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Occurrence of 80 per and polyfluorinated alkyl substances (PFAS) in muscle and liver tissues of marine mammals of the St. Lawrence Estuary and Gulf, Quebec, Canada 加拿大魁北克省圣劳伦斯河口和海湾海洋哺乳动物肌肉和肝脏组织中 80 全氟和多氟烷基物质 (PFAS) 的存在情况
Pub Date : 2024-07-04 DOI: 10.3389/fenvc.2024.1403728
N. K. Khalid, Maud Le Calvez, Mélanie Lemire, Q. Dinh, Justine Fontaine, Stéphane Lair, Sébastien Sauvé
Limited data are available for the occurrence of more recent per and polyfluorinated alkyl substances (PFAS) in marine mammals, especially from the St. Lawrence Estuary and Gulf. This study investigates the occurrence of PFAS in liver and muscle tissues of various marine mammals, including the harbor seal, gray seal, harp seal, hooded seal, harbor porpoise, white-sided dolphin, white-beaked dolphin, and True’s beaked whale. Among the 80 target PFAS (including PFCAs, PFSAs, Cyclic PFSA, FASAs/FASAAs, FTCAs/FTUCAs, FTSAs, Ether-PFAS, diPAPs, and ESI + ECF precursors) perfluorooctanoic sulfonate (PFOS) dominates in all the marine mammal species and several other long-chain PFCAs, such as PFNA, PFDA, PFUnA, PFTrDA, and PFHxDA, were detected at 100% frequency in both muscle and liver samples. PFDoA and 7:3 fluorotelomer carboxylic acid (7:3 acid) also showed a 100% detection frequency for liver samples. Harp seal tissues displayed notably low PFAS concentrations, with average total PFAS concentrations of 7 ng/g (ww: wet weight) in muscle and 44 ng/g (ww) in the liver. In contrast, the white-sided dolphin exhibited the highest average concentrations, reaching 39 ng/g (ww) in muscle and 334 ng/g (ww) in liver samples. The Pearson correlation analysis reveals a strong correlation between the concentration of PFOS, perfluoroalkyl carboxylic acids (PFCAs), and electrochemical fluorination (ECF) precursors. Species at the top of the marine food chain (harbor porpoise, white sided dolphin, and white beaked dolphin) presented the highest concentrations of PFAS, particularly PFOS and long-chain PFCAs, highlighting the need for an increased regulation of these persistent molecules in order to protect marine mammal’s health.
关于海洋哺乳动物,尤其是圣劳伦斯河口和海湾的海洋哺乳动物体内最近出现的全氟和多氟烷基物质(PFAS)的数据有限。本研究调查了各种海洋哺乳动物(包括港海豹、灰海豹、竖琴海豹、帽海豹、港湾鼠海豚、白边海豚、白喙海豚和真氏喙鲸)肝脏和肌肉组织中 PFAS 的含量。在 80 种目标 PFAS(包括 PFCAs、PFSAs、Cyclic PFSA、FASAs/FASAAs、FTCAs/FTUCAs、FTSAs、Ether-PFAS、diPAPs、全氟辛烷磺酸(PFOS)在所有海洋哺乳动物物种中均占主导地位,而其他几种长链全氟砷酸(PFNA、PFDA、PFUnA、PFTrDA 和 PFHxDA)在肌肉和肝脏样本中的检测频率均为 100%。肝脏样本中 PFDoA 和 7:3 氟代羧酸(7:3 酸)的检测频率也达到了 100%。竖琴海豹组织中的全氟辛烷磺酸浓度明显较低,肌肉中的全氟辛烷磺酸平均总浓度为 7 纳克/克(湿重),肝脏中的全氟辛烷磺酸平均总浓度为 44 纳克/克(湿重)。相比之下,白鳍豚的平均浓度最高,在肌肉和肝脏样本中分别达到 39 纳克/克(湿重)和 334 纳克/克(湿重)。Pearson 相关性分析表明,全氟辛烷磺酸、全氟烷基羧酸 (PFCAs) 和电化学氟化 (ECF) 前体的浓度之间存在很强的相关性。处于海洋食物链顶端的物种(港湾鼠海豚、白海豚和白喙海豚)体内的全氟辛烷磺酸浓度最高,尤其是全氟辛烷磺酸和长链全氟烷基羧酸,这表明有必要加强对这些持久性分子的监管,以保护海洋哺乳动物的健康。
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引用次数: 0
Method optimization for benchtop mass spectrometry imaging of lipids in Eisenia hortensis 优化台式质谱法对赤鳃藻脂质成像的方法
Pub Date : 2024-06-14 DOI: 10.3389/fenvc.2024.1334207
Kendra G. Selby, Claire E. Korte, Lauren H. Phan, Gabriel A. Bressendorff, Ashley R. Chirchirillo, K. R. Tucker
