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Unraveling the adsorption mechanisms of greenhouse gases on microporous MAF-4 nanoparticles using a statistical physics approach 利用统计物理方法揭示温室气体在微孔MAF-4纳米颗粒上的吸附机制。
IF 4.4 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2026-01-09 DOI: 10.1016/j.jconhyd.2026.104850
E.A. Elghmaz , Ghada M. Alnafesah , Mohammed Alissa , Khalil ur Rehman , Abdullah Alghamdi , Suad A. Alghamdi , Abdulkarim S. Binshaya , Ghfren S. Aloraini , Amira K. Hajri , Adil Abalkhail
The continuing struggle to reduce greenhouse gas emissions continues to be one of the most crucial obstacles in achieving both energy efficiency and sustainable, long-term environmental practices. Microporous metal azolate framework-4 nanoparticles (MAF-4 NPs) have emerged as attractive adsorbent materials with their large surface area, adjustable pore architecture, and high chemical stability. Herein we present a green and rapid synthesis of ultramicroporous MAF-4 nanoparticles via the production of no organic solvents through the use of minimal external heating. The resulting MAF-4 NPs (particle size ≥70 nm) have been characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and nitrogen physisorption analysis and demonstrate a high BET surface area of 1796 m3/g, a total pore volume of 0.75 cm3/g, and ultramicropores predominantly occurring at an average pore diameter of 0.62 nm. A number of gas adsorption behaviors have been experimentally evaluated for four different gases (CO2, SF6, CH4, and N2) and are subsequently explained using a multilayer adsorption model based on statistical physics that has recently been developed for porous metal-organic frameworks. This combination of theoretical and experimental information provides a greater understanding of how adsorption occurs within porous metal-organic frameworks. The results indicate that gas molecules (at low temperatures) are unaligned, but at higher temperatures they have primarily parallel arrangements and are able to form many layers (multilayer arrangements). The average number of adsorbed gas molecules on an active site range from 0.51 to 1.92 for each different type of gas and temperature combination, and the total number of layers varies from 1.2 to 8.0. Energy of adsorption indicates strong attractive forces for the initial layer of adsorbing molecules and a decrease in attraction for subsequent layers of adsorbing molecules, with values between 2.64 and 8.42 kJ/mol indicating the adsorptive forces are due to physisorption with significant contributions from van der Waals and London dispersion forces. Using thermodynamic evaluations of internal energy and Gibbs' free energy to estimate the spontaneity and exothermicity of the adsorption process shows that at low temperatures there is more disorder among the molecules (higher entropy) than at higher temperatures when the number of adsorbate molecules reaches saturation. This indicates that MAF-4 nanoparticles will be energy-efficient, selective, and regenerable when used for CO2 and SF6 capture and have significant capability for scale-up and increased capacity of these adsorbates.
减少温室气体排放的持续努力仍然是实现能源效率和可持续、长期环境实践的最关键障碍之一。微孔金属偶氮酸盐框架-4纳米颗粒(MAF-4 NPs)因其大表面积、可调节的孔隙结构和高化学稳定性而成为一种有吸引力的吸附材料。在这里,我们提出了一种绿色和快速合成超微孔MAF-4纳米颗粒的方法,通过使用最小的外部加热来生产无有机溶剂。通过x射线衍射(XRD)、扫描电镜(SEM)和氮物理吸附分析对制备的MAF-4 NPs(粒径≥70 nm)进行了表征,发现其BET比表面积高达1796 m3/g,总孔容为0.75 cm3/g,超微孔主要分布在平均孔径为0.62 nm处。通过实验评估了四种不同气体(CO2, SF6, CH4和N2)的许多气体吸附行为,并随后使用基于统计物理的多层吸附模型进行了解释,该模型最近已开发用于多孔金属有机框架。这种理论和实验信息的结合提供了对多孔金属有机框架内吸附如何发生的更好理解。结果表明,气体分子(在低温下)是不排列的,但在较高的温度下,它们主要是平行排列,并且能够形成许多层(多层排列)。对于不同类型的气体和温度组合,活性位点的平均吸附气体分子数在0.51 ~ 1.92之间,总层数在1.2 ~ 8.0之间。吸附能表明吸附分子的初始层具有较强的吸引力,随后的吸附分子层具有较弱的吸引力,其值在2.64 ~ 8.42 kJ/mol之间,表明吸附力是由物理吸附引起的,范德华力和伦敦色散力对吸附力的贡献很大。利用热力学热力学的内能和吉布斯自由能来估计吸附过程的自发性和放热性,结果表明,当吸附质分子数量达到饱和时,在低温下分子间的无序性更强(熵更高)。这表明MAF-4纳米颗粒在捕获二氧化碳和SF6时具有节能、选择性和可再生性,并且具有显著的扩大和增加这些吸附剂容量的能力。
