More than 13 years after the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, concerns remain about drinking water contamination from artificial radionuclides and the ongoing discharge of tritiated water into the Pacific Ocean. However, natural radionuclides unrelated to FDNPP releases can also contribute to human radiation exposure. Here, we measured radionuclides in Fukushima tap and groundwater to assess exposure from 222Rn (natural); 137Cs (artificial); and 3H (both artificial and natural). Ten years after the accident, all drinking water samples had 137Cs levels below detection limits (<0.02 Bq L–1), while only groundwater had elevated 222Rn (<3–399 Bq L–1). Trace amounts of 3H (0.07–0.55 Bq L–1) were measured in both sources, with tap water generally exhibiting higher levels. 3H levels in drinking water did not increase after several discharges of tritiated water into the Pacific Ocean. Estimated annual effective doses from tap water were 0.57 μSv (137Cs), 0.0058 μSv (3H), and 20 μSv (222Rn). For groundwater, doses were 0.57 μSv (137Cs), 0.0072 μSv (3H), and 1020 μSv (222Rn). The primary radiation exposure source is naturally occurring 222Rn from rock formations. Boiling well water in a vented area reduced radon levels by 95%, significantly mitigating exposure.
{"title":"Fukushima’s Tap and Groundwater a Decade after the Nuclear Accident with Radiocesium, Tritium, and Radon","authors":"Donovan Anderson, Yuki Oda, Yasuyuki Taira, Yasutaka Omori, Hirofumi Tazoe, Naofumi Akata, Chutima Kranrod, Ryohei Yamada, Haruka Kuwata, Yuki Tamakuma, Hiromi Kudo, Minoru Osanai, Natsuki Nishimura, Yumi Yasuoka, Tetsuya Sanada, Masahiro Hosoda, Shinji Tokonami","doi":"10.1021/acs.est.4c14601","DOIUrl":"https://doi.org/10.1021/acs.est.4c14601","url":null,"abstract":"More than 13 years after the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, concerns remain about drinking water contamination from artificial radionuclides and the ongoing discharge of tritiated water into the Pacific Ocean. However, natural radionuclides unrelated to FDNPP releases can also contribute to human radiation exposure. Here, we measured radionuclides in Fukushima tap and groundwater to assess exposure from <sup>222</sup>Rn (natural); <sup>137</sup>Cs (artificial); and <sup>3</sup>H (both artificial and natural). Ten years after the accident, all drinking water samples had <sup>137</sup>Cs levels below detection limits (<0.02 Bq L<sup>–1</sup>), while only groundwater had elevated <sup>222</sup>Rn (<3–399 Bq L<sup>–1</sup>). Trace amounts of <sup>3</sup>H (0.07–0.55 Bq L<sup>–1</sup>) were measured in both sources, with tap water generally exhibiting higher levels. <sup>3</sup>H levels in drinking water did not increase after several discharges of tritiated water into the Pacific Ocean. Estimated annual effective doses from tap water were 0.57 μSv (<sup>137</sup>Cs), 0.0058 μSv (<sup>3</sup>H), and 20 μSv (<sup>222</sup>Rn). For groundwater, doses were 0.57 μSv (<sup>137</sup>Cs), 0.0072 μSv (<sup>3</sup>H), and 1020 μSv (<sup>222</sup>Rn). The primary radiation exposure source is naturally occurring <sup>222</sup>Rn from rock formations. Boiling well water in a vented area reduced radon levels by 95%, significantly mitigating exposure.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"13 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569845","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}
Silica scaling poses a substantial challenge in the advanced treatment of industrial wastewater by reverse osmosis (RO) membranes, while the existing methods modifying RO membranes to enhance antisilica scaling performance often compromise water permeance. Herein, we fabricated a sulfonated RO membrane (SLRO) using sodium lignosulfonate as a comonomer, achieving an enhanced charge density and reduced coordination capacity. SLRO exhibited superior antisilica scaling performance, reducing scaling rates by ∼145, ∼166, and ∼157% under acidic, neutral, and alkaline conditions compared to the control. Reduced density gradient analysis confirmed that sulfonic acid groups (−SO3H) on the SLRO surface increased the repulsion of silicic acid. Moreover, the SLRO demonstrated reductions of ∼112, ∼137, and ∼133% in cation-mediated silica scaling rates under the same conditions, attributed to the weaker coordination between −SO3H and cations, which diminished the cation-bridging effect. Furthermore, SLRO membranes exhibited high pure water permeance (3.3 L m–2 h–1 bar–1) and NaCl rejection (99.2%), with a water/NaCl selectivity (7.8 bar–1) three times greater than that of the control (2.6 bar–1), primarily attributed to increased surface roughness and reduced apparent thickness of the PA layer. Our work provides a robust strategy for fabricating silica scaling-resistant RO membranes with improved perm-selectivity.
