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Organic matter concentration and characteristic dynamics in surface waters post-bushfires and cyclones: fDOM sensors for environmental monitoring and control† 火灾和气旋后地表水中有机物的浓度和特征动态:用于环境监测和控制的 fDOM 传感器
Pub Date : 2024-05-03 DOI: 10.1039/D4VA00036F
Hiua Daraei, Edoardo Bertone, Rodney A. Stewart, John Awad, Adam Leavesley, Matthew Gale, Eriita Jones, Kathy Cinque, Mark Agnew, Hugh A. Burger and John Van Leeuwen

This study presents the findings of an investigation on the dynamics of dissolved organic matter (DOM) concentration and characteristics of four Australian rivers and reservoirs after their catchments had been severely burned by bushfires (wildfires) or impacted by a tropical cyclone. Dissolved organic carbon (DOC) increased immediately following the events, and subsequently decreased. The findings indicate rapid stabilisation of water quality, based on the measured parameters, following the commencement of the first winter after the events (which occurred in mid/end summer). In the fire-affected Middle River catchment, DOC decreased from 30.7 mg L−1 to 10.2 mg L−1 over approximately seven months. In the case of the Herring Lagoon catchment, which was affected by cyclone Uesi, DOC decreased from 15.6 mg L−1 to 1.2 mg L−1 over approximately ten months. However, the DOM present in the surface water exposed to the cyclone showed higher molecular weight, coagulability and UV-vis absorbance than the DOM present in the surface water of fire-affected catchments. The observed rapid increase and then reduction in DOM concentrations after extreme climate events indicates the need for short-term and rapid responses for drinking water treatment. The fluorescence signal of a field-deployable fluorescent DOM (fDOM) sensor showed potential as an online monitoring tool for assessing DOM concentration in surface waters, including under extreme conditions. The rapid identification of high DOM loadings in surface waters following extreme climate events (e.g. using a field deployed fDOM sensor) along with its coagulability characteristics could assist in catchment management and drinking water treatment by enabling timely control decisions in response to the impacts of such events.

本研究介绍了澳大利亚四条河流和水库的集水区被丛林大火(野火)严重焚烧或受到热带气旋影响后溶解有机物(DOM)浓度和特征的动态调查结果。事件发生后,溶解有机碳 (DOC) 立即增加,随后减少。研究结果表明,根据测量参数,水质在事件发生后的第一个冬季(夏中/夏末)开始后迅速趋于稳定。在受火灾影响的中河集水区,溶解氧从 30.7 毫克/升下降到 10.2 毫克/升,历时约 7 个月。在受气旋 Uesi 影响的鲱鱼礁集水区,在大约 10 个月的时间里,溶解氧从 15.6 毫克/升-1 降至 1.2 毫克/升-1。然而,与受火灾影响的集水区地表水中的 DOM 相比,受气旋影响的地表水中的 DOM 表现出更高的分子量、凝结性和紫外可见吸收率。在极端气候事件发生后,观察到的 DOM 浓度先是快速上升,然后又下降,这表明在饮用水处理方面需要采取短期和快速的应对措施。现场部署的荧光 DOM(fDOM)传感器的荧光信号显示出作为在线监测工具评估地表水中 DOM 浓度(包括极端条件下)的潜力。在极端气候事件发生后,快速识别地表水中的高 DOM 负荷(例如使用现场部署的 fDOM 传感器)及其可凝性特征,有助于集水区管理和饮用水处理,从而针对此类事件的影响及时做出控制决策。
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引用次数: 0
Microbially mediated synthesis of vivianite by Desulfosporosinus on the way to phosphorus recovery † 脱硫孢子虫在磷回收过程中微生物介导的维维安特合成作用
Pub Date : 2024-04-30 DOI: 10.1039/D4VA00040D
Yuriy V. Knyazev, Mikhail S. Platunov, Olga P. Ikkert, Sergey V. Semenov, Oleg A. Bayukov, Anton D. Nikolenko, Vladimir P. Nazmov, Mikhail N. Volochaev, Andrey A. Dubrovskiy, Maksim S. Molokeev, Ekaterina D. Smorodina, Dmitry A. Balaev and Olga V. Karnachuk