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引用次数: 0
Long term rebound and transport of perfluorinated sulfonic acids (PFSAs) in the vadose zone following flushing 冲洗后全氟磺酸(PFSAs)在渗透区的长期反弹和运输。
IF 4.4 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2026-01-08 DOI: 10.1016/j.jconhyd.2026.104848
Charles E. Schaefer , Graig M. Lavorgna , David R. Lippincott , Shilai Hao , J. Conrad Pritchard , Christopher P. Higgins
Increases in perfluorinated sulfonic acid (PFSA) porewater concentrations over a 35 month duration following in situ flushing were monitored at an aqueous film-forming foam (AFFF) site using porous cup suction lysimeters within a highly instrumented test cell. Results provided evidence that perfluorooctane sulfonate (PFOS) slow desorption kinetics contributed to slow contaminant rebound in measured porewater concentrations. PFSAs in the shallow (0.23 m depth) highly PFSA-impacted soils migrated downward during the monitored post-flushing period, with short-chained PFSAs migrating more rapidly in porewater than long-chained PFSAs. Following flushing, apparent equilibrium porewater concentrations at a depth of 0.61 m below ground surface were attained within two months for perfluoropentane sulfonate (PFPeS), between 2 and 20 months for perfluorohexane sulfonate (PFHxS), and 25 months for PFOS. For PFPeS and PFHxS, apparent steady-state rebound concentrations (to 38% of their pre-flushing baseline levels, with no increasing or decreasing trend over time subsequently observed) were reasonably predicted based on an equilibrium model. PFOS rebound and ultimately vertical migration were highly impacted by non-equilibrium soil desorption. Excavation of elevated PFSAs in surface soils had no impact on PFSA porewater concentrations 0.38 m below the excavation over a 1.2 year post-excavation monitoring period. Together, these long-term rebound data highlight the potential importance of mass transfer-controlled processes for PFOS leaching, and suggest that removal of elevated PFSAs in surface soils may take years until PFSA discharges to groundwater are diminished.
在原位冲洗后的35个月内,在水成膜泡沫(AFFF)现场,使用高度仪器化的测试池内的多孔杯吸溶析仪监测了全氟磺酸(PFSA)孔隙水浓度的增加。结果提供了证据,证明全氟辛烷磺酸(PFOS)缓慢的解吸动力学有助于在测量的孔隙水浓度中缓慢的污染物反弹。在监测的冲洗后阶段,受pfsa影响较大的浅层(0.23 m深度)土壤中的pfsa向下迁移,短链pfsa在孔隙水中的迁移速度快于长链pfsa。冲洗后,全氟戊烷磺酸(pfpe)在2个月内达到地表以下0.61 m深度的表观平衡孔隙水浓度,全氟己烷磺酸(PFHxS)在2至20个月内达到,全氟辛烷磺酸在25个月内达到。对于PFPeS和PFHxS,基于平衡模型合理地预测了表观稳态反弹浓度(达到冲洗前基线水平的38%,随后观察到没有随时间增加或减少的趋势)。非平衡土壤解吸对全氟辛烷磺酸的回弹和最终的垂直迁移影响很大。在开挖后1.2年的监测期内,地表土壤中PFSA升高的开挖对开挖下方0.38 m的PFSA孔隙水浓度没有影响。总之,这些长期反弹数据强调了质量传递控制过程对全氟辛烷磺酸浸出的潜在重要性,并表明去除表层土壤中升高的全氟辛烷磺酸可能需要数年时间,直到向地下水排放的全氟辛烷磺酸减少。
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引用次数: 0
Anthropogenically-induced saline wetland recharge drives denitrification: Implications for nitrate attenuation in semi-arid aquifer–wetland systems 人为诱导的含盐湿地补给驱动反硝化:半干旱含水层-湿地系统中硝酸盐衰减的含义。
IF 4.4 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2026-01-08 DOI: 10.1016/j.jconhyd.2026.104840
D. Sanz , D. Salcedo , B. Toledo , I. Dountcheva , R. Margalef-Martí , N. Otero , A. Soler , J.J. Gómez-Alday
Saline wetlands are highly sensitive to anthropogenic pressures, particularly in semi-arid regions where groundwater abstraction, land use changes, and climate variability modify their hydrogeological functioning. This study focuses on the Tirez and Peñahueca hypersaline wetlands (Central Spain), which have undergone a shift from natural groundwater discharge zones to induced recharge areas due to intensive irrigation. Declining piezometric levels have reversed the hydraulic gradient between the aquifer and the wetlands, resulting in recharge conditions. A multidisciplinary approach combining hydrochemistry, (including historical monitoring data), multi-isotopic characterization (N, O, C, S), and geophysical (ERT) techniques was applied to assess groundwater