{"title":"Enhancing Silica Scaling Resistance and Perm-Selectivity of Reverse Osmosis Membranes via Increased Charge Density and Suppressed Coordination Capacity","authors":"Zhiwei Qiu, Hailan Wang, Ruobin Dai, Zhiwei Wang","doi":"10.1021/acs.est.4c13117","DOIUrl":"https://doi.org/10.1021/acs.est.4c13117","url":null,"abstract":"Silica scaling poses a substantial challenge in the advanced treatment of industrial wastewater by reverse osmosis (RO) membranes, while the existing methods modifying RO membranes to enhance antisilica scaling performance often compromise water permeance. Herein, we fabricated a sulfonated RO membrane (SLRO) using sodium lignosulfonate as a comonomer, achieving an enhanced charge density and reduced coordination capacity. SLRO exhibited superior antisilica scaling performance, reducing scaling rates by ∼145, ∼166, and ∼157% under acidic, neutral, and alkaline conditions compared to the control. Reduced density gradient analysis confirmed that sulfonic acid groups (−SO<sub>3</sub>H) on the SLRO surface increased the repulsion of silicic acid. Moreover, the SLRO demonstrated reductions of ∼112, ∼137, and ∼133% in cation-mediated silica scaling rates under the same conditions, attributed to the weaker coordination between −SO<sub>3</sub>H and cations, which diminished the cation-bridging effect. Furthermore, SLRO membranes exhibited high pure water permeance (3.3 L m<sup>–2</sup> h<sup>–1</sup> bar<sup>–1</sup>) and NaCl rejection (99.2%), with a water/NaCl selectivity (7.8 bar<sup>–1</sup>) three times greater than that of the control (2.6 bar<sup>–1</sup>), primarily attributed to increased surface roughness and reduced apparent thickness of the PA layer. Our work provides a robust strategy for fabricating silica scaling-resistant RO membranes with improved perm-selectivity.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"2 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570309","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}
Honeybees (Apis mellifera) are important pollinators. Their foraging behaviors are essential to colony sustainability. Sublethal exposure to pesticides such as neonicotinoids can significantly disrupt these behaviors, in particular pollen foraging. We investigated the effects of sublethal doses of the neonicotinoid imidacloprid on honeybee foraging, at both individual and colony levels, by integrating field experiments with artificial intelligence (AI)-based monitoring technology and mechanistic simulations using the BEEHAVE model. Our results replicated previous findings, which showed that imidacloprid selectively reduces pollen foraging at the colony level, with minimal impact on nectar foraging. Individually marked exposed honeybees exhibited prolonged pollen foraging trips, reduced pollen foraging frequency, and instances of drifting pollen foraging trips, likely due to impaired cognitive functions and altered metabolism. These behavioral changes at the individual level corroborated the previous model predictions derived from BEEHAVE, which highlights the value of combining experimental and simulation approaches to disentangle underlying mechanisms through which sublethal effects on individual foragers scale up to impact colony dynamics. Our findings have implications for future pesticide risk assessment, as we provide a robust feeding study design for evaluating pesticide effects on honeybee colonies and foraging in real landscapes, which could improve the realism of higher-tier ecological risk assessment.