Matrix selection and application is a crucial step in obtaining meaningful results with matrix-assisted laser desorption/ionization (MALDI) mass spectrometry imaging (MSI). Most instruments have a large spatial, and data with adequate spatial resolution can frequently be obtained on a benchtop instrument. The matrix application workflow has been optimized for the imaging of the earthworm (Eisenia hortensis), after exposure to various statins, a class of blood lipid-lowering agents. Lipids are nonpolar, often neutral molecules, making them difficult to ionize, and heightening the need for matrix optimization. The matrices 2,5-dihydroxybenzoic acid (DHB), α-cyano-4-hydroxycinammic acid (CHCA), 1,5-diaminonaphthalene (DAN), and 3,5-dimethoxy-4-hydroxycinnamic acid (sinapinic acid; SA) were studied. Samples were also washed in the ammonium salts of acetate, bicarbonate, formate, sulfate, or water as a control to enhance ionization and improve spatial resolution. A successful matrix for MSI is one that demonstrates homogenous tissue coverage, ionization of the analytes of interest, and does not require excessive laser power for ionization. All matrices showed sufficient tissue coverage; however, CHCA yielded unambiguous images of cholesterol and yielded sufficient signal over the lipid mass range (400–1,000 m/z), indicating that it successfully ionized endogenous lipids. Following additional optimization, the application of 50 mL of 10 mg/mL CHCA following a 5 s salt ammonium sulfate salt wash proved most successful for improving lipid ionization and enhancing spatial resolution.
基质的选择和应用是基质辅助激光解吸/电离(MALDI)质谱成像(MSI)获得有意义结果的关键步骤。大多数仪器都具有较大的空间分辨率,而且通常可以在台式仪器上获得具有足够空间分辨率的数据。针对蚯蚓(Eisenia hortensis)暴露于各种他汀类药物(一类降血脂药物)后的成像,对矩阵应用工作流程进行了优化。脂质是非极性分子,通常是中性分子,因此难以离子化,更需要对基质进行优化。我们研究了 2,5-二羟基苯甲酸(DHB)、α-氰基-4-羟基肉桂酸(CHCA)、1,5-二氨基萘(DAN)和 3,5-二甲氧基-4-羟基肉桂酸(山奈酸;SA)等基质。作为对照,样品还在醋酸盐、碳酸氢盐、甲酸盐、硫酸盐或水的铵盐中进行了洗涤,以增强离子化并提高空间分辨率。用于 MSI 的成功基质应能显示均匀的组织覆盖范围、电离感兴趣的分析物,并且不需要过高的激光电离功率。所有基质都显示出足够的组织覆盖率;然而,CHCA 能产生明确的胆固醇图像,并在脂质质量范围(400-1,000 m/z)内产生足够的信号,表明它成功地电离了内源性脂质。经过进一步优化,在进行 5 秒的硫酸铵盐洗后,使用 50 毫升 10 毫克/毫升的 CHCA,在改善脂质离子化和提高空间分辨率方面证明是最成功的。
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引用次数: 0
Air non-thermal plasma, a green approach for the treatment of contaminated water: the case of sulfamethoxazole 空气非热等离子体--处理受污染水的绿色方法:磺胺甲噁唑案例
Pub Date : 2024-06-13 DOI: 10.3389/fenvc.2024.1416702
Agata Giardina, G. Lofrano, G. Libralato, A. Siciliano, E. Marotta, C. Paradisi
Non-thermal plasma (NTP) is gaining increasing attention as a promising approach for advanced water treatment to degrade persistent organic pollutants. Aqueous solutions of sulfamethoxazole (4-amino-N-(5-methylisoxazol-3-yl)-benzensulfonamide, SMZ), an antibiotic largely employed for humans and animals and a widespread persistent pollutant of waters and wastewaters, were subjected to air NTP treatment in a dielectric barrier discharge (DBD) reactor. The effects of SMZ initial concentration and of the solution pH on SMZ decomposition kinetics and transformation products were investigated. Efficient degradation was achieved, resulting in the complete removal of SMZ (10 μM initial concentration) in less than 25 min treatments, in the exhaustive mineralization (a result never reported before in plasma treatments and seldom reached also with other advanced oxidation processes) of all organic carbon in 6 h and in an energy efficiency of 6.4 g/kWh at 50% conversion. By means of HPLC-UV/Vis and LC-ESI-MSn analyses, a number of organic transformation products was identified along the path to SMZ mineralization, all present always in very small amounts and in turn decomposed at short treatment times. The effect of the solution pH on the genesis and decay of transformation products was also investigated. Based on comparisons with literature data and on previous findings obtained with the DBD reactor used in this work, it is concluded that the major reactive species involved in the degradation of SMZ are the hydroxyl radical and ozone. Finally, toxicological analyses of water initially containing 0.5 mM SMZ and subjected to 4 h NTP treatment showed that the by-products are not toxic to Raphidocelis subcapitata and Daphnia magna, while residual toxicity was detected by Aliivibrio fischeri.