We explored the role of biomineralization in industrial waste sludge formation, using the laboratory cultivation of Desulfovibrio sp. OL sulfate reducing species isolated from the Komsomolsky waste sludge (Russia). The most frequently reported sulfate-reducing bacteria (SRB) biomineralization products are various iron sulfides. Here we present first studies of the products of Desulfosporosinus metallidurans, acidophilic SRB from acid mine drainage. We analyzed the biomineralized sample using X-ray diffraction, electron microscopy, X-ray absorption and Mössbauer spectroscopies, and magnetization measurements via First-Order Reversal Curve (FORC) diagram analysis. Our findings show that the biomineralization occurring under pure culture conditions leads to the formation of greigite (Fe3S4) nanorods, along with larger microbially mediated crystals of vivianite (Fe3(PO4)2·8H2O) and siderite (FeCO3). Energy dispersive X-ray spectroscopy revealed that the crystal sizes of vivianite and siderite were comparatively larger than those of the nanorod-shaped greigite. Transmission electron microscopy and Mössbauer spectroscopy detected ultrafine ferrihydrite (Fe2O3·nH2O) superparamagnetic nanoparticles with an average size of 2.5 nm. FORC analysis showed significant magnetic interactions among these nanoparticles, suggesting their potential for magnetic separation applications. The current study demonstrates that ferrihydrite nanoparticles have a strong magnetic affinity for other crystal phases produced by Desulfosporosinus metallidurans. Therefore, we believe that the investigated bacterial species can be exploited in advanced magnetic separation techniques. This offers a cost-effective and environmentally friendly method for purifying sediments in industrial waste sludge.

我们利用实验室培养的 Desulfovibrio sp.OL硫酸盐还原菌从共青城(俄罗斯)的废弃污泥中分离出来。最常报道的硫酸盐还原菌(SRB)生物矿化产物是各种硫化铁。在此,我们首次介绍了从酸性矿井排水中分离出的嗜酸性硫酸盐还原菌 Desulfosporosinus metallidurans 的产物。我们对生物矿化样品进行了 X 射线衍射、电子显微镜、X 射线吸收和莫斯鲍尔光谱研究以及磁化测量(一阶反转曲线(FORC)图分析)。我们确定,在纯培养条件下发生的生物矿化导致形成了格来石(Fe3S4)纳米棒,以及微生物介导的维维安岩(Fe3(PO4)2-8H2O)和菱铁矿(FeCO3)晶相。能量色散 X 射线光谱显示,维维安岩和菱铁矿以大晶体形式形成,与纳米棒状的绿泥石形成鲜明对比。透射电子显微镜和莫斯鲍尔光谱研究发现了平均尺寸为 2.5 纳米的超细铁水云母(Fe2O3 ‧ nH2O)超顺磁性纳米颗粒。此外,FORC 技术还显示出与样品中超细铁水物相对应的高水平磁相互作用,可在分离技术中加以利用。目前的研究表明,纳米铁水物对脱硫孢子虫(Desulfosporosinus metallidurans)产生的其他晶相具有很强的吸引力。因此,我们认为所研究的细菌物种可以在净化工业废渣沉积物的先进技术中加以利用。
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引用次数: 0
Nitrogen isotopes in herbaria document historical nitrogen sewage pollution in the Mersey Estuary, England† 标本馆中的氮同位素记录了英国默西河口历史上的氮污水污染情况
Pub Date : 2024-04-29 DOI: 10.1039/D4VA00015C
Freya C. Alldred, Darren R. Gröcke, Samuel E. Jackson and Geraldine Reid

A macroalgae (seaweed) herbarium nitrogen isotope (δ15N) record is produced for the River Mersey and Liverpool South Docks (England) between 1821 and 2018. A modern macroalgae δ15N record was also produced from September 2022. The herbaria δ15N record shows a stark difference from 1821 to the present. Lower δ15N in the early 1800s is attributed to agricultural and raw sewage pollution. From 1970 to the present the herbaria samples record very elevated δ15N values – peaking in 1978 at +31‰. The 1989 Water Act and privatisation of water companies in the UK had limited impact on the herbarium δ15N record but indicated a dominance of sewage nitrogen in the River Mersey. Macroalgae δ15N has become even more elevated since the last herbaria sample in 2013. The herbaria and modern data record some of the highest seaweed δ15N values (and therefore, sewage nitrogen pollution) recorded to date. This study highlights a novel use of herbaria macroalgae to document past changes in nitrogen pollution in estuarine environments. More poignantly it highlights that the River Mersey – Mersey Estuary is heavily polluted with sewage nitrogen and requires immediate action to resolve this environmental issue.

