Pub Date : 2024-08-02DOI: 10.1021/acsestwater.4c00357
Reeti Kumar, Suparna Mukherji
Photocatalysis studies were performed using graphene oxide–TiO2 (GOT) nanocomposite irradiated using 125 W UV and visible irradiation to investigate the effect of various water matrices, i.e., distilled water (DW), secondary treated wastewater (WWE), and lake water (LW) on the removal of organophosphorus pesticides from binary mixtures formulated using a 22 full factorial design. The EC60 and EC40 values of individual pesticides, determined from the dose response profile using the Ellman assay were used as the high and low concentrations, respectively. Photocatalysis was conducted at a GOT dose of 60 mg/L. For both Mixture-I, comprised of dichlorvos and malathion, and Mixture-II, comprised of parathion and phorate, degradation followed the order, DW > WWE > LW. After 80 min, the highest degradation of ∼80% was observed for Mixture I in DW under UV irradiation when the concentration of both pesticides was at EC40. Malathion displayed a higher rate and extent of degradation and mineralization compared to dichlorvos in all of the mixture combinations. Under similar reaction conditions, phorate and parathion demonstrated similar values of the first-order degradation rate constant. Dissolved organic matter (DOM) had a detrimental effect on pesticide degradation by blocking the active sites on the catalyst and by scavenging the oxidative radicals generated during irradiation. A decrease in SUVA254 in both WWE and LW during photocatalysis indicated the decomposition of aromatic moieties in DOM. After UV/visible photocatalysis, the lowest residual toxic effect, as measured in the Ellman assay, was observed in mixtures containing low initial concentration of both the pesticides.
使用 125 W 紫外线和可见光照射氧化石墨烯-二氧化钛（GOT）纳米复合材料进行光催化研究，以考察各种水基质（即蒸馏水（DW）、二级处理废水（WWE）和湖水（LW））对采用 22 全因子设计配制的二元混合物中有机磷农药的去除效果。根据埃尔曼试验的剂量反应曲线确定的单种农药的 EC60 和 EC40 值分别作为高浓度和低浓度。在 GOT 剂量为 60 毫克/升时进行光催化。由敌敌畏和马拉硫磷组成的混合物 I 和由对硫磷和甲拌磷组成的混合物 II 的降解顺序依次为 DW > WWE > LW。80 分钟后，在紫外线照射下，当两种杀虫剂的浓度均为 EC40 时，混合物 I 在 DW 中的降解率最高，达 80%。在所有混合物组合中，马拉硫磷的降解和矿化速度和程度均高于敌敌畏。在类似的反应条件下，甲拌磷和对硫磷的一阶降解速率常数值相似。溶解有机物（DOM）会阻塞催化剂上的活性位点，并清除辐照过程中产生的氧化自由基，从而对农药降解产生不利影响。在光催化过程中，WWE 和 LW 中的 SUVA254 均有所下降，这表明 DOM 中的芳香分子发生了分解。经过紫外线/可见光光催化处理后，在两种农药的初始浓度较低的混合物中观察到的残留毒性效应（通过埃尔曼检测法测量）最低。
{"title":"Assessment of Photocatalytic Efficiency of Graphene Oxide–TiO2 Nanocomposite for Removal of Binary Mixtures of Organophosphorus Pesticides from Water","authors":"Reeti Kumar, Suparna Mukherji","doi":"10.1021/acsestwater.4c00357","DOIUrl":"https://doi.org/10.1021/acsestwater.4c00357","url":null,"abstract":"Photocatalysis studies were performed using graphene oxide–TiO<sub>2</sub> (GOT) nanocomposite irradiated using 125 W UV and visible irradiation to investigate the effect of various water matrices, i.e., distilled water (DW), secondary treated wastewater (WWE), and lake water (LW) on the removal of organophosphorus pesticides from binary mixtures formulated using a 2<sup>2</sup> full factorial design. The EC<sub>60</sub> and EC<sub>40</sub> values of individual pesticides, determined from the dose response profile using the Ellman assay were used as the high and low concentrations, respectively. Photocatalysis was conducted at a GOT dose of 60 mg/L. For both Mixture-I, comprised of dichlorvos and malathion, and Mixture-II, comprised of parathion and phorate, degradation followed the order, DW > WWE > LW. After 80 min, the highest degradation of ∼80% was observed for Mixture I in DW under UV irradiation when the concentration of both pesticides was at EC<sub>40</sub>. Malathion displayed a higher rate and extent of degradation and mineralization compared to dichlorvos in all of the mixture combinations. Under similar reaction conditions, phorate and parathion demonstrated similar values of the first-order degradation rate constant. Dissolved organic matter (DOM) had a detrimental effect on pesticide degradation by blocking the active sites on the catalyst and by scavenging the oxidative radicals generated during irradiation. A decrease in SUVA<sub>254</sub> in both WWE and LW during photocatalysis indicated the decomposition of aromatic moieties in DOM. After UV/visible photocatalysis, the lowest residual toxic effect, as measured in the Ellman assay, was observed in mixtures containing low initial concentration of both the pesticides.","PeriodicalId":7078,"journal":{"name":"ACS Es&t Water","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881926","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-02DOI: 10.1021/acsestwater.4c00219
