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“Catch-and-feed”: Janus catalytic flow-through membrane enables highly efficient removal of micropollutants in water "捕捉和喂养":Janus 催化直流膜可高效去除水中的微污染物
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-09 DOI: 10.1016/j.watres.2024.122778
Yuxin Zeng , Yaxuan Gao , Tao Guo , Lifeng Yin , Michael R. Hoffmann
Micropollutants, due to their low concentrations, exceptional chemical stability, and profound toxicity, present a significant challenge in water treatment. While electrocatalysis and photocatalysis have shown promise as potential water purification techniques, their inherent limitations in mass transfer often result in elevated energy requirements and suboptimal efficiency. In this study, a Janus catalytic flow-through membrane (JCFM) was utilized to successfully remove two notorious micropollutants dichlorvos (DDVP) and azoxystrobin (AZX) from water based on the "catch-and-feed" strategy. This membrane adopts a ``sandwich'' configuration, comprising platinum-modified reduced titanium (Pt@rTO) as the electrocatalytic layer, porous titanium (Ti) as the current collector, and rTO as the photocatalytic layer. The JCFM exhibited remarkable performance, maintaining an •OH energy conversion efficiency of up to 20.12 nM and displaying catalytic activity (kJCFM = 6.97 × 10−4 s−1) in degrading AZX far superior to that of photocatalysis (kPC = 9.51 × 10−5 s−1) or electrocatalysis (kEC = 9.89 × 10−5 s−1) alone. It is evidenced that the Pt@rTO layer efficiently generates reactive oxygen species (ROS), which, along with the micropollutants, flow through the JCFM (“feed”), which strengthens mass transfer and facilitates efficient reactions within the confined space (“catch”). The ROSs then seep through the rTO layer, where they are reactivated by UV light radiation. The mechanism and the alternative reaction pathway of DDVP and AZX has also been proposed. In sequential testing, the JCFM achieved continuous and energy-efficient removal of micropollutants, exceeding 97.5 % over 200 h. The scale-up application of this technology has proven effective in the treatment of secondary biochemical effluent from municipal sewage, coking wastewater, and landfill leachate, achieving the concurrent degradation of various micropollutants.
微污染物浓度低、化学稳定性强、毒性大,给水处理带来了巨大挑战。虽然电催化和光催化有望成为潜在的水净化技术,但它们在传质方面的固有局限性往往导致能源需求增加和效率不理想。在这项研究中,利用 Janus 催化直流膜(JCFM),基于 "捕捉-进给 "策略,成功去除了水中两种臭名昭著的微污染物敌敌畏(DDVP)和唑啉草酯(AZX)。这种膜采用了 "三明治 "结构,包括作为电催化层的铂改性还原钛(Pt@rTO)、作为集流器的多孔钛(Ti)和作为光催化层的 rTO。JCFM 表现出卓越的性能,在降解 AZX 的过程中能保持高达 20.12 nM 的 -OH 能量转换效率,其催化活性(kJCFM=6.97 × 10-4 s-1)远高于光催化(kPC=9.51 × 10-5 s-1)或电催化(kEC=9.89 × 10-5 s-1)。事实证明,Pt@rTO 层能有效生成活性氧(ROS),这些活性氧与微污染物一起流经 JCFM("进料"),从而加强了传质,促进了密闭空间("捕获")内的高效反应。然后,ROS 渗过 rTO 层,在紫外线辐射下被重新激活。此外,还提出了 DDVP 和 AZX 的机理和替代反应途径。在连续测试中,JCFM 实现了连续、节能地去除微污染物,在 200 小时内去除率超过 97.5%。该技术的放大应用已在城市污水、焦化废水和垃圾填埋场渗滤液的二级生化废水处理中证明是有效的,实现了各种微污染物的同时降解。
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引用次数: 0
Explainable artificial intelligence for reliable water demand forecasting to increase trust in predictions 可解释人工智能用于可靠的水需求预测,提高预测的可信度
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-09 DOI: 10.1016/j.watres.2024.122779
Claudia Maußner , Martin Oberascher , Arnold Autengruber , Arno Kahl , Robert Sitzenfrei
The “EU Artificial Intelligence Act” sets a framework for the implementation of artificial intelligence (AI) in Europe. As a legal assessment reveals, AI applications in water supply systems are categorised as high-risk AI if a failure in the AI application results in a significant impact on physical infrastructure or supply reliability. The use case of water demand forecasts with AI for automatic tank operation is for example categorised as high-risk AI and must fulfil specific requirements regarding model transparency (traceability, explainability) and technical robustness (accuracy, reliability). To this end, six widely established machine learning models, including both transparent and opaque models, are applied to different datasets for daily water demand forecasting and the requirements regarding model accuracy, transparency and technical robustness are systematically evaluated for this use case. Opaque models generally achieve higher prediction accuracy compared to transparent models due to their ability to capture the complex relationship between parameters like for example weather data and water demand. However, this also makes them vulnerable to deviations and irregularities in weather forecasts and historical water demand. In contrast, transparent models rely mainly on historical water demand data for the utilised dataset and are less influenced by weather data, making them more robust against various data irregularities. In summary, both transparent and opaque models can fulfil the requirements regarding explainability but differ in their level of transparency and robustness to input errors. The choice of model depends also on the operator's preferences and the context of the application.
