Qi Guan,Kun Shi,R Iestyn Woolway,Boqiang Qin,Yunlin Zhang,Lishan Ran
Metabolism is an essential component of carbon cycling in river ecosystems, and understanding its response to climate change on a broad scale is imperative. Here we employ deep-learning models trained on an extensive data set to reconstruct daily metabolism in a total of 293 rivers and streams across the continental US from 1980 to 2020. Three key variables, gross primary production (GPP), ecosystem respiration (ER), and net ecosystem production (NEP), are examined to unveil long-term trends. Our analysis reveals that continental US rivers and streams experience an increase of 0.045 g O2 m-2 day-1 decade-1 in GPP from 1980 to 2020, largely driven by alterations in runoff and insolation, while ER declines more strongly at a rate of 0.078 g O2 m-2 day-1 decade-1, primarily attributed to the combined effects of discharge, thermal conditions, and temperature changes. Such changes have caused a slight decrease in the NEP over the past four decades. Moreover, our well-trained models project that NEP continues to decline at a rate of 0.017 ± 0.008 g O2 m-2 day-1 decade-1 under future climate scenarios, resulting from asymmetric and converse trends between GPP and ER. Such persistent net heterotrophy shifts would threaten aquatic biodiversity and weaken ecological resilience of flowing waters to climate change.
代谢是河流生态系统碳循环的重要组成部分，在更大范围内了解其对气候变化的响应是必要的。在这里，我们使用深度学习模型在广泛的数据集上进行训练，以重建1980年至2020年美国大陆共293条河流和溪流的日常代谢。三个关键变量，总初级生产（GPP），生态系统呼吸（ER）和净生态系统生产（NEP），研究揭示了长期趋势。我们的分析表明，从1980年到2020年，美国大陆河流和溪流的GPP增加了0.045 g O2 m-2 day-1 10年-1，这主要是由于径流和日照的变化，而ER以0.078 g O2 m-2 day-1 10年-1的速度下降更强烈，主要是由于流量、热条件和温度变化的综合影响。在过去的40年里，这些变化导致了新经济政策的小幅下降。此外，我们训练有素的模型预测，在未来气候情景下，由于GPP和ER之间的不对称和反向趋势，NEP将继续以0.017±0.008 g O2 m-2 day-1 10 -1的速率下降。这种持续的净异养变化将威胁水生生物多样性，削弱流动水体对气候变化的生态适应能力。
{"title":"Declining Predictions of Net Ecosystem Production in US Rivers and Streams Throughout the 21st Century.","authors":"Qi Guan,Kun Shi,R Iestyn Woolway,Boqiang Qin,Yunlin Zhang,Lishan Ran","doi":"10.1021/acs.est.5c05623","DOIUrl":"https://doi.org/10.1021/acs.est.5c05623","url":null,"abstract":"Metabolism is an essential component of carbon cycling in river ecosystems, and understanding its response to climate change on a broad scale is imperative. Here we employ deep-learning models trained on an extensive data set to reconstruct daily metabolism in a total of 293 rivers and streams across the continental US from 1980 to 2020. Three key variables, gross primary production (GPP), ecosystem respiration (ER), and net ecosystem production (NEP), are examined to unveil long-term trends. Our analysis reveals that continental US rivers and streams experience an increase of 0.045 g O2 m-2 day-1 decade-1 in GPP from 1980 to 2020, largely driven by alterations in runoff and insolation, while ER declines more strongly at a rate of 0.078 g O2 m-2 day-1 decade-1, primarily attributed to the combined effects of discharge, thermal conditions, and temperature changes. Such changes have caused a slight decrease in the NEP over the past four decades. Moreover, our well-trained models project that NEP continues to decline at a rate of 0.017 ± 0.008 g O2 m-2 day-1 decade-1 under future climate scenarios, resulting from asymmetric and converse trends between GPP and ER. Such persistent net heterotrophy shifts would threaten aquatic biodiversity and weaken ecological resilience of flowing waters to climate change.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"62 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145765415","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}
Rui Wang,Meng Sheng,Xitong Liu,Qiaoying Wang,Zhiwei Wang,Li Wang
