Yi Wang, Yifan Wang, Shicheng Dong, Ning Xia, Tao Deng, Hang Dong
The emerging use of ion exchange for resource recovery has repositioned spent regenerant from “waste” to the desired “product”. This transition requires a high purity regenerant for pure product recovery (e.g., ammonium recovery from urine) because the long-lasting direct contact regeneration directly mixes the eluted target ions with the regenerant. Direct contact regeneration prevents using impure regenerants such as electrochemically produced acid (containing electrolyte salts) from making a pure product, hindering the advancement of electrified ammonium recovery via ion exchange. We demonstrated a new concept of indirect contact regeneration leveraging the “proton leakage” from an anion exchange membrane to achieve tandem proton separation and resin regeneration, which enabled the recovery of pure ammonium by an impure acid. A weak acid cation exchange resin enabled multicycles over 80% regeneration efficiency by the limited proton leakage from mild acids with pH 2–3. Investigating the effects of acid purity, pH, and resin dosage revealed the critical role of aqueous pH and the dynamic balance of proton leakage and consumption in governing regeneration efficiency and kinetics. Critical insights on salt types and target pH were provided to minimize the trade-off between electrochemical acid production energy and regeneration efficiency.
{"title":"Indirect Contact Regeneration of Ion Exchangers: A New Concept for Advancing Electrified Nitrogen Recovery from Urine","authors":"Yi Wang, Yifan Wang, Shicheng Dong, Ning Xia, Tao Deng, Hang Dong","doi":"10.1021/acs.est.4c14735","DOIUrl":"https://doi.org/10.1021/acs.est.4c14735","url":null,"abstract":"The emerging use of ion exchange for resource recovery has repositioned spent regenerant from “waste” to the desired “product”. This transition requires a high purity regenerant for pure product recovery (e.g., ammonium recovery from urine) because the long-lasting direct contact regeneration directly mixes the eluted target ions with the regenerant. Direct contact regeneration prevents using impure regenerants such as electrochemically produced acid (containing electrolyte salts) from making a pure product, hindering the advancement of electrified ammonium recovery via ion exchange. We demonstrated a new concept of indirect contact regeneration leveraging the “proton leakage” from an anion exchange membrane to achieve tandem proton separation and resin regeneration, which enabled the recovery of pure ammonium by an impure acid. A weak acid cation exchange resin enabled multicycles over 80% regeneration efficiency by the limited proton leakage from mild acids with pH 2–3. Investigating the effects of acid purity, pH, and resin dosage revealed the critical role of aqueous pH and the dynamic balance of proton leakage and consumption in governing regeneration efficiency and kinetics. Critical insights on salt types and target pH were provided to minimize the trade-off between electrochemical acid production energy and regeneration efficiency.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"4 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846722","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}
Soil bacteria play a crucial role in enhancing mineral weathering, thereby facilitating the release of mineral structural ions into the environment. Pseudomonas brassicacearum NFM421, a root-isolated bacterium, produces two different siderophores in the form of pyoverdine and ornicorrugatin. We studied the interaction between this bacterium and biotite─a natural iron-bearing phyllosilicate─to assess the factors governing siderophore-mediated biogenic weathering. We demonstrated that bacterial Fe is an essential factor driving biotite weathering. Our findings suggested that the lipopeptidic siderophore ornicorrugatin might be more effective than pyoverdine as an iron-bearing mineral weathering agent. This secondary siderophore’s production is maintained even when the iron requirement of the bacteria is fulfilled. Moreover, we observed that another mechanism requiring direct physical contact might enable P. brassicacearum to acquire iron structural ions from soil minerals.