quality evolution and nitrate attenuation processes. Results show a significant increase in groundwater salinity and nitrate concentrations over the past five decades, with NO₃ levels reaching up to 245 mg/L. Average nitrate concentrations increased from ∼25 mg/L in the 1990s to over 200 mg/L in 2019–2021. Isotopic signatures indicate multiple nitrate sources, including manure, organic soil nitrogen, and synthetic fertilizers. A coupled increase of δ15N–NO₃ values ranging from +5.1 ‰ to +44 ‰ and δ18O–NO₃ from +3 ‰ to +23 ‰, along with δ34S–SO₄2− values between +16 ‰ and + 18 ‰ and δ13C–DIC from −12 ‰ to −4 ‰, suggest that heterotrophic denitrification is the main attenuation process. Electrical resistivity profiles reveal density-driven flow from the saline wetland water into the underlying aquifer, facilitating the transport of dissolved organic carbon and creating redox gradients favorable for denitrification. Maximum denitrification rates of up to 73% were estimated using literature isotopic fractionation values. Understanding the coupled hydrological and biogeochemical dynamics of saline wetland–aquifer systems is essential for developing sustainable groundwater management strategies in vulnerable arid and semi-arid regions.
盐渍湿地对人为压力高度敏感,特别是在地下水开采、土地利用变化和气候变率改变其水文地质功能的半干旱地区。本研究的重点是泰雷兹和Peñahueca高盐湿地(西班牙中部),由于集约化灌溉,这些湿地经历了从天然地下水排放区到诱导补给区的转变。压力水平的下降逆转了含水层和湿地之间的水力梯度,导致了补给条件。采用多学科方法,结合水化学(包括历史监测数据)、多同位素表征(N、O、C、S)和地球物理(ERT)技术,评估地下水质量演变和硝酸盐衰减过程。结果表明,在过去的50年里,地下水的盐度和硝酸盐浓度显著增加,NO₃-的水平达到了245毫克/升。平均硝酸盐浓度从20世纪90年代的~ 25 mg/L增加到2019-2021年的200 mg/L以上。同位素特征表明硝酸盐有多种来源,包括粪肥、有机土壤氮和合成肥料。δ15N-NO₃-从+5.1‰增加到+44‰,δ18O-NO₃-从+3‰增加到+23‰,δ34S-SO₄2-从+16‰增加到+ 18‰,δ13C-DIC从-12‰增加到-4‰,表明异养反硝化作用是主要的衰减过程。电阻率曲线揭示了从含盐湿地水进入下伏含水层的密度驱动流,促进了溶解有机碳的运输,并形成有利于反硝化的氧化还原梯度。利用文献同位素分馏值估计最大反硝化率可达73%。了解盐渍湿地-含水层系统的水文和生物地球化学耦合动力学对于制定脆弱干旱和半干旱地区可持续地下水管理战略至关重要。
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引用次数: 0
Identification of time-varying contaminant discharge rates using a data-driven Transformer model 使用数据驱动的变压器模型识别时变污染物排放率。
IF 4.4 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2026-01-07 DOI: 10.1016/j.jconhyd.2026.104847
Yaning Xu , Wenxi Lu , Liuzhi Zhu , Qingchun Yang
The identification of groundwater contamination sources (IGCS) is a critical prerequisite for the development of contamination remediation strategies and is vital for safeguarding groundwater resources. However, the recurrent neural networks (RNNs) previously applied to address IGCS have limitations due to their requirement for stepwise processing of data and inability to handle parallel processing, which restrict both accuracy and efficiency. This study applies the Transformer model to directly identify groundwater contamination source characteristics. The self-attention mechanism of the Transformer model effectively captures long-range dependencies in input data, overcoming the limitations of step-by-step data processing and supporting parallel processing of sequential information. This advantage allows the Transformer model to capture the dynamic changes in contamination source characteristics (e.g., contaminant discharge rates) across different time steps, resulting in more accurate IGCS. A hypothetical case study is conducted to compare the performance of data-driven methods (Transformer and MLP inverse mapping models) with surrogate-assisted physics-based methods (optimization and data assimilation methods), for identifying contamination source characteristics. The results indicate that the Transformer model performs better in terms of identification accuracy. The data assimilation method provides satisfactory results with a lower computational burden, making it more suitable for scenarios with strict time requirements. The optimization method requires more computational time and produces less accurate identification results compared to the other three methods.
