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Photo-aging of brominated epoxy microplastics in water under simulated solar irradiation† 模拟太阳辐照下水中溴化环氧微塑料的光老化。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-08 DOI: 10.1039/D4EM00208C
Xuefeng Hu, Hao Xie, Yujie Li and Chao Wang

Microplastics have become an increasingly concerning pollutant in aquatic environments, and photodegradation is their main degradation pathway in water. Gaining insight into the transformation process of microplastics will enhance our understanding of their behavior and destiny in natural environments. This paper studied the aging process of BER microplastics in aquatic environments under simulated sunlight and investigated the changes in the physical and chemical properties of microplastics and the changes in the leachate. During the photodegradation process, BER-MPs underwent extensive oxidation and reduction in particle size, and the originally smooth surface developed numerous voids, accompanied by yellowing. Introduction of O atoms in the molecular chains increased their hydrophilicity, resulting in the polymer chains breaking away from the plastic particles and dissolving in water. Also, once BER was excited by light, environmentally persistent free radicals are produced on its surface. Moreover, the breaking of C–Br bonds occurred during the photodegradation process of BER-MPs, which suggested that tetrabromobisphenol A would be transformed during the photoaging process of BER even if it was covalently bound to BER.

微塑料已成为水生环境中越来越令人担忧的污染物,光降解是其在水中降解的主要途径。深入了解微塑料的转化过程将加深我们对其在自然环境中的行为和归宿的理解。本文研究了 BER 微塑料在模拟阳光照射下的水生环境老化过程,并考察了微塑料物理和化学性质的变化以及渗滤液的变化。在光降解过程中,BER-MPs 发生了大面积氧化,粒径减小,原本光滑的表面出现了许多空隙,并伴有泛黄现象。在分子链中引入 O 原子增加了其亲水性,导致聚合物链从塑料粒子中断裂并溶解于水。此外,一旦 BER 被光激发,其表面就会产生环境持久性自由基。此外,在 BER-MPs 的光降解过程中,C-Br 键发生断裂,这表明即使四溴双酚 A 与 BER 共价结合,它也会在 BER 的光老化过程中发生转化。
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引用次数: 0
A CFD study on the effect of portable air cleaner placement on airborne infection control in a classroom† 关于便携式空气净化器放置位置对教室空气传播感染控制影响的 CFD 研究
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-04 DOI: 10.1039/D4EM00114A
Gen Pei, Parham Azimi, Donghyun Rim and Joseph G. Allen

The utilization of portable air cleaners (PACs) is a recommended supplemental approach to help remove airborne pathogens and mitigate disease transmission in learning environments. To improve PAC effectiveness, science-based information is needed to optimize their implementation strategies such as the deployment location, height, and number of PACs. In this study, we developed a Computational Fluid Dynamics (CFD) model to assess how PACs perform in occupied classrooms equipped with displacement and mixing ventilation systems. The results show that PACs with a flow rate of 2.6 h−1 reduce the mean aerosol intake of all students by up to 66%. A key benefit of using PACs is to facilitate air mixing and movement in indoor environments with inadequate ventilation, thereby effectively reducing high aerosol concentrations near the infector. Furthermore, our results highlight the impact of PAC location on its performance. PACs achieve the best effectiveness when placed closed to the infector (within a distance <3 m). In the absence of knowing who is infected, deploying a PAC at the center of the room is recommended. Moreover, adjusting PAC flow discharge height to the breathing height of occupants (e.g., 0.9–1.2 m for seated people) can enhance their effectiveness in spaces with poor air mixing.

