Tianle Kong, Xiaoxu Sun*, Zhibin Gu, Nie Yang, Yuqing Huang, Ling Lan, Pin Gao, Huaqing Liu, Yize Wang, Feng Jiang, Baoqin Li and Weimin Sun*,
Mine tailings are extremely oligotrophic environments frequently contaminated with elevated As and Sb, making As(III) and Sb(III) oxidation potentially important energy sources for the tailing microbiome. Although they have been proposed to share similar metabolic pathways, a systemic comparison of the As(III) and Sb(III) oxidation mechanisms and energy utilization efficiencies requires further elucidation. In this study, we employed a combination of physicochemical, molecular, and bioinformatic analyses to compare the kinetic and genetic mechanisms of As(III) and Sb(III) oxidation as well as their respective energy efficiencies for fueling the key nutrient acquisition metabolisms. Thiobacillus and Rhizobium spp. were identified as functional populations for both As(III) and Sb(III) oxidation in mine tailings by DNA-stable isotope probing. However, these microorganisms mediated As(III) and Sb(III) oxidation via different metabolic pathways, resulting in preferential oxidation of Sb(III) over As(III). Notably, both As(III) and Sb(III) oxidation can facilitate nitrogen fixation and phosphate solubilization in mine tailings, with Sb(III) oxidation being more efficient in powering these processes. Thus, this study provided novel insights into the microbial As(III) and Sb(III) oxidation mechanisms and their respective nutrient acquisition efficiencies, which may be critical for the reclamation of mine tailings.
{"title":"Differential Mechanisms of Microbial As(III) and Sb(III) Oxidation and Their Contribution to Tailings Reclamation","authors":"Tianle Kong, Xiaoxu Sun*, Zhibin Gu, Nie Yang, Yuqing Huang, Ling Lan, Pin Gao, Huaqing Liu, Yize Wang, Feng Jiang, Baoqin Li and Weimin Sun*, ","doi":"10.1021/acs.est.4c00863","DOIUrl":"10.1021/acs.est.4c00863","url":null,"abstract":"<p >Mine tailings are extremely oligotrophic environments frequently contaminated with elevated As and Sb, making As(III) and Sb(III) oxidation potentially important energy sources for the tailing microbiome. Although they have been proposed to share similar metabolic pathways, a systemic comparison of the As(III) and Sb(III) oxidation mechanisms and energy utilization efficiencies requires further elucidation. In this study, we employed a combination of physicochemical, molecular, and bioinformatic analyses to compare the kinetic and genetic mechanisms of As(III) and Sb(III) oxidation as well as their respective energy efficiencies for fueling the key nutrient acquisition metabolisms. <i>Thiobacillus</i> and <i>Rhizobium</i> spp. were identified as functional populations for both As(III) and Sb(III) oxidation in mine tailings by DNA-stable isotope probing. However, these microorganisms mediated As(III) and Sb(III) oxidation via different metabolic pathways, resulting in preferential oxidation of Sb(III) over As(III). Notably, both As(III) and Sb(III) oxidation can facilitate nitrogen fixation and phosphate solubilization in mine tailings, with Sb(III) oxidation being more efficient in powering these processes. Thus, this study provided novel insights into the microbial As(III) and Sb(III) oxidation mechanisms and their respective nutrient acquisition efficiencies, which may be critical for the reclamation of mine tailings.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141425674","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}
Tianyi Fan, Jingye Ren, Chenxi Liu, Z. Li, Jieyao Liu, Yele Sun, Yuying Wang, Xiaoai Jin and Fang Zhang*,
Surface-active organics lower the aerosol surface tension (σs/a), leading to enhanced cloud condensation nuclei (CCN) activity and potentially exerting impacts on the climate. Quantification of σs/a is mainly limited to laboratory or modeling work for particles with selected sizes and known chemical compositions. Inferred values from ambient aerosol populations are deficient. In this study, we propose a new method to derive σs/a by combining field measurements made at an urban site in northern China with the κ-Köhler theory. The results present new evidence that organics remarkably lower the surface tension of aerosols in a polluted atmosphere. Particles sized around 40 nm have an averaged σs/a of 53.8 mN m–1, while particles sized up to 100 nm show σs/a values approaching that of pure water. The dependence curve of σs/a with the organic mass resembles the behavior of dicarboxylic acids, suggesting their critical role in reducing the surface tension. The study further reveals that neglecting the σs/a lowering effect would result in lowered ultrafine CCN (diameter <100 nm) concentrations by 6.8–42.1% at a typical range of supersaturations in clouds, demonstrating the significant impact of surface tension on the CCN concentrations of urban aerosols.