制作了 1821 年至 2018 年期间默西河和利物浦南码头(英格兰)的大型藻类(海藻)标本室氮同位素(δ15N)记录。此外,还制作了自 2022 年 9 月起的现代大型藻类 δ15N 记录。标本δ15N记录显示出 1821 年至今的巨大差异。19 世纪早期较低的δ15N 可归因于农业和原始污水污染。1970 年至今,标本馆样本记录的 δ15N 值非常高,1978 年达到顶峰,为 +31‰。1989 年的《水法》和英国自来水公司的私有化对标本室的 δ15N 记录影响有限,但表明默西河中污水氮占主导地位。自 2013 年最后一次标本馆采样以来,大型藻类的 δ15N 甚至变得更高。标本馆和现代数据记录了迄今为止最高的一些海藻δ15N 值(因此也是污水氮污染)。这项研究强调了利用标本馆大型藻类记录河口环境氮污染过去变化的新方法。更重要的是,它强调了默西河-默西河口受到污水氮的严重污染,需要立即采取行动解决这一环境问题。
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引用次数: 0
Microplastic occurrence in sediments of informal settlement in Durban, South Africa: assessing the ocean impact in the aftermath of floods 南非德班非正规住区沉积物中的微塑料含量:评估洪水过后的海洋影响
Pub Date : 2024-04-29 DOI: 10.1039/D3VA00382E
Nokwanda Hendricks, Olatunde S. Olatunji and Bhekumuzi P. Gumbi

The environmental impact of microplastics is increasingly being recognized, leading to their inclusion as contaminants of emerging concern. Consequently, it is essential to identify and monitor microplastics and their impact on the ecosystem. In this study, a ball miller was employed to process plastic waste, generating microplastics for the optimisation of separation methods. Microplastics of various sizes and shapes were produced and used to spike the sediments for optimisation of the density separation method. The recovered microplastics ranged from 0.74–5 mm, as confirmed by stereomicroscopy. In addition, the types of polymers present in microplastics were confirmed using Fourier Transform Infrared Spectroscopy-Attenuated Total Reflectance (FTIR-ATR). The developed analytical method was employed to study the occurrence of microplastics in river sediments passing through informal settlements after floods. Moreover, the evaluated data confirmed that informal settlements are a major source of microplastics found in the ocean after a flood. Microplastics in river and ocean sediments were predominantly composed of polypropylene, polyethylene, and polystyrene with a size range of 0.90–5 mm. To the best of our knowledge, this study is the first to report the impacts of informal settlements on the ocean during floods in Africa.

人们日益认识到微塑料对环境的影响,并将其列为新关注的污染物。因此,识别和监测微塑料及其对生态系统的影响至关重要。本研究采用球磨机处理塑料垃圾,产生微塑料,用于优化分离方法。产生的各种尺寸和形状的微塑料被用来对沉积物进行加标处理,以优化密度分离方法。经体视显微镜确认,回收的微塑料大小在 0.74-5 毫米之间。此外,还利用傅立叶变换红外光谱-衰减全反射(FTIR-ATR)确认了微塑料中的聚合物类型。所开发的分析方法被用于研究洪水过后经过非正规居住区的河流沉积物中出现的微塑料。此外,评估数据证实,非正式定居点是洪水过后海洋中发现的微塑料的主要来源。河流和海洋沉积物中的微塑料主要由聚丙烯、聚乙烯和聚苯乙烯组成,尺寸范围为 0.90-5 毫米。据我们所知,这项研究首次报告了非洲洪水期间非正规住区对海洋的影响。
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引用次数: 0
Pesticides and transformation products in surface waters of western Montérégie, Canada: occurrence, spatial distribution and ecotoxicological risks† 加拿大 Montérégie 西部地表水中的杀虫剂和转化产物:出现、空间分布和生态毒理学风险
Pub Date : 2024-04-29 DOI: 10.1039/D3VA00231D
Xiameng Feng, Zhen Liu, Sung Vo Duy, Gabriel Munoz, Lise Parent and Sébastien Sauvé

