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Environmental drivers of monomethylmercury photodegradation along the land-to-ocean aquatic continuum† 陆地-海洋水生连续体中单甲基汞光降解的环境驱动因素。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-09 DOI: 10.1039/D4EM00636D
Sonja Gindorf, Johannes West, Andrew Graham and Sofi Jonsson

In surface waters, photodegradation is a major abiotic removal pathway of the neurotoxin monomethylmercury (MMHg), acting as a key control on the amounts of MMHg available for biological uptake. Different environmental factors can alter the rate of MMHg photodegradation. However, our understanding of how MMHg photodegradation pathways in complex matrixes along the land-to-ocean aquatic continuum respond to changes in salinity, dissolved organic carbon (DOC) concentration and dissolved organic matter (DOM) composition is incomplete. In a set of laboratory experiments combining several artificial and natural waters, we demonstrate that the interplay of DOC concentration, DOM composition, and salinity affects the photodegradation rate of MMHg. The presence of DOM was found to facilitate MMHg photodegradation, but degradation rates were not altered by varying DOC concentrations over two orders of magnitude. We found DOM composition to have a stronger effect on MMHg photodegradation rates than DOC concentration. However, at high DOC levels, where most UV radiation was lost within the first cm of the reaction vessels, lower MMHg photodegradation rates were observed. When moving from terrestrially influenced waters, characterized by a high degree of humification, towards marine conditions with a protein-rich DOM pool, MMHg photodegradation rates increased. In contrast, salinity had a stabilizing effect on MMHg. Hence, especially in systems with low salt and DOC concentrations, changes in either salinity or DOC concentration can impact the photodegradation rates of MMHg.

在地表水中,光降解是神经毒素单甲基汞(MMHg)的主要非生物去除途径,是生物吸收MMHg量的关键控制因素。不同的环境因素会改变MMHg的光降解速率。然而,我们对沿陆地-海洋水生连续体的复杂基质中MMHg光降解途径如何响应盐度、溶解有机碳(DOC)浓度和溶解有机物质(DOM)组成的变化的了解尚不完整。在一组室内实验中,我们结合了几个人工和自然水域,证明了DOC浓度、DOM组成和盐度的相互作用影响MMHg的光降解速率。DOM的存在促进了MMHg的光降解,但降解速率不会因DOC浓度超过两个数量级的变化而改变。我们发现DOM组成比DOC浓度对MMHg光降解率的影响更大。然而,在高DOC水平下,大部分紫外线辐射在反应血管的第一厘米内消失,观察到较低的MMHg光降解率。当从以高度腐殖化为特征的受陆地影响的水域向富含蛋白质的DOM池的海洋环境移动时,MMHg的光降解率增加。相比之下,盐度对MMHg有稳定作用。因此,特别是在低盐和DOC浓度的系统中,盐度或DOC浓度的变化都会影响MMHg的光降解速率。
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引用次数: 0
Accounting for in situ air cleaner utilization and performance to improve interpretation of patient outcomes in real-world indoor air cleaner intervention trials. 考虑现场空气净化器的使用和性能,以改善对现实世界室内空气净化器干预试验中患者结果的解释。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-09 DOI: 10.1039/d4em00648h
Saeed Farhoodi, Insung Kang, Yicheng Zeng, Kaveeta Jagota, Nancy Karpen, Mohammad Heidarinejad, Zane Elfessi, Israel Rubinstein, Brent Stephens

There is an increasing number of randomized clinical trials intended to assess the effectiveness of indoor air cleaners for improving participant outcomes in real-world settings. In this communication, we synthesize the current state of registered air cleaner intervention trials and call attention to the critical importance of conducting measurements to characterize the performance and in situ utilization of air cleaners in such trials to improve interpretation of exposure measurements and patient outcomes. We draw upon the existing literature and preliminary findings from our ongoing one-year, randomized, single-blind, placebo-controlled case-control trial of stand-alone air filtration in the homes of U.S. military Veterans to inform our recommendations. We demonstrate how to conduct industry-standard performance testing and how to use long-term measurements of air cleaner power draw to assess air cleaner operation. In our analysis of interim data from 53 homes to date with a mean data collection period of 275 days, we found that most air cleaners, whether active or sham, were operated predominantly at low or medium fan speeds, and most participants operated their air cleaner on predominantly one fan speed. In a few homes, air cleaners were mostly off. We estimate that air cleaner operation in these homes is providing a median additional equivalent particle loss rate of ∼0.7/h (ranging ∼0-2.8/h). Accordingly, we recommend that air cleaner intervention trials adopt the steps described herein to account for the amount of clean air delivered in real-world settings and to provide important context alongside indoor exposure measurements and analysis of patient outcomes.