地下水污染源的识别是制定污染修复策略的重要前提,对地下水资源的保护至关重要。然而,以往应用于IGCS的递归神经网络(RNNs)由于需要逐步处理数据和无法处理并行处理而存在局限性,从而限制了准确性和效率。本研究采用Transformer模型直接识别地下水污染源特征。Transformer模型的自关注机制有效地捕获输入数据中的远程依赖关系,克服了分步数据处理的限制,并支持顺序信息的并行处理。这一优势使Transformer模型能够捕获污染源特性(例如污染物排放率)在不同时间步长的动态变化,从而获得更准确的IGCS。通过一个假设的案例研究,比较了数据驱动方法(Transformer和MLP逆映射模型)与基于代理的辅助物理方法(优化和数据同化方法)在识别污染源特征方面的性能。结果表明,Transformer模型具有较好的识别精度。数据同化方法计算量小,结果令人满意,更适用于对时间要求严格的场景。与其他三种方法相比,优化方法需要更多的计算时间,并且产生的识别结果精度较低。
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引用次数: 0
Laboratory modeling of microbial and chemical clay minerals transformations of upper aquifer soils under intensive technogenic impact 在密集的技术影响下上含水层土壤微生物和化学粘土矿物转化的实验室模拟
IF 4.4 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2026-01-06 DOI: 10.1016/j.jconhyd.2026.104845
Grigory Artemiev , Nadezhda Popova , Alexey Averin , Anatoly Boguslavsky , Ivan Morozov , Olga Zakusina , Victoria Krupskaya , Alexey Safonov
Storage of nitrogen‑sulfuric acid waste from uranium ore mining and processing enterprises in sludge ponds leads to groundwater contamination by soluble components with degradation of impervious barriers. This results in a significant alteration of the geochemical environment and the mineral composition of rocks, as well as creates risks of soluble toxic components from waste entering water intakes and open hydrographic networks. Laboratory modeling of biofouling processes and subsequent alterations in soil composition from upper aquifer adjacent to the sludge repository of the Angarsk Electrolysis Chemical Plant (Angarsk, Russia) was conducted in this study. The investigation established that anthropogenic impacts resulting from elevated concentrations of nitrates, sulfates, ammonium, and bicarbonates significantly modify both the mineralogical and microbial composition of soils, consequently influencing their biogeochemical transformation characteristics. Under technogenic pollution conditions, microbial processes promote the development of more densely structured biofilms while simultaneously impeding iron reduction processes that normally facilitate more profound mineralogical alterations. The transformation of clay mineral composition plays a pivotal role in biofouling dynamics and governs subsequent mineral modification pathways. Microbial-mediated processes can induce structural reorganization of smectite minerals into tobelite-like configurations through two principal mechanisms: biologically facilitated iron dissolution and ammonium saturation of interlayer spaces resulting from dissimilatory nitrate reduction and subsequent ammonification processes.