The demand for lithium (Li) is rapidly growing as Li-ion batteries play an increasingly important role in achieving the global "net-zero emissions". Direct lithium extraction (DLE) technologies have emerged as a transformative technology for efficiently and sustainably producing Li products from brine. While numerous studies have focused on improving Li+/Mg2+ selectivity, proper Li+ concentration before carbonation is largely overlooked. In this critical review, we examine the critical performance requirements for DLE, focusing on active-control DLE technologies where external fields actively regulate extraction, including nanofiltration, electrodialysis, and electrosorption. Although all three technologies can achieve high Li+/Mg2+ selectivity with the development of advanced materials, electrodialysis and electrosorption are capable of simultaneously separating and concentrating Li+, making them more promising for realizing a real DLE process compared to nanofiltration. Furthermore, we compare the economic and environmental performance of these technologies. While the levelized cost of lithium carbonate for electrosorption (5,400 USD ton-1) is comparable to nanofiltration and electrodialysis, its global warming potential (-3911 kg CO2 eq) is markedly lower. Thus, electrosorption theoretically emerges as the most promising candidate for achieving a truly environmentally sustainable DLE process. Finally, we discuss the key challenges to industrial deployment of ES and outline potential strategies for their resolution.
{"title":"Electrosorption Theoretically Outperforms Nanofiltration and Electrodialysis for Direct Lithium Extraction from Brines.","authors":"Rui Wang,Meng Sheng,Xitong Liu,Qiaoying Wang,Zhiwei Wang,Li Wang","doi":"10.1021/acs.est.5c13571","DOIUrl":"https://doi.org/10.1021/acs.est.5c13571","url":null,"abstract":"The demand for lithium (Li) is rapidly growing as Li-ion batteries play an increasingly important role in achieving the global \"net-zero emissions\". Direct lithium extraction (DLE) technologies have emerged as a transformative technology for efficiently and sustainably producing Li products from brine. While numerous studies have focused on improving Li+/Mg2+ selectivity, proper Li+ concentration before carbonation is largely overlooked. In this critical review, we examine the critical performance requirements for DLE, focusing on active-control DLE technologies where external fields actively regulate extraction, including nanofiltration, electrodialysis, and electrosorption. Although all three technologies can achieve high Li+/Mg2+ selectivity with the development of advanced materials, electrodialysis and electrosorption are capable of simultaneously separating and concentrating Li+, making them more promising for realizing a real DLE process compared to nanofiltration. Furthermore, we compare the economic and environmental performance of these technologies. While the levelized cost of lithium carbonate for electrosorption (5,400 USD ton-1) is comparable to nanofiltration and electrodialysis, its global warming potential (-3911 kg CO2 eq) is markedly lower. Thus, electrosorption theoretically emerges as the most promising candidate for achieving a truly environmentally sustainable DLE process. Finally, we discuss the key challenges to industrial deployment of ES and outline potential strategies for their resolution.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"56 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145765450","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}
Y Lange Simmons,Jasmine M Andersen,Mo Zohrabi,Victor M Bright,Alan R Greenberg,Juliet T Gopinath
We introduce a stimulated Raman scattering (SRS) methodology designed for rapid, real-time, and in situ monitoring of RO membrane scaling adapted for bench-scale desalination flow cells. The methodology can provide new insights into membrane scaling dynamics by offering time-resolved reflection imaging of inorganic crystal growth, coupled with chemical identification from Raman spectral data. These capabilities allow for direct local measurement of the membrane surface area covered by different scalants as well as an approximation of the scalant volume using three-dimensional, integrated Raman intensity. The 2D and 3D SRS results obtained from CaSO4 scaling experiments are compared to and are in reasonable agreement with those provided by confocal microscopy. The real-time physical and chemical characterization capabilities presented here could be extended to study combinations of inorganic, organic, and biological fouling. Overall, the SRS methodology represents an advancement in real-time sensing of membrane fouling that offers the potential for improved operation, lower cost, and more resilient RO membrane systems for sustainable water management.