欧盟人工智能法》为欧洲人工智能(AI)的实施制定了框架。法律评估显示,供水系统中的人工智能应用如果出现故障,会对物理基础设施或供水可靠性造成重大影响,则被归类为高风险人工智能。例如,在水箱自动运行中使用人工智能进行水需求预测就被归类为高风险人工智能,必须满足有关模型透明度(可追溯性、可解释性)和技术稳健性(准确性、可靠性)的特定要求。为此,我们在不同的数据集上应用了六种广为流传的机器学习模型(包括透明模型和不透明模型)来进行每日需水量预测,并系统地评估了该用例对模型准确性、透明度和技术稳健性的要求。与透明模型相比,不透明模型由于能够捕捉气象数据和需水量等参数之间的复杂关系,通常能获得更高的预测精度。然而,这也使其容易受到天气预报和历史需水量的偏差和不规则性的影响。与此相反,透明模型主要依靠历史需水量数据来利用数据集,受天气数据的影响较小,因此对各种数据不规则性的抵抗能力更强。总之,透明模型和不透明模型都能满足可解释性方面的要求,但在透明度和对输入误 差的稳健性方面有所不同。模型的选择还取决于运营商的偏好和应用环境。
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引用次数: 0
Mechanism insights into metal-organic framework-derived carbon materials activating periodate for p-chlorophenol removal: The role of S and Fe co-doping 金属有机框架衍生碳材料活化高碘酸盐去除对氯苯酚的机理研究:S 和 Fe 共掺的作用
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-09 DOI: 10.1016/j.watres.2024.122735
Wenjun Xiao , Ao Chen , Min Cheng , Weiping Xiong , Yang Liu , Jun Wang , Guangfu Wang , Gaoxia Zhang , Ling Li , Hongda Liu , Qingkai Shi
Periodate (PI, IO4)-based advanced oxidation processes (AOPs) provide an economical and sustainable approach to alleviate water pollution challenges. Developing efficient and stable activators for PI is the focus of current research. Herein, S/Fe-co-doped magnetic porous carbon material (S/Fe-ZIF-950) was prepared by introducing exogenous S atoms using Fe-doped zeolitic imidazolate framework-8 (Fe-ZIF-8) as a precursor, which showed the most superior performance (100 % within 10 min) in activating PI to remove p-chlorophenol (4-CP). Quenching tests, electron spin resonance and electrochemical characterizations revealed that IO3·, 1O2, ·O2 dominated the 4-CP degradation process with Fe3C and ZnS as the main active sites. The synergistic effect of S and Fe was the main reason for the enhanced degradation performance of 4-CP in S/Fe-ZIF-950/PI system, among which the reducing S2− could effectively promote the regeneration of Fe(Ⅱ), thus facilitating the continuous generation of active species. Combined with LC-MS results and density functional theory (DFT) calculations, possible degradation routes of 4-CP in the S/Fe-ZIF-950/PI system were presented. Moreover, toxicity assessment showed that the S/Fe-ZIF-950/PI system exhibited low biotoxicity and no toxic iodine by-products were formed. In addition, S/Fe-ZIF-950/PI system demonstrated excellent activity, good stability, outstanding reusability and durability in a variety of complex water environments. This study investigated the activation mechanism of S/Fe-co-doped porous carbon materials on PI, which shed a new light on the catalytic activation of PI by heteroatom-doped Fe-loaded carbon-based materials.