铀矿开采和加工企业的氮硫酸废弃物在污泥池中储存,导致地下水被可溶性组分污染,不透水屏障降解。这导致地球化学环境和岩石矿物组成发生重大变化,并造成废物的可溶性有毒成分进入取水口和开放的水文网络的风险。本研究对安加尔斯克电解化工厂(俄罗斯安加尔斯克)污泥库附近上层含水层的生物污染过程和随后土壤成分的变化进行了实验室模拟。研究表明,由硝酸盐、硫酸盐、铵和碳酸氢盐浓度升高引起的人为影响显著改变了土壤的矿物学和微生物组成,从而影响了其生物地球化学转化特征。在技术污染条件下,微生物过程促进了结构更密集的生物膜的发展,同时阻碍了铁还原过程,而铁还原过程通常会促进更深刻的矿物学变化。粘土矿物组成的转变在生物污染动力学中起着关键作用,并支配着随后的矿物改性途径。微生物介导的过程可以通过两种主要机制诱导蒙脱石矿物的结构重组:生物促进的铁溶解和由异化硝酸还原和随后的氨化过程引起的层间空间的铵饱和。
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引用次数: 0
Vegetation type dominates slope-scale material loss under extreme rainfall: Nonlinear responses revealed by machine learning 极端降雨下植被类型主导坡面尺度物质损失:机器学习揭示的非线性响应
IF 4.4 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2026-01-06 DOI: 10.1016/j.jconhyd.2026.104846
Aipu Wu , Chunzi Ma , Shouliang Huo , Tianxiao Li , Qiang Fu
Extreme rainfall events may be intensified by climate change. These events pose significant threats to slope-scale soil erosion and non-point source (NPS) pollution in mountainous agricultural watersheds. In this study, seven years (2014–2020) of field observations from four runoff plots with different vegetation (farmland vs. shrubland) and slope types (steep vs. gentle) within the Miyun Reservoir watershed, northern China, were used to investigate material losses under contrasting rainfall patterns. Losses of soil, total nitrogen (TN), and total phosphorus (TP), along with runoff and chemical oxygen demand (COD), were quantified using a novel machine learning framework that integrated a Random Forest (RF) model with Sequential Backward Selection (SBS) and relative importance (RI) analyses. A total of 61 runoff-generating rainfall events, that included 10 rainfall events classified as extreme on the basis of the rainfall depth and 30-min maximum intensity (I30), were analyzed. Extreme rainfall accounted for only 16.4 % of the runoff events but contributed to 41.9 % in soil loss and 49.2 % in COD. Farmland was particularly vulnerable, and it had 2–5 times the losses of shrubland under extreme rainfall events. The vegetation type and 60-min rainfall intensity (I60) emerged as dominant factors that controlled losses under extreme rainfall events, while vegetation type and rainfall intensity governed material losses under normal rainfall events. A partial dependence plot (PDP) analysis revealed a nonlinear response of the material loss to I30, with sharp increases between 30 and 40 mm·h−1. This result indicated critical material loss thresholds. These results revealed the dominant role of the vegetation type in controlling material loss at the slope scale and confirmed the potential of machine learning to explain complex hydrological processes.
极端降雨事件可能因气候变化而加剧。这些事件对山地农业流域的坡面土壤侵蚀和非点源污染构成了重大威胁。本研究通过对密云水库流域4个不同植被(农田与灌丛)和坡型(陡坡与平缓坡)的径流样地7年(2014-2020年)的野外观测,研究了不同降雨模式下的物质损失。利用一种新的机器学习框架,将随机森林(RF)模型与顺序向后选择(SBS)和相对重要性(RI)分析相结合,对土壤、总氮(TN)和总磷(TP)以及径流和化学需氧量(COD)的损失进行了量化。共对61次产流降雨事件进行了分析,其中根据降雨深度和30 min最大强度(I30)划分为极端降雨事件的有10次。极端降雨仅占径流事件的16.4%,但对土壤流失量和COD的贡献率分别为41.9%和49.2%。农田尤其脆弱,在极端降雨事件下,其损失是灌木地的2-5倍。植被类型和60 min降雨强度(I60)是控制极端降雨事件下物质损失的主导因素,而植被类型和降雨强度是控制正常降雨事件下物质损失的主导因素。偏相关图(PDP)分析显示,I30对材料损耗的非线性响应,在30 ~ 40 mm·h−1之间急剧增加。这一结果表明了临界材料损失阈值。这些结果揭示了植被类型在斜坡尺度上控制物质损失方面的主导作用,并证实了机器学习解释复杂水文过程的潜力。
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引用次数: 0
Adsorption and mechanism of magnetically modified industrial hemp straw biochar on microplastics in aqueous solution 磁性改性工业大麻秸秆生物炭对微塑料的吸附及机理研究。
IF 4.4 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2026-01-05 DOI: 10.1016/j.jconhyd.2026.104844
Xi Jiang , Youxi Cai , Hanwen Deng , Xiaolei Li