有越来越多的随机临床试验旨在评估室内空气净化器对改善现实环境中参与者结果的有效性。在本文中,我们综合了已注册的空气净化器干预试验的现状,并呼吁人们注意在这些试验中进行测量以表征空气净化器的性能和原位利用的重要性,以改进对暴露测量和患者结果的解释。我们利用现有文献和我们正在进行的为期一年的、随机、单盲、安慰剂对照的病例对照试验的初步发现,在美国退伍军人家中进行独立空气过滤,以告知我们的建议。我们演示了如何进行行业标准性能测试,以及如何使用空气净化器功耗的长期测量来评估空气净化器的运行情况。在我们对迄今为止来自53个家庭的中期数据(平均数据收集期为275天)的分析中,我们发现大多数空气净化器,无论是活跃的还是假的,都主要在低或中等风扇速度下运行,并且大多数参与者主要在一个风扇速度下运行他们的空气净化器。在一些家庭中,空气净化器基本上是关闭的。我们估计,在这些家庭中,空气净化器的运行提供的额外等效颗粒损失率中位数为0.7/h(范围为~ 0-2.8/h)。因此,我们建议空气净化器干预试验采用本文所述的步骤,以解释在现实环境中输送的清洁空气量,并提供重要的背景,以及室内暴露测量和患者结果分析。
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引用次数: 0
Association of volatile organic compound metabolites with hearing loss: unveiling their potential mechanism and intervention target† 挥发性有机化合物代谢物与听力损失的关系:揭示其潜在机制和干预目标。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-08 DOI: 10.1039/D4EM00644E
Jingcheng Zhou, Guanchao Sun, Houming Zhao, Handai Qin, Yiming Bi and Xuemin Chen

Hearing loss (HL) is an otolaryngology disease susceptible to environmental pollutants. Volatile organic compounds (VOCs), as a class of chemical pollutants with evaporation propensity, pose a great threat to human health. However, the association between VOCs and HL remains unclear. This study aimed to explore the association between urinary-specific VOC metabolites and HL. It included 1048 participants from the National Health and Nutrition Examination Survey (NHANES) from 2011 to 2012. Multivariate linear regression models, smooth curve analysis, and stratified analysis were employed to investigate the relationship between urinary-specific VOC metabolite concentrations and pure tone audiometry (PTA) across three different frequencies. A two-piecewise linear regression model was employed to analyze the threshold effects of urinary-specific VOC metabolites on hearing threshold changes. Furthermore, a comparative toxicogenomics database (CTD) and functional gene enrichment were constructed. An interaction network of transcription factors, genes, and non-coding RNA was constructed to further confirm the upstream and downstream regulatory relationships. Molecular docking analyses were conducted to explore the potential binding modes and critical docking sites. Additionally, a moderation analysis was conducted to investigate the role of oxidative stress in moderating the influence of VOC metabolites on hearing. Multivariate linear regression model discerned a significant correlation between cyanide 2-aminothiazoline-4-carboxylic acid (ATCA) with speech-frequency PTA and N-acetyl-S-(3,4-dihydroxybutyl)-L-cysteine (DHBMA) with high-frequency PTA. The smoothed curve and threshold effect analysis corroborated a positive linear relationship between cyanide ATCA and speech-frequency PTA without a threshold effect only in the 20–34 age group. Additionally, the bioinformatics analysis discovered pathogenic genes related to cyanide-induced HL and suggested that oxidative stress responses play a critical role in this biological process. Furthermore, the moderation effect of total bilirubin (TB), an oxidative stress-associated molecule, was ascertained on the effects of ATCA on hearing. Our findings suggest a potential link between VOC metabolites and hearing and indicate the crucial role of oxidative stress responses in this association.