使用便携式空气净化器(PAC)是一种值得推荐的补充方法,有助于清除空气中的病原体并减少学习环境中的疾病传播。为了提高便携式空气净化器的效果,我们需要以科学为基础的信息来优化其实施策略,例如便携式空气净化器的部署位置、高度和数量。在这项研究中,我们开发了一个计算流体动力学(CFD)模型,以评估 PAC 在装有置换和混合通风系统的教室中的表现。结果表明,流速为 2.6 hr-1 的 PAC 可使所有学生的平均气溶胶摄入量减少高达 66%。使用 PAC 的一个主要好处是在通风不足的室内环境中促进空气混合和流动,从而有效降低感染者附近的高气溶胶浓度。此外,我们的研究结果还强调了 PAC 位置对其性能的影响。当 PAC 靠近感染者时(距离 3 米以内),其效果最佳。在不知道感染者是谁的情况下,建议将 PAC 部署在房间中央。此外,根据居住者的呼吸高度(如坐着的人为 0.9-1.2 米)调整 PAC 的流量排放高度,可以提高其在空气混合不佳的空间中的效果。
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引用次数: 0
New insight into the spatiotemporal distribution and ecological risk assessment of endocrine-disrupting chemicals in the Minjiang and Tuojiang rivers: perspective of watershed landscape patterns† 岷江和沱江中干扰内分泌的化学物质时空分布和生态风险评估的新见解:流域景观模式的视角。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-03 DOI: 10.1039/D4EM00052H
Weike Zhao, Peilin Li and Bo Yang

This study evaluated the pollution characteristics, spatiotemporal distribution, and ecological risks of eight endocrine-disrupting chemicals (EDCs) in the Minjiang and Tuojiang rivers. Utilizing 3S technology (ArcGIS, remote sensing, GPS) and Fragstats, the research calculated eight landscape pattern indices related to land use types along the Minjiang river and established correlations between landscape factors and EDC distribution through stepwise multiple regression. The results indicated that bisphenol A (BPA) and nonylphenol (NP) were the most concerning EDCs, with detection frequencies of 97–100% and peak concentrations up to 63.35 ng L−1, primarily located in the middle and lower reaches of the Minjiang river and the upper reaches of the Tuojiang river. There was a significant correlation between the spatial distribution of pollutants and landscape patterns, where increased fragmentation, a higher number of patches, and complex patch shapes within a 10-kilometer buffer zone were associated with elevated levels of river pollution. By integrating four classical mathematical models to fit curves for acute and chronic toxicity data of BPA and NP, the findings suggested that BPA posed a higher ecological risk. This interdisciplinary research provided essential theoretical insights for investigating river pollution and its influencing factors, offering a new perspective on simultaneous river pollution control, urban functional zoning, and adjustment of watershed landscape spatial patterns from an urban planning standpoint.

本研究评估了岷江和沱江中八种干扰内分泌的化学物质(EDCs)的污染特征、时空分布和生态风险。研究利用 3S 技术(ArcGIS、遥感、GPS)和 Fragstats,计算了与岷江沿岸土地利用类型相关的 8 个景观格局指数,并通过逐步多元回归建立了景观因子与 EDC 分布之间的相关性。结果表明,双酚 A(BPA)和壬基酚(NP)是关注度最高的 EDCs,检出率为 97%-100%,峰值浓度高达 63.35 ng L-1,主要分布在岷江中下游和沱江上游。污染物的空间分布与景观格局之间存在明显的相关性,在10公里的缓冲区内,破碎化程度增加、斑块数量增多、斑块形状复杂与河流污染水平升高有关。通过整合四个经典数学模型来拟合双酚 A 和 NP 的急性和慢性毒性数据曲线,研究结果表明双酚 A 对生态环境的风险更高。这项跨学科研究为研究河流污染及其影响因素提供了重要的理论依据,从城市规划的角度为同时进行河流污染控制、城市功能分区和流域景观空间格局调整提供了新的视角。
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引用次数: 0
Association between polycyclic aromatic hydrocarbon exposure and cognitive performance in older adults: a cross-sectional study from NHANES 2011–2014† 多环芳烃暴露与老年人认知能力之间的关系:2011-2014 年 NHANES 横截面研究。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-02 DOI: 10.1039/D4EM00290C
Zerong Guan, Xueqiong Weng, Ligang Zhang and Peiran Feng