非热等离子体(NTP)作为一种降解持久性有机污染物的先进水处理方法,正受到越来越多的关注。磺胺甲噁唑(4-氨基-N-(5-甲基异恶唑-3-基)-苯磺酰胺,SMZ)是一种主要用于人类和动物的抗生素,也是一种广泛存在于水体和废水中的持久性污染物。研究了 SMZ 初始浓度和溶液 pH 值对 SMZ 分解动力学和转化产物的影响。在不到 25 分钟的处理过程中,SMZ(初始浓度为 10 μM)被完全去除,所有有机碳在 6 小时内被完全矿化(这是等离子体处理过程中从未报道过的结果,其他高级氧化过程也很少达到这一结果),50% 转化时的能效为 6.4 g/kWh。通过 HPLC-UV/Vis 和 LC-ESI-MSn 分析,在 SMZ 矿化过程中发现了许多有机转化产物,它们的含量都很低,并且在很短的处理时间内就会被分解。此外,还研究了溶液 pH 值对转化产物的生成和分解的影响。根据与文献数据的比较以及之前使用 DBD 反应器得出的结论,参与 SMZ 降解的主要反应物是羟基自由基和臭氧。最后,对最初含有 0.5 毫摩尔 SMZ 并经过 4 小时 NTP 处理的水进行的毒理学分析表明,副产品对 Raphidocelis subcapitata 和 Daphnia magna 没有毒性,而对 Aliivibrio fischeri 有残留毒性。
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引用次数: 0
A review of per- and polyfluoroalkyl substances in biosolids: geographical distribution and regulations 审查生物固体中的全氟和多氟烷基物质:地理分布和法规
Pub Date : 2024-06-13 DOI: 10.3389/fenvc.2024.1383185
T. Saliu, Sébastien Sauvé
Applying sewage sludge and biosolids to agricultural lands has become an increasingly essential aspect of sustainable waste management and circular economy as it contributes positively to nutrient recycling, soil fertility and environmental health. Due to the widespread presence of per and poly-fluoroalkyl substances (PFAS) globally, wastewater treatment plants have become a sink for PFAS. PFAS resist degradation by conventional wastewater treatment processes and are usually adsorbed to sewage sludge and biosolids. However, there have been significant concerns that land application of sewage sludge and biosolids could become a probable pathway for PFAS to enter the food chain. This article assessed the global sewage sludge/biosolids generation and country-to-country management methods through a systematic review. The global occurrence, distribution and prevalence of different classes of PFAS were assessed. We also evaluate the factors influencing PFAS contamination in sewage sludge/biosolids and the existing regulations on the upper limit of PFAS in biosolids before their disposal or application to farmland (or other usages). Additionally, most reports revealed high PFAS concentrations in influent, effluent, sewage sludge and biosolids generated worldwide. Overall, recorded PFAS concentration on a global scale varied from 2.2 to 2,156 ng/L (influents), 1.9–4,800 ng/L (effluents) and 2.1–500,000 ng/g (biosolids). While most studies focused on legacy PFAS detection, recent studies have revealed the prevalence of diPAPs in high concentrations in sewage sludge and biosolids, contributing from 40% to 95% of the total PFAS concentration. Across all PFAS classes, PFAAs and diPAPs were the dominant groups exhibiting elevated detection rates (35%–95%). Due to documented PFAS contamination in agricultural lands, rigorous regulations need to be instituted to govern the application of these biowastes on agricultural lands. However, several countries lack data on the level of PFAS in the sewage sludges they generate, and there are currently few or no regulations guiding their application to farmlands. Notably, the diPAPs class of PFAS was shown to be present in biosolids and sewage sludge; their inclusion in the list of PFAS required in standardized analytical methods and risk assessment becomes imperative.