基于高碘酸盐(PI,IO4-)的高级氧化工艺(AOPs)为缓解水污染挑战提供了一种经济、可持续的方法。开发高效稳定的高碘酸盐活化剂是当前研究的重点。本文以掺杂 Fe 的唑基咪唑啉框架-8(Fe-ZIF-8)为前驱体,通过引入外源 S 原子制备了 S/Fe 共掺杂磁性多孔碳材料(S/Fe-ZIF-950),该材料在活化 PI 去除对氯苯酚(4-CP)方面表现出了最优异的性能(10 分钟内 100% 去除)。淬灭试验、电子自旋共振和电化学特性分析表明,IO3-、1O2、-O2- 主导了 4-CP 的降解过程,Fe3C 和 ZnS 是主要的活性位点。S和Fe的协同作用是S/Fe-ZIF-950/PI体系中4-CP降解性能增强的主要原因,其中还原性S2-能有效促进Fe(Ⅱ)的再生,从而促进活性物种的不断生成。结合 LC-MS 结果和密度泛函理论(DFT)计算,提出了 4-CP 在 S/Fe-ZIF-950/PI 体系中的可能降解途径。此外,毒性评估表明,S/Fe-ZIF-950/PI 系统具有较低的生物毒性,并且没有形成有毒的碘副产物。此外,S/Fe-ZIF-950/PI 系统在各种复杂的水环境中表现出卓越的活性、良好的稳定性、出色的可重复使用性和耐久性。本研究探讨了 S/Fe 共掺杂多孔碳材料对 PI 的活化机理,为杂质原子掺杂的 Fe 负载碳基材料催化活化 PI 提供了新的思路。
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引用次数: 0
A novel approach for immobilizing Ag/ZnO nanorods on a glass substrate: Application in solar light-driven degradation of micropollutants in water 在玻璃基底上固定 Ag/ZnO 纳米棒的新方法:在太阳光驱动的水中微污染物降解中的应用
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-09 DOI: 10.1016/j.watres.2024.122736
Yanan Li , Isaac Sánchez-Montes , Lingling Yang , Mohamed Gamal El-Din , Xuehua Zhang
One of the main challenges in applying photocatalysts for water treatment is the complex separation and recycling process. In this study, we developed highly stable, porous zinc oxide nanorods (ZnO NRs) immobilized on glass vials using a solvent exchange process (SEP) and hydrothermal calcination. Key parameters, including oleic acid concentration and hydrothermal growth time, were optimized to maximize the active surface area, significantly enhancing photodegradation performance. Under the best conditions, ZnO NRs-coated vials achieved nearly 100% degradation of sulfamethoxazole (SMX) in 10 h of simulated solar irradiation. Depositing silver nanoparticles on the surface of ZnO NRs (Ag/ZnO NRs) further improved performance, reducing degradation time to 4 h and increasing photocatalyst stability. The Ag/ZnO NRs-coated vials, optimized with an Ag precursor concentration of 0.05 M, also demonstrated high degradation rates (>99%) for eight organic micropollutants at environmentally relevant concentrations over multiple reuse cycles and with minimal metal leaching. This study presents an innovative, tunable method for immobilizing photocatalysts on glass substrates, offering high surface area, excellent photocatalytic activity, and mechanical properties, making it highly suitable for water treatment applications.