{"title":"Reduced Honeybee Pollen Foraging under Neonicotinoid Exposure: Exploring Reproducible Individual and Colony Level Effects in the Field Using AI and Simulation","authors":"Ming Wang, Frederic Tausch, Katharina Schmidt, Matthias Diehl, Silvio Knaebe, Holger Bargen, Farnaz Faramarzi, Volker Grimm","doi":"10.1021/acs.est.4c13656","DOIUrl":"https://doi.org/10.1021/acs.est.4c13656","url":null,"abstract":"Honeybees (<i>Apis mellifera</i>) are important pollinators. Their foraging behaviors are essential to colony sustainability. Sublethal exposure to pesticides such as neonicotinoids can significantly disrupt these behaviors, in particular pollen foraging. We investigated the effects of sublethal doses of the neonicotinoid imidacloprid on honeybee foraging, at both individual and colony levels, by integrating field experiments with artificial intelligence (AI)-based monitoring technology and mechanistic simulations using the BEEHAVE model. Our results replicated previous findings, which showed that imidacloprid selectively reduces pollen foraging at the colony level, with minimal impact on nectar foraging. Individually marked exposed honeybees exhibited prolonged pollen foraging trips, reduced pollen foraging frequency, and instances of drifting pollen foraging trips, likely due to impaired cognitive functions and altered metabolism. These behavioral changes at the individual level corroborated the previous model predictions derived from BEEHAVE, which highlights the value of combining experimental and simulation approaches to disentangle underlying mechanisms through which sublethal effects on individual foragers scale up to impact colony dynamics. Our findings have implications for future pesticide risk assessment, as we provide a robust feeding study design for evaluating pesticide effects on honeybee colonies and foraging in real landscapes, which could improve the realism of higher-tier ecological risk assessment.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"34 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143575411","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}
Nienke Meekel, Anneli Kruve, Marja H. Lamoree, Frederic M. Been
Nontarget screening (NTS) with liquid chromatography high-resolution mass spectrometry (LC-HRMS) is commonly used to detect unknown organic micropollutants in the environment. One of the main challenges in NTS is the prioritization of relevant LC-HRMS features. A novel prioritization strategy based on structural alerts to select NTS features that correspond to potentially hazardous chemicals is presented here. This strategy leverages raw tandem mass spectra (MS2) and machine learning models to predict the probability that NTS features correspond to chemicals with structural alerts. The models were trained on fragments and neutral losses from the experimental MS2 data. The feasibility of this approach is evaluated for two groups: aromatic amines and organophosphorus structural alerts. The neural network classification model for organophosphorus structural alerts achieved an Area Under the Curve of the Receiver Operating Characteristics (AUC-ROC) of 0.97 and a true positive rate of 0.65 on the test set. The random forest model for the classification of aromatic amines achieved an AUC-ROC value of 0.82 and a true positive rate of 0.58 on the test set. The models were successfully applied to prioritize LC-HRMS features in surface water samples, showcasing the high potential to develop and implement this approach further.