Thilini Maheshika Herath, Bei Zhang, Dhimas Dwinandha, Manabu Fujii
As a complementary or alternative approach to experiments, theoretical computation of adsorption between carbon materials and emerging aromatic organic contaminants (AOCs) is increasingly important in elucidating adsorption mechanisms and characteristics, as well as their predictions. In this study, the adsorption energies between graphene and 112 AOCs were first analyzed by density functional theory (DFT-D). By the use of quantum molecular descriptors, different machine learning (ML) algorithms were developed. EXtreme gradient boosting exhibited the best performance among the four ML algorithms investigated, showing the lowest root-mean-square percentage error of 4.5% for the test data set. Accordingly, the interpretable ML technique (i.e., SHAP) assessed the importance and dependence of descriptors in the adsorption mechanisms of AOCs to graphene. The global interpretation confirmed that the molecular-volume-induced van der Waals interactions including π–π stacking are dominant, whereas the other interactions (e.g., induced hydrogen and electrostatic interactions) are comparably less significant in the adsorption of most AOCs on graphene. In contrast, using local interpretation, hydrogen bonds and induced dipole interactions with surrounding water were identified as important explanatory variables in the adsorption of AOCs containing carbonyl and sulfur functional groups. Therefore, the developed DFT-D-based ML models could be a reference model for theoretical and experimental studies.
作为实验的补充或替代方法，碳材料与新出现的芳香族有机污染物（AOC）之间的吸附理论计算在阐明吸附机理、特征及其预测方面越来越重要。本研究首先利用密度泛函理论（DFT-D）分析了石墨烯与 112 种芳香族有机污染物之间的吸附能。利用量子分子描述符，开发了不同的机器学习（ML）算法。在所研究的四种 ML 算法中，EXtreme gradient boosting 算法表现最佳，在测试数据集上显示出最低的均方根百分比误差（4.5%）。因此，可解释的 ML 技术（即 SHAP）评估了描述符在 AOC 对石墨烯吸附机制中的重要性和依赖性。全局解释证实，在大多数 AOCs 在石墨烯上的吸附过程中，分子体积诱导的范德华相互作用（包括 π-π 堆积）占主导地位，而其他相互作用（如诱导的氢相互作用和静电相互作用）的重要性则相对较低。相反，通过局部解释，氢键和与周围水的诱导偶极相互作用被认为是含羰基和硫官能团的 AOC 吸附过程中的重要解释变量。因此，所建立的基于 DFT-D 的 ML 模型可以作为理论和实验研究的参考模型。
{"title":"Elucidating Adsorption Mechanisms and Characteristics of Emerging Aromatic Organic Contaminants to Graphene Material by Quantum Chemical Calculation Integrated with Interpretable Machine Learning","authors":"Thilini Maheshika Herath, Bei Zhang, Dhimas Dwinandha, Manabu Fujii","doi":"10.1021/acsestwater.4c00219","DOIUrl":"https://doi.org/10.1021/acsestwater.4c00219","url":null,"abstract":"As a complementary or alternative approach to experiments, theoretical computation of adsorption between carbon materials and emerging aromatic organic contaminants (AOCs) is increasingly important in elucidating adsorption mechanisms and characteristics, as well as their predictions. In this study, the adsorption energies between graphene and 112 AOCs were first analyzed by density functional theory (DFT-D). By the use of quantum molecular descriptors, different machine learning (ML) algorithms were developed. EXtreme gradient boosting exhibited the best performance among the four ML algorithms investigated, showing the lowest root-mean-square percentage error of 4.5% for the test data set. Accordingly, the interpretable ML technique (i.e., SHAP) assessed the importance and dependence of descriptors in the adsorption mechanisms of AOCs to graphene. The global interpretation confirmed that the molecular-volume-induced van der Waals interactions including π–π stacking are dominant, whereas the other interactions (e.g., induced hydrogen and electrostatic interactions) are comparably less significant in the adsorption of most AOCs on graphene. In contrast, using local interpretation, hydrogen bonds and induced dipole interactions with surrounding water were identified as important explanatory variables in the adsorption of AOCs containing carbonyl and sulfur functional groups. Therefore, the developed DFT-D-based ML models could be a reference model for theoretical and experimental studies.","PeriodicalId":7078,"journal":{"name":"ACS Es&t Water","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881924","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-02DOI: 10.1021/acsestwater.4c00185
