Yuntao Wu, Josep Peñuelas, Jalaid Naersige, Jie Luo, Heng Ge, Xingming Zhang, Pengfei Chang, Ping Li, Lingli Liu
Intensified aridity beyond a critical threshold could disrupt vegetation, microbial, and soil processes, reshaping the mechanisms controlling soil carbon (C) storage in drylands. However, the aridity threshold at which the transition occurs and how the controls over different soil C fractions shift remain unclear. Here, we conducted a 2400 km transect survey across 45 sites spanning a broad aridity gradient in temperate grasslands of China. We identified a pronounced shift in the dominant drivers of soil C storage at an aridity threshold of 0.749. Below this threshold, complex vegetation structures enhanced soil C by promoting microbial activity and mineral abundance, which stimulated the accumulation of both POM and MAOM, with a stronger effect on POM. Above the threshold, fine roots dominated soil biochemical processes, sustaining microbial activity and mineral formation that indirectly stabilized SOC, particularly via MAOM. Across the entire aridity gradient, vegetation structure mediated surface soil susceptibility to wind erosion with complex structures providing effective protection, while simpler structures offered limited buffering. These findings highlight the dual role of vegetation-mediated C input and wind erosion protection in sustaining soil stocks in drylands, underscoring the need to account for canopy and root structure when species are selected for dryland restoration.
{"title":"Vegetation-Mediated Carbon Inputs and Erosion Protection Shape Soil Carbon Dynamics across Aridity Thresholds","authors":"Yuntao Wu, Josep Peñuelas, Jalaid Naersige, Jie Luo, Heng Ge, Xingming Zhang, Pengfei Chang, Ping Li, Lingli Liu","doi":"10.1021/acs.est.5c07643","DOIUrl":"https://doi.org/10.1021/acs.est.5c07643","url":null,"abstract":"Intensified aridity beyond a critical threshold could disrupt vegetation, microbial, and soil processes, reshaping the mechanisms controlling soil carbon (C) storage in drylands. However, the aridity threshold at which the transition occurs and how the controls over different soil C fractions shift remain unclear. Here, we conducted a 2400 km transect survey across 45 sites spanning a broad aridity gradient in temperate grasslands of China. We identified a pronounced shift in the dominant drivers of soil C storage at an aridity threshold of 0.749. Below this threshold, complex vegetation structures enhanced soil C by promoting microbial activity and mineral abundance, which stimulated the accumulation of both POM and MAOM, with a stronger effect on POM. Above the threshold, fine roots dominated soil biochemical processes, sustaining microbial activity and mineral formation that indirectly stabilized SOC, particularly via MAOM. Across the entire aridity gradient, vegetation structure mediated surface soil susceptibility to wind erosion with complex structures providing effective protection, while simpler structures offered limited buffering. These findings highlight the dual role of vegetation-mediated C input and wind erosion protection in sustaining soil stocks in drylands, underscoring the need to account for canopy and root structure when species are selected for dryland restoration.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"92 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101999","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 Tibetan Plateau (TP), a critical sentinel for tracking long-range atmospheric transport (LRAT) of anthropogenic pollutants, provides indispensable archives for evaluating historical pollutant dynamics in pristine ecosystems. This study investigated temporal variations of 26 per- and polyfluoroalkyl substances (PFASs) in four alpine lake sediment cores across the TP spanning 1952–2020. Total PFAS concentrations ranged from 43.7 to 1428 pg g–1 of dw. Linear regression of log-transformed PFAS concentration revealed a significant elevation-dependent trend across the studied lakes (R2 = 0.58, p < 0.01) after excluding the lower-altitude, more human-impacted Qinghai Lake (3190 m), supporting mountain cold-trapping of these pollutants in high-altitude environments. Ranwu Lake demonstrated a unique PFAS profile dominated by perfluorobutanoic acid (PFBA), which contributed 48% of total PFASs on average, reflecting the predominant influence of glacier meltwater input pathways. The deposition flux exhibited an overall increasing trend, with fluctuations between 7.62 and 258 pg cm–2 a–1 during the studied period. Following a phase of relative stability or slight decline in the 1980s–1990s, all lakes showed a pronounced and sustained rise after 2000. Notably, the doubling time of short-chain PFBA (C4) flux in these lakes was estimated to be 7.4–15.6 years since the post-2000 period. Compositional analysis revealed a global shift from long-chain to short-chain PFASs in TP lake sediments, as reflected by declining PFOS (C8) and rapidly increasing levels of PFBA. The sedimentary record reveals temporal PFAS trends that closely track the historical evolution of global and regional PFAS emissions. Our findings provide crucial insights into the long-term trends of PFAS pollution in high-altitude ecosystems, contributing to global PFAS management efforts by assessing the effectiveness of regulations and the environmental impacts of industrial relocations.