{"title":"Machine Learning-based Classification for the Prioritization of Potentially Hazardous Chemicals with Structural Alerts in Nontarget Screening","authors":"Nienke Meekel, Anneli Kruve, Marja H. Lamoree, Frederic M. Been","doi":"10.1021/acs.est.4c10498","DOIUrl":"https://doi.org/10.1021/acs.est.4c10498","url":null,"abstract":"Nontarget screening (NTS) with liquid chromatography high-resolution mass spectrometry (LC-HRMS) is commonly used to detect unknown organic micropollutants in the environment. One of the main challenges in NTS is the prioritization of relevant LC-HRMS features. A novel prioritization strategy based on structural alerts to select NTS features that correspond to potentially hazardous chemicals is presented here. This strategy leverages raw tandem mass spectra (MS<sup>2</sup>) and machine learning models to predict the probability that NTS features correspond to chemicals with structural alerts. The models were trained on fragments and neutral losses from the experimental MS<sup>2</sup> data. The feasibility of this approach is evaluated for two groups: aromatic amines and organophosphorus structural alerts. The neural network classification model for organophosphorus structural alerts achieved an Area Under the Curve of the Receiver Operating Characteristics (AUC-ROC) of 0.97 and a true positive rate of 0.65 on the test set. The random forest model for the classification of aromatic amines achieved an AUC-ROC value of 0.82 and a true positive rate of 0.58 on the test set. The models were successfully applied to prioritize LC-HRMS features in surface water samples, showcasing the high potential to develop and implement this approach further.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"9 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569839","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}
Susan Hartmann, Roland Schrödner, Brandon T. Hassett, Markus Hartmann, Manuela van Pinxteren, Khanneh Wadinga Fomba, Frank Stratmann, Hartmut Herrmann, Mira Pöhlker, Sebastian Zeppenfeld
Remote marine regions are characterized by a high degree of cloud cover that greatly impacts Earth’s radiative budget. It is highly relevant for climate projections to represent the ice formation in these clouds. Therefore, it is crucial to understand the sources of ice-nucleating particles (INPs) that enable primary ice formation. Here, we report polysaccharides produced by four different aquatic eukaryotic microorganisms (Thraustochytrium striatum, Tausonia pullulans, Naganishia diffluens, Penicillium chrysogenum) as responsible ice-nucleating macromolecules (INMs) in these samples originating from the marine biosphere. By deriving a classical nucleation theory-based parametrization of these polysaccharidic INMs and applying it to global model simulations, a comparison to currently available marine atmospheric INP observations demonstrates a 44% contribution of polysaccharides to the total INPs of marine origin within −15 to −20 °C. The results highlight the relevance of biological INMs as part of the INP population in remote marine regions.
{"title":"Polysaccharides─Important Constituents of Ice-Nucleating Particles of Marine Origin","authors":"Susan Hartmann, Roland Schrödner, Brandon T. Hassett, Markus Hartmann, Manuela van Pinxteren, Khanneh Wadinga Fomba, Frank Stratmann, Hartmut Herrmann, Mira Pöhlker, Sebastian Zeppenfeld","doi":"10.1021/acs.est.4c08014","DOIUrl":"https://doi.org/10.1021/acs.est.4c08014","url":null,"abstract":"Remote marine regions are characterized by a high degree of cloud cover that greatly impacts Earth’s radiative budget. It is highly relevant for climate projections to represent the ice formation in these clouds. Therefore, it is crucial to understand the sources of ice-nucleating particles (INPs) that enable primary ice formation. Here, we report polysaccharides produced by four different aquatic eukaryotic microorganisms (<i>Thraustochytrium striatum</i>, <i>Tausonia pullulans</i>, <i>Naganishia diffluens</i>, <i>Penicillium chrysogenum</i>) as responsible ice-nucleating macromolecules (INMs) in these samples originating from the marine biosphere. By deriving a classical nucleation theory-based parametrization of these polysaccharidic INMs and applying it to global model simulations, a comparison to currently available marine atmospheric INP observations demonstrates a 44% contribution of polysaccharides to the total INPs of marine origin within −15 to −20 °C. The results highlight the relevance of biological INMs as part of the INP population in remote marine regions.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"58 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570308","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}
Chuanhua Ren, Xin Huang, Yanan Wang, Li Zhang, Xueyu Zhou, Weihang Sun, Haoran Zhang, Tengyu Liu, Aijun Ding, Tao Wang