The objective of this study was to investigate the occurrence, spatial distribution, and ecotoxicological risk of pesticides and transformation products in surface waters of western Montérégie (Quebec, Canada). A total of 29 samples were collected from 11 rivers during the summers of 2019 and 2021, and the samples were analyzed for 48 pesticides and 8 transformation products. The downstream data were used to assess the ecotoxicological risks based on Quebec's acute or chronic aquatic life criterion (AALC or CALC). Overall, 9 herbicides (glyphosate, S-metolachlor, 2,4-D, metribuzin, atrazine, MCPA, prometryn, dimethenamid, simazine), 3 insecticides (clothianidin, imidacloprid, chlorantraniliprole), and 4 fungicides (azoxystrobin, fluxapyroxad, tebuconazole, carbendazim) were detected at all sampling sites, demonstrating their widespread use in western Montérégie. Glyphosate (87–4095 ng L−1), S-metolachlor (6–2519 ng L−1), and 2,4-D (6–1094 ng L−1) were identified as the most abundant pesticides in surface water. Furthermore, 6 pesticide transformation products (metolachlor ESA, AMPA, metolachlor OA, desethylatrazine, atrazine-2-hydroxy, desisopropylatrazine) were detected at all sampling sites. The concentration of transformation products accounted for 51% on average of the total concentration, demonstrating the abundance of transformation products in surface waters. Neonicotinoids exhibited the highest ecotoxicological risk in the surface water samples with an average CALC risk quotient of 28 for 2019 and 12 for 2021, respectively. The present study offers insights into pesticides occurrence and their ecological impacts on surface waters of western Montérégie and allows for supporting future pesticide management and ecotoxicological risk mitigation strategies.

本研究旨在调查加拿大魁北克省蒙特雷吉西部地表水中农药和转化产物的发生、空间分布和生态毒理学风险。在 2019 年和 2021 年夏季,共从 11 条河流中采集了 29 份样本,并对样本中的 48 种农药和 8 种转化产物进行了分析。下游数据用于根据魁北克省急性或慢性水生生物标准(AALC 或 CALC)评估生态毒理学风险。总体而言,在所有采样点都检测到了 9 种除草剂(草甘膦、S-甲草胺、2,4-D、甲萘威、莠去津、MCPA、丙炔草酯、二甲戊灵、西玛津)、3 种杀虫剂(噻虫嗪、吡虫啉、氯虫苯甲酰胺)和 4 种杀菌剂(唑螨酯、氟螨脲、戊唑醇、多菌灵),这表明它们在蒙泰雷吉省西部被广泛使用。草甘膦(87-4095 纳克/升)、S-甲草胺(6-2519 纳克/升)和 2,4-D (6-1094 纳克/升)是地表水中含量最高的农药。此外,在所有采样点还检测到 6 种农药转化产物(甲草胺 ESA、甲草胺 AMPA、甲草胺 OA、去乙基atrazine、阿特拉津-2-羟基、去异丙基atrazine)。转化产物的浓度平均占总浓度的 51%,这表明转化产物在地表水中的含量很高。新烟碱类在蒙特雷盖省西部地表水中的生态毒理学风险最高,2019 年和 2021 年的平均 CALC 风险商数分别为 28 和 12。本研究有助于深入了解农药的发生及其对蒙泰雷吉省西部地表水的生态影响,并为未来的农药管理和生态毒理学风险缓解战略提供支持。
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引用次数: 0
The effects of lead, copper, and iron corrosion products on antibiotic resistant bacteria and antibiotic resistance genes† 铅、铜和铁腐蚀产物对抗生素耐药细菌和抗生素耐药基因的影响
Pub Date : 2024-04-24 DOI: 10.1039/D4VA00026A
Veronika Folvarska, San Marie Thomson, Zihao Lu, Maya Adelgren, Adam Schmidt, Ryan J. Newton, Yin Wang and Patrick J. McNamara