听力损失是一种易受环境污染物影响的耳鼻喉科疾病。挥发性有机化合物(VOCs)作为一类具有蒸发倾向的化学污染物,对人类健康构成了巨大威胁。然而,挥发性有机化合物与HL之间的关系尚不清楚。本研究旨在探讨尿特异性VOC代谢物与HL之间的关系。该研究包括2011年至2012年全国健康与营养检查调查(NHANES)的1048名参与者。采用多元线性回归模型、平滑曲线分析和分层分析等方法,探讨了三种不同频率下尿液特异性VOC代谢物浓度与纯音听力学(PTA)的关系。采用双分段线性回归模型分析尿特异性VOC代谢物对听阈变化的阈值效应。此外,构建了比较毒理学基因组数据库(CTD)和功能基因富集。构建了转录因子、基因和非编码RNA的相互作用网络,进一步确认了上下游调控关系。通过分子对接分析,探索潜在的结合模式和关键对接位点。此外,我们还进行了调节分析,以探讨氧化应激在调节VOC代谢物对听力的影响中的作用。多元线性回归模型发现,氰化物2-氨基噻唑-4-羧酸(ATCA)与语音频率PTA、n -乙酰- s -(3,4-二羟基丁基)- l-半胱氨酸(DHBMA)与高频PTA存在显著相关性。平滑曲线和阈值效应分析证实,氰化物ATCA与语音频率PTA呈正线性关系,仅在20-34岁年龄组无阈值效应。此外,生物信息学分析发现了氰化物诱导HL的相关致病基因,提示氧化应激反应在这一生物学过程中起关键作用。此外,还确定了氧化应激相关分子总胆红素(TB)对ATCA对听力的影响的调节作用。我们的研究结果表明VOC代谢物与听力之间存在潜在的联系,并表明氧化应激反应在这种联系中起着至关重要的作用。
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引用次数: 0
A review on environmental contamination of petroleum hydrocarbons, its effects and remediation approaches
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-03 DOI: 10.1039/D4EM00548A
Bzhwen Khalid Majeed, Dler M.S Shwan and Khasraw Abdullah Rashid

Oil leakage into soil is a major environmental concern, affecting its physical, chemical, biological, and geotechnical properties, which threatens soil fertility. Remediating contaminated sites helps mitigate risks to human health, the environment, and the economy, while also enabling land reuse for development or agriculture. Petroleum spills generally occur during production, processing, transportation, and storage. This review discusses the impact of hydrocarbon contamination on soil and its surrounding environment and examines various remediation techniques, including physical–chemical methods (soil excavation, soil washing, soil vapor extraction, thermal treatment, and chemical oxidation), biological methods (bioremediation and phytoremediation), nanotechnology-based approaches, and integrated methods. The effectiveness, limitations, and applicability of these techniques are critically analyzed, providing a comprehensive framework for managing soil contamination by petroleum hydrocarbons.

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引用次数: 0
Seasonal effect of PM2.5 exposure in patients with COPD: a multicentre panel study. PM2.5暴露对COPD患者的季节性影响:一项多中心小组研究
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-02 DOI: 10.1039/d4em00376d
Jin-Young Huh, Hajeong Kim, Shinhee Park, Seung Won Ra, Sung-Yoon Kang, Bock Hyun Jung, Mihye Kim, Sang Min Lee, Sang Pyo Lee, Dirga Kumar Lamichhane, Young-Jun Park, Seon-Jin Lee, Jae Seung Lee, Yeon-Mok Oh, Hwan-Cheol Kim, Sei Won Lee