Background: polycyclic aromatic hydrocarbons (PAHs) are classified as neurotoxins, but the relationship between exposure to PAHs and cognition in adults is unclear, and their non-linear and mixed exposure association hasn't been explored. Objective: to evaluate the non-linear and joint association between co-exposure to PAHs and multiple cognitive tests in U.S. older people. Methods: restricted cubic spline (RCS) and Bayesian kernel machine regression (BKMR) were conducted to evaluate the non-linear and mixed exposure association, based on the cross-sectional data from NHANES 2011–2014: 772 participants over 60 years old, 4 cognitive test scores, including the Immediate Recall Test (IRT), Delayed Recall Test (DRT), Animal Fluency Test (AFT), and Digit Symbol Substitution test (DSST), and 5 urinary PAH metabolites. Results: a V-shaped nonlinear relationship was found between 3-hydroxyfluorene (3-FLUO), 2-hydroxyfluorene (2-FLUO), and DRT. Negative trends between mixed PAH exposure and IRT, DRT, and DSST scores were observed. 2-FLUO contributed the most to the negative association of multiple PAHs with IRT and DRT scores and 2-hydroxynaphthalene (2-NAP) played the most important role in the decreasing relationship between mixed PAH exposure and DSST scores. Conclusion: our study suggested that PAH exposure in the U.S. elderly might be related to their poor performances in IRT, DRT and DSST. Further prospective studies are needed to validate the association.

背景:多环芳烃(PAHs)被归类为神经毒素,但成人暴露于多环芳烃与认知能力之间的关系尚不清楚,其非线性和混合暴露关联也尚未得到探讨。目的:评估美国老年人共同暴露于多环芳烃与多种认知测试之间的非线性联合关系。方法:基于 NHANES 2011-2014 年的横截面数据,采用受限立方样条曲线(RCS)和贝叶斯核机器回归(BKMR)来评估非线性和混合暴露关联:研究对象包括 772 名 60 岁以上的参与者、4 项认知测试得分(包括即时回忆测试 (IRT)、延迟回忆测试 (DRT)、动物流畅性测试 (AFT) 和数字符号替换测试 (DSST))以及 5 种尿 PAH 代谢物。结果:3-羟基芴(3-FLUO)、2-羟基芴(2-FLUO)和 DRT 之间呈 V 型非线性关系。混合 PAH 暴露与 IRT、DRT 和 DSST 分数之间呈负相关趋势。2-FLUO 对多种 PAHs 与 IRT 和 DRT 分数之间的负相关关系贡献最大,而 2-hydroxynaphthalene (2-NAP) 在混合 PAH 暴露与 DSST 分数之间的递减关系中起着最重要的作用。结论:我们的研究表明,美国老年人的 PAH 暴露可能与他们在 IRT、DRT 和 DSST 中的不良表现有关。需要进一步的前瞻性研究来验证这种关联。
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引用次数: 0
The chemical assessment of surfaces and air (CASA) study: using chemical and physical perturbations in a test house to investigate indoor processes. 表面和空气化学评估(CASA)研究:利用试验房中的化学和物理扰动来研究室内过程。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-02 DOI: 10.1039/d4em00209a
Delphine K Farmer, Marina E Vance, Dustin Poppendieck, Jon Abbatt, Michael R Alves, Karen C Dannemiller, Cholaphan Deeleepojananan, Jenna Ditto, Brian Dougherty, Olivia R Farinas, Allen H Goldstein, Vicki H Grassian, Han Huynh, Deborah Kim, Jon C King, Jesse Kroll, Jienan Li, Michael F Link, Liora Mael, Kathryn Mayer, Andrew B Martin, Glenn Morrison, Rachel O'Brien, Shubhrangshu Pandit, Barbara J Turpin, Marc Webb, Jie Yu, Stephen M Zimmerman

The Chemical Assessment of Surfaces and Air (CASA) study aimed to understand how chemicals transform in the indoor environment using perturbations (e.g., cooking, cleaning) or additions of indoor and outdoor pollutants in a well-controlled test house. Chemical additions ranged from individual compounds (e.g., gaseous ammonia or ozone) to more complex mixtures (e.g., a wildfire smoke proxy and a commercial pesticide). Physical perturbations included varying temperature, ventilation rates, and relative humidity. The objectives for CASA included understanding (i) how outdoor air pollution impacts indoor air chemistry, (ii) how wildfire smoke transports and transforms indoors, (iii) how gases and particles interact with building surfaces, and (iv) how indoor environmental conditions impact indoor chemistry. Further, the combined measurements under unperturbed and experimental conditions enable investigation of mitigation strategies following outdoor and indoor air pollution events. A comprehensive suite of instruments measured different chemical components in the gas, particle, and surface phases throughout the study. We provide an overview of the test house, instrumentation, experimental design, and initial observations - including the role of humidity in controlling the air concentrations of many semi-volatile organic compounds, the potential for ozone to generate indoor nitrogen pentoxide (N2O5), the differences in microbial composition between the test house and other occupied buildings, and the complexity of deposited particles and gases on different indoor surfaces.

