Weiyi Pan,Kaiyue Li,Junwei Zhang,Yanghua Duan,Ruoyu Wang,Jouke E. Dykstra,Menachem Elimelech
Electrodialysis (ED) is an electrically driven separation technology that has been widely applied in various industrial sectors (e.g., desalination and food processing). While recent research has focused on developing novel ion-exchange membrane (IEM) materials, the detrimental effects of inorganic scaling in ED systems, particularly on energy consumption and ion selectivity, remain largely overlooked. In this study, we systematically investigated the impact of inorganic scaling (i.e., gypsum) on ED performance under varying operating conditions, including applied current densities ranging from 20% to 100% of the limiting current density and flow rates ranging from 4 to 12 mL min–1 (linear velocities from 0.33 to 1 cm min–1). Through precise measurements of input energy, solution composition evolution, and solid-phase characterization, we found that scaling not only increased energy consumption (up to 3-fold compared to nonscaling conditions) but also significantly changed selectivity. Specifically, we found that sodium–calcium and chloride–sulfate selectivities exhibited up to a 7-fold change relative to the initial value when the salt removal from the diluate solution reached approximately 30%. By integrating process modeling with experimental data, we confirmed that these changes in selectivity were directly attributable to gypsum formation on the surface of the IEM. These findings advance our understanding of inorganic scaling effects in ED and offer valuable guidance for optimizing real-world ED operation.
电渗析（ED）是一种电驱动分离技术，已广泛应用于各种工业部门（如海水淡化和食品加工）。虽然最近的研究集中在开发新型离子交换膜（IEM）材料上，但无机结垢在ED系统中的有害影响，特别是对能量消耗和离子选择性的影响，在很大程度上仍然被忽视。在本研究中，我们系统地研究了无机结垢（即石膏）在不同操作条件下对ED性能的影响，包括应用电流密度为极限电流密度的20%至100%，流速为4至12 mL min-1（线速度为0.33至1 cm min-1）。通过精确测量输入能量，溶液组成演变和固相表征，我们发现缩放不仅增加了能量消耗（与非缩放条件相比高达3倍），而且显着改变了选择性。具体来说，我们发现当稀溶液中的盐去除率达到约30%时，钠-钙和氯化物-硫酸盐的选择性相对于初始值表现出高达7倍的变化。通过将过程建模与实验数据相结合，我们证实了这些选择性的变化直接归因于IEM表面的石膏形成。这些发现促进了我们对ED中无机结垢效应的理解，并为优化实际ED操作提供了有价值的指导。
{"title":"Inorganic Scaling in Electrodialysis: Mechanistic Insights and Impact on Energy Efficiency and Ion Selectivity","authors":"Weiyi Pan,Kaiyue Li,Junwei Zhang,Yanghua Duan,Ruoyu Wang,Jouke E. Dykstra,Menachem Elimelech","doi":"10.1021/acs.est.5c16084","DOIUrl":"https://doi.org/10.1021/acs.est.5c16084","url":null,"abstract":"Electrodialysis (ED) is an electrically driven separation technology that has been widely applied in various industrial sectors (e.g., desalination and food processing). While recent research has focused on developing novel ion-exchange membrane (IEM) materials, the detrimental effects of inorganic scaling in ED systems, particularly on energy consumption and ion selectivity, remain largely overlooked. In this study, we systematically investigated the impact of inorganic scaling (i.e., gypsum) on ED performance under varying operating conditions, including applied current densities ranging from 20% to 100% of the limiting current density and flow rates ranging from 4 to 12 mL min–1 (linear velocities from 0.33 to 1 cm min–1). Through precise measurements of input energy, solution composition evolution, and solid-phase characterization, we found that scaling not only increased energy consumption (up to 3-fold compared to nonscaling conditions) but also significantly changed selectivity. Specifically, we found that sodium–calcium and chloride–sulfate selectivities exhibited up to a 7-fold change relative to the initial value when the salt removal from the diluate solution reached approximately 30%. By integrating process modeling with experimental data, we confirmed that these changes in selectivity were directly attributable to gypsum formation on the surface of the IEM. These findings advance our understanding of inorganic scaling effects in ED and offer valuable guidance for optimizing real-world ED operation.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"15 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147493162","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tian Tao,Bo-Xuan Zhang,Zhiyang Li,Qiuju Li,Xiaojie Wei,Ziwei Ye,Boyang Zong,Xiang-Zhou Meng,Shun Mao