Background: Exposure to particulate matter <2.5 μm (PM2.5) is linked to chronic obstructive pulmonary disease (COPD), but most studies lack individual PM2.5 measurements. Seasonal variation and their impact on clinical outcomes remain understudied. Objective: This study investigated the impact of PM2.5 concentrations on COPD-related clinical outcomes and their seasonal changes. Methods: A multicentre panel study enrolled 105 COPD patients (age range: 46-82) from July 2019 to August 2020. Their mean forced expiratory volume in 1 second after bronchodilation was 53.9%. Individual PM2.5 levels were monitored continuously with indoor measurements at residences and outdoor data from the National Ambient Air Quality Monitoring Information System. Clinical parameters, including pulmonary function tests, symptom questionnaires (CAT and SGRQ-C), and impulse oscillometry (IOS), were assessed every three months over the course of one year. Statistical analysis was conducted using a linear mixed-effect model to account for repeated measurements and control for confounding variables, including age, sex, smoking status and socioeconomic status. Results: The mean indoor and outdoor PM2.5 concentrations were 16.2 ± 8.4 μg m-3 and 17.2 ± 5.0 μg m-3, respectively. Winter had the highest PM2.5 concentrations (indoor, 18.8 ± 11.7 μg m3; outdoor, 22.5 ± 5.0 μg m-3). Higher PM2.5 concentrations significantly correlated with poorer St. George's Respiratory Questionnaire for COPD (SGRQ-C) scores and increased acute exacerbations, particularly in winter. Patients of lower socioeconomic status were more vulnerable. Increased PM2.5 concentrations were also associated with amplified small airway resistance (R5-R20). Conclusions: PM2.5 concentration changes are positively correlated with poorer SGRQ-C scores and increased acute exacerbations in COPD patients with significant seasonal variations, especially in winter.

背景:暴露于颗粒物质2.5与慢性阻塞性肺疾病(COPD)有关,但大多数研究缺乏个体PM2.5测量。季节变化及其对临床结果的影响仍未得到充分研究。目的:研究PM2.5浓度对copd相关临床结局的影响及其季节变化。方法:2019年7月至2020年8月,一项多中心小组研究纳入了105名COPD患者(年龄范围:46-82岁)。支气管扩张后1秒平均用力呼气量为53.9%。通过住宅室内测量和国家环境空气质量监测信息系统的室外数据,连续监测个人PM2.5水平。临床参数,包括肺功能测试、症状问卷(CAT和SGRQ-C)和脉冲振荡测量(IOS),在一年的过程中每三个月评估一次。采用线性混合效应模型进行统计分析,以解释重复测量和控制混杂变量,包括年龄、性别、吸烟状况和社会经济状况。结果:室内和室外PM2.5平均浓度分别为16.2±8.4 μg m-3和17.2±5.0 μg m-3。冬季PM2.5浓度最高(室内为18.8±11.7 μg m3;室外22.5±5.0 μg m-3)。较高的PM2.5浓度与较差的圣乔治慢性阻塞性肺病呼吸问卷(SGRQ-C)评分和急性加重程度增加显著相关,尤其是在冬季。社会经济地位较低的患者更容易受到伤害。PM2.5浓度升高也与小气道阻力增大相关(R5-R20)。结论:PM2.5浓度变化与COPD患者SGRQ-C评分较差、急性加重程度增加呈正相关,且季节变化明显,尤其是冬季。
{"title":"Seasonal effect of PM<sub>2.5</sub> exposure in patients with COPD: a multicentre panel study.","authors":"Jin-Young Huh, Hajeong Kim, Shinhee Park, Seung Won Ra, Sung-Yoon Kang, Bock Hyun Jung, Mihye Kim, Sang Min Lee, Sang Pyo Lee, Dirga Kumar Lamichhane, Young-Jun Park, Seon-Jin Lee, Jae Seung Lee, Yeon-Mok Oh, Hwan-Cheol Kim, Sei Won Lee","doi":"10.1039/d4em00376d","DOIUrl":"https://doi.org/10.1039/d4em00376d","url":null,"abstract":"<p><p><i>Background</i>: Exposure to particulate matter <2.5 μm (PM<sub>2.5</sub>) is linked to chronic obstructive pulmonary disease (COPD), but most studies lack individual PM<sub>2.5</sub> measurements. Seasonal variation and their impact on clinical outcomes remain understudied. <i>Objective</i>: This study investigated the impact of PM<sub>2.5</sub> concentrations on COPD-related clinical outcomes and their seasonal changes. <i>Methods</i>: A multicentre panel study enrolled 105 COPD patients (age range: 46-82) from July 2019 to August 2020. Their mean forced expiratory volume in 1 second after bronchodilation was 53.9%. Individual PM<sub>2.5</sub> levels were monitored continuously with indoor measurements at residences and outdoor data from the National Ambient Air Quality Monitoring Information System. Clinical parameters, including pulmonary function tests, symptom questionnaires (CAT and SGRQ-C), and impulse oscillometry (IOS), were assessed every three months over the course of one year. Statistical analysis was conducted using a linear mixed-effect model to account for repeated measurements and control for confounding variables, including age, sex, smoking status and socioeconomic status. <i>Results</i>: The mean indoor and outdoor PM<sub>2.5</sub> concentrations were 16.2 ± 8.4 μg m<sup>-3</sup> and 17.2 ± 5.0 μg m<sup>-3</sup>, respectively. Winter had the highest PM<sub>2.5</sub> concentrations (indoor, 18.8 ± 11.7 μg m<sup>3</sup>; outdoor, 22.5 ± 5.0 μg m<sup>-3</sup>). Higher PM<sub>2.5</sub> concentrations significantly correlated with poorer St. George's Respiratory Questionnaire for COPD (SGRQ-C) scores and increased acute exacerbations, particularly in winter. Patients of lower socioeconomic status were more vulnerable. Increased PM<sub>2.5</sub> concentrations were also associated with amplified small airway resistance (<i>R</i>5-<i>R</i>20). <i>Conclusions</i>: PM<sub>2.5</sub> concentration changes are positively correlated with poorer SGRQ-C scores and increased acute exacerbations in COPD patients with significant seasonal variations, especially in winter.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" ","pages":""},"PeriodicalIF":4.3,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142913256","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}
引用次数: 0
Photodegradation of typical psychotropic drugs in the aquatic environment: a critical review
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-02 DOI: 10.1039/D4EM00669K
Chuanguang Wang, Ruonan Guo, Changsheng Guo, Hailong Yin and Jian Xu