表面和空气化学评估(CASA)研究旨在通过在控制良好的试验房中进行扰动(如烹饪、清洁)或添加室内外污染物,了解化学物质在室内环境中是如何转化的。添加的化学物质包括单个化合物(如气态氨或臭氧)和更复杂的混合物(如野火烟雾代理和商业杀虫剂)。物理扰动包括不同的温度、通风率和相对湿度。CASA 的目标包括了解 (i) 室外空气污染如何影响室内空气化学,(ii) 野火烟雾如何在室内传播和转化,(iii) 气体和颗粒物如何与建筑物表面相互作用,以及 (iv) 室内环境条件如何影响室内化学。此外,在无干扰和实验条件下进行的综合测量有助于研究室外和室内空气污染事件后的缓解策略。在整个研究过程中,一整套仪器对气体、颗粒物和表面阶段的不同化学成分进行了测量。我们将概述试验室、仪器、实验设计和初步观测结果,包括湿度在控制空气中多种半挥发性有机化合物浓度方面的作用、臭氧产生室内五氧化二氮(N2O5)的可能性、试验室与其他有人居住的建筑物之间微生物成分的差异,以及不同室内表面沉积颗粒和气体的复杂性。
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引用次数: 0
Criteria for distinguishing heterogeneous from homogeneous conditions for aromatic diisocyanates in water† 区分芳香族二异氰酸酯在水中的异质和均质条件的标准。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-01 DOI: 10.1039/D4EM00200H
Patrick M. Plehiers, Hans-Georg Pirkl, Lauren Ward and Christian Bögi

Environmental fate and toxicity testing typically requires knowledge of the water solubility of the test substances. Determining the solubility of aromatic diisocyanates in water poses great challenges because of their hydrophobic nature and water-reactivity. The reactive dissolution process is dynamic and the establishment of a steady-state equilibrium cannot readily be observed. In preparation of experimental work, computer simulation was used to derive and evaluate criteria that enable distinguishing homogeneous (i.e., substances would be fully dissolved in water) from heterogeneous (i.e., a separate organic phase would be present) conditions. The simulation utilized available kinetic information and models representing the main physical and chemical processes taking place. It was found that the transition to heterogeneous conditions (i.e., the exceedance of the solubility limit with increasing loading) can be identified by observing either a rapid decline in ultimate yield of the diamine hydrolysis product from near-stoichiometric to much lower values, or a decrease in rate of formation of the diamine hydrolysis product relative to its ultimate yield. The latter criterion is expected to be the more powerful indicator. These criteria can be used in future work to define and interpret an experimental program for determining solubility limits for aromatic diisocyanates or other poorly-soluble, water-reactive substances.

环境归宿和毒性测试通常需要了解测试物质的水溶性。由于芳香族二异氰酸酯具有疏水性和水反应性,因此确定其在水中的溶解度是一项巨大的挑战。反应溶解过程是动态的,无法轻易观察到稳态平衡的建立。在准备实验工作的过程中,利用计算机模拟来推导和评估能够区分均相条件(即物质完全溶解在水中)和异相条件(即存在独立的有机相)的标准。模拟利用了现有的动力学信息和代表所发生的主要物理和化学过程的模型。结果发现,向异构条件的过渡(即随着负载量的增加而超过溶解度极限)可以通过以下两种情况来确定:一是二胺水解产物的最终产率从接近化学计量值迅速下降到更低的值,二是二胺水解产物的形成率相对于其最终产率有所下降。预计后一种标准是更有力的指标。在今后的工作中,可以利用这些标准来确定和解释用于确定芳香族二异氰酸酯或其他溶解性差、水反应性物质溶解度极限的实验方案。
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引用次数: 0
Critical review of fluorescence and absorbance measurements as surrogates for the molecular weight and aromaticity of dissolved organic matter† 荧光和吸收率测量作为溶解有机物分子量和芳香性替代物的批判性评述
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-27 DOI: 10.1039/D4EM00183D
Julie A. Korak and Garrett McKay