{"title":"Pseudomonas brassicacearum-Induced Biotite Weathering: Role of Iron Homeostasis and Two Siderophores","authors":"Tom Girard, Isabelle Basile-Doelsch, Sylvain Fochesato, Adrien Duvivier, Emmanuel Doelsch, Thierry Heulin, Wafa Achouak","doi":"10.1021/acs.est.4c07951","DOIUrl":"https://doi.org/10.1021/acs.est.4c07951","url":null,"abstract":"Soil bacteria play a crucial role in enhancing mineral weathering, thereby facilitating the release of mineral structural ions into the environment. <i>Pseudomonas brassicacearum</i> NFM421, a root-isolated bacterium, produces two different siderophores in the form of pyoverdine and ornicorrugatin. We studied the interaction between this bacterium and biotite─a natural iron-bearing phyllosilicate─to assess the factors governing siderophore-mediated biogenic weathering. We demonstrated that bacterial Fe is an essential factor driving biotite weathering. Our findings suggested that the lipopeptidic siderophore ornicorrugatin might be more effective than pyoverdine as an iron-bearing mineral weathering agent. This secondary siderophore’s production is maintained even when the iron requirement of the bacteria is fulfilled. Moreover, we observed that another mechanism requiring direct physical contact might enable <i>P. brassicacearum</i> to acquire iron structural ions from soil minerals.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"43 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846720","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}
Jinling Li, Miaomiao Liu, Yuli Shan, Jianxun Yang, Wen Fang, Zongwei Ma, Jun Bi
Local water scarcity shocks can threaten supply chains by triggering cascading economic risks embedded in the flow of goods and services. However, the lack of cascading risk modeling techniques makes it challenging to determine how disruptions in one economic sector propagate to others through the supply chain. In this study, we construct a national multilayer cascading risk model using 2017 multiregional input–output data from China and simulate shock propagation. Our results show that the originating sector and geographic location of a shock are critical in determining the collapse’s effects. The probability of a large avalanche (>1000 collapsed nodes) varies from 2 to 80% across provinces and from 1 to 96% across layers. Food production and processing, chemical smelting, and energy supply are critical layers that amplify the cascade effects of shocks. Grain regions like Henan and Hunan, manufacturing hubs such as Guangdong, and water and energy suppliers like Sichuan and Hubei face high cascading risks. Our scenario analyses show that reducing output dependence on nodes decreases the system’s avalanche size by 20–40% while improving water production efficiency reduces it by 10–22%. These results highlight the importance of diversifying supply sources and optimizing water use efficiency to enhance network resilience.
{"title":"Mapping the Water-Economic Cascading Risks within a Multilayer Network of Supply Chains in China","authors":"Jinling Li, Miaomiao Liu, Yuli Shan, Jianxun Yang, Wen Fang, Zongwei Ma, Jun Bi","doi":"10.1021/acs.est.5c01545","DOIUrl":"https://doi.org/10.1021/acs.est.5c01545","url":null,"abstract":"Local water scarcity shocks can threaten supply chains by triggering cascading economic risks embedded in the flow of goods and services. However, the lack of cascading risk modeling techniques makes it challenging to determine how disruptions in one economic sector propagate to others through the supply chain. In this study, we construct a national multilayer cascading risk model using 2017 multiregional input–output data from China and simulate shock propagation. Our results show that the originating sector and geographic location of a shock are critical in determining the collapse’s effects. The probability of a large avalanche (>1000 collapsed nodes) varies from 2 to 80% across provinces and from 1 to 96% across layers. Food production and processing, chemical smelting, and energy supply are critical layers that amplify the cascade effects of shocks. Grain regions like Henan and Hunan, manufacturing hubs such as Guangdong, and water and energy suppliers like Sichuan and Hubei face high cascading risks. Our scenario analyses show that reducing output dependence on nodes decreases the system’s avalanche size by 20–40% while improving water production efficiency reduces it by 10–22%. These results highlight the importance of diversifying supply sources and optimizing water use efficiency to enhance network resilience.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"23 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846727","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}
The influence of ground-level O3, which possesses a higher oxidative concentration than other ambient pollutants, on reproductive health has received relatively limited scrutiny. In this study, we collected information on reproductive history, sociodemographic profiles, lifestyle, and residential details of 10,153 couples at risk of pregnancy. Each participant’s 1-year, 3-year, and 5-year average O3 exposure levels were estimated using a previously developed randomized trees model. We used discrete-time Cox proportional hazards models to estimate the fecundability odds ratio (FOR) for each 10 μg/m3 change in the O3, adjusting for a set of demographics, lifestyle, and environmental covariables. We observed that a 10 μg/m3 increase in the annual average level of exposure to O3 was associated with a 16% reduction in fecundity (FOR: 0.84; 95% CI: 0.82–0.85). We also observed a 40% increase in the odds of infertility (OR: 1.40; 95% CI: 1.34–1.46) for each 10 μg/m3 rise in the annual mean of O3 exposure. After adjustment for fine particulate matter, the strong association between O3 exposure of fecundity to O3 persisted. Given the increasing epidemic of infertility, we strongly advocate for heightened consideration of O3’s impact on reproductive health, as it may partially counterbalance the health benefits gained from improved PM2.5 levels in a middle-income setting.