{"title":"Temporal Trends of Per- and Polyfluoroalkyl Substances (PFASs) in Tibetan Plateau Sediment Cores (1952–2020): Tracking Global Emission History and Industrial Transformation in PFAS Production","authors":"Tengfei Cui, Yu Chen, Qianchen Fu, Xinyi Chen, Wei Luo, Yiyao Pan, Yifan Chen, Yali Shi, Ruiqiang Yang, Qinghua Zhang, Guibin Jiang","doi":"10.1021/acs.est.5c11161","DOIUrl":"https://doi.org/10.1021/acs.est.5c11161","url":null,"abstract":"The Tibetan Plateau (TP), a critical sentinel for tracking long-range atmospheric transport (LRAT) of anthropogenic pollutants, provides indispensable archives for evaluating historical pollutant dynamics in pristine ecosystems. This study investigated temporal variations of 26 per- and polyfluoroalkyl substances (PFASs) in four alpine lake sediment cores across the TP spanning 1952–2020. Total PFAS concentrations ranged from 43.7 to 1428 pg g<sup>–1</sup> of dw. Linear regression of log-transformed PFAS concentration revealed a significant elevation-dependent trend across the studied lakes (<i>R</i><sup>2</sup> = 0.58, <i>p</i> < 0.01) after excluding the lower-altitude, more human-impacted Qinghai Lake (3190 m), supporting mountain cold-trapping of these pollutants in high-altitude environments. Ranwu Lake demonstrated a unique PFAS profile dominated by perfluorobutanoic acid (PFBA), which contributed 48% of total PFASs on average, reflecting the predominant influence of glacier meltwater input pathways. The deposition flux exhibited an overall increasing trend, with fluctuations between 7.62 and 258 pg cm<sup>–2</sup> a<sup>–1</sup> during the studied period. Following a phase of relative stability or slight decline in the 1980s–1990s, all lakes showed a pronounced and sustained rise after 2000. Notably, the doubling time of short-chain PFBA (C<sub>4</sub>) flux in these lakes was estimated to be 7.4–15.6 years since the post-2000 period. Compositional analysis revealed a global shift from long-chain to short-chain PFASs in TP lake sediments, as reflected by declining PFOS (C<sub>8</sub>) and rapidly increasing levels of PFBA. The sedimentary record reveals temporal PFAS trends that closely track the historical evolution of global and regional PFAS emissions. Our findings provide crucial insights into the long-term trends of PFAS pollution in high-altitude ecosystems, contributing to global PFAS management efforts by assessing the effectiveness of regulations and the environmental impacts of industrial relocations.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"87 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146102007","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}
Kasuni H. H. Gamage,Ganga M. Hettiarachchi,Evan Heronemus,Prathap Parameswaran
The increasing demand for phosphorus (P) sources and concerns about surface water quality raise the need to explore safe and efficient secondary P fertilizer sources. This study evaluated the effectiveness of a Ca-based recovered nutrient product (RNP) from synthetic swine wastewater using an innovative anaerobic membrane bioreactor (AnMBR) technology. This study aimed to characterize and compare the dissolution, transformations, and potential bioavailability of P in RNP with conventional P fertilizers (monoammonium phosphate; MAP, triple superphosphate; TSP) in selected soils over time by using short-term laboratory incubation studies in Petri dishes. Soil samples sectioned from the point of application were assessed for pH, total P, resin-extractable P, and selected samples by using X-ray absorption near-edge structure spectroscopy. The RNP treatment showed that over 90%, 70%, and 80% of added P remained in the center section in calcareous, neutral, and acid soils, respectively, where the potential plant-available P was greater than the control in all soils and similar to the MAP treatment only in acid soil after 5 weeks of incubation. The hydroxyapatite-like species dominated P speciation in both RNP and RNP-added soils, leading to less solubility. These results underscore the potential of Ca-based RNP as a P source for tested soils, and process modifications could yield a series of viable secondary P sources for agriculture.