Microplastics (MPs) originating from plastic waste in groundwater have attracted much attention worldwide due to their wide distribution, small particle size and high mobility, as well as their potential threat to organisms. In this study, a magnetically modified biochar adsorbent for the removal of microplastics was prepared using KOH-activated industrial hemp straw biochar as a precursor. For polystyrene (PS) microspheres (1 μm, 60 mg/L) in aqueous solution, magnetic biochar (MBC) removed 89.97 %, which was 9.30 times higher removal rate compared to pristine biochar (BC). It is hypothesized that the adsorption process was a result of electrostatic interactions and chemical bonding interactions between microplastics and biochar. The adsorption process was affected by solution pH and interfering ions, and the MBC had good stability, and its removal efficiency of MPs remained above 80 % after 5 cycles. Kinetic, isothermal and thermodynamic modeling analyses showed that the adsorption reaction was spontaneous, higher temperature contributed to the enhancement of adsorption, and the adsorption mechanism involved electrostatic interactions, surface complexation, metal-O-MPs complexation and π-π interactions. These results would provide an idea for obtaining MBC to remove the MPs from aqueous systems.
来源于地下水中塑料垃圾的微塑料因其分布广泛、粒径小、流动性强以及对生物的潜在威胁而受到世界各国的广泛关注。本研究以koh活化的工业大麻秸秆生物炭为前驱体,制备了一种用于去除微塑料的磁性改性生物炭吸附剂。磁性生物炭(MBC)对聚苯乙烯(PS)微球(1 μm, 60 mg/L)的去除率为89.97%,是原始生物炭(BC)的9.30倍。假设吸附过程是微塑料与生物炭之间静电相互作用和化学键相互作用的结果。吸附过程受溶液pH和干扰离子的影响,MBC具有良好的稳定性,循环5次后对MPs的去除率保持在80%以上。动力学、等温和热力学模型分析表明,吸附反应是自发的,温度升高有助于吸附的增强,吸附机理涉及静电相互作用、表面络合作用、金属- o - mps络合作用和π-π相互作用。这些结果将为获得从水体系中去除MPs的MBC提供思路。
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引用次数: 0
Fate, chlorination kinetics, and comprehensive risk assessment of pharmaceuticals and personal care products in drinking water distribution systems 饮用水分配系统中药品和个人护理产品的命运、氯化动力学和综合风险评估
IF 4.4 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2026-01-05 DOI: 10.1016/j.jconhyd.2026.104842
Zhenglin Li , Nan Li , Fei Wang , Minru Xiao , Anlei Wei
The widespread occurrence of pharmaceuticals and personal care products (PPCPs) in aquatic environments has emerged as a global concern due to their potential threats to water security and ecological health. Despite increasing attention, their fate and associated risks in drinking water systems remain insufficiently understood. The occurrence, transformation behavior, and ecological and human health risks of 19 PPCPs were investigated across drinking water treatment and distribution systems in this study. Eighteen PPCPs were ubiquitously detected in raw water, with high detection frequencies (>70 %), whereas both the number of detected compounds and their concentrations were markedly reduced in finished water (five compounds) and tap water (eleven compounds). These results demonstrate the substantial effectiveness of conventional treatment processes in reducing both the diversity and concentrations of PPCPs. To further elucidate their potential transformation during water treatment, chlorination kinetics of eight structurally diverse PPCPs were evaluated under controlled conditions. Four compounds (atenolol, sulpiride, paroxetine, and nadolol) exhibited pseudo-first-order kinetics with residual chlorine, while the others exhibited significant resistance to chlorination. Degradation efficiency was found to depend on both the water matrix conditions and their molecular properties, highlighting the combined roles of intrinsic chemical properties and environmental complexity. Ecological risk assessment revealed ibuprofen posed a moderate ecological risk, a risk quotient (RQ) of 0.335, while triclocarban presented a high ecological risk (RQ = 4.6031). Mixture toxicity assessment based on the cumulative toxic unit (ΣTU) further indicated a potential ecological risk (ΣTU > 1) in raw water. Human health risk assessment showed minimal risks across all age groups (RQ 〈10−3). However, infants were identified as the most susceptible population, likely due to their higher exposure relative to body weight. Among the detected PPCPs, meclofenamic acid was identified as the compound of highest concern, with average relative risk indices exceeding >10−4. These findings provide critical insights into the fate and transformation of PPCPs in drinking water systems and offer scientific guidance for optimizing treatment processes and risk management strategies.