Perfluoroalkyl substances (PFASs) pose significant environmental risk due to their persistence and toxicity, while the structural similarity among congeners complicates selective detection in complex matrices. This study presents a β-cyclodextrin (β-CD)-oriented molecular imprinting strategy integrated with an extended gate field-effect transistor (EGFET) sensor. The approach leverages the hydrophobic cavity of β-CD to achieve preorientation of PFAS template molecules followed by electropolymerization of o-phenylenediamine (o-PD) in the presence of [BMIM][BF4] ionic liquid (IL) to form molecularly imprinted polymers (MIPs) with enhanced recognition specificity. PFAS binding to imprinted sites induces interfacial charge redistribution, which is amplified through field-effect modulation and converted to measurable threshold voltage shift. This multiple recognition enables differential binding patterns for structurally similar PFAS molecules, achieving femtomolar detection limits (25 fM for perfluorooctanesulfonate, 73 fM for perfluorodecanoic acid) with excellent selectivity. The sensors demonstrate robust performance across diverse environmental matrices, including tap water, river water, chromium electroplating wastewater, and surrounding groundwater. Real-world application of the sensor to industrial electroplating sites reveals distinct contamination levels spanning 10-9 to 10-5 M in wastewater and 10-12 to 10-7 M in groundwater, which represent outstanding analytical correlation validated against liquid chromatography-tandem mass spectrometry (LC-MS/MS). The developed sensor provides a practical solution for rapid, simplified PFAS screening in a contaminated environmental medium.
{"title":"Femtomolar Congener-Selective Detection of Perfluoroalkyl Substances in Water by a Cyclodextrin-Oriented Molecularly Imprinted Transistor Sensor.","authors":"Tian Tao,Bo-Xuan Zhang,Zhiyang Li,Qiuju Li,Xiaojie Wei,Ziwei Ye,Boyang Zong,Xiang-Zhou Meng,Shun Mao","doi":"10.1021/acs.est.5c15581","DOIUrl":"https://doi.org/10.1021/acs.est.5c15581","url":null,"abstract":"Perfluoroalkyl substances (PFASs) pose significant environmental risk due to their persistence and toxicity, while the structural similarity among congeners complicates selective detection in complex matrices. This study presents a β-cyclodextrin (β-CD)-oriented molecular imprinting strategy integrated with an extended gate field-effect transistor (EGFET) sensor. The approach leverages the hydrophobic cavity of β-CD to achieve preorientation of PFAS template molecules followed by electropolymerization of o-phenylenediamine (o-PD) in the presence of [BMIM][BF4] ionic liquid (IL) to form molecularly imprinted polymers (MIPs) with enhanced recognition specificity. PFAS binding to imprinted sites induces interfacial charge redistribution, which is amplified through field-effect modulation and converted to measurable threshold voltage shift. This multiple recognition enables differential binding patterns for structurally similar PFAS molecules, achieving femtomolar detection limits (25 fM for perfluorooctanesulfonate, 73 fM for perfluorodecanoic acid) with excellent selectivity. The sensors demonstrate robust performance across diverse environmental matrices, including tap water, river water, chromium electroplating wastewater, and surrounding groundwater. Real-world application of the sensor to industrial electroplating sites reveals distinct contamination levels spanning 10-9 to 10-5 M in wastewater and 10-12 to 10-7 M in groundwater, which represent outstanding analytical correlation validated against liquid chromatography-tandem mass spectrometry (LC-MS/MS). The developed sensor provides a practical solution for rapid, simplified PFAS screening in a contaminated environmental medium.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"92 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147495110","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Matt S. Sparks,James D. East,Fernando Garcia-Menendez,Erwan Monier,Rebecca K. Saari
Without emission reductions, climate change may increase ozone and PM2.5 air pollution in the United States; however, we do not know how this will affect air quality alerts that prompt people to stay indoors. Here, we use an integrated modeling framework to find distributions of daily Air Quality Index (AQI) during the smog season at the start, middle, and end-of-century. Considering natural variability, climate change may cause air quality alerts to double (increase by a factor of 2 ± 0.2) by 2100. Days when both ozone and PM2.5 exceed alert thresholds quadruple (4.3 ± 1.2). More than 100,000,000 (±45,000,000) people experience mean air pollution deemed “Unhealthy for Sensitive Groups”, a growth of 7 (±3) times compared to 2000. If people follow alerts by staying inside, they reduce exposure to outdoor-generated pollutants. Their health benefits are similar whether the alert is caused by ozone or PM2.5. Senior (age 65+) populations receive much higher benefits per day by adapting (e.g., 95CI for PM2.5: $4.60 to $147) as young adults (age 18–35; 95CI: $0.15 to $4.22)─more than 45 times higher on average. This disproportionate impact requires targeted messaging and guidance, especially as climate-related risks rise.