{"title":"Recovered Calcium-Based Phosphorus Products from Synthetic Swine Wastewater: Fate and Behavior in Soils","authors":"Kasuni H. H. Gamage,Ganga M. Hettiarachchi,Evan Heronemus,Prathap Parameswaran","doi":"10.1021/acs.est.5c05565","DOIUrl":"https://doi.org/10.1021/acs.est.5c05565","url":null,"abstract":"The increasing demand for phosphorus (P) sources and concerns about surface water quality raise the need to explore safe and efficient secondary P fertilizer sources. This study evaluated the effectiveness of a Ca-based recovered nutrient product (RNP) from synthetic swine wastewater using an innovative anaerobic membrane bioreactor (AnMBR) technology. This study aimed to characterize and compare the dissolution, transformations, and potential bioavailability of P in RNP with conventional P fertilizers (monoammonium phosphate; MAP, triple superphosphate; TSP) in selected soils over time by using short-term laboratory incubation studies in Petri dishes. Soil samples sectioned from the point of application were assessed for pH, total P, resin-extractable P, and selected samples by using X-ray absorption near-edge structure spectroscopy. The RNP treatment showed that over 90%, 70%, and 80% of added P remained in the center section in calcareous, neutral, and acid soils, respectively, where the potential plant-available P was greater than the control in all soils and similar to the MAP treatment only in acid soil after 5 weeks of incubation. The hydroxyapatite-like species dominated P speciation in both RNP and RNP-added soils, leading to less solubility. These results underscore the potential of Ca-based RNP as a P source for tested soils, and process modifications could yield a series of viable secondary P sources for agriculture.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"17 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098139","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}
To assess associations between multiple environmental factors and depressive symptoms (DS) among children and adolescents, we conducted a school-based longitudinal study among 1,418 Chinese students aged 9–14 years, with baseline and follow-up surveys conducted from 2022 to 2023. Twenty outdoor environmental exposures from three domains, air pollutants, meteorological conditions, and geographical features were assessed. DS was measured using the Center for Epidemiologic Studies Depression Scale. An exposome-wide association study was used to explore associations and identify important environmental exposures related to DS, followed by eXtreme Gradient Boosting to rank their relative importance. Composite scores for three environmental domains were constructed to assess their joint impacts on DS. Exposure to PM2.5, PM10, temperature, wind speed, artificial light at night, and building density were significantly associated with increased odds of DS, while higher relative humidity, and higher greenness indicators (Normalized Difference Vegetation Index [NDVI], forest-shrub-grass coverage, and cropland coverage) were inversely associated. Among all exposures, building density showed the greatest contribution in the model ranking. Considering the joint impacts, unfavorable environmental profiles across all three domains were significantly associated with higher odds of DS, particularly among children with abnormal weight or higher metabolic risk. Importantly, population attributable fraction analysis indicates that improving environmental profiles could theoretically reduce 14.22–29.41% of DS cases, with geographical factors showing the largest theoretical contribution. These findings underscore the importance of incorporating environmental considerations into mental health strategies and support urban design and air quality improvements as tailored interventions for vulnerable populations to reduce the burden of DS.