{"title":"Maternal Exposure to Surface Ozone and Reduced Fecundity in China: Evidence from a Nationwide Survey","authors":"Qin Li, Rui Yang, Qingqing Tao, Hongping Wu, Suxin Xu, Yuefan Kang, Yunxia Cao, Xiujuan Chen, Yimin Zhu, Shuguang Xu, Zi-Jiang Chen, Ping Liu, Rong Li, Jie Qiao","doi":"10.1021/acs.est.5c01974","DOIUrl":"https://doi.org/10.1021/acs.est.5c01974","url":null,"abstract":"The influence of ground-level O<sub>3</sub>, which possesses a higher oxidative concentration than other ambient pollutants, on reproductive health has received relatively limited scrutiny. In this study, we collected information on reproductive history, sociodemographic profiles, lifestyle, and residential details of 10,153 couples at risk of pregnancy. Each participant’s 1-year, 3-year, and 5-year average O<sub>3</sub> exposure levels were estimated using a previously developed randomized trees model. We used discrete-time Cox proportional hazards models to estimate the fecundability odds ratio (FOR) for each 10 μg/m<sup>3</sup> change in the O<sub>3</sub>, adjusting for a set of demographics, lifestyle, and environmental covariables. We observed that a 10 μg/m<sup>3</sup> increase in the annual average level of exposure to O<sub>3</sub> was associated with a 16% reduction in fecundity (FOR: 0.84; 95% CI: 0.82–0.85). We also observed a 40% increase in the odds of infertility (OR: 1.40; 95% CI: 1.34–1.46) for each 10 μg/m<sup>3</sup> rise in the annual mean of O<sub>3</sub> exposure. After adjustment for fine particulate matter, the strong association between O<sub>3</sub> exposure of fecundity to O<sub>3</sub> persisted. Given the increasing epidemic of infertility, we strongly advocate for heightened consideration of O<sub>3</sub>’s impact on reproductive health, as it may partially counterbalance the health benefits gained from improved PM<sub>2.5</sub> levels in a middle-income setting.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"12 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143849878","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}
The uptake of heavy metals by unicellular organisms can lead to the bioaccumulation of these metals in higher organisms, detrimentally affecting organismal health and ultimately impacts the ecosystems. By studying the uptake and accumulation of heavy metals in unicellular organisms, we gain insights into potential risks associated with low-dose heavy metal exposure in aquatic environments. Thus, to investigate the accumulation characteristics of Mo, Ag, Cd, Sn, Sb, Hg, Tl, and Pb mixtures in single Tetrahymena thermophila cells, we developed a label-free approach for the simultaneous absolute quantification of multiple metals in a single cell using mass cytometry. Our results demonstrated the dynamic changes in metal concentrations in T. thermophila, and the competition between metals in uptake and excretory pathways resulted in heterogeneous accumulation and bioconcentration of these metals. Additionally, our findings revealed the limited capacity of T. thermophila to excrete Cd and Hg, suggesting a higher risk for T. thermophila cells when exposed to Cd and Hg over an extended period. Therefore, the current study provides valuable data for a more comprehensive understanding of the impact of low-dose heavy metals on aquatic ecosystems.
