Mafina and Maya Al-Sid-Cheikh*, 

Detecting and quantifying tire wear particles (TWPs) in the environment pose a unique environmental challenge due to their chemical complexity. There are emerging concerns around TWPs due to their potential high numbers of particles released, outnumbering microplastics, as well as the leaching of toxic additives such as 6-PPD which has been linked to the death of salmon even when present at very low levels (<0.1 μg/L). Analytical techniques such as pyrolysis gas chromatography mass spectrometry (Py-GC/MS) and thermal extraction-desorption gas chromatography mass spectrometry (TED-GC/MS) have been used but also demonstrate limitations including low sample mass, low sample throughput, and complex characterization and quantification procedures. This work aims to overcome these challenges by developing a new approach which utilizes a coupling between thermogravimetric analysis (TGA) and gas chromatography–mass spectrometry (GC/MS). This work is the first to harness conventional TGA-GC/MS for the analysis of tire rubber, with the detection of additives such as 6-PPD, while also pioneering a novel mode of operation, PyroTGA-GC/MS, using fast heating to enable robust quantitative analysis of TWPs in road dust. The limits of detection and quantification of 0.08/0.16 μg and 0.20/0.40 μg for SBR and PI, respectively, are lower than those achieved using Py-GC/MS and TED-GC/MS for SBR and align with those achieved for PI. This study reveals a clear link between the ratio of PI to SBR and the proportion of heavy goods vehicles. This work solves key issues in tire particle analysis related to sample size and throughput. By overcoming these limitations, we introduce a technique that provides an economically viable solution for large-scale commercial analysis of tire rubber and particles.

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引用次数: 0
More Frequent Runoff and Connected Sources in Headwaters Promote Browning of Northern Freshwaters
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-11 DOI: 10.1021/acs.estlett.4c0093910.1021/acs.estlett.4c00939
Stefano Basso*, Andreas Musolff and Heleen A. de Wit, 

Sustained browning of northern waters has prompted inquiries into the drivers of increasing concentrations of organic matter. While reduced sulfur deposition is a key cause, an increasing role of hydrologic mechanisms as a result of cleaner air and progressing climate change has been repeatedly suggested. How these controls act remains however unclear. Here we examine over 30 years of organic carbon concentration and discharge data from four reference streams located across Norway to pinpoint consistent hydrologic changes that may promote water browning. Stable slopes with changing intercepts of the concentration-discharge relations indicate that the influence of air pollution on soil solution chemistry is plausible, supporting available chemical explanations from a hydrologic perspective. Decreasing ratios of concentration to discharge variability, observed in autumn over the years, point to less spatial heterogeneity of the sources of organic carbon. A clear rise in the frequency of runoff events, which increases the opportunities for dissolved organic carbon to transit from soil to streams, also indicates higher hydrologic connectivity and more even mobilization of carbon sources. More connected sources and more frequent runoff events, which jointly enhance the likelihood of organic carbon reaching rivers, may thus contribute to the observed browning of northern waters.

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引用次数: 0
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Environmental Science & Technology Letters Environ.
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