将污水污泥和生物固体应用于农业用地已日益成为可持续废物管理和循环经济的一个重要方面,因为这对养分循环、土壤肥力和环境健康都有积极的促进作用。由于全氟烷基和多氟烷基物质(PFAS)在全球广泛存在,污水处理厂已成为全氟烷基和多氟烷基物质的汇集地。传统的废水处理工艺无法降解 PFAS,通常会将其吸附在污水污泥和生物固体中。然而,污水污泥和生物固体的土地应用可能成为 PFAS 进入食物链的可能途径,这引起了人们的极大关注。本文通过系统回顾评估了全球污水污泥/生物固体的产生情况和各国的管理方法。评估了不同类别的 PFAS 在全球的发生、分布和流行情况。我们还评估了影响污水污泥/生物固体中 PFAS 污染的因素,以及在处置生物固体或将其用于农田(或其他用途)之前,有关生物固体中 PFAS 上限的现行法规。此外,大多数报告显示,世界各地产生的进水、出水、污水污泥和生物固体中的 PFAS 浓度都很高。总体而言,全球范围内记录的 PFAS 浓度分别为 2.2-2,156 纳克/升(进水)、1.9-4,800 纳克/升(出水)和 2.1-500,000 纳克/克(生物固体)。虽然大多数研究都侧重于检测遗留的全氟辛烷磺酸,但最近的研究显示,污水污泥和生物固体中普遍存在高浓度的二全氟辛烷磺酸,占全氟辛烷磺酸总浓度的 40% 至 95%。在所有 PFAS 类别中,PFAAs 和 diPAPs 是检出率较高的主要类别(35%-95%)。由于农田中存在有据可查的 PFAS 污染,因此需要制定严格的法规来管理这些生物废料在农田中的应用。然而,一些国家缺乏有关其产生的污水淤泥中 PFAS 含量的数据,目前也很少或根本没有指导其在农田中应用的法规。值得注意的是,diPAPs 类 PFAS 已被证明存在于生物固体和污水污泥中;将其纳入标准化分析方法和风险评估所需的 PFAS 清单已势在必行。
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引用次数: 0
Performance of pitcher-type POU filters for the removal of 75 PFAS from drinking water: comparing different water sources 壶式 POU 过滤器去除饮用水中 75 种全氟辛烷磺酸的性能:不同水源的比较
Pub Date : 2024-06-04 DOI: 10.3389/fenvc.2024.1376079
Termeh Teymoorian, Q. Dinh, Benoit Barbeau, Sébastien Sauvé
This study presents a comprehensive assessment of the performance of popular pitcher-type point-of-use (POU) water filters to remove PFAS contaminants from tap waters. The evaluated filters, Brita (Elite and Standard), ZeroWater, Aquagear, and ClearlyFiltered, were tested for their efficacy in removing 75 targeted PFAS, total organic carbon (TOC), total dissolved solids (TDS), chloride, and sulfate from two Canadian tap waters with background Σ75 PFAS concentrations of 13 and 56 ng/L. Overall, the performances of the filters varied depending on the structure of the filter media, the water source, and the specific contaminants present. ZeroWater was the top performer in the case of total PFAS removal. The volume-weighted average removal of total PFAS after 160 L of filtration using Saint-Donat tap water was 99% for ZeroWater, 99% for ClearlyFiltered, 77% for Aquagear, and 20% for Brita (Elite). In the case of Montreal tap water, which had different water characteristics and lower total PFAS levels, the volume-weighted average removal for PFAS was ≈100% for ZeroWater, 96% for ClearlyFiltered, 60% for Aquagear, 48% for Brita (Elite), and 38% for Brita (Standard). Both laboratory and home tests involving ZeroWater filters yielded similar high-performance results using Montreal tap water. Although ZeroWater exhibited high PFAS removal (99%) in Saint-Donat water, TDS and TOC desorption and a significant drop