Nitrogen fertilizer application is accompanied by intense release of multiple reactive nitrogen (Nr) gases such as nitrous acid (HONO), ammonia (NH3), and nitric oxide (NO) from the soil, influencing atmospheric chemistry and air pollution. In current emission inventories, postfertilization soil emissions are poorly characterized due to inaccurate identification of fertilization timing and location. Moreover, pre-existing studies predominantly focus on individual Nr gases, and a comprehensive understanding of simultaneously emitted Nr gases from fertilization and their impacts on air quality is still limited. Here, we developed a novel method to identify the dryland fertilization activity based on satellite and reanalysis data sets. Then, we updated a dynamic soil Nr emissions model (WRF-SoilN-Chem) with lab-derived parametrization and applied it to analyze the time- and space-varying Nr emissions and their effects on air quality. It is estimated that the Nr emissions from a typical fertilization event in the Yangtze River Delta (YRD) region increased ozone (O3) and nitrate concentrations by 2.5 and 18.2%, respectively. HONO and NH3 emissions jointly enhanced nitrate production via gas–particle partitioning. An accurate representation of fertilization and meteorology–emission–chemistry coupled modeling would greatly improve the understanding of the soil Nr emissions and their impacts on regional air pollution.
{"title":"Enhanced Soil Emissions of Reactive Nitrogen Gases by Fertilization and Their Impacts on Secondary Air Pollution in Eastern China","authors":"Chuanhua Ren, Xin Huang, Yanan Wang, Li Zhang, Xueyu Zhou, Weihang Sun, Haoran Zhang, Tengyu Liu, Aijun Ding, Tao Wang","doi":"10.1021/acs.est.4c12324","DOIUrl":"https://doi.org/10.1021/acs.est.4c12324","url":null,"abstract":"Nitrogen fertilizer application is accompanied by intense release of multiple reactive nitrogen (Nr) gases such as nitrous acid (HONO), ammonia (NH<sub>3</sub>), and nitric oxide (NO) from the soil, influencing atmospheric chemistry and air pollution. In current emission inventories, postfertilization soil emissions are poorly characterized due to inaccurate identification of fertilization timing and location. Moreover, pre-existing studies predominantly focus on individual Nr gases, and a comprehensive understanding of simultaneously emitted Nr gases from fertilization and their impacts on air quality is still limited. Here, we developed a novel method to identify the dryland fertilization activity based on satellite and reanalysis data sets. Then, we updated a dynamic soil Nr emissions model (WRF-SoilN-Chem) with lab-derived parametrization and applied it to analyze the time- and space-varying Nr emissions and their effects on air quality. It is estimated that the Nr emissions from a typical fertilization event in the Yangtze River Delta (YRD) region increased ozone (O<sub>3</sub>) and nitrate concentrations by 2.5 and 18.2%, respectively. HONO and NH<sub>3</sub> emissions jointly enhanced nitrate production via gas–particle partitioning. An accurate representation of fertilization and meteorology–emission–chemistry coupled modeling would greatly improve the understanding of the soil Nr emissions and their impacts on regional air pollution.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"49 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569922","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}
Atmospheric ammonia (NH3) has multiple impacts on the environment, climate change, and human health. China is the largest emitter of NH3 globally, with the dynamic inventory of NH3 emissions remaining uncertain. Here, we use the second national agricultural pollution source censuses, integrated satellite data, 15N isotope source apportionment, and multiple models to better understand those key features of NH3 emissions and its environmental impacts in China. Our results show that the total NH3 emissions were estimated to be 11.2 ± 1.1 million tonnes in 2020, with three emission peaks in April, June, and October, primarily driven by agricultural sources, which contributed 74% of the total emissions. Furthermore, employing a series of quantitative analyses, we estimated the contribution of NH3 emissions to ecosystem impacts. The NH3 emissions have contributed approximately 22% to secondary PM2.5 formation and a 16.6% increase in nitrogen loading of surface waters, while ammonium deposition led to a decrease in soil pH by 0.0032 units and an increase in the terrestrial carbon sink by 44.6 million tonnes in 2020. Reducing agricultural NH3 emissions in China would contribute to the mitigation of air and water pollution challenges, saving damage costs estimated at around 22 billion US dollars due to avoided human and ecosystem health impacts.