{"title":"Air Quality Alerts, Health Impacts, and Adaptation Implications Under Varying Climate Policy","authors":"Matt S. Sparks,James D. East,Fernando Garcia-Menendez,Erwan Monier,Rebecca K. Saari","doi":"10.1021/acs.est.5c12522","DOIUrl":"https://doi.org/10.1021/acs.est.5c12522","url":null,"abstract":"Without emission reductions, climate change may increase ozone and PM2.5 air pollution in the United States; however, we do not know how this will affect air quality alerts that prompt people to stay indoors. Here, we use an integrated modeling framework to find distributions of daily Air Quality Index (AQI) during the smog season at the start, middle, and end-of-century. Considering natural variability, climate change may cause air quality alerts to double (increase by a factor of 2 ± 0.2) by 2100. Days when both ozone and PM2.5 exceed alert thresholds quadruple (4.3 ± 1.2). More than 100,000,000 (±45,000,000) people experience mean air pollution deemed “Unhealthy for Sensitive Groups”, a growth of 7 (±3) times compared to 2000. If people follow alerts by staying inside, they reduce exposure to outdoor-generated pollutants. Their health benefits are similar whether the alert is caused by ozone or PM2.5. Senior (age 65+) populations receive much higher benefits per day by adapting (e.g., 95CI for PM2.5: $4.60 to $147) as young adults (age 18–35; 95CI: $0.15 to $4.22)─more than 45 times higher on average. This disproportionate impact requires targeted messaging and guidance, especially as climate-related risks rise.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"60 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147493154","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jane A. Sedlak, Eric Siciliano Rego, Sarah Aarons, Vicki H. Grassian
Atmospheric processing of Biomass Burning Aerosols (BBAs) changes the chemical composition of these aerosols, potentially affecting iron (Fe) solubility. To probe these changes, we conducted laboratory experiments using maghemite nanoparticles as a representative iron oxide phase. Dissolved Fe(II) concentrations were approximately 3 times higher, and total dissolved Fe was 1.4 times higher, when both catechol and oxalate were present compared to experiments with one organic compound (48 h, pH 2, HCl). In situ attenuated total reflectance Fourier transform infrared spectroscopy of the maghemite-aqueous interface shows that oxalate initially outcompetes catechol for surface binding, but as the reaction progresses, catechol forms inner-sphere complexes, promoting reductive dissolution. Iron isotope measurements indicate that oxalate-assisted dissolution accounts for most of the iron released during the first 6 h of the reaction, while catechol-assisted dissolution contributes substantially in later stages. The observed synergy in Fe(II) and total dissolved Fe arises from a combination of solution phase and surface reactions that occur when both compounds are present. These results suggest that the dark atmospheric processing of BBA can increase dissolved Fe(II) and total dissolved Fe, potentially contributing to the adverse health effects of smoke. These findings also highlight that mixtures produce outcomes not predictable from single compounds alone.