Continuous consumption combined with incomplete removal during wastewater treatment means residues of psychotropic drugs (PDs), including antidepressants, antipsychotics, antiepileptics and illicit drugs, are continuously entering the aquatic environment, where they have the potential to affect non-target organisms. Photochemical transformation is an important aspect to consider when evaluating the environmental persistence of PDs, particularly for those present in sunlit surface waters. This review summarizes the latest research on the photodegradation of typical PDs under environmentally relevant conditions. According to the analysis results, four classes of PDs discussed in this paper are influenced by direct and indirect photolysis. Indirect photodegradation has been more extensively studied for antidepressants and antiepileptics compared to antipsychotics and illicit drugs. Particularly, the photosensitization process of dissolved organic materials (DOM) in natural waters has received significant research attention due to its ubiquity and specificity. The direct photolysis pathway plays a less significant role, but it is still relevant for most PDs discussed in this paper. The photodegradation rates and pathways of PDs are influenced by various water constituents and parameters such as DOM, nitrate and pH value. The contradictory results reported in some studies can be attributed to differences in experimental conditions. Based on this analysis of the existing literature, the review also identifies several key aspects that warrant further research on PD photodegradation. These results and recommendations contribute to a better understanding of the environmental role of water matrixes and provide important new insights into the photochemical fate of PDs in aquatic environments.

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引用次数: 0
Environmental impact of an acid-forming alum shale waste rock legacy site in Norway† 挪威产酸明矾页岩废石遗址的环境影响。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-02 DOI: 10.1039/D4EM00298A
Mila K. Pelkonen, Estela Reinoso-Maset, Gareth T. W. Law, Ole Christian Lind and Lindis Skipperud