{"title":"Stimulated Raman Scattering Microscopy: Real-Time In-Situ Physical and Chemical Characterization of Reverse Osmosis Desalination Membrane Scaling.","authors":"Y Lange Simmons,Jasmine M Andersen,Mo Zohrabi,Victor M Bright,Alan R Greenberg,Juliet T Gopinath","doi":"10.1021/acs.est.5c10405","DOIUrl":"https://doi.org/10.1021/acs.est.5c10405","url":null,"abstract":"We introduce a stimulated Raman scattering (SRS) methodology designed for rapid, real-time, and in situ monitoring of RO membrane scaling adapted for bench-scale desalination flow cells. The methodology can provide new insights into membrane scaling dynamics by offering time-resolved reflection imaging of inorganic crystal growth, coupled with chemical identification from Raman spectral data. These capabilities allow for direct local measurement of the membrane surface area covered by different scalants as well as an approximation of the scalant volume using three-dimensional, integrated Raman intensity. The 2D and 3D SRS results obtained from CaSO4 scaling experiments are compared to and are in reasonable agreement with those provided by confocal microscopy. The real-time physical and chemical characterization capabilities presented here could be extended to study combinations of inorganic, organic, and biological fouling. Overall, the SRS methodology represents an advancement in real-time sensing of membrane fouling that offers the potential for improved operation, lower cost, and more resilient RO membrane systems for sustainable water management.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"20 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145759882","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}
Maodian Liu,Qianru Zhang,Alexander V Zhulidov,Tatiana Yu Gurtovaya,Xingrui Cai,Wenzhe Guo,Lyudmila S Kosmenko,Nadezhda A Pavlova,Hehao Qin,Vladimir V Shamov,Alexander I Shiklomanov,Igor K Volkov,Xuejun Wang,Changhao Xiao,Zhihao Zhang,Sergey V Berdnikov,Peter A Raymond
Rivers deliver substantial mercury to coastal oceans, significantly impacting seafood safety. However, the time frame for mercury levels and fluxes in large rivers to return to a stable, low-pollution state following long-term industrial pollution remains unclear. The Amur River, the world's fifth longest and one of the largest temperate rivers, originates in Mongolia and flows along the China-Russia border. Heavy industrial wastewater discharges in the 1960s-1970s severely contaminated the river, while strict controls implemented in the late 1970s created a rare opportunity to evaluate how quickly a large river recovers from severe anthropogenic mercury pollution. Here, we present an unprecedented 43-year time series of monthly observations of particulate mercury export to determine the river's recovery time frame. We find that mercury concentrations at the river mouth tripled due to wastewater discharges. After a 90% cut in wastewater discharges, mercury levels remained at peak levels for four years, returning to near-background within approximately 15 years, representing the initial flushing of mobile mercury from the drainage network ("Baseline Recovery"). However, after the initial flushing, legacy mercury from historic wastewater discharges was remobilized by hydrologic events, triggering episodic pulses ("Disturbance Recovery") that peaked ∼20 years after controls and reached up to three times the levels of the 1960s-1970s industrial peak. This remobilization was driven by agricultural expansion that enhanced soil disturbance and erosion, compounded by intensified droughts followed by heavy rainfall. This study provides evidence of slow and pulsed recovery of mercury fluxes in heavily polluted large rivers, highlighting that historical Hg pollution in some major rivers has likely been underestimated and reinforcing the need for sustainable, long-term management.