Dissolved organic matter (DOM) is ubiquitous in aquatic environments and challenging to characterize due to its heterogeneity. Optical measurements (i.e., absorbance and fluorescence spectroscopy) are popular characterization tools, because they are non-destructive, require small sample volumes, and are relatively inexpensive and more accessible compared to other techniques (e.g., high resolution mass spectrometry). To make inferences about DOM chemistry, optical surrogates have been derived from absorbance and fluorescence spectra to describe differences in spectral shape (e.g., E2:E3 ratio, spectral slope, fluorescence indices) or quantify carbon-normalized optical responses (e.g., specific absorbance (SUVA) or specific fluorescence intensity (SFI)). The most common interpretations relate these optical surrogates to DOM molecular weight or aromaticity. This critical review traces the genesis of each of these interpretations and, to the extent possible, discusses additional lines of evidence that have been developed since their inception using datasets comparing diverse DOM sources or strategic endmembers. This review draws several conclusions. More caution is needed to avoid presenting surrogates as specific to either molecular weight or aromaticity, as these physicochemical characteristics are often correlated or interdependent. Many surrogates are proposed using narrow contexts, such as fractionation of a limited number of samples or dependence on isolates. Further study is needed to determine if interpretations are generalizable to whole-waters. Lastly, there is a broad opportunity to identify why endmembers with low abundance of aromatic carbon (e.g., effluent organic matter, Antarctic lakes) often do not follow systematic trends with molecular weight or aromaticity as observed in endmembers from terrestrial environments with higher plant inputs.

溶解有机物(DOM)在水生环境中无处不在,由于其异质性,对其进行表征具有挑战性。光学测量(即吸光度和荧光光谱)是常用的表征工具,因为它们不具破坏性,所需样本量小,而且相对便宜,与其他技术(如高分辨率质谱法)相比更容易获得。为了推断 DOM 化学性质,人们从吸收光谱和荧光光谱中推导出光学代用指标,以描述光谱形状的差异(如 E2:E3 比值、光谱斜率、荧光指数)或量化碳归一化光学响应(如特定吸收光谱(SUVA)或特定荧光强度(SFI))。最常见的解释是将这些光学代用指标与 DOM 分子量或芳香度联系起来。本评论追溯了每种解释的起源,并尽可能讨论了自这些解释出现以来,利用比较不同 DOM 来源或战略内含物的数据集开发出的其他证据。本综述得出了几个结论。需要更加谨慎,避免把代用指标说成是分子量或芳香度的特异性指标,因为这些理化特征往往是相互关联或相互依存的。许多代用指标都是在狭窄的范围内提出的。例如,对数量有限的样本进行分馏或依赖于分离物并将解释推广到整个水体的做法值得进一步研究。最后,我们还有很多机会来确定为什么芳香碳含量较低的内含物(如南极湖泊中的排出有机物)通常不会像植物投入量较高的陆地环境中的内含物那样,随着分子量或芳香度的增加而呈现系统化趋势。
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引用次数: 0
A sustainable method for oxidizing phenanthrene in tropical soil using natural iron as a catalyst in a slurry phase reactor with persulfate assistance† 在有过硫酸盐辅助的浆相反应器中使用天然铁作为催化剂氧化热带土壤中菲的可持续方法
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-25 DOI: 10.1039/D4EM00328D
Mohammad Qutob, Mohd Rafatullah, Syahidah Akmal Muhammad, Masoom Raza Siddiqui and Mahboob Alam

The presence of impurities is a significant restriction to the use of natural iron minerals as catalysts in the advanced oxidation process (AOP), especially if applied for soil remediation. This study evaluated the catalytic activity of tropical soil, which has relatively low impurities and naturally contains iron, for the remediation of phenanthrene (PHE) contamination. The system showed good performance, and the best result was 81% PHE removal after 24 h under experimental conditions of pH 7, [PHE]0 = 300 mg/50 g soil, temperature 55 °C, air flow = 260 mL min−1, and [persulfate]0 = 20 mg kg−1, while the mineralization was 61%. Nevertheless, certain limitations were noted in the soil matrix following the remediation procedure, including the appearance of cracks in the soil aggregate, reduction in the crystal size of the soil particles, and decline in the iron and aluminium contents. The results confirmed that the radicals play a major role in the remediation process. SO4˙ was more dominant than O2˙, while HO˙ played a minor role. Additionally, the by-products were detected by gas chromatography-mass spectroscopy (GC-MS), and the degradation pathway of PHE is proposed. Toxicity assessment tests were performed by using a computational method. In spite of the challenges, this research achieved notable progress in soil remediation, taking a significant step forward in implementing the AOP without catalysts to activate oxidants and remove PHE within the soil. Also, this approach supports sustainability by reducing the need for extra materials and providing an environmentally friendly way of soil remediation.