将光催化剂用于水处理的主要挑战之一是复杂的分离和回收过程。在这项研究中,我们利用溶剂交换工艺(SEP)和水热煅烧技术开发了固定在玻璃瓶上的高稳定性多孔氧化锌纳米棒(ZnO NRs)。对油酸浓度和水热生长时间等关键参数进行了优化,以最大限度地增加活性表面积,从而显著提高光降解性能。在最佳条件下,ZnO NRs 涂层小瓶在模拟太阳照射 10 小时后,磺胺甲噁唑(SMX)的降解率接近 100%。在 ZnO NRs(Ag/ZnO NRs)表面沉积银纳米粒子可进一步提高性能,将降解时间缩短至 4 小时,并提高光催化剂的稳定性。经过优化的 Ag/ZnO NRs 涂层小瓶(Ag 前体浓度为 0.05 M)在多个重复使用周期内对环境相关浓度的八种有机微污染物具有很高的降解率(>>99%),且金属浸出极少。这项研究提出了一种在玻璃基底上固定光催化剂的创新可调方法,它具有高表面积、出色的光催化活性和机械性能,非常适合水处理应用。
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引用次数: 0
Time series-based machine learning for forecasting multivariate water quality in full-scale drinking water treatment with various reagent dosages 基于时间序列的机器学习用于预测采用不同试剂剂量的全规模饮用水处理中的多元水质
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-09 DOI: 10.1016/j.watres.2024.122777
Hongjiao Pang , Yawen Ben , Yong Cao , Shen Qu , Chengzhi Hu
Accurately predicting drinking water quality is critical for intelligent water supply management and for maintaining the stability and efficiency of water treatment processes. This study presents an optimized time series machine learning approach for accurately predicting multivariate drinking water quality, explicitly considering the time-dependent effects of reagent dosing. By leveraging data from a full-scale treatment plant, we constructed feature-engineered time series datasets incorporating influent water quality parameters, reagent dosages and effluent water characteristics. Seven predictive models, including both traditional machine learning (ML) and deep learning (DL) models were developed and rigorously evaluated against a naive mean baseline model. Our results demonstrate that traditional ML models, enhanced with time feature engineering, rivaled the performance of both widely used DL models and the naive mean baseline model. Specifically, an XGBoost model achieved superior prediction accuracy in dynamically forecasting four water quality characteristics at a 12-hour time lag step, outperforming the naive baseline model by 3–4 % in terms of Mean Absolute Percentage Error (MAPE). This finding underscores the importance of incorporating a 12-hour interval to effectively capture the delayed impact of reagent dosing on water quality prediction. Furthermore, SHAP model interpretability analysis provided valuable insights into the XGBoost model's decision-making process, revealing its strong data-driven foundation aligned with established water treatment principles. This research highlights the significant potential of optimized machine learning techniques for enhancing water purification processes and enabling more informed, data-driven decision-making in the water supply industry.
准确预测饮用水水质对于智能供水管理以及保持水处理工艺的稳定性和效率至关重要。本研究提出了一种优化的时间序列机器学习方法,用于准确预测多元饮用水水质,并明确考虑了试剂投加的时间依赖效应。通过利用全规模处理厂的数据,我们构建了包含进水水质参数、试剂剂量和出水特征的特征工程时间序列数据集。我们开发了七种预测模型,包括传统的机器学习(ML)模型和深度学习(DL)模型,并对照天真平均基线模型进行了严格评估。结果表明,通过时间特征工程增强的传统 ML 模型的性能可与广泛使用的 DL 模型和天真平均基线模型相媲美。具体来说,XGBoost 模型在以 12 小时时滞步长动态预测四种水质特征时取得了更高的预测精度,在平均绝对百分比误差 (MAPE) 方面比天真的基线模型高出 3-4%。这一发现强调了加入 12 小时间隔以有效捕捉试剂投加对水质预测的延迟影响的重要性。此外,SHAP 模型可解释性分析为 XGBoost 模型的决策过程提供了有价值的见解,揭示了其与既定水处理原则相一致的强大数据驱动基础。这项研究凸显了优化机器学习技术在增强水净化过程和实现供水行业更明智的数据驱动决策方面的巨大潜力。
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引用次数: 0
The role of bacteriophages in facilitating the horizontal transfer of antibiotic resistance genes in municipal wastewater treatment plants 噬菌体在促进城市污水处理厂抗生素耐药性基因水平转移中的作用
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-09 DOI: 10.1016/j.watres.2024.122776
Qiang Wang , Min Wang , Qingxiang Yang , Lingran Feng , Hao Zhang , Ruifei Wang , Ruimin Wang