{"title":"Evidence of Surface-Tension Lowering of Atmospheric Aerosols by Organics from Field Observations in an Urban Atmosphere: Relation to Particle Size and Chemical Composition","authors":"Tianyi Fan, Jingye Ren, Chenxi Liu, Z. Li, Jieyao Liu, Yele Sun, Yuying Wang, Xiaoai Jin and Fang Zhang*, ","doi":"10.1021/acs.est.4c03141","DOIUrl":"10.1021/acs.est.4c03141","url":null,"abstract":"<p >Surface-active organics lower the aerosol surface tension (σ<sub>s/a</sub>), leading to enhanced cloud condensation nuclei (CCN) activity and potentially exerting impacts on the climate. Quantification of σ<sub>s/a</sub> is mainly limited to laboratory or modeling work for particles with selected sizes and known chemical compositions. Inferred values from ambient aerosol populations are deficient. In this study, we propose a new method to derive σ<sub>s/a</sub> by combining field measurements made at an urban site in northern China with the κ-Köhler theory. The results present new evidence that organics remarkably lower the surface tension of aerosols in a polluted atmosphere. Particles sized around 40 nm have an averaged σ<sub>s/a</sub> of 53.8 mN m<sup>–1</sup>, while particles sized up to 100 nm show σ<sub>s/a</sub> values approaching that of pure water. The dependence curve of σ<sub>s/a</sub> with the organic mass resembles the behavior of dicarboxylic acids, suggesting their critical role in reducing the surface tension. The study further reveals that neglecting the σ<sub>s/a</sub> lowering effect would result in lowered ultrafine CCN (diameter <100 nm) concentrations by 6.8–42.1% at a typical range of supersaturations in clouds, demonstrating the significant impact of surface tension on the CCN concentrations of urban aerosols.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141425677","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}
Wanlin Guo, Hong Ching Kwok, Stephen M. Griffith, Stefan Nagl, Dragan Milovanović, Miljana Pavlović, Nikola M. Pavlović*, Jian Zhen Yu, Peter C. Dedon and Wan Chan*,
Tens of thousands of people in southern Europe suffer from Balkan endemic nephropathy (BEN), and four times as many are at risk. Incidental ingestion of aristolochic acids (AAs), stemming from the ubiquitousAristolochia clematitis(birthwort) weed in the region, leads to DNA adduct-induced toxicity in kidney cells, the primary cause of BEN. Numerous cofactors, including toxic organics and metals, have been investigated, but all have shown small contributions to the overall BEN relative to non-BEN village distribution gradients. Here, we reveal that combustion-derived pollutants from wood and coal burning in Serbia also contaminate arable soil and test as plausible causative factors of BEN. Using a GC–MS screening method, biomass-burning-derived furfural and coal-burning-derived medium-chain alkanes were detected in soil samples from BEN endemic areas levels at up to 63-times and 14-times higher, respectively, than in nonendemic areas. Significantly higher amounts were also detected in colocated wheat grains. Coexposure studies with cultured kidney cells showed that these pollutants enhance DNA adduct formation by AA, – the cause of AA nephrotoxicity and carcinogenicity. With the coincidence of birthwort-derived AAs and the widespread practice of biomass and coal burning for household cooking and heating purposes and agricultural burning in rural low-lying flood-affected areas in the Balkans, these results implicate combustion-derived pollutants in promoting the development of BEN.