{"title":"Integrating Iron Isotope and Oxidation State Measurements with In Situ Vibrational Spectroscopy to Understand Iron Dissolution during Atmospheric Processing of Iron Oxides in Wildfire Smoke","authors":"Jane A. Sedlak, Eric Siciliano Rego, Sarah Aarons, Vicki H. Grassian","doi":"10.1021/acs.est.5c15449","DOIUrl":"https://doi.org/10.1021/acs.est.5c15449","url":null,"abstract":"Atmospheric processing of Biomass Burning Aerosols (BBAs) changes the chemical composition of these aerosols, potentially affecting iron (Fe) solubility. To probe these changes, we conducted laboratory experiments using maghemite nanoparticles as a representative iron oxide phase. Dissolved Fe(II) concentrations were approximately 3 times higher, and total dissolved Fe was 1.4 times higher, when both catechol and oxalate were present compared to experiments with one organic compound (48 h, pH 2, HCl). In situ attenuated total reflectance Fourier transform infrared spectroscopy of the maghemite-aqueous interface shows that oxalate initially outcompetes catechol for surface binding, but as the reaction progresses, catechol forms inner-sphere complexes, promoting reductive dissolution. Iron isotope measurements indicate that oxalate-assisted dissolution accounts for most of the iron released during the first 6 h of the reaction, while catechol-assisted dissolution contributes substantially in later stages. The observed synergy in Fe(II) and total dissolved Fe arises from a combination of solution phase and surface reactions that occur when both compounds are present. These results suggest that the dark atmospheric processing of BBA can increase dissolved Fe(II) and total dissolved Fe, potentially contributing to the adverse health effects of smoke. These findings also highlight that mixtures produce outcomes not predictable from single compounds alone.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"13 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147493015","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xin Lin, Canru Li, David A. Hutchins, Haodong Luo, Ningxin Yan, Yan Li, Yuan Jiang, Zhimian Cao, Minhan Dai
Ocean alkalinity enhancement (OAE) via olivine addition is a promising carbon dioxide (CO2) removal strategy, yet its impact on phytoplankton-driven biogeochemical processes remains unclear. We investigated the effects of olivine on the diatom Thalassiosira pseudonana (T. pseudonana) and the coccolithophore Emiliania huxleyi (E. huxleyi;calcifying and noncalcifying strains). Olivine addition increased total alkalinity across all cultures, although the increase was less pronounced in calcifying E. huxleyi. Notably, olivine stimulated growth and particulate organic carbon production in T. pseudonana and calcifying E. huxleyi, while noncalcifying strains showed no significant response. Olivine addition dramatically accelerated sinking rates, which increased 9.36-fold for T. pseudonana and 2.39-fold for calcifying E. huxleyi. This enhancement was driven by distinct mechanisms: silicon-mediated ballasting in diatoms and extracellular polysaccharide-induced cell–olivine aggregation in coccolithophores, alongside minor silicon deposition on coccoliths. These results indicate that olivine-based OAE could increase CO2 drawdown through two independent mechanisms and may potentially strengthen the biological pump by accelerating organic matter export. Our findings suggest that olivine addition could serve as a potent approach for enhancing carbon export efficiency, with diatoms exhibiting a stronger response than coccolithophores, although its ecological impacts will require further investigation.
{"title":"Olivine-Induced Alkalinity Enhancement Amplifies Phytoplankton Carbon Export Efficiency","authors":"Xin Lin, Canru Li, David A. Hutchins, Haodong Luo, Ningxin Yan, Yan Li, Yuan Jiang, Zhimian Cao, Minhan Dai","doi":"10.1021/acs.est.6c02131","DOIUrl":"https://doi.org/10.1021/acs.est.6c02131","url":null,"abstract":"Ocean alkalinity enhancement (OAE) via olivine addition is a promising carbon dioxide (CO<sub>2</sub>) removal strategy, yet its impact on phytoplankton-driven biogeochemical processes remains unclear. We investigated the effects of olivine on the diatom <i>Thalassiosira pseudonana</i> (<i>T. pseudonana</i>) and the coccolithophore <i>Emiliania huxleyi</i> (<i>E. huxleyi</i>;calcifying and noncalcifying strains). Olivine addition increased total alkalinity across all cultures, although the increase was less pronounced in calcifying <i>E. huxleyi</i>. Notably, olivine stimulated growth and particulate organic carbon production in <i>T. pseudonana</i> and calcifying <i>E. huxleyi</i>, while noncalcifying strains showed no significant response. Olivine addition dramatically accelerated sinking rates, which increased 9.36-fold for <i>T. pseudonana</i> and 2.39-fold for calcifying <i>E. huxleyi</i>. This enhancement was driven by distinct mechanisms: silicon-mediated ballasting in diatoms and extracellular polysaccharide-induced cell–olivine aggregation in coccolithophores, alongside minor silicon deposition on coccoliths. These results indicate that olivine-based OAE could increase CO<sub>2</sub> drawdown through two independent mechanisms and may potentially strengthen the biological pump by accelerating organic matter export. Our findings suggest that olivine addition could serve as a potent approach for enhancing carbon export efficiency, with diatoms exhibiting a stronger response than coccolithophores, although its ecological impacts will require further investigation.