{"title":"Managing Ammonia for Multiple Benefits Based on Verified High-Resolution Emission Inventory in China","authors":"Chen Wang, Zehui Liu, Xiuming Zhang, Lin Zhang, Feng Zhou, Chaopu Ti, Wulahati Adalibieke, Lingyun Peng, Xiaoying Zhan, Stefan Reis, Hongbin Liu, Zhiping Zhu, Hongmin Dong, Jianming Xu, Baojing Gu","doi":"10.1021/acs.est.4c12558","DOIUrl":"https://doi.org/10.1021/acs.est.4c12558","url":null,"abstract":"Atmospheric ammonia (NH<sub>3</sub>) has multiple impacts on the environment, climate change, and human health. China is the largest emitter of NH<sub>3</sub> globally, with the dynamic inventory of NH<sub>3</sub> emissions remaining uncertain. Here, we use the second national agricultural pollution source censuses, integrated satellite data, <sup>15</sup>N isotope source apportionment, and multiple models to better understand those key features of NH<sub>3</sub> emissions and its environmental impacts in China. Our results show that the total NH<sub>3</sub> emissions were estimated to be 11.2 ± 1.1 million tonnes in 2020, with three emission peaks in April, June, and October, primarily driven by agricultural sources, which contributed 74% of the total emissions. Furthermore, employing a series of quantitative analyses, we estimated the contribution of NH<sub>3</sub> emissions to ecosystem impacts. The NH<sub>3</sub> emissions have contributed approximately 22% to secondary PM<sub>2.5</sub> formation and a 16.6% increase in nitrogen loading of surface waters, while ammonium deposition led to a decrease in soil pH by 0.0032 units and an increase in the terrestrial carbon sink by 44.6 million tonnes in 2020. Reducing agricultural NH<sub>3</sub> emissions in China would contribute to the mitigation of air and water pollution challenges, saving damage costs estimated at around 22 billion US dollars due to avoided human and ecosystem health impacts.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"46 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569923","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}
Xicheng He, Elaine D. Flynn, Jeffrey G. Catalano, Daniel E. Giammar
Selenium (Se) contamination is widespread, and Se(VI) removal from water is particularly challenging. This study evaluated Se(VI) removal using iron electrocoagulation (EC) in a flow-through reactor under various water chemistry and operating conditions. Effective Se(VI) removal (>98% from 1000 μg/L Se) was achieved under anoxic conditions with an iron dose as low as 30 mg/L and an EC reactor residence time as short as 11 s that was followed by a 1-h settling period. The removal remained stable over an extended operating time (24 h) and involved the generation of reactive Fe(II)/Fe(III) solids (green rust and magnetite). Oxic conditions were less effective for Se removal because of limited Se adsorption at the elevated pH of the effluent. The immobilized Se in the solids was in a reduced form (-II or 0), but about 70% of Se was oxidized after air exposure. Despite the reduced forms of Se being oxidized, very little Se was released from the solids and the toxicity characteristic leaching procedure indicated that EC-generated solids can be classified as nonhazardous. This study highlights the potential of flow-through iron EC to produce iron-containing adsorbents and reductants that can be tailored for Se(VI) and other oxyanion removal. It also offers practical insights into designing effective treatment systems and ensuring the safe disposal of EC-generated residual solids in real-world applications.