Md. Moklesur Rahman, Marc Peipoch, Jinjun Kan, Matthew Sena, Bisesh Joshi, Dipankar Dwivedi, Arthur J. Gold, Peter M. Groffman, Joseph G. Galella, Shreeram Inamdar
Denitrification (DNF) and dissimilatory nitrate reduction to ammonium (DNRA) compete in reducing sediment conditions where DNF permanently removes nitrogen (N), while DNRA retains N with the conversion of nitrate (NO3–) to ammonium (NH4+). Thus, an increase in the level of DNRA can undermine permanent N removal. We investigated the relative magnitude and controls of these two processes at two milldam-affected riparian sites. DNRA (5.2–37.6 μg L–1 h–1) accounted for 10–79% of total NO3– reduction and was highest in riparian sediments with higher iron (Fe) and sodium (Na+) in groundwater. DNF was the primary mechanism for NO3– reduction when Fe and Na+ concentrations were low but when NO3– was elevated. DNRA rates were higher for treatments with higher dissolved organic carbon (DOC):NO3– and Fe:NO3– ratios, indicating the stimulation of both heterotrophic and Fe2+ driven autotrophic DNRA. DNF and DNRA rates and their microbial functional genes decreased with increasing sediment depths. These findings imply that hydrologically stagnant and persistently reducing conditions associated with relict milldams and similar anthropogenic structures may enhance DNRA at the expense of DNF and undermine permanent N removal in riparian zones. Thus, the effects of such structures need to be accounted for in watershed N management strategies.
{"title":"Dissimilatory Nitrate Reduction to Ammonium (DNRA) Can Undermine Nitrogen Removal Effectiveness of Persistently Reducing Riparian Sediments","authors":"Md. Moklesur Rahman, Marc Peipoch, Jinjun Kan, Matthew Sena, Bisesh Joshi, Dipankar Dwivedi, Arthur J. Gold, Peter M. Groffman, Joseph G. Galella, Shreeram Inamdar","doi":"10.1021/acsestwater.4c00185","DOIUrl":"https://doi.org/10.1021/acsestwater.4c00185","url":null,"abstract":"Denitrification (DNF) and dissimilatory nitrate reduction to ammonium (DNRA) compete in reducing sediment conditions where DNF permanently removes nitrogen (N), while DNRA retains N with the conversion of nitrate (NO<sub>3</sub><sup>–</sup>) to ammonium (NH<sub>4</sub><sup>+</sup>). Thus, an increase in the level of DNRA can undermine permanent N removal. We investigated the relative magnitude and controls of these two processes at two milldam-affected riparian sites. DNRA (5.2–37.6 μg L<sup>–1</sup> h<sup>–1</sup>) accounted for 10–79% of total NO<sub>3</sub><sup>–</sup> reduction and was highest in riparian sediments with higher iron (Fe) and sodium (Na<sup>+</sup>) in groundwater. DNF was the primary mechanism for NO<sub>3</sub><sup>–</sup> reduction when Fe and Na<sup>+</sup> concentrations were low but when NO<sub>3</sub><sup>–</sup> was elevated. DNRA rates were higher for treatments with higher dissolved organic carbon (DOC):NO<sub>3</sub><sup>–</sup> and Fe:NO<sub>3</sub><sup>–</sup> ratios, indicating the stimulation of both heterotrophic and Fe<sup>2+</sup> driven autotrophic DNRA. DNF and DNRA rates and their microbial functional genes decreased with increasing sediment depths. These findings imply that hydrologically stagnant and persistently reducing conditions associated with relict milldams and similar anthropogenic structures may enhance DNRA at the expense of DNF and undermine permanent N removal in riparian zones. Thus, the effects of such structures need to be accounted for in watershed N management strategies.","PeriodicalId":7078,"journal":{"name":"ACS Es&t Water","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881977","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-02DOI: 10.1021/acsestwater.4c00262
Wellington Arthur, Zach Morgan, Marco Reina Antillon, Edward Drabold, Daniel E. Wells, Dianna V. Bourassa, Qichen Wang, Brendan T. Higgins