in pH were observed after 80 L, a phenomenon which was explained by the higher total concentration of anions in this water. In contrast, no desorption was observed in Montreal tap water for TDS and TOC due to the lower concentrations of anions. The Aquagear filter demonstrated an unusual increase in concentrations of sulfate after the initial 20 L, which needs further evaluation. This study discusses individual filter performance, the influence of tap water characteristics, and the potential to meet the new NSF guidelines, which provides valuable insights for consumers seeking to choose an appropriate easy-to-use water filtration system to ensure safe and clean drinking water in different regions.
本研究全面评估了流行的投壶式使用点(POU)滤水器去除自来水中 PFAS 污染物的性能。对接受评估的滤水器(Brita(精英型和标准型)、ZeroWater、Aquagear 和 ClearlyFiltered)进行了测试,以了解它们在去除加拿大两种自来水中 75 种目标 PFAS、总有机碳 (TOC)、总溶解固体 (TDS)、氯化物和硫酸盐方面的功效,这两种自来水的 PFAS Σ75 背景浓度分别为 13 纳克/升和 56 纳克/升。总体而言,过滤器的性能因过滤介质的结构、水源和存在的特定污染物而异。在去除全氟辛烷磺酸总量方面,ZeroWater 表现最佳。使用 Saint-Donat 自来水过滤 160 升后,ZeroWater 对总 PFAS 的体积加权平均去除率为 99%,ClearlyFiltered 为 99%,Aquagear 为 77%,Brita(Elite)为 20%。蒙特利尔的自来水具有不同的水质特征,PFAS 总含量较低,在这种情况下,零水公司对 PFAS 的体积加权平均去除率≈100%,ClearlyFiltered 为 96%,Aquagear 为 60%,Brita(精英型)为 48%,Brita(标准型)为 38%。在使用蒙特利尔自来水进行的实验室和家庭测试中,零度水过滤器都取得了类似的高性能结果。尽管零水公司在圣多纳特(Saint-Donat)自来水中对 PFAS 的去除率很高(99%),但在 80 升水后发现 TDS 和 TOC 被解吸,pH 值显著下降,这种现象的原因是这种水中的阴离子总浓度较高。相比之下,蒙特利尔自来水中的 TDS 和 TOC 由于阴离子浓度较低而未出现解吸现象。Aquagear 过滤器显示,在最初的 20 升水之后,硫酸盐的浓度异常增加,这需要进一步评估。这项研究讨论了单个过滤器的性能、自来水特性的影响以及满足新的美国国家卫生基金会准则的潜力,为消费者选择合适的易用型水过滤系统以确保不同地区安全清洁的饮用水提供了有价值的见解。
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引用次数: 0
Erratum: Study on the degradation and metabolic mechanism of four quinolone antibiotics by mixed strains 勘误:混合菌株对四种喹诺酮类抗生素的降解及代谢机制研究
Pub Date : 2024-05-07 DOI: 10.3389/fenvc.2024.1425407
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引用次数: 0
Erratum: State-of-the-art multimodal scanning hard X-ray imaging and tomography sheds light at multiple length-scales on biomineralization related processes 勘误:最先进的多模态扫描硬 X 射线成像和断层扫描技术在多个长度尺度上揭示了生物矿化的相关过程
Pub Date : 2024-05-07 DOI: 10.3389/fenvc.2024.1425379
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引用次数: 0
Editorial: Advanced characterization of dissolved organic matter in natural aquatic environments and water/wastewater treatment processes 编辑:自然水生环境和水/废水处理过程中溶解有机物的高级表征
Pub Date : 2024-04-11 DOI: 10.3389/fenvc.2024.1399083
Kang Xiao, Yingxun Du, Xing Zheng, Qing Ding
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引用次数: 0
Editorial: Women in environmental chemistry 社论:环境化学领域的女性