{"title":"Impact of Outdoor Environmental Exposome on Depressive Symptoms Among Children Aged 9–14 in China","authors":"Yaqi Wang,Di Shi,Jiajia Dang,Jieyu Liu,Yunfei Liu,Ziyue Chen,Jianhui Guo,Xinyao Lian,Yihang Zhang,Xinxin Wang,Jieyun Song,Yanhui Dong,Jing Li,Yi Song","doi":"10.1021/acs.est.5c10618","DOIUrl":"https://doi.org/10.1021/acs.est.5c10618","url":null,"abstract":"To assess associations between multiple environmental factors and depressive symptoms (DS) among children and adolescents, we conducted a school-based longitudinal study among 1,418 Chinese students aged 9–14 years, with baseline and follow-up surveys conducted from 2022 to 2023. Twenty outdoor environmental exposures from three domains, air pollutants, meteorological conditions, and geographical features were assessed. DS was measured using the Center for Epidemiologic Studies Depression Scale. An exposome-wide association study was used to explore associations and identify important environmental exposures related to DS, followed by eXtreme Gradient Boosting to rank their relative importance. Composite scores for three environmental domains were constructed to assess their joint impacts on DS. Exposure to PM2.5, PM10, temperature, wind speed, artificial light at night, and building density were significantly associated with increased odds of DS, while higher relative humidity, and higher greenness indicators (Normalized Difference Vegetation Index [NDVI], forest-shrub-grass coverage, and cropland coverage) were inversely associated. Among all exposures, building density showed the greatest contribution in the model ranking. Considering the joint impacts, unfavorable environmental profiles across all three domains were significantly associated with higher odds of DS, particularly among children with abnormal weight or higher metabolic risk. Importantly, population attributable fraction analysis indicates that improving environmental profiles could theoretically reduce 14.22–29.41% of DS cases, with geographical factors showing the largest theoretical contribution. These findings underscore the importance of incorporating environmental considerations into mental health strategies and support urban design and air quality improvements as tailored interventions for vulnerable populations to reduce the burden of DS.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"4 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098137","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}
Photocatalytic degradation of volatile organic compounds (VOCs) using visible light has been widely investigated, but its practical implementation remains constrained by several limiting factors. Here, we prepared carboxymethyl-β-cyclodextrin (CMCD)-anchored WO3 that enabled visible-light-driven mineralization of acetaldehyde even under O2-free conditions. Anchoring CMCD on WO3 facilitated interfacial charge separation, enhancing the photocatalytic performance. Spectroscopic and electrochemical analyses revealed that loading CMCD on WO3 induced the formation of a charge-transfer complex via C-O-W bonding and extended the charge carrier lifetime by trapping electrons in CMCD. CMCD/WO3 sustained •OH generation under visible light (λ > 420 nm) and fully mineralized acetaldehyde even in the absence of O2. It also produced dioxygen from water oxidation in O2-free conditions, supplying O2 needed to fully mineralize VOCs to CO2, and it enabled an unconventional three-electron reduction of O2 to •OH. CMCD/WO3 exhibited a visible light degradation efficiency comparable to that of Pt-loaded WO3. In particular, CMCD/WO3 exhibited a higher carbon mass balance for acetaldehyde degradation than Pt/WO3, and this value remained nearly unchanged under both oxygen-rich and oxygen-free conditions. CMCD/WO3 also demonstrated long-term stability across repeated photocatalytic cycles with no decomposition of the CMCD structure. These findings highlight a supramolecular design strategy for developing an unconventional visible-light-active photocatalyst for indoor air purification, especially in enclosed or oxygen-depleted environments where conventional photocatalysts fail to operate.