在高级氧化工艺(AOP)中使用天然铁矿物作为催化剂,尤其是用于土壤修复时,杂质的存在是一个重要的限制因素。本研究评估了杂质相对较少且天然含铁的热带土壤对菲(PHE)污染修复的催化活性。在 pH 值为 7、[PHE]0 = 300 mg/50 g 土壤、温度为 55 ℃、气流 = 260 mL/min、[过硫酸盐]0 = 20 mg/kg 的实验条件下,24 小时后 PHE 去除率达到 81%,矿化度为 61%。不过,修复过程后的土壤基质也出现了一些问题,包括土壤团聚体出现裂缝、土壤颗粒的晶体尺寸减小、铁和铝含量下降等。结果证实,自由基在修复过程中发挥了重要作用。SO_4^(--) 是最主要的自由基,其次是 O_2^(--),而 HO^- 的作用较小。此外,还利用气相色谱-质谱法(GC-MS)检测了副产品,并提出了 PHE 的降解途径。利用计算方法进行了毒性评估测试。尽管面临诸多挑战,但这项研究在土壤修复方面取得了显著进展,在实施无催化剂 AOP 以激活氧化剂并去除土壤中 PHE 方面迈出了重要一步。此外,这种方法还减少了对额外材料的需求,为土壤修复提供了一种环境友好型方法,从而支持了可持续发展。
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引用次数: 0
Reduced greenhouse gas emissions from particulate organic matter degradation in iron-enriched sediments† 富铁沉积物中颗粒有机物降解减少温室气体排放。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-18 DOI: 10.1039/D4EM00185K
Giulia Kommana, Michael Hupfer, Jason Nicholas Woodhouse, Hans-Peter Grossart and Tobias Goldhammer

Iron (Fe) plays an important role in the biogeochemical cycling of carbon and nutrients in aquatic systems. Reactive Fe phases can interact with organic carbon and facilitate the removal of carbon from the biogeochemical cycle; however, this important ecosystem function is often strongly controlled by Fe availability. Due to pollution from lignite mining in the Lusatian province in Northeast Germany, large amounts of iron and sulfate are released into the fluvial-lacustrine system of the Spree River. It was hypothesized that the input of freshly precipitated iron oxyhydroxides from mining areas (e.g., ferrihydrite) alter the biodegradation of particulate organic matter (POM) in downstream lacustrine sediments. To investigate the Fe-dependent degradation of POM, slurries mimicking iron-polluted sediments (85 mg Fe per g, 116 mg Fe per g, and 149 mg Fe per g dry weight) were incubated with plankton or leaf POM under anoxic and oxic headspace conditions, and CO2 and CH4 emissions, water chemistry, and stable isotopes of dissolved inorganic carbon were measured. The experiments revealed that (i) with an increasing Fe content, the CO2 and CH4 emissions were gradually reduced, (ii) CO2 and CH4 production was higher during plankton degradation than during leaf decomposition, and (iii) under oxic conditions, CO2 production was higher and CH4 production was lower when compared to the treatments under anoxic conditions. These findings demonstrate that while benthic mineralization of fresh POM typically releases greenhouse gases into the water column, the availability of iron oxyhydroxides can contribute to reduced greenhouse gas emissions from sediments. This is of considerable relevance for future carbon budgets of similar mining-affected, iron-polluted fluvial-lacustrine river systems.