{"title":"Half-Century Observations Reveal Slow and Pulsed Recovery from Heavy Mercury Pollution in a Major Temperate River.","authors":"Maodian Liu,Qianru Zhang,Alexander V Zhulidov,Tatiana Yu Gurtovaya,Xingrui Cai,Wenzhe Guo,Lyudmila S Kosmenko,Nadezhda A Pavlova,Hehao Qin,Vladimir V Shamov,Alexander I Shiklomanov,Igor K Volkov,Xuejun Wang,Changhao Xiao,Zhihao Zhang,Sergey V Berdnikov,Peter A Raymond","doi":"10.1021/acs.est.5c09152","DOIUrl":"https://doi.org/10.1021/acs.est.5c09152","url":null,"abstract":"Rivers deliver substantial mercury to coastal oceans, significantly impacting seafood safety. However, the time frame for mercury levels and fluxes in large rivers to return to a stable, low-pollution state following long-term industrial pollution remains unclear. The Amur River, the world's fifth longest and one of the largest temperate rivers, originates in Mongolia and flows along the China-Russia border. Heavy industrial wastewater discharges in the 1960s-1970s severely contaminated the river, while strict controls implemented in the late 1970s created a rare opportunity to evaluate how quickly a large river recovers from severe anthropogenic mercury pollution. Here, we present an unprecedented 43-year time series of monthly observations of particulate mercury export to determine the river's recovery time frame. We find that mercury concentrations at the river mouth tripled due to wastewater discharges. After a 90% cut in wastewater discharges, mercury levels remained at peak levels for four years, returning to near-background within approximately 15 years, representing the initial flushing of mobile mercury from the drainage network (\"Baseline Recovery\"). However, after the initial flushing, legacy mercury from historic wastewater discharges was remobilized by hydrologic events, triggering episodic pulses (\"Disturbance Recovery\") that peaked ∼20 years after controls and reached up to three times the levels of the 1960s-1970s industrial peak. This remobilization was driven by agricultural expansion that enhanced soil disturbance and erosion, compounded by intensified droughts followed by heavy rainfall. This study provides evidence of slow and pulsed recovery of mercury fluxes in heavily polluted large rivers, highlighting that historical Hg pollution in some major rivers has likely been underestimated and reinforcing the need for sustainable, long-term management.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"20 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145759883","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}
Josephine Meibom, Natalie Wichmann, Aina Astorch-Cardona, Michael Zumstein, Tamar Kohn
Lakewater microorganisms secrete proteases which contribute to the turnover of dissolved organic matter and the degradation of peptidic contaminants. However, little is known about the identities and substrate specificities of these proteases. Herein, we sought to characterize the global proteolytic fingerprint of the extracellular proteases present in Lake Geneva, the largest freshwater body in Central Europe. Using Multiplex Substrate Profiling by Mass Spectrometry (MSP-MS), we identified preferred enzymatic cleavage next to positively charged and certain nonpolar amino acids, while cleavage next to negatively charged residues was disfavored. Specifically, the detected dominant cleavage sites were surrounded by arginine and lysine, consistent with a trypsin-like substrate specificity. This pattern was conserved across seasons and water depths and was shared with two other Swiss lakes. In contrast, we observed variability in the numbers and types of less prevalent cleavage sites across samples, suggesting that the degree of heterogeneity in proteolytic substrate specificity varies spatially and temporally. Using class-specific inhibitors, we found that serine and metalloproteases contribute to both exo- and endoproteolytic activity in lakewater. Our findings expand our understanding of protein stability in lake ecosystems and may be used to predict the fate of peptidic contaminants in the environment.