Poultry processing wastewater (PPW) is a nutrient-rich effluent with the potential for reuse in crop irrigation. This study investigated transforming PPW into a hydroponic nutrient solution using a pilot scale “poultryponics” system operated continuously for 222 days. The system treated ∼57 L d–1 of real PPW and consisted of bioreactors (inoculated with a consortium of microalgae and nitrifying bacteria), clarifiers, membrane filters, a UV disinfection unit, and a deep-water hydroponic system. The system was evaluated in terms of nitrogen transformation, organic removal efficiency, and pathogen levels. Although soluble organic removal efficiencies (sCOD) were high (>80%) in all bioreactors, nitrification was limited due to high organic loading (350–800 mg sCOD L–1), relatively short retention time (24 h), and low dissolved oxygen levels (<3.5 mg O2 L–1). Grow beds showed significant nitrification, indicating the importance of upstream organic removal. CO2 supplementation (0.5% v/v) in bioreactors did not promote nitrification in the bioreactors but was beneficial for nitrification in grow beds due to pH-modulating effects. Microbiological analyses showed no Salmonella detection in bioreactors and substantial reductions in total coliform (∼40%) and aerobic plate counts (∼30%) after UV treatment. These findings demonstrate the sustainable and safe reuse of nutrient-rich industrial effluents in agriculture.
{"title":"Pilot-Scale Evaluation of Poultryponics: Insights into Nitrogen Utilization and Food Pathogen Dynamics","authors":"Wellington Arthur, Zach Morgan, Marco Reina Antillon, Edward Drabold, Daniel E. Wells, Dianna V. Bourassa, Qichen Wang, Brendan T. Higgins","doi":"10.1021/acsestwater.4c00262","DOIUrl":"https://doi.org/10.1021/acsestwater.4c00262","url":null,"abstract":"Poultry processing wastewater (PPW) is a nutrient-rich effluent with the potential for reuse in crop irrigation. This study investigated transforming PPW into a hydroponic nutrient solution using a pilot scale “poultryponics” system operated continuously for 222 days. The system treated ∼57 L d<sup>–1</sup> of real PPW and consisted of bioreactors (inoculated with a consortium of microalgae and nitrifying bacteria), clarifiers, membrane filters, a UV disinfection unit, and a deep-water hydroponic system. The system was evaluated in terms of nitrogen transformation, organic removal efficiency, and pathogen levels. Although soluble organic removal efficiencies (sCOD) were high (>80%) in all bioreactors, nitrification was limited due to high organic loading (350–800 mg sCOD L<sup>–1</sup>), relatively short retention time (24 h), and low dissolved oxygen levels (<3.5 mg O<sub>2</sub> L<sup>–1</sup>). Grow beds showed significant nitrification, indicating the importance of upstream organic removal. CO<sub>2</sub> supplementation (0.5% v/v) in bioreactors did not promote nitrification in the bioreactors but was beneficial for nitrification in grow beds due to pH-modulating effects. Microbiological analyses showed no <i>Salmonella</i> detection in bioreactors and substantial reductions in total coliform (∼40%) and aerobic plate counts (∼30%) after UV treatment. These findings demonstrate the sustainable and safe reuse of nutrient-rich industrial effluents in agriculture.","PeriodicalId":7078,"journal":{"name":"ACS Es&t Water","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881925","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-02DOI: 10.1021/acsestwater.4c00214
Suffiyan Safdar, Anne J. Jefferson, David M. Costello, Andrew Blinn
Suspended sediment is a critical water quality parameter and an indicator of geomorphic processes, but suspended sediment dynamics in urban streams may not conform to the first-flush model widely used for other pollutants. We analyzed discharge and turbidity data for 367 events from three urban watersheds (impervious cover 16–45%) in Cleveland, Ohio (USA). Less intensely urbanized watersheds exhibit higher turbidity compared to that of the most highly urbanized watershed. Proportionally, more counterclockwise hysteresis is observed in the two less urbanized watersheds, and more clockwise hysteresis occurs in the highly urbanized watershed. However, hysteresis patterns are driven by different mechanisms in each watershed, and geomorphic analysis was critical to identifying the underlying mechanisms. In the least urbanized watershed, spatial rainfall variability controls sediment hysteresis. In the intermediate watershed, the erosion of upstream weathered shale banks during dry periods plays a significant role in the sediment supply and shaping hysteresis. In the most urbanized watershed, high eroding banks in downstream reaches lead to more frequent clockwise hysteresis. Overall, we suggest that as the impervious surfaces increase, the availability of instream sediments (bed and banks) plays an increased role in suspended sediment dynamics, and geomorphology remains essential for guiding management decisions.