{"title":"Heterogeneous Single-Cell Distribution of Trace-Level Metal Mixtures in Tetrahymena thermophila Using Mass Cytometry","authors":"Qi Wu, Shiyang Cheng, Wenchao Zhang, Jing Zhao, Liu Zhang, Meilin Lv, Junjie Ma, Jie Ding, Shunhao Wang, Xuehan Zheng, Jie Gao, Rui Liu, Yongguang Yin, Jianbo Shi, Guangbo Qu, Guibin Jiang","doi":"10.1021/acs.est.4c12818","DOIUrl":"https://doi.org/10.1021/acs.est.4c12818","url":null,"abstract":"The uptake of heavy metals by unicellular organisms can lead to the bioaccumulation of these metals in higher organisms, detrimentally affecting organismal health and ultimately impacts the ecosystems. By studying the uptake and accumulation of heavy metals in unicellular organisms, we gain insights into potential risks associated with low-dose heavy metal exposure in aquatic environments. Thus, to investigate the accumulation characteristics of Mo, Ag, Cd, Sn, Sb, Hg, Tl, and Pb mixtures in single <i>Tetrahymena thermophila</i> cells, we developed a label-free approach for the simultaneous absolute quantification of multiple metals in a single cell using mass cytometry. Our results demonstrated the dynamic changes in metal concentrations in <i>T. thermophila</i>, and the competition between metals in uptake and excretory pathways resulted in heterogeneous accumulation and bioconcentration of these metals. Additionally, our findings revealed the limited capacity of <i>T. thermophila</i> to excrete Cd and Hg, suggesting a higher risk for <i>T. thermophila</i> cells when exposed to Cd and Hg over an extended period. Therefore, the current study provides valuable data for a more comprehensive understanding of the impact of low-dose heavy metals on aquatic ecosystems.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"7 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143849883","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}
Mei Fei Zeng, Andreas Zuend, Nealan G. A. Gerrebos, Pengfei Yu, Gregory P. Schill, Daniel M. Murphy, Allan K. Bertram
Understanding the viscosity and phase state of biomass-burning organic aerosol (BBOA) from wildfires and pyrocumulonimbus (pyroCb) events in the stratosphere is critical for predicting their role in stratospheric multiphase chemistry and ozone depletion. However, the viscosity and phase state of BBOA under stratospheric conditions, including interactions with sulfuric acid (H2SO4), remain largely unquantified. In this study, we combine laboratory data with a thermodynamic model to predict the viscosity and phase state of BBOA under stratospheric conditions. Our results suggest that BBOA with a H2SO4-to-BBOA mass ratio of 0.37─an estimated upper limit for pyroCb smoke in the lower stratosphere after two months of aging─is highly viscous and frequently exists in a glassy state. Even at a higher H2SO4-to-BBOA mass ratio of 0.79─an estimated upper limit after nine months of aging─BBOA can still transition to a glassy state under certain stratospheric conditions. In the glassy state, bulk reactions are suppressed, and multiphase chemistry may be limited to the particle surfaces. We also highlight key areas for future research needed to better constrain the viscosity and phase state of BBOA in the stratosphere and its subsequent impact on ozone.
{"title":"Viscosity and Phase State of Wildfire Smoke Particles in the Stratosphere from Pyrocumulonimbus Events: An Initial Assessment","authors":"Mei Fei Zeng, Andreas Zuend, Nealan G. A. Gerrebos, Pengfei Yu, Gregory P. Schill, Daniel M. Murphy, Allan K. Bertram","doi":"10.1021/acs.est.4c10597","DOIUrl":"https://doi.org/10.1021/acs.est.4c10597","url":null,"abstract":"Understanding the viscosity and phase state of biomass-burning organic aerosol (BBOA) from wildfires and pyrocumulonimbus (pyroCb) events in the stratosphere is critical for predicting their role in stratospheric multiphase chemistry and ozone depletion. However, the viscosity and phase state of BBOA under stratospheric conditions, including interactions with sulfuric acid (H<sub>2</sub>SO<sub>4</sub>), remain largely unquantified. In this study, we combine laboratory data with a thermodynamic model to predict the viscosity and phase state of BBOA under stratospheric conditions. Our results suggest that BBOA with a H<sub>2</sub>SO<sub>4</sub>-to-BBOA mass ratio of 0.37─an estimated upper limit for pyroCb smoke in the lower stratosphere after two months of aging─is highly viscous and frequently exists in a glassy state. Even at a higher H<sub>2</sub>SO<sub>4</sub>-to-BBOA mass ratio of 0.79─an estimated upper limit after nine months of aging─BBOA can still transition to a glassy state under certain stratospheric conditions. In the glassy state, bulk reactions are suppressed, and multiphase chemistry may be limited to the particle surfaces. We also highlight key areas for future research needed to better constrain the viscosity and phase state of BBOA in the stratosphere and its subsequent impact on ozone.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"4 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841133","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}