{"title":"Oxygen-Independent Mineralization of Acetaldehyde by a Cyclodextrin-Anchored WO<sub>3</sub> Photocatalyst under Visible Light.","authors":"Woojung Jeon, Seunghyun Weon, Ye He, Wonyong Choi","doi":"10.1021/acs.est.5c14689","DOIUrl":"https://doi.org/10.1021/acs.est.5c14689","url":null,"abstract":"<p><p>Photocatalytic degradation of volatile organic compounds (VOCs) using visible light has been widely investigated, but its practical implementation remains constrained by several limiting factors. Here, we prepared carboxymethyl-β-cyclodextrin (CMCD)-anchored WO<sub>3</sub> that enabled visible-light-driven mineralization of acetaldehyde even under O<sub>2</sub>-free conditions. Anchoring CMCD on WO<sub>3</sub> facilitated interfacial charge separation, enhancing the photocatalytic performance. Spectroscopic and electrochemical analyses revealed that loading CMCD on WO<sub>3</sub> induced the formation of a charge-transfer complex via C-O-W bonding and extended the charge carrier lifetime by trapping electrons in CMCD. CMCD/WO<sub>3</sub> sustained <sup>•</sup>OH generation under visible light (λ > 420 nm) and fully mineralized acetaldehyde even in the absence of O<sub>2</sub>. It also produced dioxygen from water oxidation in O<sub>2</sub>-free conditions, supplying O<sub>2</sub> needed to fully mineralize VOCs to CO<sub>2</sub>, and it enabled an unconventional three-electron reduction of O<sub>2</sub> to <sup>•</sup>OH. CMCD/WO<sub>3</sub> exhibited a visible light degradation efficiency comparable to that of Pt-loaded WO<sub>3</sub>. In particular, CMCD/WO<sub>3</sub> exhibited a higher carbon mass balance for acetaldehyde degradation than Pt/WO<sub>3</sub>, and this value remained nearly unchanged under both oxygen-rich and oxygen-free conditions. CMCD/WO<sub>3</sub> also demonstrated long-term stability across repeated photocatalytic cycles with no decomposition of the CMCD structure. These findings highlight a supramolecular design strategy for developing an unconventional visible-light-active photocatalyst for indoor air purification, especially in enclosed or oxygen-depleted environments where conventional photocatalysts fail to operate.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":11.3,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146103107","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}
Xiong Luo,Yan Lan,Ming Gao,Mingzhu Xu,Shuhao Liu,Shixue Zheng,Mingshun Li
Microbial oxidation of environmental antimonite (Sb(III)) to antimonate (Sb(V)) is a key antimony (Sb) detoxification mechanism. Comamonas testosteroni JL40 oxidizes Sb(III) to Sb(V) under oxic conditions via an uncharacterized mechanism. A redox-related enzyme identified via differential proteomics was designated AntO. The antO transcription was significantly upregulated upon addition of Sb(III). AntO is predicted to be a catalase-like heme-binding peroxidase, similar to the uncharacterized SrpA. Phylogenetic analysis indicates that AntO represents a novel Sb(III) oxidase or catalase. In E. coli AW3110(Δars), AntO confers Sb(III) resistance and oxidation activity and is induced by Sb(III) and H2O2. Further analysis confirms that antO mediates Sb(III) oxidation and H2O2 decomposition in JL40. Purified AntO catalyzes Sb(III) oxidation (with NADP+ as an electron acceptor) and H2O2 decomposition in vitro. Molecular docking shows that these reactions occur in distinct AntO structural domains. In summary, AntO has dual roles: Sb(III) oxidation for detoxification and H2O2 decomposition. This study identifies AntO as a novel environmental Sb(III) oxidase that facilitates Sb(III) detoxification, alleviates Sb(III)-induced oxidative stress, and advances understanding of microbial contributions to antimony biogeochemical cycling.
{"title":"Novel Bifunctional Enzyme AntO Catalyzes Antimonite Oxidation and H2O2 Decomposition in Environmental Antimony Detoxification","authors":"Xiong Luo,Yan Lan,Ming Gao,Mingzhu Xu,Shuhao Liu,Shixue Zheng,Mingshun Li","doi":"10.1021/acs.est.5c12342","DOIUrl":"https://doi.org/10.1021/acs.est.5c12342","url":null,"abstract":"Microbial oxidation of environmental antimonite (Sb(III)) to antimonate (Sb(V)) is a key antimony (Sb) detoxification mechanism. Comamonas testosteroni JL40 oxidizes Sb(III) to Sb(V) under oxic conditions via an uncharacterized mechanism. A redox-related enzyme identified via differential proteomics was designated AntO. The antO transcription was significantly upregulated upon addition of Sb(III). AntO is predicted to be a catalase-like heme-binding peroxidase, similar to the uncharacterized SrpA. Phylogenetic analysis indicates that AntO represents a novel Sb(III) oxidase or catalase. In E. coli AW3110(Δars), AntO confers Sb(III) resistance and oxidation activity and is induced by Sb(III) and H2O2. Further analysis confirms that antO mediates Sb(III) oxidation and H2O2 decomposition in JL40. Purified AntO catalyzes Sb(III) oxidation (with NADP+ as an electron acceptor) and H2O2 decomposition in vitro. Molecular docking shows that these reactions occur in distinct AntO structural domains. In summary, AntO has dual roles: Sb(III) oxidation for detoxification and H2O2 decomposition. This study identifies AntO as a novel environmental Sb(III) oxidase that facilitates Sb(III) detoxification, alleviates Sb(III)-induced oxidative stress, and advances understanding of microbial contributions to antimony biogeochemical cycling.