{"title":"Selenium(VI) Removal by Continuous Flow-Through Iron Electrocoagulation: Effects of Operating Conditions and Stability of Selenium in Residual Solids","authors":"Xicheng He, Elaine D. Flynn, Jeffrey G. Catalano, Daniel E. Giammar","doi":"10.1021/acs.est.4c12305","DOIUrl":"https://doi.org/10.1021/acs.est.4c12305","url":null,"abstract":"Selenium (Se) contamination is widespread, and Se(VI) removal from water is particularly challenging. This study evaluated Se(VI) removal using iron electrocoagulation (EC) in a flow-through reactor under various water chemistry and operating conditions. Effective Se(VI) removal (>98% from 1000 μg/L Se) was achieved under anoxic conditions with an iron dose as low as 30 mg/L and an EC reactor residence time as short as 11 s that was followed by a 1-h settling period. The removal remained stable over an extended operating time (24 h) and involved the generation of reactive Fe(II)/Fe(III) solids (green rust and magnetite). Oxic conditions were less effective for Se removal because of limited Se adsorption at the elevated pH of the effluent. The immobilized Se in the solids was in a reduced form (-II or 0), but about 70% of Se was oxidized after air exposure. Despite the reduced forms of Se being oxidized, very little Se was released from the solids and the toxicity characteristic leaching procedure indicated that EC-generated solids can be classified as nonhazardous. This study highlights the potential of flow-through iron EC to produce iron-containing adsorbents and reductants that can be tailored for Se(VI) and other oxyanion removal. It also offers practical insights into designing effective treatment systems and ensuring the safe disposal of EC-generated residual solids in real-world applications.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"53 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560773","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}
Katherine H Jordan, Paulina Jaramillo, Valerie J Karplus, Peter J Adams, Nicholas Z Muller
This study investigates the role of hydrogen as a decarbonization strategy for the iron and steel industry in the United States (U.S.) in the presence of an economy-wide net zero CO2 emissions target. Our analysis shows that hydrogen-based direct reduced iron (H2DRI) provides a cost-effective decarbonization strategy only under a relatively narrow set of conditions. Using today’s best estimates of the capital and variable costs of alternative decarbonized iron and steelmaking technologies in a U.S. economy-wide simulation framework, we find that carbon capture technologies can achieve comparable decarbonization levels by 2050 and greater cumulative emissions reductions from iron and steel production at a lower cost. Simulations suggest hydrogen contributes to economy-wide decarbonization, but H2DRI is not the preferred use case for hydrogen in most scenarios. The average abatement cost for U.S. iron and steel production could be as low as $70/tonne CO2 with existing technologies plus carbon capture, while the cost with H2DRI rises to over $500/tonne CO2. We also find that IRA tax credits are insufficient to spur hydrogen use in steelmaking in our model and that a green steel production tax credit would need to be as high as $300/tonne steel to lead to sustained H2DRI use.
{"title":"The Role of Hydrogen in Decarbonizing U.S. Iron and Steel Production","authors":"Katherine H Jordan, Paulina Jaramillo, Valerie J Karplus, Peter J Adams, Nicholas Z Muller","doi":"10.1021/acs.est.4c05756","DOIUrl":"https://doi.org/10.1021/acs.est.4c05756","url":null,"abstract":"This study investigates the role of hydrogen as a decarbonization strategy for the iron and steel industry in the United States (U.S.) in the presence of an economy-wide net zero CO<sub>2</sub> emissions target. Our analysis shows that hydrogen-based direct reduced iron (H<sub>2</sub>DRI) provides a cost-effective decarbonization strategy only under a relatively narrow set of conditions. Using today’s best estimates of the capital and variable costs of alternative decarbonized iron and steelmaking technologies in a U.S. economy-wide simulation framework, we find that carbon capture technologies can achieve comparable decarbonization levels by 2050 and greater cumulative emissions reductions from iron and steel production at a lower cost. Simulations suggest hydrogen contributes to economy-wide decarbonization, but H<sub>2</sub>DRI is not the preferred use case for hydrogen in most scenarios. The average abatement cost for U.S. iron and steel production could be as low as $70/tonne CO<sub>2</sub> with existing technologies plus carbon capture, while the cost with H<sub>2</sub>DRI rises to over $500/tonne CO<sub>2</sub>. We also find that IRA tax credits are insufficient to spur hydrogen use in steelmaking in our model and that a green steel production tax credit would need to be as high as $300/tonne steel to lead to sustained H<sub>2</sub>DRI use.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"30 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560767","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}