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"60 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147493016","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Disinfection is essential for safe drinking water, yet it generates hundreds of disinfection byproducts (DBPs); many unregulated DBPs are more toxic than those currently regulated. This study provides a nationwide assessment of multiple DBP classes across 24 U.S. water utilities, linking their occurrence with distribution system dynamics and calculated cytotoxicity. Among 61 measured species, dichloroacetonitrile (DCAN), dibromoacetonitrile (DBAN), bromochloroacetonitrile (BCAN), dibromoacetamide (DBAM), monobromoacetic acid (MBAA), and dichloroacetamide (DCAM) emerged as the dominant calculated additive toxicity (CAT) drivers. CAT increased by 40-50% in the distribution systems of chlorination plants, indicating elevated CAT at distal locations relative to the point of entry within the measured DBP framework. In contrast, chloraminated plants exhibited more variable CAT behavior, including net decreases or delayed downstream peaks. Halogen-specific analyses revealed total organic bromine (TOBr) as a robust screening-level indicator of CAT, while total organic iodine (TOI) showed situational predictive value in iodide-rich, chloraminated waters. High CAT values were consistently associated with elevated halides, wastewater, and algal contributions, as well as select operational practices such as preozonation and short chlorine contact times before ammonia addition to form chloramines. Source-water dissolved organic carbon (DOC) and the Br/DOC ratio emerged as central, actionable controls linking precursor availability to halogen substitution pathways. These findings suggest a holistic approach of bromide control, organic precursor control, optimized treatment, and adoption of DOC, Br/DOC ratio, and TOBr-based monitoring is needed to produce better water for public consumption.
{"title":"From the Source to Tap: Exploring the Nationwide Occurrence and Calculated Cytotoxicity of Regulated and Unregulated DBPs in U.S. Water Systems.","authors":"Peng Dai,Sehnaz Sule Kaplan-Bekaroglu,Habibullah Uzun,Tanju Karanfil","doi":"10.1021/acs.est.5c13253","DOIUrl":"https://doi.org/10.1021/acs.est.5c13253","url":null,"abstract":"Disinfection is essential for safe drinking water, yet it generates hundreds of disinfection byproducts (DBPs); many unregulated DBPs are more toxic than those currently regulated. This study provides a nationwide assessment of multiple DBP classes across 24 U.S. water utilities, linking their occurrence with distribution system dynamics and calculated cytotoxicity. Among 61 measured species, dichloroacetonitrile (DCAN), dibromoacetonitrile (DBAN), bromochloroacetonitrile (BCAN), dibromoacetamide (DBAM), monobromoacetic acid (MBAA), and dichloroacetamide (DCAM) emerged as the dominant calculated additive toxicity (CAT) drivers. CAT increased by 40-50% in the distribution systems of chlorination plants, indicating elevated CAT at distal locations relative to the point of entry within the measured DBP framework. In contrast, chloraminated plants exhibited more variable CAT behavior, including net decreases or delayed downstream peaks. Halogen-specific analyses revealed total organic bromine (TOBr) as a robust screening-level indicator of CAT, while total organic iodine (TOI) showed situational predictive value in iodide-rich, chloraminated waters. High CAT values were consistently associated with elevated halides, wastewater, and algal contributions, as well as select operational practices such as preozonation and short chlorine contact times before ammonia addition to form chloramines. Source-water dissolved organic carbon (DOC) and the Br/DOC ratio emerged as central, actionable controls linking precursor availability to halogen substitution pathways. These findings suggest a holistic approach of bromide control, organic precursor control, optimized treatment, and adoption of DOC, Br/DOC ratio, and TOBr-based monitoring is needed to produce better water for public consumption.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"11 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147483492","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Andong Hu,Bing Li,Shang Yang,Ruili Li,Yuefei Huang,Shungui Zhou,Guangqian Wang