Alum shale formations in Scandinavia are generally enriched in uranium (U) and, when exposed to air and water, may produce acidic rock drainage (ARD), releasing potentially harmful elements into the environment. Taraldrud is a legacy site in southeast Norway where approx. 51 000 m3 of alum shale was deposited in the 1980s–1990s. In 2006, ARD formation became obvious after high concentrations of leachable elements and low environmental pH were measured in a nearby stream. A manmade precipitation pond and liming treatments attempt to address the environmental pollution, but the site remains non-remediated. This study aimed to evaluate the extent of contamination caused by ARD and examine environmental and human health risks caused by mobilized trace elements and radionuclides. Surface water, sediment, soil, and biota samples were collected in the area and chemically and/or radiochemically analyzed to assess the prevailing concentrations within different environmental compartments. The elemental distribution and variation patterns were studied using principal component analysis. Most of the leachable elements were present in highly mobile and bioavailable forms in the pond water, out of which Cd, Mn, Ni, and U exceeded drinking water regulations. The highest enrichment in soil and sediment was for U, which was associated with the sulfide-bearing soil fraction, Fe, Cu, Mo, and As. No changes in water quality were observed between up- and downstream from the site, indicating that the Fe and S rich phases in the pond retain the leachable elements effectively under prevailing environmental conditions. This study provides valuable insights into the risks and challenges associated with ARD and where U is the main pollutant of concern.

斯堪的纳维亚的明矾页岩通常富含铀(U),当暴露于空气和水中时,可能产生酸性岩石排水(ARD),将潜在的有害元素释放到环境中。塔拉德鲁德是挪威东南部的一个遗产遗址,大约有200万人口。20世纪80年代至90年代沉积了5.1万立方米的明矾页岩。2006年,在附近的一条溪流中测量了高浓度的可浸出元素和低环境pH后,ARD的形成变得明显。一个人工沉淀池和石灰处理试图解决环境污染,但该场地仍未得到修复。本研究旨在评价放射性放射性污染物的污染程度,探讨其对环境和人体健康的危害。在该地区收集了地表水、沉积物、土壤和生物群样本,并进行了化学和/或放射化学分析,以评估不同环境隔间内的主要浓度。采用主成分分析方法研究了元素分布和变化规律。池水中可浸出元素大部分以高流动性和生物可利用性形式存在,其中Cd、Mn、Ni和U超过饮用水标准。U在土壤和沉积物中富集程度最高,与含硫化物的土壤组分、Fe、Cu、Mo和As有关。上游和下游的水质没有变化,这表明在当时的环境条件下,池塘中的富铁和富S相有效地保留了可浸出元素。这项研究为与ARD相关的风险和挑战以及U是主要污染物的地方提供了有价值的见解。
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引用次数: 0
Chemical characterization of polymer and chloride content in waste plastic materials using pyrolysis – direct analysis in real time – high-resolution mass spectrometry† 利用热解-实时直接分析-高分辨率质谱法对废塑料材料中聚合物和氯化物含量进行化学表征。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-12-30 DOI: 10.1039/D4EM00501E
Emily Halpern, Lauren Heirty, Christopher West, Yitao Li, Won M. Kim, Anthony S. Mennito and Alexander Laskin

The increasing global demand for plastic has raised the need for effective waste plastic management due to its long lifetime and resistance to environmental degradation. There is a need for rapid plastic identification to improve the mechanical waste plastic sorting process. This study presents a novel application of Temperature-Programmed Desorption-Direct Analysis in Real Time-High Resolution Mass Spectrometry (TPD-DART-HRMS) that enables rapid characterization of various plastics. This technique was applied on four commercially available reference polymers (polyethylene, polypropylene, polystyrene, polyvinyl chloride) as well as three “waste” plastic samples of mixed origin. These waste plastic samples were obtained as discards from various industrial processes with limited analytical characterization data. Through the application of CH2 Kendrick mass defect (KMD) grouping, characteristic trends in the mass spectra of each sample were identified, allowing for a simplified numerical comparison. This approach utilized a robust statistical approach using the Tanimoto coefficient, allowing for the quantitative measures of similarity between standards and unknown samples. The application of this mathematical evaluation methodology was used to identify plastic types and to distinguish structurally similar polymers. Additionally, we report that a chloride ion clustering effect with copper substrate can identify chlorinated polymer PVC (polyvinyl chloride) utilizing pyro-(−)DART-HRMS mode. PVC polymer is of particular interest in recycling due to its high chloride content, which can present technical challenges for some types of recycling. We found that chloride ion clusters are a good screening marker for the presence of chlorinated polymers in mixed waste plastic samples. This study can possibly help advance rapid and accurate analytical techniques for identifying the composition of waste plastics to advance the effectiveness of the waste plastic sorting process.