Wenfeng Huang, Jingyi Zhang, Bo Chen, Xiangyang Gui, Zehong Zhang, Liyang Hu, Jun Liang, Xinde Cao, Xiaoyun Xu
Humification of exogenous soil organic matter (ESOM) remodels the organic compositions and microbial communities of soil, thus exerting potential impacts on the biogeochemical transformation of iron (hydr)oxides and associated trace metals. Here, we conducted a 70-day incubation experiment to investigate how aerobic straw humification influenced the repartitioning of arsenic (As) associated with ferrihydrite in paddy soil. Results showed that the humification was characterized by rapid OM degradation (1–14 days) and subsequent slow maturation (14–70 days). During the degradation stage, considerable As (13.1 mg·L–1) was released into the aqueous phase, which was reimmobilized to the solid phase in the maturation stage. Meanwhile, the low-crystalline structural As/Fe was converted to a more stable species, with a subtle crystalline phase transformation. The generated highly unsaturated and phenolic compounds and enriched Enterobacter and Sphingomonas induced ferrihydrite (∼3.1%) and As(V) reduction, leading to As release during the degradation stage. In the maturation stage, carboxylic-rich alicyclic molecules facilitated the aqueous As reimmobilization. Throughout the humification process, organo-mineral complexes formed between OM and ferrihydrite via C–O–Fe bond contributed to the solid-phase As/Fe stabilization. Collectively, this work highlighted the ESOM humification-driven iron (hydr)oxide transformation and associated As redistribution, advancing our understanding of the coupled biogeochemical behaviors of C, Fe, and As in soil.
{"title":"Release and Redistribution of Arsenic Associated with Ferrihydrite Driven by Aerobic Humification of Exogenous Soil Organic Matter","authors":"Wenfeng Huang, Jingyi Zhang, Bo Chen, Xiangyang Gui, Zehong Zhang, Liyang Hu, Jun Liang, Xinde Cao, Xiaoyun Xu","doi":"10.1021/acs.est.4c13919","DOIUrl":"https://doi.org/10.1021/acs.est.4c13919","url":null,"abstract":"Humification of exogenous soil organic matter (ESOM) remodels the organic compositions and microbial communities of soil, thus exerting potential impacts on the biogeochemical transformation of iron (hydr)oxides and associated trace metals. Here, we conducted a 70-day incubation experiment to investigate how aerobic straw humification influenced the repartitioning of arsenic (As) associated with ferrihydrite in paddy soil. Results showed that the humification was characterized by rapid OM degradation (1–14 days) and subsequent slow maturation (14–70 days). During the degradation stage, considerable As (13.1 mg·L<sup>–1</sup>) was released into the aqueous phase, which was reimmobilized to the solid phase in the maturation stage. Meanwhile, the low-crystalline structural As/Fe was converted to a more stable species, with a subtle crystalline phase transformation. The generated highly unsaturated and phenolic compounds and enriched <i>Enterobacter</i> and <i>Sphingomonas</i> induced ferrihydrite (∼3.1%) and As(V) reduction, leading to As release during the degradation stage. In the maturation stage, carboxylic-rich alicyclic molecules facilitated the aqueous As reimmobilization. Throughout the humification process, organo-mineral complexes formed between OM and ferrihydrite via C–O–Fe bond contributed to the solid-phase As/Fe stabilization. Collectively, this work highlighted the ESOM humification-driven iron (hydr)oxide transformation and associated As redistribution, advancing our understanding of the coupled biogeochemical behaviors of C, Fe, and As in soil.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"264 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841140","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}
With the increasing prevalence of plastic pollution, including microplastics (MPs, particles <5 mm), the pursuit of safer and more sustainable alternatives gains increasing traction. While a substantial portion of MPs in the environment arises from the degradation of plastic litter and the wear of polymer-containing materials (secondary MPs), deliberate incorporation of MPs in certain products (primary MPs) also represents a considerable source, and targeted measures can be implemented to minimize human exposure and environmental releases. Improved policies for managing macroplastic waste help mitigate secondary MPs, but addressing primary MPs requires distinct strategies. Globally, various approaches, such as bans or restrictions on primary MPs, have been proposed, including the recent EU regulation under REACH, which groups intentionally added MPs together based on their diverse uses and properties. However, applying the Essential Use Concept (EUC) provides a more refined regulatory approach; balancing environmental health, technical feasibility, and innovation. This perspective explores the potential, challenges, and limitations of implementing the EUC for primary MPs. By examining four use cases─controlled-release medicines, agricultural seed coatings, personal care products, and artificial turf infill─we highlight how the EUC can prioritize essential and beneficial applications while phasing out nonessential uses.