The mobilization of abundant but immobilized phosphorus into bioavailable forms is conventionally attributed to microbial metabolite production. Yet the persistence of reductive transformations in hydrodynamically active environments with limited microbial metabolism implies a previously overlooked abiotic pathway. Here, we reveal hydrodynamic-driven phosphorus mobilization via a piezoelectric energy-transduction pathway. Hydrodynamic forces enhanced phosphate release 3-fold in natural intertidal sediments, whereas ultrasonic treatment further elevated the release through processes operating independently of microbial activity. Mechanistic investigation confirmed that piezoelectrically generated electrons directly reduce Fe(III) species, releasing mineral-bound phosphate while simultaneously facilitating secondary mineral formation. This pathway fundamentally challenges the established paradigm of biologically dominated phosphorus cycling and establishes hydrodynamic energy as a primary driver of phosphorus transformation. Given the global distribution of hydrodynamic energy and piezoelectric minerals, this mechanism likely operates worldwide, particularly under climate-intensified hydrodynamic conditions. These processes may elevate aquatic nutrient fluxes and eutrophication risks, highlighting the need to quantify their environmental significance and develop management strategies. In addition, our findings could advance the interpretation of historical phosphorus cycling while enabling sustainable phosphorus recovery through piezoelectric processes.
{"title":"Hydrodynamic Forces as an Overlooked Driver of Phosphorus Mobilization via Piezoelectric Activation.","authors":"Andong Hu,Bing Li,Shang Yang,Ruili Li,Yuefei Huang,Shungui Zhou,Guangqian Wang","doi":"10.1021/acs.est.5c17156","DOIUrl":"https://doi.org/10.1021/acs.est.5c17156","url":null,"abstract":"The mobilization of abundant but immobilized phosphorus into bioavailable forms is conventionally attributed to microbial metabolite production. Yet the persistence of reductive transformations in hydrodynamically active environments with limited microbial metabolism implies a previously overlooked abiotic pathway. Here, we reveal hydrodynamic-driven phosphorus mobilization via a piezoelectric energy-transduction pathway. Hydrodynamic forces enhanced phosphate release 3-fold in natural intertidal sediments, whereas ultrasonic treatment further elevated the release through processes operating independently of microbial activity. Mechanistic investigation confirmed that piezoelectrically generated electrons directly reduce Fe(III) species, releasing mineral-bound phosphate while simultaneously facilitating secondary mineral formation. This pathway fundamentally challenges the established paradigm of biologically dominated phosphorus cycling and establishes hydrodynamic energy as a primary driver of phosphorus transformation. Given the global distribution of hydrodynamic energy and piezoelectric minerals, this mechanism likely operates worldwide, particularly under climate-intensified hydrodynamic conditions. These processes may elevate aquatic nutrient fluxes and eutrophication risks, highlighting the need to quantify their environmental significance and develop management strategies. In addition, our findings could advance the interpretation of historical phosphorus cycling while enabling sustainable phosphorus recovery through piezoelectric processes.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"34 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147483496","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yoan Carreira Mendes Da Silva,Maria Angelaki,Adrien Gandolfo,D James Donaldson,Christian George
An increasing number of studies report on the spontaneous production of OH radicals and H2O2 at the air/water interface of aqueous droplets. However, none of these studies have investigated OH production in droplets containing nitrate (NO3-) or nitrite (NO2-) anions. Those two ions, in particular NO3-, play a key role in atmospheric chemistry. The goal of this work was to study the spontaneous production of H2O2 in water droplets containing these two anions under dark conditions. Compared to ions that we have already studied (i.e., Cl- and Br-), H2O2 production in droplets containing NO2- or NO3- can be either enhanced or inhibited depending on the NO2- or NO3- concentrations. These findings suggest that, below a certain concentration, NO2- and NO3- enhance the H2O2 production due to their ability to disrupt the water structure at the interface, where at larger concentrations, a specific interfacial NO2- or NO3- chemistry starts to be important, producing gas-phase species such as HONO and NO2. By monitoring H2O2 and several other gas-phase products, we propose a mechanism to explain this specific interfacial chemistry of NO2- and NO3-. This chemistry may not be significant during day time due the photolysis of these two anions, but it can have an important impact during night time.