{"title":"Urbanization and Suspended Sediment Transport Dynamics: A Comparative Study of Watersheds with Varying Degree of Urbanization Using Concentration-Discharge Hysteresis","authors":"Suffiyan Safdar, Anne J. Jefferson, David M. Costello, Andrew Blinn","doi":"10.1021/acsestwater.4c00214","DOIUrl":"https://doi.org/10.1021/acsestwater.4c00214","url":null,"abstract":"Suspended sediment is a critical water quality parameter and an indicator of geomorphic processes, but suspended sediment dynamics in urban streams may not conform to the first-flush model widely used for other pollutants. We analyzed discharge and turbidity data for 367 events from three urban watersheds (impervious cover 16–45%) in Cleveland, Ohio (USA). Less intensely urbanized watersheds exhibit higher turbidity compared to that of the most highly urbanized watershed. Proportionally, more counterclockwise hysteresis is observed in the two less urbanized watersheds, and more clockwise hysteresis occurs in the highly urbanized watershed. However, hysteresis patterns are driven by different mechanisms in each watershed, and geomorphic analysis was critical to identifying the underlying mechanisms. In the least urbanized watershed, spatial rainfall variability controls sediment hysteresis. In the intermediate watershed, the erosion of upstream weathered shale banks during dry periods plays a significant role in the sediment supply and shaping hysteresis. In the most urbanized watershed, high eroding banks in downstream reaches lead to more frequent clockwise hysteresis. Overall, we suggest that as the impervious surfaces increase, the availability of instream sediments (bed and banks) plays an increased role in suspended sediment dynamics, and geomorphology remains essential for guiding management decisions.","PeriodicalId":7078,"journal":{"name":"ACS Es&t Water","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881930","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-02DOI: 10.1021/acsestwater.4c00198
Mahlet M. Kebede, Leigh G. Terry, T. Prabhakar Clement, Mesfin M. Mekonnen
Per- and polyfluoroalkyl substances (PFAS) released from common consumer products, such as cosmetics and carpets, are nonpoint sources of environmental contamination. However, detailed information on PFAS mass and emission rates from these products is limited. Here, we propose a methodology to develop PFAS footprint from the manufacturing and supply chain data of cosmetics and carpets. Our analysis combines geospatial and statistical assessments to understand how the production and consumption of these products contribute to existing PFAS contamination hotspots in the Continental United States (CONUS). Statewide mass estimations revealed that North Carolina and New York contribute to the major PFAS mass released from cosmetics, while Georgia and California contribute to the major PFAS mass released from carpets. The average per capita PFAS footprint from carpets and cosmetics is about 103 mg/year. Upon disposal, over 60% of the mass eventually ends up in landfills. The accumulation of PFAS stocks in landfills, primarily from carpets and to some extent from cosmetics, highlights the critical need to cease the production and use of PFAS in consumer products. Coastal counties are particularly vulnerable due to higher population and therefore higher consumption of these PFAS-tainted consumer products. Additionally, counties with densely populated areas and with preexisting contamination sources would face increased vulnerability to PFAS contamination released from various consumer products.