{"title":"Exploring the Essential Use Concept for Primary Microplastics Regulation in the EU","authors":"Stefano Amberg, Denise M. Mitrano","doi":"10.1021/acs.est.4c10830","DOIUrl":"https://doi.org/10.1021/acs.est.4c10830","url":null,"abstract":"With the increasing prevalence of plastic pollution, including microplastics (MPs, particles <5 mm), the pursuit of safer and more sustainable alternatives gains increasing traction. While a substantial portion of MPs in the environment arises from the degradation of plastic litter and the wear of polymer-containing materials (secondary MPs), deliberate incorporation of MPs in certain products (primary MPs) also represents a considerable source, and targeted measures can be implemented to minimize human exposure and environmental releases. Improved policies for managing macroplastic waste help mitigate secondary MPs, but addressing primary MPs requires distinct strategies. Globally, various approaches, such as bans or restrictions on primary MPs, have been proposed, including the recent EU regulation under REACH, which groups intentionally added MPs together based on their diverse uses and properties. However, applying the Essential Use Concept (EUC) provides a more refined regulatory approach; balancing environmental health, technical feasibility, and innovation. This perspective explores the potential, challenges, and limitations of implementing the EUC for primary MPs. By examining four use cases─controlled-release medicines, agricultural seed coatings, personal care products, and artificial turf infill─we highlight how the EUC can prioritize essential and beneficial applications while phasing out nonessential uses.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"16 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846723","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}
Shirin Saffar-Avval, Mahsa Modiri Gharehveran, Rodrigo Alvarez Ruiz, Linda S. Lee, Brian P. Chaplin
This study investigated the electrochemical oxidation of per- and polyfluoroalkyl substances (PFAS) using a Ti4O7 anode in centrate from sludge dewatering. Synthetic solutions containing perfluorooctanoic acid (PFOA), other PFAS, and inorganic constituents (phosphate, ammonium, chloride, carbonate, and acetate salts) found in centrate were studied to assess their impact on the oxidation process. PFOA removal decreased from 95% in a stable electrolyte (NaClO4) to 81% in a Na2HPO4 electrolyte and 30% in a solution mimicking concentrated centrate. X-ray photoelectron spectroscopy detected phosphate and nitrogen species on the electrode surface. At potentials required to oxidize PFAS (>3.0 V/SHE), phosphate and ammonium were oxidized to radicals that blocked electrode sites, inhibiting PFAS removal and shifting PFOA oxidation from first-order kinetics. The kinetics were accurately modeled using a Langmuir–Hinshelwood approach with a transient inhibition term. Results suggested that phosphate, ammonium, and bicarbonate ions reduced hydroxyl radical availability, thereby limiting PFOA defluorination. In concentrated centrate, 95% of the chemical oxygen demand and 93% of total PFAS were removed after 233 s of electrolysis at 30 mA cm–2. However, partial degradation of perfluorohexanoic acid and accumulation of perfluoroheptanoic acid, attributed to inorganic electrode fouling, suggested the need for a multistage reactor system for more complete PFAS mineralization.