Bacteriophages play integral roles in the ecosystem; however, their precise involvement in horizontal gene transfer and the spread of antibiotic resistance genes (ARGs) are not fully understood. In this study, a coculture system involving consortia of bacteriophages and multidrug-resistant bacteria from an aerobic tank in a municipal wastewater treatment plant (WWTP) was established to investigate the functions of bacteriophages in ARG transfer and spread. The results of the cocultivation of the MRB and bacteriophage consortia indicated that the bacterial community remained stable throughout the whole process, but the addition of bacteriophages significantly increased ARG abundance, especially in bacteriophage DNA. Nine out of the 11 identified ARGs significantly increased, indicating that more bacteriophage particles carried ARGs in the system after cocultivation. In addition, 686 plasmids were detected during cocultivation, of which only 3.36 % were identified as conjugative plasmids, which is significantly lower than the proportion found among previously published plasmids (25.2 %, totaling 14,029 plasmids). Our findings revealed that bacteriophages may play important roles in the horizontal transfer of ARGs through both bacteriophage-mediated conduction and an increase in extracellular ARGs; however, conjugative transfer may not be the main mechanism by which multidrug-resistant bacteria acquire and spread ARGs. Unlike in most previous reports, a coculture system of diverse bacteria and bacteriophages was established in this study to assess bacteriophage functions in ARG transfer and dissemination in the environment, overcoming the limitations associated with the isolation of bacteria and bacteriophages, as well as the specificity of bacteriophage hosts.
噬菌体在生态系统中发挥着不可或缺的作用;然而,人们对噬菌体参与水平基因转移和抗生素耐药基因(ARGs)传播的确切情况还不完全了解。本研究建立了一个由噬菌体和来自城市污水处理厂好氧池的多重耐药菌组成的共培养系统,以研究噬菌体在 ARG 转移和传播中的功能。MRB和噬菌体联合培养的结果表明,细菌群落在整个过程中保持稳定,但噬菌体的加入显著增加了ARG的丰度,尤其是噬菌体DNA中的ARG。在 11 个已确定的 ARGs 中,有 9 个明显增加,这表明共培养后系统中有更多的噬菌体颗粒携带 ARGs。此外,在共培养过程中还检测到了 686 个质粒,其中只有 3.36% 被鉴定为共轭质粒,这一比例明显低于之前公布的质粒比例(25.2%,共 14,029 个质粒)。我们的研究结果表明,噬菌体可能通过噬菌体介导的传导和细胞外ARGs的增加在ARGs的水平转移中发挥重要作用;然而,共轭转移可能并不是耐多药细菌获得和传播ARGs的主要机制。与以往大多数报告不同的是,本研究建立了一个由多种细菌和噬菌体组成的共培养系统,以评估噬菌体在环境中传递和传播 ARG 的功能,克服了细菌和噬菌体分离的局限性以及噬菌体宿主的特异性。
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引用次数: 0
Self-catalytic enhancement of Cu-EDTA decomplexation and simultaneous Cu recovery via a dual-cathode electrochemical process 通过双阴极电化学过程自催化增强 Cu-EDTA 解络合并同时回收 Cu
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-09 DOI: 10.1016/j.watres.2024.122775
Ran Mao , Ke Hu , Hongshuai Kan , Li Yan , Rongsen Chen , Xu Zhao
Heavy metals that are readily chelated with coexisting organic ligands in industrial wastewaters impose threats to environment and human health but are also valuable metal resources. Traditional treatment methods generally require additional chemicals and generate secondary contaminants. Here, a reagent-free dual-cathode electrochemical system was proposed for the efficient destruction of Cu-organic complexes and synchronous cathodic recovery of Cu, whereby in situ production of H2O2 at carbon aerogel (CA) cathode was coupled with the reduction of Cu(II) to Cu(I) and finally to Cu(0) at Ti cathode. The intermediate Cu(II) complexes enabled the self-reinforced degradation owing to their higher activities toward •OH generation by activating H2O2 in contrast to initial Cu-ethylenediaminetetraacetic acid (Cu-EDTA). The enhanced production of Cu(I) by Ti cathode facilitated both •OH and Cu(III) formation, and the copper redox cycle was realized in the self-reinforced system, maintaining its sustainable catalytic activity. The energy cost of the dual-cathode system is 0.011 kWh/g for decomplexation and 0.057 kWh/g for Cu recovery, which is much lower than single Ti or CA cathode system. This established process provides a prospective approach for cost-effective destruction of chelating metal complexes and metal resources recovery from heavy metal wastewaters.