Pub Date : 2024-04-05 DOI: 10.3389/fenvc.2024.1403643
E. Bontempi, C. M. R. Almeida, C. Futalan, Varsha Srivastava
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引用次数: 0
Photocatalytic degradation of naproxen using TiO2 single nanotubes 利用 TiO2 单纳米管光催化降解萘普生
Pub Date : 2024-03-13 DOI: 10.3389/fenvc.2024.1373320
Marcela Sepúlveda, Joanna Musiał, Ivan Saldan, P. K. Chennam, J. Rodríguez-Pereira, H. Sopha, Beata J. Stanisz, J. Macák
Herein, TiO2 single-tube (TiO2 ST-NT) powders with and without magnetite Fe3O4 nanoparticles (TiO2 ST-NT@Fe3O4NPs) are presented for the first time as excellent photocatalysts for the degradation of one of the most popular non-steroidal anti-inflammatory drugs (NSAIDs), naproxen (NPX). The TiO2 ST-NT powders were synthesized by anodization followed by etching of the double wall, bending, sonication, ultra-centrifugation, and finally annealing at 600°C. A part of the obtained TiO2 ST-NT powders was decorated with Fe3O4 nanoparticles using a simple one-step decoration process. The best photocatalytic performance of TiO2 ST-NT and TiO2 ST-NT@Fe3O4NPs powders was obtained under the white light (6.2 × 10−4 s-1) and the blue light (2.7 × 10−4 s-1), respectively. During NPX photodegradation using TiO2 ST-NT powders, three main NPX transformation products (P1, P2, and P3) were detected. Upon excitation with the blue light illumination, TiO2 ST-NT@ Fe3O4NPs powders exhibited higher performance (∼80%) than TiO2 ST-NT powders (∼23%) within 1 h, resulting in an approximately three times increased photocatalytic rate constant. Moreover, under simulated sunlight conditions, TiO2 ST-NT powders demonstrated remarkable activity, achieving a 94% NPX degradation within 1 h. TiO2 ST-NT and TiO2 ST-NT@Fe3O4NPs powders represent excellent photocatalysts for NPX degradation.
本文首次提出了含有或不含磁铁矿 Fe3O4 纳米颗粒的 TiO2 单管(TiO2 ST-NT)粉末(TiO2 ST-NT@Fe3O4NPs ),作为降解最常用的非甾体抗炎药(NSAID)之一--萘普生(NPX)的优良光催化剂。TiO2 ST-NT 粉末是通过阳极氧化法合成的,然后进行双壁蚀刻、弯曲、超声、超速离心,最后在 600°C 下退火。采用简单的一步装饰工艺,在获得的部分 TiO2 ST-NT 粉末上装饰了 Fe3O4 纳米粒子。TiO2 ST-NT 和 TiO2 ST-NT@Fe3O4NPs 粉末分别在白光(6.2 × 10-4 s-1)和蓝光(2.7 × 10-4 s-1)下获得了最佳光催化性能。在使用 TiO2 ST-NT 粉末进行 NPX 光降解的过程中,检测到了三种主要的 NPX 转化产物(P1、P2 和 P3)。在蓝光照射下,TiO2 ST-NT@ Fe3O4NPs 粉末在 1 小时内的光催化性能(∼80%)高于 TiO2 ST-NT 粉末(∼23%),光催化速率常数提高了约三倍。TiO2 ST-NT 和 TiO2 ST-NT@Fe3O4NPs 粉末是降解 NPX 的优良光催化剂。
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引用次数: 0
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Frontiers in environmental chemistry
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