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"8 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098134","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 widespread application and unavoidable atmospheric release of transitional metal dichalcogenides (TMDCs) pose significant inhalation-related health risks. During respiration, atmospheric aging of nanoparticles occurs first; nonetheless, the hazard of air-aged TMDCs and the effect of postbiotransformation in the microenvironment following inhalation remain unclear. By mimicking atmospheric conditions and respiratory media, we discovered that air-aged molybdenum disulfide (A-MoS2) and tungsten disulfide (A-WS2) underwent biotransformation in artificial nasal fluids and Gamble’s solution, increasing the hydrophobicity and roughness of the nanosheets. The oxidized products (31.7% in A-MoS2 and 44.5% in A-WS2) were partially converted to sulfidation-state species via thiol-mediated reduction. Both biotransformed and air-aged TMDCs were localized to macrophage lysosomes at approximate concentrations, whereas the lysosomal membrane damage and ferrous ion (Fe2+) release were more significant for biotransformed forms. Transcriptome and lipidomics analyses indicated that ferroprotein degradation and ferroportin1 inhibition also facilitated Fe2+ overload, along with glutathione peroxidase 4 inhibition, lipid acylation, and phospholipid biosynthesis activation, worsening lipid peroxidation (154.3–225.6%). Shapley Additive Explanations substantiated the reduction of oxidized species, 1T-phase stabilization, and increased hydrophobicity as major contributors to ferroptosis aggravation of biotransformed TMDCs. Our findings highlight the necessity of incorporating biotransformation into risk assessment, rather than merely relying on the versions of nanomaterials following environmental processes as the testing endpoints.
{"title":"Biotransformation of Atmospheric-Aged Metal-Sulfide Nanosheets in Respiratory Tract Fluids Potentiates Ferroptosis toward Alveolar Macrophages","authors":"Wei Zou,Yishuang Chang,Jiahui Wang,Xingli Zhang,Caixia Jin,Jiawei Wang,Guoqing Zhang,Shaohu Ouyang,Zhiguo Cao,Qixing Zhou","doi":"10.1021/acs.est.5c13859","DOIUrl":"https://doi.org/10.1021/acs.est.5c13859","url":null,"abstract":"The widespread application and unavoidable atmospheric release of transitional metal dichalcogenides (TMDCs) pose significant inhalation-related health risks. During respiration, atmospheric aging of nanoparticles occurs first; nonetheless, the hazard of air-aged TMDCs and the effect of postbiotransformation in the microenvironment following inhalation remain unclear. By mimicking atmospheric conditions and respiratory media, we discovered that air-aged molybdenum disulfide (A-MoS2) and tungsten disulfide (A-WS2) underwent biotransformation in artificial nasal fluids and Gamble’s solution, increasing the hydrophobicity and roughness of the nanosheets. The oxidized products (31.7% in A-MoS2 and 44.5% in A-WS2) were partially converted to sulfidation-state species via thiol-mediated reduction. Both biotransformed and air-aged TMDCs were localized to macrophage lysosomes at approximate concentrations, whereas the lysosomal membrane damage and ferrous ion (Fe2+) release were more significant for biotransformed forms. Transcriptome and lipidomics analyses indicated that ferroprotein degradation and ferroportin1 inhibition also facilitated Fe2+ overload, along with glutathione peroxidase 4 inhibition, lipid acylation, and phospholipid biosynthesis activation, worsening lipid peroxidation (154.3–225.6%). Shapley Additive Explanations substantiated the reduction of oxidized species, 1T-phase stabilization, and increased hydrophobicity as major contributors to ferroptosis aggravation of biotransformed TMDCs. Our findings highlight the necessity of incorporating biotransformation into risk assessment, rather than merely relying on the versions of nanomaterials following environmental processes as the testing endpoints.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"184 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098132","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}
Martin Scheringer,Hans Peter H. Arp,Ian T. Cousins
The planetary-scale risks posed by “chemicals of global concern” have deep historical roots that predate the literature on the Planetary Boundaries concept. Two largely separate scientific and regulatory tracks emerged from mid-20th-century research: an atmospheric track (exemplified by chlorofluorocarbons and stratospheric ozone depletion) and an aquatic-terrestrial/ecotoxicological track (exemplified by DDT, PCBs and other bioaccumulative organohalogens). Both tracks produced early warnings, scientific consensus, and eventual multilateral environmental agreements (the Montreal Protocol and Stockholm Convention). In this Perspective, we synthesize the historical evidence, link it to the planetary-boundaries and limits-to-growth narratives, highlight why chemical regulation repeatedly failed to prevent widespread contamination, and propose a set of pragmatic policy instruments, including targeted premarket controls such as the application of the Safe and Sustainable by Design framework, class-based phase-outs to speed up the removal of hazardous substances from the market, and global burden sharing to better manage planetary-scale chemical problems.