工业废水中容易与共存有机配体螯合的重金属对环境和人类健康构成威胁,但同时也是宝贵的金属资源。传统的处理方法通常需要额外的化学品,并会产生二次污染。在此,我们提出了一种无试剂双阴极电化学系统,用于高效破坏铜有机络合物并同步阴极回收铜,即在碳气凝胶(CA)阴极原位产生 H2O2,同时在钛阴极将 Cu(II) 还原成 Cu(I) 并最终还原成 Cu(0)。与最初的铜-乙二胺四乙酸(Cu-EDTA)相比,中间的 Cu(II) 复合物通过激活 H2O2 生成-OH 的活性更高,因此能够实现自我强化降解。钛阴极产生的 Cu(I)的增强促进了 -OH 和 Cu(III)的形成,在自增强系统中实现了铜氧化还原循环,保持了其可持续的催化活性。双阴极系统的解络合能耗为 0.011 kWh/g,铜回收能耗为 0.057 kWh/g,远低于单 Ti 或 CA 阴极系统。这种成熟的工艺为经济有效地销毁螯合金属络合物和从重金属废水中回收金属资源提供了一种前景广阔的方法。
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引用次数: 0
Adsorbability of a wide range of per- and polyfluoroalkyl substances on granular activated carbon, ion exchange resin, and surface modified clay 颗粒活性炭、离子交换树脂和表面改性粘土对多种全氟和多氟烷基物质的吸附性
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-09 DOI: 10.1016/j.watres.2024.122774
Bahareh Tajdini , Hooman Vatankhah , Ethan R. Pezoulas , Chuhui Zhang , Christopher P Higgins , Christopher Bellona
The increased detection of understudied per- and polyfluoroalkyl substances (PFAS) in environmental matrices has highlighted the need to evaluate the treatability of a wide-range of PFAS by sorption-based processes. This study investigated the efficacy of three commercial adsorbents (i.e., granular activated carbon (GAC), surface modified clay (SMC), and anionic exchange resin (AER)) for the removal of a wide range of cationic, zwitterionic, and anionic PFAS from an aqueous film forming foam (AFFF)-impacted groundwater employing rapid small-scale column tests (RSSCTs) coupled with high resolution mass spectrometry (HRMS) and suspect screening analysis (SQ). AER exhibited later breakthrough times for the majority of anionic and zwitterionic PFAS compared to SMC and GAC. However, both AER and SMC exhibited negligible removal of cationic PFAS presumably due to the reliance of these adsorbents on electrostatic interactions and the counteraction of hydrophobic forces caused by the repulsion between cationic PFAS and positively charged surfaces of AER and SMC. GAC, being a non-selective adsorbent, was largely unaffected by the ionic charge of the evaluated PFAS with molecular structure having a bigger impact on adsorbability. The detection of a variety of PFAS classes in the investigated AFFF-impacted groundwater enabled assessment of the relative impact of chemical structure on adsorptive removal of PFAS. Chain-length dependent adsorption was observed across all investigated anionic and zwitterionic PFAS classes. The PFAS structures possessing hydroxyl and/or methyl functional groups exhibited later breakthrough times compared to their homologues lacking these functional groups and cyclic/unsaturated structures were removed less efficiently compared to their linear/saturated homologues. In the case of perfluoroalkyl acid (PFAA)-derivative structures, hydrogen-substituted classes (i.e., H-PFAAs) were removed more efficiency than PFAAs while keto-substituted structures (i.e., K-PFSA) and pentahydrido-fluoroalkane sulfates (PeH-FAOS) exhibited lower adsorbability compared to PFAAs for all adsorbents. Oxa-PFAAs (O-PFSA; isomer class of PFA-OS) on the other hand demonstrated higher adsorbability compared to PFAAs in the case of AER-like adsorbents, while this trend was reversed for GAC.