Antibiotic resistance is a public health crisis. Antibiotic resistant bacteria (ARB) and antibiotic resistance genes (ARGs) are present in drinking water distribution systems. Metals are known selective pressures for antibiotic resistance, and metallic corrosion products are found within drinking water distribution systems due to the corrosion of metal pipes. While corrosion products are a source of metals, the impact of specific corrosion products on antibiotic resistance has not been investigated. The objective of this study was to determine the impact of six corrosion products—CuO, Cu2O, Pb5(PO4)3OH, β-PbO2, Fe3O4, and α-FeOOH—on the abundance of ARB and ARGs. Lab-scale microcosms were seeded with source water from Lake Michigan and amended with individual corrosion products. In general, copper and lead corrosion products increased antibiotic resistance, although not universally across different ARB and ARG types. Concentration and speciation of copper and lead corrosion products were found to have an impact on antibiotic resistance profiles. Meanwhile, iron corrosion products had minimal impact on antibiotic resistance. Overall, this study sheds light on how pipe materials may impact antibiotic resistance as a result of corrosion products.

抗生素耐药性是一场公共卫生危机。抗生素耐药细菌 (ARB) 和抗生素耐药基因 (ARG) 存在于饮用水输配系统中。金属是抗生素耐药性的已知选择性压力,由于金属管道的腐蚀,在饮用水输水系统中发现了金属腐蚀产物。虽然腐蚀产物是金属的一种来源,但具体腐蚀产物对抗生素耐药性的影响尚未进行调查。本研究旨在确定六种腐蚀产物(CuO、Cu2O、Pb5(PO4)3OH、β-PbO2、Fe3O4 和 α-FeOOH)对 ARB 和 ARG 丰度的影响。在实验室规模的微生态系统中加入了密歇根湖的原水,并用各种腐蚀产物进行了修正。一般来说,铜和铅腐蚀产物会增加抗生素耐药性,但在不同的 ARB 和 ARG 类型中并不普遍。研究发现,铜和铅腐蚀产物的浓度和种类对抗生素耐药性特征有影响。同时,铁腐蚀产物对抗生素耐药性的影响很小。总之,这项研究揭示了管道材料如何因腐蚀产物而影响抗生素耐药性。
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引用次数: 0
Cross-cutting research and future directions under the GAPS networks† 全球行动计划网络下的横向研究和未来方向
Pub Date : 2024-04-16 DOI: 10.1039/D4VA00034J
Tom Harner, Amandeep Saini, Pourya Shahpoury, Anita Eng, Jasmin K. Schuster, Egide Kalisa and Jacob Mastin

The Global Atmospheric Passive Sampling (GAPS) network and GAPS Megacities network (GAPS-MC) are the only global-scale air monitoring programs for persistent organic pollutants (POPs), which support the Global Monitoring Plan (GMP) of the Stockholm Convention on POPs. The GAPS data represents all five United Nation regions and informs the spatial and temporal trends of listed POPs, their long-range transport in air, and new priorities for POPs monitoring and research. This information contributes to the Effectiveness Evaluation of the Stockholm Convention, which is assessed every six years. To ensure its long-term sustainability and relevance, the GAPS network is engaging in cross-cutting studies across fields of science and policy – leading to more holistic and integrative work on air pollution, health, climate science, and biodiversity. Future work under GAPS will continue to advance areas of intersection and tap-into topics and expertise in areas such as non-target analysis (chemical mixture approaches including transformation products in air), advanced data analysis and land-use assessment methods, top-down and inverse global modeling, global air health assessment/warning systems, and citizen science and outreach.

全球大气被动采样(GAPS)网络和全球大气被动采样大城市网络(GAPS-MC)是全球范围内唯一的持久性有机污染物(POPs)空气监测计划,为《关于持久性有机污染物的斯德哥尔摩公约》的全球监测计划(GMP)提供支持。全球空气监测计划的数据代表了联合国所有五个地区的数据,并为所列持久性有机污染物的空间和时间趋势、其在空气中的长程飘移以及持久性有机污染物监测和研究的新优先事项提供了信息。这些信息有助于每六年一次的《斯德哥尔摩公约》成效评估。为确保其长期可持续性和相关性,全球大气污染战略网络正在开展跨科学和政策领域的横向研究,从而在空气污染、健康、气候科学和生物多样性方面开展更加全面和综合的工作。GAPS 下的未来工作将继续推进交叉领域的工作,并挖掘非目标分析(化学混合物方法,包括空气中的转化产物)、高级数据分析和土地利用评估方法、自上而下和逆向全球建模、全球空气健康评估/预警系统以及公民科学和外联等领域的主题和专业知识。
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引用次数: 0
Fabrication of a novel palladium membrane sensor for its determination in environmental and biological samples 制作新型钯膜传感器以测定环境和生物样品中的钯含量
Pub Date : 2024-04-13 DOI: 10.1039/D4VA00056K
Adil O. S. Bahathiq, Ahmad O. Babalghith, Alaa S. Amin and Abdelrazek M. Askar