{"title":"Boundaries, Limits, Global Threats – How Can the Impacts of Global Synthetic Pollutants Be Reduced?","authors":"Martin Scheringer,Hans Peter H. Arp,Ian T. Cousins","doi":"10.1021/acs.est.5c13807","DOIUrl":"https://doi.org/10.1021/acs.est.5c13807","url":null,"abstract":"The planetary-scale risks posed by “chemicals of global concern” have deep historical roots that predate the literature on the Planetary Boundaries concept. Two largely separate scientific and regulatory tracks emerged from mid-20th-century research: an atmospheric track (exemplified by chlorofluorocarbons and stratospheric ozone depletion) and an aquatic-terrestrial/ecotoxicological track (exemplified by DDT, PCBs and other bioaccumulative organohalogens). Both tracks produced early warnings, scientific consensus, and eventual multilateral environmental agreements (the Montreal Protocol and Stockholm Convention). In this Perspective, we synthesize the historical evidence, link it to the planetary-boundaries and limits-to-growth narratives, highlight why chemical regulation repeatedly failed to prevent widespread contamination, and propose a set of pragmatic policy instruments, including targeted premarket controls such as the application of the Safe and Sustainable by Design framework, class-based phase-outs to speed up the removal of hazardous substances from the market, and global burden sharing to better manage planetary-scale chemical problems.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"82 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098133","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 N. Scherer,Madison Feshuk,James M. Armitage,Jon A. Arnot,David Crizer,Michael DeVito,Stephen S. Ferguson,Kimberly Freeman,Gregory S. Honda,Joshua A. Harrill,Alessandro Sangion,Caroline Tebes-Stevens,Katie Paul Friedman,John F. Wambaugh
The aim of in vitro - in vivo extrapolation (IVIVE) of dose is to predict potential whole animal effects from perturbations observed in vitro. Reliance on nominal (administered) concentration (assumed dose) does not account for chemical distribution to cellular and noncellular elements of an in vitro assay system. Chemical distribution can reduce the free concentration available to cause effects and can result in an inaccurate estimate of the intracellular concentration causing any observed perturbations. There are mathematical, chemical property-based partitioning models for predicting cellular concentrations when not measured experimentally. This work evaluated two of these in vitro disposition models, Armitage et al., 2021 and Kramer et al., 2010, using a total of 153 experimental intracellular concentration measurements of 43 chemicals, along with parameters describing measurement conditions, from 12 peer reviewed studies in addition to data generated for this study. Intracellular concentrations were more accurately predicted by both the Armitage model (root mean squared log10 error (RMSLE) = 1.12) and the Kramer model (RMSLE = 1.30) than by the nominal concentration (RMSLE = 1.45). Although limited by the amount of available measurement data, these results indicate that mathematical modeling of in vitro distribution can improve the accuracy of IVIVE for toxicology.