环境基质中检测到的未充分研究的全氟和多氟烷基物质(PFAS)越来越多,这凸显了通过基于吸附的工艺来评估各种全氟和多氟烷基物质的可处理性的必要性。本研究采用快速小规模柱试验 (RSSCT)、高分辨率质谱分析 (HRMS) 和疑似筛选分析 (SQ),调查了三种商用吸附剂(即颗粒活性炭 (GAC)、表面改性粘土 (SMC) 和阴离子交换树脂 (AER))去除受水成膜泡沫 (AFFF) 影响的地下水中各种阳离子、齐聚阴离子和阴离子 PFAS 的功效。与 SMC 和 GAC 相比,AER 对大多数阴离子和齐聚物 PFAS 的突破时间较晚。不过,AER 和 SMC 对阳离子全氟辛烷磺酸的去除几乎可以忽略不计,这可能是由于这些吸附剂依赖于静电相互作用以及阳离子全氟辛烷磺酸与 AER 和 SMC 带正电的表面之间的排斥力所产生的疏水力的反作用。作为一种非选择性吸附剂,GAC 基本上不受所评估的全氟辛烷磺酸离子电荷的影响,而分子结构对吸附性的影响更大。在所调查的受 AFFF 影响的地下水中检测到了各种类别的 PFAS,这有助于评估化学结构对吸附去除 PFAS 的相对影响。在所有调查的阴离子和齐聚物全氟辛烷磺酸类别中,都观察到了链长依赖性吸附。与缺乏羟基和/或甲基官能团的同系物相比,具有羟基和/或甲基官能团的 PFAS 结构的突破时间较晚,与线性/饱和同系物相比,环状/不饱和结构的去除效率较低。就全氟烷基酸(PFAA)衍生物结构而言,氢取代类(即 H-PFAA)的去除效率高于全氟烷基酸,而酮取代结构(即 K-PFSA)和五水氟烷硫酸盐(PeH-FAOS)在所有吸附剂中的吸附性均低于全氟烷基酸。另一方面,在类似 AER 的吸附剂中,Oxa-PFAAs(O-PFSA;PFA-OS 的异构体类别)与 PFAAs 相比具有更高的吸附性,而对于 GAC 而言,这一趋势正好相反。
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引用次数: 0
Modeling Nitrogen Recovery and Water Transport in Gas-Permeable Membranes 透气膜中的氮回收和水传输建模
IF 12.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-08 DOI: 10.1016/j.watres.2024.122771
C. Da Silva, A. Serra-Toro, V. Pelizzaro, F. Valentino, S. Astals, F. Mas, J. Dosta
This study presents a new modeling approach for nitrogen recovery for gas-permeable membrane (GPM) contactors, including both ammonia and water transport dynamics. A distinct feature of the model is its capacity to model water transport across the membrane, which has been overlooked in most publications. Osmotic pressure differences are used to predict the behavior of ammonia and water transport in the GPM. Experiments carried out to develop, test and calibrate the model examined the dynamics of ammonia and water transport through the GPM at various nitrogen concentrations. Specifically, the GPM contactor was tested for nitrogen recovery from high-strength synthetic wastewaters (2.4-10.6 g N/L) at 35°C and at pH 9. The initial volume of the trapping solution (diluted H2SO4) was 10 times lower than that of the synthetic wastewater, aiming to concentrate the recovered nitrogen. The estimated ammonia transport constant (Km) ranged between (1.2 – 2.1)·10-6 m/s and water transport constant Kw between (2.8 – 8.2)·10-10 m/(s bar). Numerical determination of the model parameters revealed high R² values, demonstrating strong agreement with experimental data.