{"title":"Matrix Effects on Electrochemical Oxidation of Per- and Polyfluoroalkyl Substances in Sludge Centrate","authors":"Shirin Saffar-Avval, Mahsa Modiri Gharehveran, Rodrigo Alvarez Ruiz, Linda S. Lee, Brian P. Chaplin","doi":"10.1021/acs.est.4c13720","DOIUrl":"https://doi.org/10.1021/acs.est.4c13720","url":null,"abstract":"This study investigated the electrochemical oxidation of per- and polyfluoroalkyl substances (PFAS) using a Ti<sub>4</sub>O<sub>7</sub> anode in centrate from sludge dewatering. Synthetic solutions containing perfluorooctanoic acid (PFOA), other PFAS, and inorganic constituents (phosphate, ammonium, chloride, carbonate, and acetate salts) found in centrate were studied to assess their impact on the oxidation process. PFOA removal decreased from 95% in a stable electrolyte (NaClO<sub>4</sub>) to 81% in a Na<sub>2</sub>HPO<sub>4</sub> electrolyte and 30% in a solution mimicking concentrated centrate. X-ray photoelectron spectroscopy detected phosphate and nitrogen species on the electrode surface. At potentials required to oxidize PFAS (>3.0 V/SHE), phosphate and ammonium were oxidized to radicals that blocked electrode sites, inhibiting PFAS removal and shifting PFOA oxidation from first-order kinetics. The kinetics were accurately modeled using a Langmuir–Hinshelwood approach with a transient inhibition term. Results suggested that phosphate, ammonium, and bicarbonate ions reduced hydroxyl radical availability, thereby limiting PFOA defluorination. In concentrated centrate, 95% of the chemical oxygen demand and 93% of total PFAS were removed after 233 s of electrolysis at 30 mA cm<sup>–2</sup>. However, partial degradation of perfluorohexanoic acid and accumulation of perfluoroheptanoic acid, attributed to inorganic electrode fouling, suggested the need for a multistage reactor system for more complete PFAS mineralization.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"22 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846724","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}
Cholaphan Deeleepojananan, Shubhrangshu Pandit, Jienan Li, Dylan A. Schmidt, Delphine K. Farmer, Vicki H. Grassian
Indoor environments are affected during wildfire events due to the infiltration of smoke. In this study, the fate of wildfire smoke, including gases and particles, on indoor surfaces was investigated through laboratory and field experiments. Fresh smoke was generated from the burning of ponderosa pine woodchips, which produced well-established wildfire and biomass burning tracers, such as levoglucosan, 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA), and 5-hydroxymethylfurfural. The interactions of smoke particles and gases were observed on different indoor-relevant building material surfaces, including glass (windows), rutile (paint and self-cleaning surfaces), and kaolinite (cement proxy and clay). However, the relative abundance of surface-bound species varied depending on the nature of these surfaces, suggesting that preferential adsorption of volatile species and particle deposition onto relevant surfaces play a key role in indoor chemistry and indoor air quality following smoke intrusion. Kaolinite surfaces, in particular, exhibited the formation of surface-initiated products during fresh smoke exposure. Furthermore, the formation of larger particles on a rutile surface was observed following ozone-aged smoke exposure, potentially resulting from the interaction of secondary organic aerosol formed during ozonolysis. Overall, this study demonstrates that different indoor-relevant material surfaces interact uniquely with smoke compounds, leading to distinct chemical transformations.
{"title":"Chemical Transformations of Infiltrated Wildfire Smoke on Indoor-Relevant Surfaces","authors":"Cholaphan Deeleepojananan, Shubhrangshu Pandit, Jienan Li, Dylan A. Schmidt, Delphine K. Farmer, Vicki H. Grassian","doi":"10.1021/acs.est.4c11771","DOIUrl":"https://doi.org/10.1021/acs.est.4c11771","url":null,"abstract":"Indoor environments are affected during wildfire events due to the infiltration of smoke. In this study, the fate of wildfire smoke, including gases and particles, on indoor surfaces was investigated through laboratory and field experiments. Fresh smoke was generated from the burning of ponderosa pine woodchips, which produced well-established wildfire and biomass burning tracers, such as levoglucosan, 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA), and 5-hydroxymethylfurfural. The interactions of smoke particles and gases were observed on different indoor-relevant building material surfaces, including glass (windows), rutile (paint and self-cleaning surfaces), and kaolinite (cement proxy and clay). However, the relative abundance of surface-bound species varied depending on the nature of these surfaces, suggesting that preferential adsorption of volatile species and particle deposition onto relevant surfaces play a key role in indoor chemistry and indoor air quality following smoke intrusion. Kaolinite surfaces, in particular, exhibited the formation of surface-initiated products during fresh smoke exposure. Furthermore, the formation of larger particles on a rutile surface was observed following ozone-aged smoke exposure, potentially resulting from the interaction of secondary organic aerosol formed during ozonolysis. Overall, this study demonstrates that different indoor-relevant material surfaces interact uniquely with smoke compounds, leading to distinct chemical transformations.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"60 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841136","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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