由于药品和个人护理产品(PPCPs)对水安全和生态健康的潜在威胁,它们在水生环境中的广泛存在已成为全球关注的问题。尽管受到越来越多的关注,但它们的命运和饮用水系统中的相关风险仍然没有得到充分的了解。本研究调查了19种PPCPs在饮用水处理和配水系统中的发生、转化行为以及生态和人类健康风险。在原水中普遍检测到18种PPCPs,检测频率高(> 70%),而在成品水(5种化合物)和自来水(11种化合物)中检测到的化合物数量和浓度均显著降低。这些结果表明,传统处理工艺在减少ppcp的多样性和浓度方面具有实质性的有效性。为了进一步阐明它们在水处理过程中的潜在转化,在受控条件下评估了8种结构不同的PPCPs的氯化动力学。四种化合物(阿替洛尔、舒必利、帕罗西汀和纳多洛尔)对余氯表现出准一级动力学,而其他化合物对氯化反应表现出明显的抗性。研究发现,降解效率取决于水基质条件及其分子性质,突出了内在化学性质和环境复杂性的综合作用。生态风险评价结果显示,布洛芬具有中等生态风险,RQ为0.335;三氯卡班具有较高生态风险,RQ为4.6031。基于累积毒性单位(ΣTU)的混合毒性评价进一步表明原水存在潜在的生态风险(ΣTU > 1)。人类健康风险评估显示,所有年龄组的风险最小(RQ < 10−3)。然而,婴儿被确定为最易受影响的人群,可能是因为他们相对于体重的接触量更高。在检测到的PPCPs中,甲氯芬酸被确定为最受关注的化合物,其平均相对风险指数超过10−4。这些发现为饮用水系统中ppcp的命运和转变提供了重要见解,并为优化处理过程和风险管理策略提供了科学指导。
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引用次数: 0
Distinguishing natural from mining-related metal sources by including streambank groundwater data in a stream mass loading study 通过在河流质量负荷研究中包括河岸地下水数据来区分自然与采矿相关的金属来源
IF 4.4 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2026-01-05 DOI: 10.1016/j.jconhyd.2026.104841
Andrew H. Manning , Robert L. Runkel , Jean M. Morrison , Sara Warix , Richard B. Wanty , Katherine Walton-Day , Michael Snook
Distinguishing stream metal loading caused by mine features from that caused by natural background sources remains challenging, yet this distinction is essential for making effective remedial decisions at many legacy mine sites. We combine a stream tracer injection and synoptic sampling study with data from shallow near-stream groundwater wells to estimate left-bank versus right-bank metal loading contributions at the 100-m spatial scale. The study was performed in the East Mancos River, a mountain headwater stream in Colorado, USA. The dominant source of elevated stream metal concentrations could be either groundwater infiltration through right-bank Doyle Mine waste piles or natural acid rock drainage from hydrothermally altered bedrock located mainly on the left bank. For the five metals of concern (Cu, Al, Zn, Cd, and Mn), we find that 15 % of the load contributed by diffuse groundwater inputs in the section potentially influenced by Doyle mine waste originates from the right bank. This right-bank potential mine contribution equates to only 3 % of the total watershed instream load for these metals. Furthermore, apparent 3H/3He groundwater ages in segments contributing most of the right-bank metal loading are sufficiently old (9–12 yr) to suggest that infiltration through the waste piles, located only 140–180 m from the stream, is unlikely. Estimated potential Doyle mine loading contributions can therefore be considered maximum values. Study results thus indicate that Doyle mine waste piles are a minor source of metal loading under low-flow conditions, and streambank groundwater data can provide valuable additional information in stream mass loading studies.