本研究介绍了气体渗透膜(GPM)接触器氮气回收的新建模方法,包括氨气和水的传输动力学。该模型的一个显著特点是它能够模拟水在膜上的传输,而这一点在大多数出版物中都被忽视了。渗透压差用于预测 GPM 中氨和水的传输行为。为开发、测试和校准模型而进行的实验研究了不同氮浓度下氨和水通过 GPM 的动态迁移。具体而言,在 35°C 和 pH 值为 9 的条件下,测试了 GPM 接触器从高浓度合成废水(2.4-10.6 克氮/升)中回收氮的情况。捕集溶液(稀 H2SO4)的初始体积比合成废水低 10 倍,目的是浓缩回收的氮。估计的氨迁移常数 (Km) 在 (1.2 - 2.1)-10-6 m/s 之间,水迁移常数 Kw 在 (2.8 - 8.2)-10-10 m/(s bar)之间。对模型参数的数值测定显示出很高的 R² 值,表明与实验数据非常吻合。
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引用次数: 0
Ambient solar-driven selenate reduction and removal from industrial brine using TiO2-based buoyant photocatalysts 利用基于 TiO2 的浮力光催化剂实现环境太阳能驱动的硒酸盐还原和工业盐水中的硒酸盐去除
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-08 DOI: 10.1016/j.watres.2024.122761
Aldrich Ngan , Zi Qi Chen , Aaron Bleasdale-Pollowy , Christopher Chan , Frank Gu
Selenium (Se), released from mining, power generation, and agriculture, is an environmentally and ecologically concerning contaminant due to its toxicity at elevated concentrations. Se oxyanions are highly soluble and mobile in aquatic ecosystems, and have a strong tendency to bioaccumulate and biomagnify, leading to acute and chronic toxicity in animals and humans. Photocatalysis presents a promising sustainable Se treatment solution and has successfully reduced and removed Se from mining-influenced matrices using UV-powered slurry photoreactor systems. Despite its potential, active photocatalytic water treatment faces significant challenges, particularly high operating costs and limited development of scalable deployment strategies, which hinder its real-world application. Herein, we adapt photocatalytic Se reduction and removal towards an easily deployable solar-driven semi-passive application using TiO2-based buoyant photocatalysts (BPCs). The results demonstrate successful semi-passive photocatalytic selenium reduction and removal using BPCs under ambient solar conditions, achieving up to 99.6 % removal of Se from an industrial brine matrix containing ∼3.5 mg/L of Se, despite challenges from dissolved oxygen and reactive oxygen species (ROS). We advance the mechanistic understanding of the ambient Se reduction pathway, successfully identifying Se(IV) as a reduction intermediate, and uncovering the role formic acid plays in suppressing the oxidative effects of ROS, enabling the complete reduction of Se. We address the major challenges to both Se treatment and environmental photocatalysis and highlight the potential of sustainable solar-driven and semi-passive photocatalytic processes to address environmental challenges like selenium.
采矿、发电和农业中释放的硒(Se)因其浓度升高时的毒性而成为一种环境和生态方面的污染物。硒氧阴离子在水生生态系统中具有高溶解性和流动性,极易发生生物累积和生物放大,从而导致动物和人类的急性和慢性中毒。光催化技术是一种很有前景的可持续硒处理解决方案,利用紫外线驱动的浆料光反应系统已成功减少和去除采矿影响基质中的硒。尽管具有潜力,但活性光催化水处理仍面临重大挑战,尤其是高昂的运营成本和可扩展部署策略的有限开发,阻碍了其在现实世界中的应用。在本文中,我们利用基于二氧化钛的浮力光催化剂(BPCs),将光催化还原和去除 Se 的方法调整为易于部署的太阳能驱动半被动式应用。结果表明,尽管面临溶解氧和活性氧(ROS)的挑战,在环境太阳能条件下使用 BPCs 成功实现了半被动光催化硒还原和去除,从含硒 3.5 mg/L 的工业盐水基质中去除高达 99.6% 的硒。我们推进了对环境硒还原途径的机理认识,成功确定了作为还原中间体的硒(IV),并揭示了甲酸在抑制 ROS 氧化作用方面的作用,从而实现了硒的完全还原。我们探讨了硒处理和环境光催化面临的主要挑战,并强调了可持续的太阳能驱动和半被动光催化过程在应对硒等环境挑战方面的潜力。
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引用次数: 0
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Water Research
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