{"title":"Specific Ion Chemistry at the Air-Water Interface of Nitrite/Nitrate-Containing Droplets.","authors":"Yoan Carreira Mendes Da Silva,Maria Angelaki,Adrien Gandolfo,D James Donaldson,Christian George","doi":"10.1021/acs.est.5c15074","DOIUrl":"https://doi.org/10.1021/acs.est.5c15074","url":null,"abstract":"An increasing number of studies report on the spontaneous production of OH radicals and H2O2 at the air/water interface of aqueous droplets. However, none of these studies have investigated OH production in droplets containing nitrate (NO3-) or nitrite (NO2-) anions. Those two ions, in particular NO3-, play a key role in atmospheric chemistry. The goal of this work was to study the spontaneous production of H2O2 in water droplets containing these two anions under dark conditions. Compared to ions that we have already studied (i.e., Cl- and Br-), H2O2 production in droplets containing NO2- or NO3- can be either enhanced or inhibited depending on the NO2- or NO3- concentrations. These findings suggest that, below a certain concentration, NO2- and NO3- enhance the H2O2 production due to their ability to disrupt the water structure at the interface, where at larger concentrations, a specific interfacial NO2- or NO3- chemistry starts to be important, producing gas-phase species such as HONO and NO2. By monitoring H2O2 and several other gas-phase products, we propose a mechanism to explain this specific interfacial chemistry of NO2- and NO3-. This chemistry may not be significant during day time due the photolysis of these two anions, but it can have an important impact during night time.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"312 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147483493","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
High temporal frequency global positioning system (GPS) data are increasingly employed in mobility-based exposure assessments, yet their advantages over lower-frequency data remain uncertain for long-term applications. Understanding how GPS sampling rates affect exposure estimates is crucial for identifying the temporal scale at which human daily mobility affects exposure assessments and for informing practical strategies for GPS data collection. This study evaluated the influence of sampling rates on long-term personal exposure to air pollution, noise, green space, and fast food environments. We collected 2-week GPS data from 345 Dutch adults at 20 s (i.e., benchmark data) and systematically down-sampled the data to 1-25 min (i.e., resampled data). Exposure estimates from benchmark and resampled data were compared using Bland-Altman plots, showing minimal impact of sampling rate on personal exposures (mean biases ≈ 0 and concordance correlation coefficients = 1). We found that over 80% of air pollution, noise, and green space exposures originated from the two activity locations where participants spent most of their time, whereas in-transit periods were the dominant source of fast food exposure. These findings indicate that high-frequency GPS data are not essential for estimating long-term, time-weighted personal exposures. Activity location-based approaches can effectively approximate long-term personal exposures to air pollution, noise, and green space and present a promising pathway to facilitate scalable, person-centered exposure studies across large populations.