A novel sensitive, specific, and reversible optical sensor for the palladium(II) ion was created by impregnating an agarose membrane with 4-(2-amino-3-hydroxypyridine-4-ylazo)1,5-dimethyl-2-phenyl-1,2-dihydropyrazol-3-one (AHDDO). Spectrophotometric studies of complex formation between the AHDDO base ligand and Mn2+, Cd2+, Co2+ Hg2+, Zn2+, Cu2+, Pd2+, Sr2+, Al3+, Fe3+, Au3+, and Ag+ metal ions in an ethanolic solution indicated a substantially larger stability for the palladium ion complex. Therefore, the AHDDO was immobilized on a clear agarose film and used as a suitable ionophore for building a selective Pd2+ optical sensor. By combining the sensing membrane with Pd2+ ions at pH 5.75, a transparent color change from orange to violet was observed. On the immobilization of AHDDO, the effects of ionophore concentration, pH, temperature, stirring, and reaction time were investigated. A linear relationship was observed between the membrane absorbance at 633 nm and Pd2+ concentrations in a range from 15 to 225 ng mL−1 with detection (3σ) and quantification (10σ) limits of 4.25 and 14.25 ng mL−1, respectively. For the determination of Pd2+ ions, no significant interference from at least 400-fold excess concentrations of a number of possibly interfering ions was found. The sensor exhibits remarkable selectivity for Pd2+ ions and can be regenerated through exposure to 0.15 M HNO3. The sensor has been successfully used to find palladium in biological, soil, road, and water samples.

通过在琼脂糖膜上浸渍 4-(2-氨基-3-羟基吡啶-4-偶氮)1,5-二甲基-2-苯基-1,2-二氢吡唑-3-酮(AHDDO),制备了一种新型灵敏、特异和可逆的钯(II)离子光学传感器。分光光度法研究了 AHDDO 碱配体与 Mn2+、Cd2+、Co2+、Hg2+、Zn2+、Cu2+、Pd2+、Sr2+、Al3+、Fe3+、Au3+ 和 Ag+ 金属离子在乙醇溶液中形成的络合物,结果表明钯离子络合物具有更高的稳定性。因此,AHDDO 被固定在透明的琼脂糖薄膜上,并被用作构建选择性 Pd2+ 光学传感器的合适离子载体。在 pH 值为 5.75 时,将传感膜与 Pd2+ 离子结合,可观察到明显的橙色到紫色的颜色变化。研究了离子源浓度、pH 值、温度、搅拌和反应时间对固定 AHDDO 的影响。在 15-225 ng mL-1 的范围内,膜在 633 nm 处的吸光度与 Pd2+ 浓度之间呈线性关系,检测限(3σ)和定量限(10σ)分别为 4.25 和 14.25 ng mL-1。在测定 Pd2+ 离子时,没有发现浓度为 400 倍的多种可能的干扰离子的明显干扰。该传感器已成功用于生物、土壤、道路和水样中钯的检测。
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引用次数: 0
Microbially-mediated aerobic oxidation of trace element-bearing pyrite in neutral-pH sandstone aquifer sediments† 中性pH砂岩含水层沉积物中含微量元素黄铁矿的微生物介导好氧氧化作用
Pub Date : 2024-04-12 DOI: 10.1039/D3VA00399J
Lisa Haas, Matthew Ginder-Vogel, James J. Zambito, David Hart and Eric E. Roden