区分由矿山特征引起的金属流载荷与自然背景源引起的金属流载荷仍然具有挑战性,但这种区分对于在许多遗留矿区做出有效的补救决策至关重要。我们将河流示踪剂注入和天气抽样研究与浅层近溪流地下水井的数据相结合,以估计100米空间尺度上左岸与右岸金属载荷的贡献。该研究是在美国科罗拉多州的山源河流东曼科斯河进行的。河流金属浓度升高的主要来源可能是通过右岸Doyle矿山废渣堆渗透的地下水或主要位于左岸的热液蚀变基岩的天然酸性岩石排水。对于关注的五种金属(Cu、Al、Zn、Cd和Mn),我们发现在可能受Doyle矿山废弃物影响的断面中,漫射地下水输入所贡献的负荷中有15%来自右岸。这一右岸潜在的矿山贡献仅相当于这些金属的流域河流总负荷的3%。此外,在贡献大部分右岸金属负荷的部分,明显的3H/3He地下水年龄足够老(9-12年),表明通过距离溪流仅140-180米的废物堆渗透的可能性不大。因此,估计的潜在多伊尔矿负荷贡献可视为最大值。研究结果表明,Doyle矿山废渣桩是低流量条件下金属载荷的次要来源,河岸地下水数据可以为河流质量载荷研究提供有价值的附加信息。
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引用次数: 0
Nitrate dynamics in the Dongjiang River watershed: Human impacts in the context of an Anthropocene River 东江流域硝酸盐动态:人类世河流背景下的人类影响
IF 4.4 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2026-01-04 DOI: 10.1016/j.jconhyd.2026.104843
Yaotong Gao , Bingjun Liu , Qian Tan , Kai He , Wei Ouyang , Yaling Yu
Rivers in the Anthropocene are increasingly impacted by human activities, with nitrate (NO3) pollution posing a significant threat to water quality and ecosystem health. This study investigates the Dongjiang River watershed as a representative example of such systems impacted by human activities. Using nitrate dual isotopes (δ15N-NO3 and δ18O-NO3) and a Bayesian mixing model (MixSIAR), we identified the sources and transformation processes of NO3 in the downstream Dongjiang River. Our results indicate that manure and sewage (MS) account for the majority of NO3 inputs (64.52 %), followed by soil nitrogen (SN) at 18.88 %. The influence of MS is amplified in catchments with higher urbanization, while forested areas show more significant contributions from SN. Seasonal variations in nitrate sources were also observed, with MS dominating during the dry season and SN contributions increasing during the wet season. Nitrification and denitrification were relatively weak during our sampling periods, as indicated by the absence of a characteristic δ15N-NO3 versus δ18O-NO3 slope (∼50 %) and by low extent of denitrification values at most sites; thus, external inputs were likely the primary drivers of NO3 dynamics. Furthermore, we link socio-economic factors and water consumption patterns to specific NO3 sources, highlighting the role of urbanization, economic development, and agricultural practices in shaping nitrate pollution. These findings provide critical insights for managing water quality and mitigating anthropogenic impacts on the Dongjiang River in the Anthropocene.
人类世的河流受到人类活动的影响越来越大,硝酸盐(NO3−)污染对水质和生态系统健康构成了重大威胁。本文以东江流域为研究对象,研究了受人类活动影响的生态系统。利用硝酸盐双同位素(δ15N-NO3−和δ18O-NO3−)和贝叶斯混合模型(MixSIAR),确定了东江下游NO3−的来源和转化过程。结果表明,粪肥和污水(MS)占NO3−输入的大部分(64.52%),其次是土壤氮(SN),占18.88%。城市化程度越高的流域,MS的影响越大,而森林地区SN的贡献越显著。硝态氮源在旱季以MS为主,而在雨季硝态氮的贡献增加。在我们的采样期间,硝化和反硝化作用相对较弱,这表明缺乏δ15N-NO3−与δ18O-NO3−的特征斜率(~ 50%),并且大多数地点的反硝化值程度较低;因此,外部输入可能是NO3−动力学的主要驱动因素。此外,我们将社会经济因素和水消费模式与特定的NO3−来源联系起来,强调了城市化、经济发展和农业实践在形成硝酸盐污染中的作用。这些发现为人类世的水质管理和减轻对东江的人为影响提供了重要的见解。
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引用次数: 0
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Journal of contaminant hydrology
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