{"title":"Proteolytic Activity and Substrate Specificity of Lake Geneva.","authors":"Josephine Meibom, Natalie Wichmann, Aina Astorch-Cardona, Michael Zumstein, Tamar Kohn","doi":"10.1021/acs.est.5c06582","DOIUrl":"https://doi.org/10.1021/acs.est.5c06582","url":null,"abstract":"<p><p>Lakewater microorganisms secrete proteases which contribute to the turnover of dissolved organic matter and the degradation of peptidic contaminants. However, little is known about the identities and substrate specificities of these proteases. Herein, we sought to characterize the global proteolytic fingerprint of the extracellular proteases present in Lake Geneva, the largest freshwater body in Central Europe. Using Multiplex Substrate Profiling by Mass Spectrometry (MSP-MS), we identified preferred enzymatic cleavage next to positively charged and certain nonpolar amino acids, while cleavage next to negatively charged residues was disfavored. Specifically, the detected dominant cleavage sites were surrounded by arginine and lysine, consistent with a trypsin-like substrate specificity. This pattern was conserved across seasons and water depths and was shared with two other Swiss lakes. In contrast, we observed variability in the numbers and types of less prevalent cleavage sites across samples, suggesting that the degree of heterogeneity in proteolytic substrate specificity varies spatially and temporally. Using class-specific inhibitors, we found that serine and metalloproteases contribute to both exo- and endoproteolytic activity in lakewater. Our findings expand our understanding of protein stability in lake ecosystems and may be used to predict the fate of peptidic contaminants in the environment.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":11.3,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145766498","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}
Tianjie Ao,Yiping Luo,Javier Remón,Jie Wu,Fang Deng,Dong Li,Chenguang Liu,Fengwu Bai
Conventional biorefining of lignocellulosic biomass, such as corn stover (CS), is hampered by poor carbon efficiency, as nearly half of the substrate carbon is lost as CO2 during ethanol fermentation. This study presents a holistically integrated cascade process designed to capture and valorize all major carbon streams. The system synergistically couples three stages: (1) high-productivity ethanol fermentation (1.68 g/L/h) using the engineered yeast Saccharomyces cerevisiae CE10; (2) anaerobic digestion of the resulting stillage, which efficiently converted residual organics into methane (171 L/kg COD) with ca. 80% COD removal; and (3) cultivation of the cyanobacterium Desertifilum tharense BERC03 using the nutrient-rich digestate and captured fermentation CO2. This integrated approach boosted the carbon utilization from a baseline of 48% to 62%. A comprehensive techno-economic analysis of an industrial-scale (2000 t/d) facility projected a Minimum Ethanol Selling Price (MESP) of $2.44 per gallon, a value approaching current market competitiveness. The analysis identified the feedstock (30%) and cellulase (17%) as the primary cost drivers. These findings demonstrate a validated biorefinery model that significantly enhances carbon recovery and outlines a viable pathway for the coproduction of multiple biofuels from lignocellulosic resources.
{"title":"Valorizing Every Carbon Atom: A Cascade Bioprocess for Advanced Biofuels from Corn-Stover-Derived Lignocellulose.","authors":"Tianjie Ao,Yiping Luo,Javier Remón,Jie Wu,Fang Deng,Dong Li,Chenguang Liu,Fengwu Bai","doi":"10.1021/acs.est.5c14410","DOIUrl":"https://doi.org/10.1021/acs.est.5c14410","url":null,"abstract":"Conventional biorefining of lignocellulosic biomass, such as corn stover (CS), is hampered by poor carbon efficiency, as nearly half of the substrate carbon is lost as CO2 during ethanol fermentation. This study presents a holistically integrated cascade process designed to capture and valorize all major carbon streams. The system synergistically couples three stages: (1) high-productivity ethanol fermentation (1.68 g/L/h) using the engineered yeast Saccharomyces cerevisiae CE10; (2) anaerobic digestion of the resulting stillage, which efficiently converted residual organics into methane (171 L/kg COD) with ca. 80% COD removal; and (3) cultivation of the cyanobacterium Desertifilum tharense BERC03 using the nutrient-rich digestate and captured fermentation CO2. This integrated approach boosted the carbon utilization from a baseline of 48% to 62%. A comprehensive techno-economic analysis of an industrial-scale (2000 t/d) facility projected a Minimum Ethanol Selling Price (MESP) of $2.44 per gallon, a value approaching current market competitiveness. The analysis identified the feedstock (30%) and cellulase (17%) as the primary cost drivers. These findings demonstrate a validated biorefinery model that significantly enhances carbon recovery and outlines a viable pathway for the coproduction of multiple biofuels from lignocellulosic resources.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"43 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145765446","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}
Karolina Cysneiros de Carvalho,Kelley C Barsanti,Justin D Hamlin,Kimberly A Prather,William C Porter
The San Diego-Tijuana border region has experienced rapid urbanization and industrial growth with unmitigated environmental consequences. For nearly a century, the Tijuana River (TR) has carried untreated sewage and industrial waste into the United States, contributing to a long-recognized and ongoing water pollution crisis. However, the impact of this pollution on air quality has been almost entirely overlooked until very recently. Analysis of low-cost air sensor data reveals that gases released from the polluted TR directly contribute to the formation of fine aerosols, increasing PM1 (particulate matter <1 μm) concentrations, particularly when river flow is high and atmospheric dispersion is low. Analysis of PM1 size distributions revealed the enhancement of smaller particle fractions, and persistently high PM1-to-PM2.5 ratios (≥0.56 ± 0.15) showed that submicrometer particles constitute the majority of fine PM mass. Combined with recent evidence of elevated gas-phase emissions from the polluted TR, these results point to secondary aerosol formation─driven by the chemical transformations of river-emitted gaseous precursors─as a major source of PM1. Concentrations peaked near a turbulent riverine hotspot, particularly at night when intensified flow and stable conditions promoted secondary aerosol formation. These findings identify a previously unrecognized source of urban air pollution, showing that the river-to-air transfer of particulate precursors can perpetuate poor air quality and heighten environmental justice and public health concerns.