南欧有数万人患有巴尔干地方性肾病(BEN),其中四倍的人面临患病风险。意外摄入的马兜铃酸(AAs)源自该地区无处不在的马兜铃科(birthwort)杂草,会导致肾细胞中的 DNA 加合物诱发毒性,这是 BEN 的主要病因。对包括有毒有机物和金属在内的许多辅助因子进行了研究,但所有辅助因子都显示,相对于非 BEN 村的分布梯度,它们对整个 BEN 的贡献很小。在这里,我们揭示了塞尔维亚木材和煤炭燃烧产生的污染物也污染了耕地土壤,并测试出这些污染物可能是 BEN 的致病因素。利用气相色谱-质谱筛选方法,在 BEN 流行区的土壤样本中检测到了生物质燃烧产生的糠醛和煤燃烧产生的中链烷烃,其含量分别比非流行区高 63 倍和 14 倍。在同位小麦粒中也检测到了显著较高的含量。用培养的肾脏细胞进行的共暴露研究表明,这些污染物会增强 AA 形成的 DNA 加合物,这是 AA 肾毒性和致癌性的原因。在巴尔干地区的农村低洼洪涝灾区,家庭烹饪和取暖普遍使用生物质和燃煤,农业焚烧也很普遍。
{"title":"Combustion-Derived Pollutants Linked with Kidney Disease in Low-Lying Flood-Affected Areas in the Balkans","authors":"Wanlin Guo, Hong Ching Kwok, Stephen M. Griffith, Stefan Nagl, Dragan Milovanović, Miljana Pavlović, Nikola M. Pavlović*, Jian Zhen Yu, Peter C. Dedon and Wan Chan*, ","doi":"10.1021/acs.est.4c02848","DOIUrl":"10.1021/acs.est.4c02848","url":null,"abstract":"<p >Tens of thousands of people in southern Europe suffer from Balkan endemic nephropathy (BEN), and four times as many are at risk. Incidental ingestion of aristolochic acids (AAs), stemming from the ubiquitous<i>Aristolochia clematitis</i>(birthwort) weed in the region, leads to DNA adduct-induced toxicity in kidney cells, the primary cause of BEN. Numerous cofactors, including toxic organics and metals, have been investigated, but all have shown small contributions to the overall BEN relative to non-BEN village distribution gradients. Here, we reveal that combustion-derived pollutants from wood and coal burning in Serbia also contaminate arable soil and test as plausible causative factors of BEN. Using a GC–MS screening method, biomass-burning-derived furfural and coal-burning-derived medium-chain alkanes were detected in soil samples from BEN endemic areas levels at up to 63-times and 14-times higher, respectively, than in nonendemic areas. Significantly higher amounts were also detected in colocated wheat grains. Coexposure studies with cultured kidney cells showed that these pollutants enhance DNA adduct formation by AA, – the cause of AA nephrotoxicity and carcinogenicity. With the coincidence of birthwort-derived AAs and the widespread practice of biomass and coal burning for household cooking and heating purposes and agricultural burning in rural low-lying flood-affected areas in the Balkans, these results implicate combustion-derived pollutants in promoting the development of BEN.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141430740","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}
Yarong Bai, Chuhan Miao, Haiqiang Wang* and Zhongbiao Wu,
We developed a simple strategy for preparing IrSn bimetallic clusters encapsulated in pure silicon zeolites via a one-pot hydrothermal synthesis by using diethylamine as a stabilizing agent. A series of investigations verified that metal species have been confined successfully in the inner of MFI zeolites. IrSn bimetallic cluster catalysts were efficient for the CO selective catalytic reduction of NOx in the presence of excess O2. Furthermore, the 13CO temperature-programmed surface reaction results demonstrated that NO2 and N2O could form when most of the CO was transformed into CO2 and that Sn modification could passivate CO oxidation on the IrSn bimetallic clusters, leading to more reductants that could be used for NOx reduction at high temperatures. Furthermore, SO2 can also influence the NOx conversion by inhibiting the oxidation of CO. This study provides a new strategy for preparing efficient environmental catalysts with a high dispersion of metal species.
我们开发了一种简单的策略,以二乙胺为稳定剂,通过一锅水热合成法制备封装在纯硅沸石中的 IrSn 双金属团簇。一系列研究证实,金属物种已成功地被限制在 MFI 沸石内部。IrSn 双金属簇催化剂在过量 O2 存在的情况下能有效地进行 CO 选择性催化还原氮氧化物。此外,13CO 温度编程表面反应结果表明,当大部分 CO 转化为 CO2 时,会形成 NO2 和 N2O,而 Sn 修饰可钝化 IrSn 双金属簇上的 CO 氧化,从而产生更多可用于高温还原 NOx 的还原剂。此外,二氧化硫也会通过抑制 CO 的氧化作用影响氮氧化物的转化。这项研究为制备金属物种高度分散的高效环保催化剂提供了一种新策略。
{"title":"IrSn Bimetallic Clusters Confined in MFI Zeolites for CO Selective Catalytic Reduction of NOx in the Presence of Excess O2","authors":"Yarong Bai, Chuhan Miao, Haiqiang Wang* and Zhongbiao Wu, ","doi":"10.1021/acs.est.4c02540","DOIUrl":"10.1021/acs.est.4c02540","url":null,"abstract":"<p >We developed a simple strategy for preparing IrSn bimetallic clusters encapsulated in pure silicon zeolites via a one-pot hydrothermal synthesis by using diethylamine as a stabilizing agent. A series of investigations verified that metal species have been confined successfully in the inner of MFI zeolites. IrSn bimetallic cluster catalysts were efficient for the CO selective catalytic reduction of NO<sub><i>x</i></sub> in the presence of excess O<sub>2</sub>. Furthermore, the <sup>13</sup>CO temperature-programmed surface reaction results demonstrated that NO<sub>2</sub> and N<sub>2</sub>O could form when most of the CO was transformed into CO<sub>2</sub> and that Sn modification could passivate CO oxidation on the IrSn bimetallic clusters, leading to more reductants that could be used for NO<sub><i>x</i></sub> reduction at high temperatures. Furthermore, SO<sub>2</sub> can also influence the NO<sub><i>x</i></sub> conversion by inhibiting the oxidation of CO. This study provides a new strategy for preparing efficient environmental catalysts with a high dispersion of metal species.