Detritusphere is a hotspot of carbon cycling in terrestrial ecosystems, yet the mineralization of soil organic carbon (SOC) within this microregion associated with reactive oxygen species (ROS) remains unclear. Herein, we investigated ROS production and distribution in the detritusphere of six representative soils and evaluated their contributions to SOC mineralization. We found that ROS production was significantly correlated with several soil chemical and biological factors, including pH, water-soluble phenols, water-extractable organic carbon, phenol oxidase activity, surface-bound or complexed Fe(II) and Fe(II) in low-crystalline minerals, highly crystalline Fe(II)-bearing minerals, and SOC. These factors collectively contributed to 99.6% of the variation in ROS production, as revealed by redundancy analyses. Among ROS, hydroxyl radicals (•OH) were key contributors to SOC mineralization, responsible for 10.4%–38.7% of CO2 emissions in ROS quenching experiments. Inhibiting •OH production decreased C-degrading enzyme activities, indicating that •OH stimulates CO2 emissions by increasing enzyme activity. Structural equation modeling further demonstrated that •OH promotes C-degrading enzyme activities by degrading water-soluble phenols to unlock the “enzyme latch” and by increasing SOC availability to upregulate C-degrading gene expression. These pathways contributed equally to SOC mineralization and exceeded its direct effect. These findings provide detailed insight into the mechanistic pathways of •OH-mediated carbon dynamics within the detritusphere.
{"title":"A Novel Perspective on the Role of Hydroxyl Radicals in Soil Organic Carbon Mineralization within the Detritusphere: Stimulating C-Degrading Enzyme Activities","authors":"Kangjie Yang, Bin Jia, Jinbo Liu, Kecheng Zhu, Junhao Qin, Hanzhong Jia","doi":"10.1021/acs.est.4c13619","DOIUrl":"https://doi.org/10.1021/acs.est.4c13619","url":null,"abstract":"Detritusphere is a hotspot of carbon cycling in terrestrial ecosystems, yet the mineralization of soil organic carbon (SOC) within this microregion associated with reactive oxygen species (ROS) remains unclear. Herein, we investigated ROS production and distribution in the detritusphere of six representative soils and evaluated their contributions to SOC mineralization. We found that ROS production was significantly correlated with several soil chemical and biological factors, including pH, water-soluble phenols, water-extractable organic carbon, phenol oxidase activity, surface-bound or complexed Fe(II) and Fe(II) in low-crystalline minerals, highly crystalline Fe(II)-bearing minerals, and SOC. These factors collectively contributed to 99.6% of the variation in ROS production, as revealed by redundancy analyses. Among ROS, hydroxyl radicals (<sup>•</sup>OH) were key contributors to SOC mineralization, responsible for 10.4%–38.7% of CO<sub>2</sub> emissions in ROS quenching experiments. Inhibiting <sup>•</sup>OH production decreased C-degrading enzyme activities, indicating that <sup>•</sup>OH stimulates CO<sub>2</sub> emissions by increasing enzyme activity. Structural equation modeling further demonstrated that <sup>•</sup>OH promotes C-degrading enzyme activities by degrading water-soluble phenols to unlock the “enzyme latch” and by increasing SOC availability to upregulate C-degrading gene expression. These pathways contributed equally to SOC mineralization and exceeded its direct effect. These findings provide detailed insight into the mechanistic pathways of <sup>•</sup>OH-mediated carbon dynamics within the detritusphere.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"24 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560770","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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