{"title":"Contaminated Tijuana River Contributes to Regional Particulate Matter (PM) Levels Highlighting Overlooked Water-Air Transfer of Gaseous PM Precursors.","authors":"Karolina Cysneiros de Carvalho,Kelley C Barsanti,Justin D Hamlin,Kimberly A Prather,William C Porter","doi":"10.1021/acs.est.5c08369","DOIUrl":"https://doi.org/10.1021/acs.est.5c08369","url":null,"abstract":"The San Diego-Tijuana border region has experienced rapid urbanization and industrial growth with unmitigated environmental consequences. For nearly a century, the Tijuana River (TR) has carried untreated sewage and industrial waste into the United States, contributing to a long-recognized and ongoing water pollution crisis. However, the impact of this pollution on air quality has been almost entirely overlooked until very recently. Analysis of low-cost air sensor data reveals that gases released from the polluted TR directly contribute to the formation of fine aerosols, increasing PM1 (particulate matter <1 μm) concentrations, particularly when river flow is high and atmospheric dispersion is low. Analysis of PM1 size distributions revealed the enhancement of smaller particle fractions, and persistently high PM1-to-PM2.5 ratios (≥0.56 ± 0.15) showed that submicrometer particles constitute the majority of fine PM mass. Combined with recent evidence of elevated gas-phase emissions from the polluted TR, these results point to secondary aerosol formation─driven by the chemical transformations of river-emitted gaseous precursors─as a major source of PM1. Concentrations peaked near a turbulent riverine hotspot, particularly at night when intensified flow and stable conditions promoted secondary aerosol formation. These findings identify a previously unrecognized source of urban air pollution, showing that the river-to-air transfer of particulate precursors can perpetuate poor air quality and heighten environmental justice and public health concerns.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"62 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145765447","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}
Anna K Mahony,Tyler A Clair,Miguel A Mendez,Patrick J McNamara,William A Arnold
Quaternary ammonium compounds (QACs) are high production volume chemicals used in consumer and industrial products, including disinfectants. Influent, effluent, and biosolid samples were collected from 12 wastewater treatment plants (WWTPs) from 2020 to 2023 and analyzed for 21 QACs to assess influent loadings and discharges to the environment via effluent and biosolids. The median total QAC concentrations in liquid influents ranged from 18 to 194 μg/L, while liquid effluent concentrations were substantially lower (0.15 to 1.1 μg/L). Median biosolid concentrations were substantial (26-430 mg QAC/kg solids dry wt; maximum ∼1 g/kg). For many WWTPs, the mass loadings of QACs in biosolids were of similar magnitude as those in influents, indicating that sorption plays a large role in the removal of QACs. At most plants, ≥98% of QACs were removed by a combination of sorption (9-72%) and degradation (28-91%). One plant that used aerobic digestion had only 1% of the initial QACs in the biosolids. On a national scale, 1900 tons of QACs were estimated to enter WWTPs in liquid influents annually, 30 tons were estimated to be discharged with liquid effluents, and 770 tons were estimated to leave with biosolids, of which 640 tons are land applied or landfilled.