{"title":"Mapping Per- and Polyfluoroalkyl Substance Footprint from Cosmetics and Carpets across the Continental United States","authors":"Mahlet M. Kebede, Leigh G. Terry, T. Prabhakar Clement, Mesfin M. Mekonnen","doi":"10.1021/acsestwater.4c00198","DOIUrl":"https://doi.org/10.1021/acsestwater.4c00198","url":null,"abstract":"Per- and polyfluoroalkyl substances (PFAS) released from common consumer products, such as cosmetics and carpets, are nonpoint sources of environmental contamination. However, detailed information on PFAS mass and emission rates from these products is limited. Here, we propose a methodology to develop PFAS footprint from the manufacturing and supply chain data of cosmetics and carpets. Our analysis combines geospatial and statistical assessments to understand how the production and consumption of these products contribute to existing PFAS contamination hotspots in the Continental United States (CONUS). Statewide mass estimations revealed that North Carolina and New York contribute to the major PFAS mass released from cosmetics, while Georgia and California contribute to the major PFAS mass released from carpets. The average per capita PFAS footprint from carpets and cosmetics is about 103 mg/year. Upon disposal, over 60% of the mass eventually ends up in landfills. The accumulation of PFAS stocks in landfills, primarily from carpets and to some extent from cosmetics, highlights the critical need to cease the production and use of PFAS in consumer products. Coastal counties are particularly vulnerable due to higher population and therefore higher consumption of these PFAS-tainted consumer products. Additionally, counties with densely populated areas and with preexisting contamination sources would face increased vulnerability to PFAS contamination released from various consumer products.","PeriodicalId":7078,"journal":{"name":"ACS Es&t Water","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881979","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-01DOI: 10.1021/acsestwater.4c00566
Ying Jie Zheng, Liang Rui Zhu, Jun Jiang Luo, Hao Lin Zou, Hong Qun Luo, Nian Bing Li, Bang Lin Li
On-site analysis of bacteria is important, but high-practicality methods are challenging due to their limited sensitivity and weak anti-interference. Herein, nitrocellulose (NC) membranes with hydrophilic characteristics and porous structures are utilized to filter those small coexisting substances in samples and selectively enrich target bacteria at the NC surfaces. To visualize bacteria with enhanced stability and sensitivity, the in situ growth of plasmonic Au nanocrystals on bacteria is implemented via the incubation of the bacterium-loaded NC membranes in Au reaction solutions. The bacteria are remarkably stained by the plasmonic Au nanocrystals, exhibiting responsive color changes for quantitative analysis. First, bacteria are visualized by in situ grown Au nanocrystals. In comparison with the presynthetic Au nanocrystals, those chemicals in Au reaction solutions are more stable, which ensures comparable stability and reproductivity. Second, the bacterium responses are amplified via plasmonic chemical reactions. Those Au nanocrystals are considered not only visual probes but also signal amplifiers. Overall, the protocol of Au-stained bacteria on NC membranes facilitates the on-site microbial analysis with characteristics of high simplicity, speediness, sensitivity, stability, and anti-interference, largely contributing to the progress of nanotechnologies from fundamental research to practical applications.
{"title":"In Situ Grown Gold Nanoparticles Enable Plasmonic Staining of Bacteria for High-Performance On-Site Microbial Analysis in Drinking Water","authors":"Ying Jie Zheng, Liang Rui Zhu, Jun Jiang Luo, Hao Lin Zou, Hong Qun Luo, Nian Bing Li, Bang Lin Li","doi":"10.1021/acsestwater.4c00566","DOIUrl":"https://doi.org/10.1021/acsestwater.4c00566","url":null,"abstract":"On-site analysis of bacteria is important, but high-practicality methods are challenging due to their limited sensitivity and weak anti-interference. Herein, nitrocellulose (NC) membranes with hydrophilic characteristics and porous structures are utilized to filter those small coexisting substances in samples and selectively enrich target bacteria at the NC surfaces. To visualize bacteria with enhanced stability and sensitivity, the in situ growth of plasmonic Au nanocrystals on bacteria is implemented via the incubation of the bacterium-loaded NC membranes in Au reaction solutions. The bacteria are remarkably stained by the plasmonic Au nanocrystals, exhibiting responsive color changes for quantitative analysis. First, bacteria are visualized by in situ grown Au nanocrystals. In comparison with the presynthetic Au nanocrystals, those chemicals in Au reaction solutions are more stable, which ensures comparable stability and reproductivity. Second, the bacterium responses are amplified via plasmonic chemical reactions. Those Au nanocrystals are considered not only visual probes but also signal amplifiers. Overall, the protocol of Au-stained bacteria on NC membranes facilitates the on-site microbial analysis with characteristics of high simplicity, speediness, sensitivity, stability, and anti-interference, largely contributing to the progress of nanotechnologies from fundamental research to practical applications.","PeriodicalId":7078,"journal":{"name":"ACS Es&t Water","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881931","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The contamination of natural water bodies with dyes and other refractory compounds is a menacing issue in developing nations. Despite stringent laws, industrial effluent is not managed efficiently, as it incurs additional cost. Hence, the present research focuses on sustainable mitigation of refractory contaminants using a self-driven bioelectro-Fenton (BEF) system. The iron-activated charcoal (Gt-Fe/AC) cathode-cum-Fenton catalyst used in this investigation was synthesized using waste green tea extract as a biogenic agent. The green catalyst-driven BEF system (Gt-Fe/AC-MFC) achieved a maximum power density of 111.7 ± 3.1 mW/m2 and a maximum operating voltage of 108 ± 3 mV, while parallelly degrading 20 mg/L of Coomassie Brilliant Blue (CBB) dye almost entirely in 300 min at a neutral pH. Additionally, high removal of Congo red dye (96.8 ± 1.2%) and methylparaben (90.9 ± 0.6%) was attained under similar operating conditions. Moreover, the Fe-AC-catalyzed BEF performed fairly well in treating spiked real wastewater and exhibited remarkable stability, with only a 3% decrease in CBB removal efficiency after 10 continuous cycles and 0.11% drop in cathodic current per cycle. Hence, this BEF system can be a sustainable oxidative technology to tackle refractory wastewater in resource-constricted regions.