由于塑料的使用寿命长,耐环境退化,全球对塑料的需求不断增加,因此需要对废塑料进行有效的管理。需要快速识别塑料,以改进机械废塑料分类过程。本研究提出了一种新的应用程序的温度编程解吸直接分析实时高分辨率质谱(TPD-DART-HRMS),使各种塑料的快速表征。该技术应用于四种市售参考聚合物(聚乙烯、聚丙烯、聚苯乙烯、聚氯乙烯)以及三种混合来源的“废”塑料样品。这些废塑料样品是从各种工业过程中获得的,分析表征数据有限。通过应用CH2 Kendrick质量缺陷(KMD)分组,确定了每个样品的质谱特征趋势,从而简化了数值比较。这种方法利用了一种稳健的统计方法,使用谷本系数,允许对标准和未知样本之间的相似性进行定量测量。该数学评价方法的应用被用于识别塑料类型和区分结构相似的聚合物。此外,我们报告了氯离子与铜衬底的聚类效应可以利用pyro-(-)DART-HRMS模式识别氯化聚合物PVC(聚氯乙烯)。PVC聚合物由于其氯化物含量高,因此对回收特别感兴趣,这可能对某些类型的回收提出技术挑战。我们发现氯离子簇是一个很好的筛选标记氯代聚合物的存在在混合废塑料样品。这项研究可能有助于推进快速准确的分析技术来识别废塑料的成分,从而提高废塑料分类过程的有效性。
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引用次数: 0
A mechanistic model for determining factors that influence inorganic nitrogen fate in corn cultivation† 玉米栽培中影响无机氮命运因素的机制模型。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-12-26 DOI: 10.1039/D4EM00566J
Patrick J. Dunn and Leanne M. Gilbertson

Conventional practices for inorganic nitrogen fertilizer are highly inefficient leading to excess nitrogen in the environment. Excess environmental nitrogen induces ecological (e.g., hypoxia, eutrophication) and public health (e.g., nitrate contaminated drinking water) consequences, motivating adoption of management strategies to improve fertilizer use efficiency. Yet, how to limit the environmental impacts from inorganic nitrogen fertilizer while maintaining crop yields is a persistent challenge. The lack of empirical data on the fate and transport of nitrogen in an agriculture soil-crop system and how transport changes under varying conditions limits our ability to address this challenge. To this end, we developed a mechanistic model to assess how various parameters within a soil-crop system affect where nitrogen goes and inform how we can perturb the system to improve crop nitrogen content while reducing nitrogen emissions to the environment. The model evaluates nitrogen transport and distribution in the soil-corn plant system on a conventional Iowa corn farm. Simulations determine the amount of applied nitrogen fertilizer acquired by the crop root system, leached to groundwater, lost to tile drainage, and denitrified. Through scenario modeling, it was found that reducing application rates from 200 kg ha−1 to 160 kg ha−1 had limited impact on plant nitrogen content, while decreasing wasted nitrogen fertilizer by 25%. Delayed application until June significantly increased the f-NUE and denitrification while reducing the amount of fertilizer leached and exported through tile drainage. The value in a model like the one presented herein, is the ability to perturb the system through manipulation of variables representative of a specific scenario of interest to inform how one can improve crop-based nitrogen management.