{"title":"Quaternary Ammonium Compounds in Wastewater Influents, Effluents, and Biosolids: Analysis from Twelve Wastewater Treatment Plants from 2020 to 2023.","authors":"Anna K Mahony,Tyler A Clair,Miguel A Mendez,Patrick J McNamara,William A Arnold","doi":"10.1021/acs.est.5c14775","DOIUrl":"https://doi.org/10.1021/acs.est.5c14775","url":null,"abstract":"Quaternary ammonium compounds (QACs) are high production volume chemicals used in consumer and industrial products, including disinfectants. Influent, effluent, and biosolid samples were collected from 12 wastewater treatment plants (WWTPs) from 2020 to 2023 and analyzed for 21 QACs to assess influent loadings and discharges to the environment via effluent and biosolids. The median total QAC concentrations in liquid influents ranged from 18 to 194 μg/L, while liquid effluent concentrations were substantially lower (0.15 to 1.1 μg/L). Median biosolid concentrations were substantial (26-430 mg QAC/kg solids dry wt; maximum ∼1 g/kg). For many WWTPs, the mass loadings of QACs in biosolids were of similar magnitude as those in influents, indicating that sorption plays a large role in the removal of QACs. At most plants, ≥98% of QACs were removed by a combination of sorption (9-72%) and degradation (28-91%). One plant that used aerobic digestion had only 1% of the initial QACs in the biosolids. On a national scale, 1900 tons of QACs were estimated to enter WWTPs in liquid influents annually, 30 tons were estimated to be discharged with liquid effluents, and 770 tons were estimated to leave with biosolids, of which 640 tons are land applied or landfilled.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"22 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145765448","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}
Weixin Zhang,Da Pan,I-Ting Ku,Yong Zhou,Jeffrey R Pierce,Jeffrey L Collett
Oil and gas (O&G) development in the U.S. has accelerated in the past two decades, aided by unconventional extraction techniques. Potential environmental and health impacts of volatile organic compounds (VOCs) originating from O&G activities have raised concerns, but emission estimates remain highly uncertain. This study offers new insights into operation-specific VOC emission rates during unconventional O&G development (UOGD). We utilize dispersion model simulations with a new emission inversion method to analyze four years (2019-2022) of weekly air canister samples, measuring 48 VOCs at 10 monitoring sites in Broomfield, Colorado, where several large multiwell pads were drilled, completed, and entered production during the study period. Emissions are characterized for well drilling, hydraulic fracturing, coiled tubing/millout, flowback, and production operations. Drilling using synthetic drilling muds and coiled tubing operations exhibit the highest NMVOC emission rates, with median values of 2.8 g/s and 1.1 g/s, respectively. NMVOC and benzene emission rates during flowback were 96% and 98% lower, respectively, than previously reported values, highlighting the effectiveness of improved management practices in reducing air pollutant emissions from what used to be often the most significant emission source during UOGD. Our findings provide the first report of VOC emissions from coiled tubing/millout operations and show that the EPA's nonpoint oil and gas emission estimation tool underestimates VOC emissions from drilling mud volatilization and flowback green completions.