{"title":"Green-Activated Charcoal-Anchored Iron Oxide-Driven Microbial Electro-Fenton System for Sustainable Mitigation of Refractory Contaminants","authors":"Rishabh Raj, Anil Dhanda, Sovik Das, Makarand Madhao Ghangrekar","doi":"10.1021/acsestwater.4c00402","DOIUrl":"https://doi.org/10.1021/acsestwater.4c00402","url":null,"abstract":"The contamination of natural water bodies with dyes and other refractory compounds is a menacing issue in developing nations. Despite stringent laws, industrial effluent is not managed efficiently, as it incurs additional cost. Hence, the present research focuses on sustainable mitigation of refractory contaminants using a self-driven bioelectro-Fenton (BEF) system. The iron-activated charcoal (Gt-Fe/AC) cathode-cum-Fenton catalyst used in this investigation was synthesized using waste green tea extract as a biogenic agent. The green catalyst-driven BEF system (Gt-Fe/AC-MFC) achieved a maximum power density of 111.7 ± 3.1 mW/m<sup>2</sup> and a maximum operating voltage of 108 ± 3 mV, while parallelly degrading 20 mg/L of Coomassie Brilliant Blue (CBB) dye almost entirely in 300 min at a neutral pH. Additionally, high removal of Congo red dye (96.8 ± 1.2%) and methylparaben (90.9 ± 0.6%) was attained under similar operating conditions. Moreover, the Fe-AC-catalyzed BEF performed fairly well in treating spiked real wastewater and exhibited remarkable stability, with only a 3% decrease in CBB removal efficiency after 10 continuous cycles and 0.11% drop in cathodic current per cycle. Hence, this BEF system can be a sustainable oxidative technology to tackle refractory wastewater in resource-constricted regions.","PeriodicalId":7078,"journal":{"name":"ACS Es&t Water","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881928","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Current research on advanced oxidation processes often focuses on removing individual organic contaminants, sometimes overlooking the impact of microplastics (MPs) on mass transfer. Real-time and precise monitoring through experimental measurements is challenging. In this study, we used computational fluid dynamics simulations to examine the effect of MPs on mass transfer in a flow-through electro-peroxone process. Our findings revealed that MPs decreased the concentration of hydroxyl radicals at the electrochemical cathode/solution interface. However, there was no significant impact on the concentrations and diffusion pathways of O3 in the inlet gas phase and hydrogen peroxide on the electrochemical cathode surface. Additionally, the average size of MPs increased from 135.0 to 750.0 μm, and their count rose from 7474 to 10,924 particles/L. This was accompanied by increases in average turbulent kinetic energy and turbulent dissipation rate by 0.027 and 0.018 km2/s2, and 0.041 and 0.702 m2/s3, respectively. These changes suggested that the enlargement and increased count of MPs hindered liquid flow, reducing the efficiency of converting gaseous O3 to aqueous O3. Consequently, this diminished the removal efficiency of pollutants in the electro-peroxone process. These insights are crucial for developing more efficient advanced oxidation processes for the simultaneous removal of MPs and pollutants.