{"title":"High-Temporal-Resolution Global Positioning System Data Are Not Necessary for Mobility-Based Assessments of Long-Term Outdoor Personal Exposures.","authors":"Lai Wei,Marco Helbich,Roel Vermeulen","doi":"10.1021/acs.est.5c16790","DOIUrl":"https://doi.org/10.1021/acs.est.5c16790","url":null,"abstract":"High temporal frequency global positioning system (GPS) data are increasingly employed in mobility-based exposure assessments, yet their advantages over lower-frequency data remain uncertain for long-term applications. Understanding how GPS sampling rates affect exposure estimates is crucial for identifying the temporal scale at which human daily mobility affects exposure assessments and for informing practical strategies for GPS data collection. This study evaluated the influence of sampling rates on long-term personal exposure to air pollution, noise, green space, and fast food environments. We collected 2-week GPS data from 345 Dutch adults at 20 s (i.e., benchmark data) and systematically down-sampled the data to 1-25 min (i.e., resampled data). Exposure estimates from benchmark and resampled data were compared using Bland-Altman plots, showing minimal impact of sampling rate on personal exposures (mean biases ≈ 0 and concordance correlation coefficients = 1). We found that over 80% of air pollution, noise, and green space exposures originated from the two activity locations where participants spent most of their time, whereas in-transit periods were the dominant source of fast food exposure. These findings indicate that high-frequency GPS data are not essential for estimating long-term, time-weighted personal exposures. Activity location-based approaches can effectively approximate long-term personal exposures to air pollution, noise, and green space and present a promising pathway to facilitate scalable, person-centered exposure studies across large populations.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"59 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147490184","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shanqi Shen,Siya Zhao,Zhong He,Xueying An,Jian Dong,Leyi Wang,Wenxiang Ji,Aimin Li
The coexpression of antibiotic resistance and virulence traits in aquatic bacteria represents an emerging ecological and public health threat, yet the mechanisms underlying their coordinated regulation under complex environmental pressures remain unclear. In this work, we integrated metagenomic, proteomic, and metabolomic data sets from surface water samples across the Yangtze River Basin in Jiangsu Province to elucidate the drivers of resistance-virulence convergence under multipollutant stress. Among 392 multidrug-resistant (MDR; resistant to ≥3 antibiotic classes) isolates, approximately 5% were identified as "culturable superhost precursors" exhibiting pandrug-resistant (PDR; resistant to ≥10 antibiotic classes) phenotypes. Multiomics analyses indicated frequent colocalization and synchronous activation of antibiotic resistance genes (ARGs) and virulence factors (VFs) in these environmental reservoirs. Functional assays under subinhibitory antibiotic exposure demonstrated enhanced cytotoxicity and efflux activity, accompanied by the upregulation of tolC and two-component regulators evgA/evgS. Together, these results characterize a putative redox-coupled efflux-two-component system (TCS)-virulence functional axis that synchronizes adaptive gene expression under pollution stress. Crucially, our findings challenge traditional antimicrobial resistance (AMR) surveillance approaches, which rely primarily on static gene abundance metrics, by demonstrating that the dynamic regulatory activation of this axis provides a more sensitive indicator of environmental health risks. Furthermore, tolC and evgA were identified as potential transcript-level biomarkers, providing a proof of concept for environmental antimicrobial resistance early warning tools within the One Health framework.
{"title":"The Efflux-Two-Component System (TCS)-Virulence Axis Drives Resistance-Virulence Convergence in Aquatic \"Superhost Precursors\" under Pollution Stress.","authors":"Shanqi Shen,Siya Zhao,Zhong He,Xueying An,Jian Dong,Leyi Wang,Wenxiang Ji,Aimin Li","doi":"10.1021/acs.est.5c09604","DOIUrl":"https://doi.org/10.1021/acs.est.5c09604","url":null,"abstract":"The coexpression of antibiotic resistance and virulence traits in aquatic bacteria represents an emerging ecological and public health threat, yet the mechanisms underlying their coordinated regulation under complex environmental pressures remain unclear. In this work, we integrated metagenomic, proteomic, and metabolomic data sets from surface water samples across the Yangtze River Basin in Jiangsu Province to elucidate the drivers of resistance-virulence convergence under multipollutant stress. Among 392 multidrug-resistant (MDR; resistant to ≥3 antibiotic classes) isolates, approximately 5% were identified as \"culturable superhost precursors\" exhibiting pandrug-resistant (PDR; resistant to ≥10 antibiotic classes) phenotypes. Multiomics analyses indicated frequent colocalization and synchronous activation of antibiotic resistance genes (ARGs) and virulence factors (VFs) in these environmental reservoirs. Functional assays under subinhibitory antibiotic exposure demonstrated enhanced cytotoxicity and efflux activity, accompanied by the upregulation of tolC and two-component regulators evgA/evgS. Together, these results characterize a putative redox-coupled efflux-two-component system (TCS)-virulence functional axis that synchronizes adaptive gene expression under pollution stress. Crucially, our findings challenge traditional antimicrobial resistance (AMR) surveillance approaches, which rely primarily on static gene abundance metrics, by demonstrating that the dynamic regulatory activation of this axis provides a more sensitive indicator of environmental health risks. Furthermore, tolC and evgA were identified as potential transcript-level biomarkers, providing a proof of concept for environmental antimicrobial resistance early warning tools within the One Health framework.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"12 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147483490","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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