{"title":"Using Ambient Concentration Measurements to Quantify Volatile Organic Compound Emissions from Unconventional Oil and Gas Operations.","authors":"Weixin Zhang,Da Pan,I-Ting Ku,Yong Zhou,Jeffrey R Pierce,Jeffrey L Collett","doi":"10.1021/acs.est.5c03994","DOIUrl":"https://doi.org/10.1021/acs.est.5c03994","url":null,"abstract":"Oil and gas (O&G) development in the U.S. has accelerated in the past two decades, aided by unconventional extraction techniques. Potential environmental and health impacts of volatile organic compounds (VOCs) originating from O&G activities have raised concerns, but emission estimates remain highly uncertain. This study offers new insights into operation-specific VOC emission rates during unconventional O&G development (UOGD). We utilize dispersion model simulations with a new emission inversion method to analyze four years (2019-2022) of weekly air canister samples, measuring 48 VOCs at 10 monitoring sites in Broomfield, Colorado, where several large multiwell pads were drilled, completed, and entered production during the study period. Emissions are characterized for well drilling, hydraulic fracturing, coiled tubing/millout, flowback, and production operations. Drilling using synthetic drilling muds and coiled tubing operations exhibit the highest NMVOC emission rates, with median values of 2.8 g/s and 1.1 g/s, respectively. NMVOC and benzene emission rates during flowback were 96% and 98% lower, respectively, than previously reported values, highlighting the effectiveness of improved management practices in reducing air pollutant emissions from what used to be often the most significant emission source during UOGD. Our findings provide the first report of VOC emissions from coiled tubing/millout operations and show that the EPA's nonpoint oil and gas emission estimation tool underestimates VOC emissions from drilling mud volatilization and flowback green completions.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"24 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145765449","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}
Meredith M Brehob,Michael J Pennino,Jana E Compton,Qian Zhang,Marc H Weber,Ryan A Hill,Selia Markley,Brian Pickard,Maddie Keefer,Sarah M Stackpoole,Lauren A Knose,Gerardo J Ruiz-Mercado,Christopher M Clark,Anne W Rea,James N Carleton,Jiajia Lin,Jesse O Bash,Kristen M Foley,Christian Hogrefe,Robert D Sabo
Efforts to constrain the negative environmental impacts of excess nitrogen (N) and phosphorus (P) are costly and challenging, due in part to inconsistent reporting of nutrient sources at temporal and spatial scales relevant for local decision making. To meet this challenge, the U.S. Environmental Protection Agency's National Nutrient Inventory provides estimates of major agricultural, urban, atmospheric, and natural nutrient fluxes for the contiguous United States at county and HUC12 scales annually from 1987 (from 1950 for agriculture) to 2017. Since the late 1980s, total N emissions and atmospheric N deposition have declined 22% and 15%, respectively, despite increased agricultural emissions. Over the same period, municipal wastewater N and P loads remained largely stable, despite population increases, through wastewater treatment upgrades and the phaseout of phosphorus-containing detergents. Improved agricultural efficiency allowed for dramatic increases in agricultural production and crop harvest since 1987 (∼25% for N and P), with little change in surplus nutrients left on fields. Overall, a combination of innovative technologies and management has stemmed or even decreased major sources of nutrient pollution to the environment over the last several decades, representing an important shift that, if continued, may contribute to improved air, land, and water quality and human health.
{"title":"The US EPA's National Nutrient Inventory: Critical Shifts in US Nutrient Pollution Sources from 1987 to 2017.","authors":"Meredith M Brehob,Michael J Pennino,Jana E Compton,Qian Zhang,Marc H Weber,Ryan A Hill,Selia Markley,Brian Pickard,Maddie Keefer,Sarah M Stackpoole,Lauren A Knose,Gerardo J Ruiz-Mercado,Christopher M Clark,Anne W Rea,James N Carleton,Jiajia Lin,Jesse O Bash,Kristen M Foley,Christian Hogrefe,Robert D Sabo","doi":"10.1021/acs.est.5c08196","DOIUrl":"https://doi.org/10.1021/acs.est.5c08196","url":null,"abstract":"Efforts to constrain the negative environmental impacts of excess nitrogen (N) and phosphorus (P) are costly and challenging, due in part to inconsistent reporting of nutrient sources at temporal and spatial scales relevant for local decision making. To meet this challenge, the U.S. Environmental Protection Agency's National Nutrient Inventory provides estimates of major agricultural, urban, atmospheric, and natural nutrient fluxes for the contiguous United States at county and HUC12 scales annually from 1987 (from 1950 for agriculture) to 2017. Since the late 1980s, total N emissions and atmospheric N deposition have declined 22% and 15%, respectively, despite increased agricultural emissions. Over the same period, municipal wastewater N and P loads remained largely stable, despite population increases, through wastewater treatment upgrades and the phaseout of phosphorus-containing detergents. Improved agricultural efficiency allowed for dramatic increases in agricultural production and crop harvest since 1987 (∼25% for N and P), with little change in surplus nutrients left on fields. Overall, a combination of innovative technologies and management has stemmed or even decreased major sources of nutrient pollution to the environment over the last several decades, representing an important shift that, if continued, may contribute to improved air, land, and water quality and human health.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"21 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145759886","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：