{"title":"Characterizing Accuracy of Model Predictions for Chemical Concentration in High Throughput Screening Assays","authors":"Meredith N. Scherer,Madison Feshuk,James M. Armitage,Jon A. Arnot,David Crizer,Michael DeVito,Stephen S. Ferguson,Kimberly Freeman,Gregory S. Honda,Joshua A. Harrill,Alessandro Sangion,Caroline Tebes-Stevens,Katie Paul Friedman,John F. Wambaugh","doi":"10.1021/acs.est.5c10195","DOIUrl":"https://doi.org/10.1021/acs.est.5c10195","url":null,"abstract":"The aim of in vitro - in vivo extrapolation (IVIVE) of dose is to predict potential whole animal effects from perturbations observed in vitro. Reliance on nominal (administered) concentration (assumed dose) does not account for chemical distribution to cellular and noncellular elements of an in vitro assay system. Chemical distribution can reduce the free concentration available to cause effects and can result in an inaccurate estimate of the intracellular concentration causing any observed perturbations. There are mathematical, chemical property-based partitioning models for predicting cellular concentrations when not measured experimentally. This work evaluated two of these in vitro disposition models, Armitage et al., 2021 and Kramer et al., 2010, using a total of 153 experimental intracellular concentration measurements of 43 chemicals, along with parameters describing measurement conditions, from 12 peer reviewed studies in addition to data generated for this study. Intracellular concentrations were more accurately predicted by both the Armitage model (root mean squared log10 error (RMSLE) = 1.12) and the Kramer model (RMSLE = 1.30) than by the nominal concentration (RMSLE = 1.45). Although limited by the amount of available measurement data, these results indicate that mathematical modeling of in vitro distribution can improve the accuracy of IVIVE for toxicology.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"91 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098136","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}
Kush Paliwal,Antoine F. Aubeneau,Rao S. Govindaraju
Environmental DNA (eDNA) has emerged as a powerful marker for assessing species presence in flowing waters; however, estimating the spatial and temporal origins of these signals remains a challenge. This study presents a set of laboratory experiments examining the role of bottom substrates and hyporheic exchange on eDNA fate and transport. A conceptual model is proposed wherein eDNA transport is governed by competition between adsorption/desorption processes and hydrodynamic forces which remobilize eDNA across the water column and sediment storage zones. Retention experiments were conducted for plane and gravel beds, while breakthrough experiments were performed across both bed types and two hydraulic regimes. To quantify eDNA settling rates and validate the conceptual model, an independent experiment under quiescent conditions was performed. Breakthrough curves were analyzed using a continuous time random walk (CTRW) model. Enhanced exchange and retention rates were observed for eDNA in the gravel bed, showing that surface–subsurface interactions and turbulence influenced downstream transport distances. Effective velocities were significantly lower for eDNA than for a conservative tracer across both bed types at low flows. These results underscore that parafluvial processes, including hyporheic exchange and storage in sediments, play a crucial role in eDNA transport dynamics within slow-moving lotic environments.
{"title":"Laboratory Study on Fate and Transport of Water-Borne eDNA: A Tale of Tempered Tails and Parafluvial Processes","authors":"Kush Paliwal,Antoine F. Aubeneau,Rao S. Govindaraju","doi":"10.1021/acs.est.5c11215","DOIUrl":"https://doi.org/10.1021/acs.est.5c11215","url":null,"abstract":"Environmental DNA (eDNA) has emerged as a powerful marker for assessing species presence in flowing waters; however, estimating the spatial and temporal origins of these signals remains a challenge. This study presents a set of laboratory experiments examining the role of bottom substrates and hyporheic exchange on eDNA fate and transport. A conceptual model is proposed wherein eDNA transport is governed by competition between adsorption/desorption processes and hydrodynamic forces which remobilize eDNA across the water column and sediment storage zones. Retention experiments were conducted for plane and gravel beds, while breakthrough experiments were performed across both bed types and two hydraulic regimes. To quantify eDNA settling rates and validate the conceptual model, an independent experiment under quiescent conditions was performed. Breakthrough curves were analyzed using a continuous time random walk (CTRW) model. Enhanced exchange and retention rates were observed for eDNA in the gravel bed, showing that surface–subsurface interactions and turbulence influenced downstream transport distances. Effective velocities were significantly lower for eDNA than for a conservative tracer across both bed types at low flows. These results underscore that parafluvial processes, including hyporheic exchange and storage in sediments, play a crucial role in eDNA transport dynamics within slow-moving lotic environments.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"42 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098135","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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