铁(Fe)在水生系统中碳和营养物质的生物地球化学循环中发挥着重要作用。反应性铁相可与有机碳相互作用,促进生物地球化学循环中碳的去除;然而,这一重要的生态系统功能往往受到铁供应量的强烈控制。由于德国东北部卢萨特省褐煤开采造成的污染,大量铁和硫酸盐被释放到施普雷河的河道-湖泊系统中。据推测,矿区新析出的铁氧氢氧化物(如铁酸盐)会改变下游湖沼沉积物中颗粒有机物(POM)的生物降解。为了研究 POM 的铁依赖性降解,在缺氧和缺氧顶空条件下,模拟铁污染沉积物(每克含铁 85 毫克、每克含铁 116 毫克和每克干重含铁 149 毫克)的泥浆与浮游生物或叶片 POM 一起培养,并测量 CO2 和 CH4 排放、水化学和溶解无机碳的稳定同位素。实验结果表明:(i) 随着铁含量的增加,CO2 和 CH4 的排放量逐渐减少;(ii) 浮游生物降解过程中 CO2 和 CH4 的产生量高于叶片分解过程中;(iii) 与缺氧条件下的处理相比,缺氧条件下 CO2 的产生量更高,CH4 的产生量更低。这些研究结果表明,虽然新鲜 POM 的底栖矿化通常会将温室气体释放到水体中,但铁氧氢氧化物的存在有助于减少沉积物的温室气体排放。这对类似受采矿影响、铁污染的河流-湖泊系统未来的碳预算具有重要意义。
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引用次数: 0
Emerging investigator series: nontargeted screening of aryl hydrocarbon receptor agonists in endangered beluga whales from the St. Lawrence Estuary: beyond legacy contaminants† 新晋研究人员系列:圣劳伦斯河口濒危白鲸体内芳基烃受体激动剂的非靶向筛选:超越遗留污染物。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-17 DOI: 10.1039/D4EM00243A
Holly Barrett, Jianxian Sun, Yuhao Chen, Diwen Yang, Jonathan Verreault, Magali Houde, Frank Wania and Hui Peng

The elevated concentrations of organohalogen contaminants in the endangered St. Lawrence Estuary (SLE) belugas have prompted the hypothesis that aryl hydrocarbon receptor (AhR) activity may be a contributor towards their potential adverse effects. While indirect associations between AhR and contaminant levels have been reported in SLE beluga tissues, AhR activity was never directly measured. Using bioassays and nontargeted analysis, this study contrasted AhR activity and agonist profiles between pooled tissue extracts of endangered SLE and non-threatened Arctic belugas. Tissue extracts of SLE belugas exhibited significantly higher overall AhR activity than that of Arctic belugas, with a 2000s SLE beluga liver extract exerting significantly higher activity than blubber extracts of SLE and Arctic belugas from the same time period. Contrary to our expectations, well-known AhR agonists detected by nontargeted analysis, including polychlorinated biphenyls (PCBs), were only minor contributors to the observed AhR activity. Instead, Tox21 suspect screening identified more polar chemicals, such as dyes and natural indoles, as potential contributors. Notably, the natural product bromoindole was selectively detected in SLE beluga liver at high abundance and was further confirmed as an AhR agonist. These findings highlighted the significance of the AhR-mediated toxicity pathway in belugas and underscored the importance of novel AhR agonists, particularly polar compounds, in its induction.

濒危的圣劳伦斯河口(SLE)白鲸体内有机卤素污染物浓度的升高引发了一种假设,即芳基烃受体(AhR)活性可能是造成其潜在不良影响的一个因素。虽然有报道称 SLE 白鲸组织中的 AhR 与污染物水平存在间接联系,但从未直接测量过 AhR 的活性。本研究采用生物测定和非目标分析方法,对比了濒危系统性红斑狼疮白鲸和未受威胁的北极白鲸的集合组织提取物中的 AhR 活性和激动剂特征。系统性红斑狼疮白鲸组织提取物的总体AhR活性明显高于北极白鲸,2000年代的系统性红斑狼疮白鲸肝脏提取物的活性明显高于同一时期的系统性红斑狼疮白鲸和北极白鲸鲸脂提取物。与我们的预期相反,通过非靶向分析检测到的众所周知的 AhR 激动剂(包括多氯联苯 (PCB))对观察到的 AhR 活性的贡献很小。相反,Tox21 可疑筛选发现了更多极性化学物质,如染料和天然吲哚,它们是潜在的促成因素。值得注意的是,在系统性红斑狼疮白鲸肝脏中选择性地检测到了高丰度的天然产物溴吲哚,并进一步证实其是一种 AhR 激动剂。这些发现凸显了白鲸体内AhR介导的毒性途径的重要性,并强调了新型AhR激动剂(尤其是极性化合物)在诱导毒性途径中的重要性。
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Environmental Science: Processes & Impacts
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