{"title":"Effect of Microplastics on the Flow-Through Electro-Peroxone Process: A Computational Fluid Dynamics Simulation","authors":"Jingjing Yao, Dong-Sheng Li, Jianbei Qiu, Xuhui Xu, Haipu Li, Hui Ying Yang","doi":"10.1021/acsestwater.4c00079","DOIUrl":"https://doi.org/10.1021/acsestwater.4c00079","url":null,"abstract":"Current research on advanced oxidation processes often focuses on removing individual organic contaminants, sometimes overlooking the impact of microplastics (MPs) on mass transfer. Real-time and precise monitoring through experimental measurements is challenging. In this study, we used computational fluid dynamics simulations to examine the effect of MPs on mass transfer in a flow-through electro-peroxone process. Our findings revealed that MPs decreased the concentration of hydroxyl radicals at the electrochemical cathode/solution interface. However, there was no significant impact on the concentrations and diffusion pathways of O<sub>3</sub> in the inlet gas phase and hydrogen peroxide on the electrochemical cathode surface. Additionally, the average size of MPs increased from 135.0 to 750.0 μm, and their count rose from 7474 to 10,924 particles/L. This was accompanied by increases in average turbulent kinetic energy and turbulent dissipation rate by 0.027 and 0.018 km<sup>2</sup>/s<sup>2</sup>, and 0.041 and 0.702 m<sup>2</sup>/s<sup>3</sup>, respectively. These changes suggested that the enlargement and increased count of MPs hindered liquid flow, reducing the efficiency of converting gaseous O<sub>3</sub> to aqueous O<sub>3</sub>. Consequently, this diminished the removal efficiency of pollutants in the electro-peroxone process. These insights are crucial for developing more efficient advanced oxidation processes for the simultaneous removal of MPs and pollutants.","PeriodicalId":7078,"journal":{"name":"ACS Es&t Water","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881927","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The reuse of ozone-treated wastewater, especially for agricultural irrigation, is a crucial strategy to address water scarcity. However, the storage of ozone-treated wastewater contributes to the growth of potentially pathogenic bacteria. This study explores using nanosilver-loaded hydrogels as liners in storage containers to provide sustained antibacterial effects. The results indicate that the antibacterial effect of nanosilver-loaded hydrogels, possessing a three-dimensional porous network structure, is more efficient due to a relatively low concentration of nanosilver in the stored water while increasing the concentration in the immediate vicinity of K-12 Escherichia coli (E. coli) anchored in the pores. The antibacterial mechanism of nanosilver against K-12 E. coli involves a process termed pseudo cuproptosis. Nanosilver did not lead to a significant reduction in basal or ATP-linked respiration, but it did notably decrease the spare capacity of respiration and disrupt bacterial metabolism by binding to lipoylated proteins, including 2-oxoglutarate dehydrogenase E2 subunit (sucB) and dihydrolipoamide S-acetyltransferase (aceF), which are related to the tricarboxylic acid cycle. It also leads to the oligomerization of aceF, and finally causes proteotoxicity to the K-12 E. coli. This process is distinct from known bacterial growth stasis pathways. By understanding this mechanism, the dosage of nanosilver can be effectively controlled, ensuring the safety and efficacy of wastewater reuse for agricultural purposes in the near future.
{"title":"Nanosilver-Induced Pseudo Cuproptosis of Potentially Pathogenic Bacteria during the Storage of Ozone-Treated Wastewater","authors":"Qiang Sun, Qiang He, Xuebin Hu, Hong Li, Yufei Li, Qiquan Zheng, Muxinjian Luo, Qixin Pan, Sarfaraz Khan, Liangliang Dai, Yujiao Dong","doi":"10.1021/acsestwater.4c00235","DOIUrl":"https://doi.org/10.1021/acsestwater.4c00235","url":null,"abstract":"The reuse of ozone-treated wastewater, especially for agricultural irrigation, is a crucial strategy to address water scarcity. However, the storage of ozone-treated wastewater contributes to the growth of potentially pathogenic bacteria. This study explores using nanosilver-loaded hydrogels as liners in storage containers to provide sustained antibacterial effects. The results indicate that the antibacterial effect of nanosilver-loaded hydrogels, possessing a three-dimensional porous network structure, is more efficient due to a relatively low concentration of nanosilver in the stored water while increasing the concentration in the immediate vicinity of K-12 <i>Escherichia coli</i> (<i>E. coli</i>) anchored in the pores. The antibacterial mechanism of nanosilver against K-12 <i>E. coli</i> involves a process termed pseudo cuproptosis. Nanosilver did not lead to a significant reduction in basal or ATP-linked respiration, but it did notably decrease the spare capacity of respiration and disrupt bacterial metabolism by binding to lipoylated proteins, including 2-oxoglutarate dehydrogenase E2 subunit (sucB) and dihydrolipoamide S-acetyltransferase (aceF), which are related to the tricarboxylic acid cycle. It also leads to the oligomerization of aceF, and finally causes proteotoxicity to the K-12 <i>E. coli</i>. This process is distinct from known bacterial growth stasis pathways. By understanding this mechanism, the dosage of nanosilver can be effectively controlled, ensuring the safety and efficacy of wastewater reuse for agricultural purposes in the near future.","PeriodicalId":7078,"journal":{"name":"ACS Es&t Water","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141862750","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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