Pyrite (FeS2) is the most abundant sulfide mineral on Earth and represents a significant reservoir of iron and sulfur in modern and ancient sediments. Oxidation of pyrite in the terrestrial subsurface is commonly associated with lowering of groundwater pH and release of constituent trace elements to solution. Although the central role of microbial activity in pyrite oxidation is well understood in acid mine/rock drainage and other low-pH (e.g. pH < 2) environments, the role of microorganisms in mediating pyrite oxidation under circumneutral pH conditions is not well understood. Here we demonstrate the potential for aerobic microbial metabolism to promote circumneutral pH oxidation of trace element-bearing pyrite in Cambrian-age sandstones from Trempealeau County, WI (USA). Microbial activity accelerated ca. 2–5 fold the rate and extent of sulfate release (a direct measure of pyrite oxidation) from reduced pyrite-bearing sediments. pH values dropped to 3 in biotic microcosms which contained limited carbonate (dolomite) buffering capacity. The overall surface area-specific rate constant for pyrite oxidation inferred from batch reaction modeling of these microcosms (10−7.8 mol m−2 s−1) was ca. 25-fold higher than for the corresponding abiotic reactors (10−9.2 mol m−2 s−1). Calcium and magnesium were proportionally released to solution with sulfate as a result of carbonate and/or Ca-aluminosilicate dissolution by acid generated from pyrite oxidation. When the amount of acid from pyrite oxidation exceeded the system buffering capacity, metals were selectively released from the geological material. No significant release of trace metals took place in abiotic reactors, which showed much lower rates of pyrite oxidation. These findings suggest that groundwaters in contact with pyrite-containing geological formations contain microorganisms capable of accelerating the oxidation of native pyrite in those formations. Analysis of microbial community composition in the microcosms by 16S rRNA gene amplicon sequencing showed enrichment in organisms related to taxa associated with chemolithotrophic metabolism (Candidatus Tenderia electrophaga, Thioprofundum lithophicum, and Thiobacillus thioparus) from background levels (<2%) to up to 40% of total sequence reads. A reactive transport modeling exercise demonstrated how microbial acceleration of pyrite oxidation could have a crucial, near-term (<10 years) impact on pH decline and trace element release in response to influx of oxygenated groundwater into previously reduced geological strata. Our results have key implications for controls on the onset of low-pH conditions and associated changes in groundwater quality in drinking water wells located within pyrite-bearing geo

黄铁矿(FeS2)是地球上最丰富的硫化物矿物,是现代和远古沉积物中重要的铁和硫储层。黄铁矿在陆地地下的氧化通常与地下水 pH 值降低和向溶液释放微量元素有关。虽然微生物活动在黄铁矿氧化过程中的核心作用在酸性矿山/岩石排水和其他低 pH 值(如 pH 值为 2)环境中已得到很好的理解,但在中性 pH 值条件下,微生物介导黄铁矿氧化的潜力还没有得到很好的理解。在这里,我们展示了有氧微生物新陈代谢促进美国威斯康星州 Trempealeau 县寒武纪砂岩中含微量元素黄铁矿环中性 pH 氧化的潜力。微生物活动使含黄铁矿的还原沉积物中硫酸盐释放(黄铁矿氧化的直接测量指标)的速度和程度加快了约 5 倍。在含有有限碳酸盐(白云石)缓冲能力的微生态系统中,pH 值降至 3。黄铁矿氧化产生的酸溶解碳酸盐和/或钙铝硅酸盐后,钙和镁与硫酸盐一起按比例释放到溶液中。当黄铁矿氧化产生的酸量超过系统缓冲能力时,地质材料中的金属就会有选择性地释放出来。在非生物反应器中,痕量金属没有明显释放,黄铁矿氧化的速率要低得多。这些发现表明,与含黄铁矿地质构造接触的地下水中含有能够加速这些地质构造中原生黄铁矿氧化的微生物。一项反应迁移建模工作表明,微生物活动导致黄铁矿氧化率增加几倍,会对含氧地下水流入先前还原地质层的短期反应产生重大影响。我们的研究结果对控制含黄铁矿地质层内饮用水井的低 PH 值条件和相关地下水质量变化具有重要意义。
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引用次数: 0
2023 Outstanding Papers published in the Environmental Science journals of the Royal Society of Chemistry 在英国皇家化学学会《环境科学》期刊上发表 2023 篇优秀论文
Pub Date : 2024-04-09 DOI: 10.1039/D4VA90010C
Zongwei Cai, Neil Donahue, Graham Gagnon, Kevin C. Jones, Célia Manaia, Elsie Sunderland and Peter J. Vikesland

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引用次数: 0
期刊
Environmental science. Advances
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