无机氮肥的传统做法效率极低,导致环境中氮过量。过量的环境氮引起生态(如缺氧、富营养化)和公共卫生(如硝酸盐污染的饮用水)后果,促使采取管理战略以提高肥料利用效率。然而,如何在保持作物产量的同时限制无机氮肥对环境的影响是一个持久的挑战。缺乏农业土壤-作物系统中氮的命运和运输以及运输在不同条件下如何变化的经验数据限制了我们应对这一挑战的能力。为此,我们开发了一个机制模型来评估土壤-作物系统中的各种参数如何影响氮的去向,并告知我们如何干扰该系统以提高作物氮含量,同时减少对环境的氮排放。该模型评估了爱荷华州传统玉米农场土壤-玉米植株系统中氮的运输和分布。模拟确定了作物根系获得的氮肥用量,这些氮肥会渗入地下水,流失到排水系统中,并被反硝化。通过情景模拟发现,将施用量从200 kg ha-1降低到160 kg ha-1对植株氮含量影响有限,但氮肥浪费减少25%。推迟到6月施用显著提高了氮肥利用效率和反硝化作用,同时减少了肥料的沥滤和通过排水出口的数量。像本文所介绍的模型的价值在于,能够通过操纵代表感兴趣的特定场景的变量来干扰系统,从而告知如何改进基于作物的氮管理。
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引用次数: 0
Mitigating matrix effects in oil and gas wastewater analysis: LC-MS/MS method for ethanolamines† 缓解基质在油气废水分析中的影响:乙醇胺的LC-MS/MS方法。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-12-26 DOI: 10.1039/D4EM00716F
Glen Andrew D. de Vera, Loredana Caldiero, Giovanni Conte and Desirée L. Plata

The high salinity and organic content in oil and gas wastewaters can cause ion suppression during liquid chromatography mass spectrometry (LC/MS) analysis, diminishing the sensitivity and accuracy of measurements in available methods. This suppression is severe for low molecular weight organic compounds such as ethanolamines (e.g., monoethanolamine (MEA), diethanolamine (DEA), triethanolamine (TEA), N-methyldiethanolamine (MDEA), and N,N-ethyldiethanolamine (EDEA)). Here, we deployed solid phase extraction (SPE), mixed-mode LC, triple quadrupole MS with positive electrospray ionization (ESI), and a suite of stable isotope standards (i.e., one per target compound) to correct for ion suppression by salts and organic matter, SPE losses, and instrument variability. The method was evaluated in produced water samples from Italy (NaCl salinity from 8110–18 100 mg L−1; diesel range organic compounds ranging from 5.1–7.9 mg L−1). After correcting for matrix effects, ethanolamines in produced water samples were quantified. The first batch of samples (March 2019) had 37–646 μg L−1 total ethanolamines. The second batch of samples (September 2019) had greater ethanolamine content of 77–3976 μg L−1 which was attributed to a reduced water cut during oil production, enhancing the proportionate abundance of these compounds in the aqueous phase. In all samples, DEA and MEA were the dominant ethanolamine species. Possible sources (e.g., corrosion inhibitor and biotransformation) and natural attenuation potential during storage (e.g., at different temperatures, acidification, and addition of sodium azide) were investigated. The developed analytical method enables further investigation of the fate of low molecular weight organic additives in oil and gas development and provides an enhanced ability to evaluate risks associated with chemical release to the environment.

油气废水中的高盐度和高有机含量会在液相色谱-质谱(LC/MS)分析过程中导致离子抑制,从而降低现有方法测量的灵敏度和准确性。这种抑制对于低分子量有机化合物如乙醇胺(例如,单乙醇胺(MEA),二乙醇胺(DEA),三乙醇胺(TEA), N-甲基二乙醇胺(MDEA)和N,N-乙基二乙醇胺(EDEA))是严重的。在这里,我们部署了固相萃取(SPE)、混合模式LC、三重四极杆质谱与正电喷雾电离(ESI),以及一套稳定同位素标准(即每个目标化合物一个)来纠正盐和有机物的离子抑制、SPE损失和仪器可变性。对意大利采出水样进行了评价(NaCl盐度为8110 ~ 18 100 mg L-1;柴油的有机化合物含量在5.1-7.9 mg L-1之间。校正基质效应后,对采出水样中的乙醇胺进行定量。第一批样品(2019年3月)总乙醇胺含量为37 ~ 646 μg。第二批样品(2019年9月)的乙醇胺含量更高,为77-3976 μ L-1,这是由于采油过程中含水减少,提高了这些化合物在水相中的比例丰度。在所有样品中,DEA和MEA是乙醇胺的优势种。研究了可能的来源(如缓蚀剂和生物转化)和储存过程中的自然衰减电位(如不同温度、酸化和添加叠氮化钠)。开发的分析方法可以进一步研究低分子量有机添加剂在油气开发中的命运,并提高评估化学物质释放到环境中的风险的能力。
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Environmental Science: Processes & Impacts
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