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141425678","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}
Placental DNA methylation (DNAm) may be a potential mechanism underlying the effects of prenatal bisphenol analogues (BPs) exposure on reproductive health. Based on the Shanghai-Minhang Birth Cohort Study (S-MBCS), this study investigated associations of placental DNAm at reproduction-related genes with prenatal BPs exposure and children’s digit ratios at age 4 using multiple linear regression models, and mediation analysis was further used to examine the mediating role of placental DNAm in the associations between prenatal BPs exposure and digit ratios among 345 mother–child pairs. Prenatal exposure to bisphenol A (BPA) was associated with hypermethylation at Protocadherin 8 (PCDH8), RBMX Like 2 (RBMXL2), and Sperm Acrosome Associated 1 (SPACA1), while bisphenol F (BPF) exposure was associated with higher methylation levels of Fibroblast Growth Factor 13 (FGF13). Consistent patterns were found in associations between higher DNAm at the 4 genes and increased digit ratios. Further mediation analysis showed that about 15% of the effect of BPF exposure on increased digit ratios was mediated by placental FGF13 methylation. In conclusion, the altered placental DNAm status might be a mediator underlying the feminizing effect of prenatal BPs exposure.
{"title":"The Role of Placental DNA Methylation at Reproduction-Related Genes in Associations between Prenatal Bisphenol Analogues Exposure and the Digit Ratio in Children at Age 4: A Birth Cohort Study","authors":"Jiaxian Chen, Haijun Zhu, Yafei Chen, Shuqin Pan, Hong Liang, Xiuxia Song, Qihan Wu, Wei Yuan, Maohua Miao and Ziliang Wang*, ","doi":"10.1021/acs.est.4c03764","DOIUrl":"10.1021/acs.est.4c03764","url":null,"abstract":"<p >Placental DNA methylation (DNAm) may be a potential mechanism underlying the effects of prenatal bisphenol analogues (BPs) exposure on reproductive health. Based on the Shanghai-Minhang Birth Cohort Study (S-MBCS), this study investigated associations of placental DNAm at reproduction-related genes with prenatal BPs exposure and children’s digit ratios at age 4 using multiple linear regression models, and mediation analysis was further used to examine the mediating role of placental DNAm in the associations between prenatal BPs exposure and digit ratios among 345 mother–child pairs. Prenatal exposure to bisphenol A (BPA) was associated with hypermethylation at Protocadherin 8 (<i>PCDH8</i>), RBMX Like 2 (<i>RBMXL2</i>), and Sperm Acrosome Associated 1 (<i>SPACA1</i>), while bisphenol F (BPF) exposure was associated with higher methylation levels of Fibroblast Growth Factor 13 (<i>FGF13</i>). Consistent patterns were found in associations between higher DNAm at the 4 genes and increased digit ratios. Further mediation analysis showed that about 15% of the effect of BPF exposure on increased digit ratios was mediated by placental <i>FGF13</i> methylation. In conclusion, the altered placental DNAm status might be a mediator underlying the feminizing effect of prenatal BPs exposure.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141425685","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 microbial oxidation of short-chain gaseous alkanes (SCGAs, consisting of ethane, propane, and butane) serves as an efficient sink to mitigate these gases’ emission to the atmosphere, thus reducing their negative impacts on air quality and climate. “Candidatus Alkanivorans nitratireducens” are recently found to mediate nitrate-dependent anaerobic ethane oxidation (n-DAEO). In natural ecosystems, anaerobic ammonium-oxidizing (anammox) bacteria may consume nitrite generated from nitrate reduction by “Ca. A. nitratireducens”, thereby alleviating the inhibition caused by nitrite accumulation on the metabolism of “Ca. A. nitratireducens”. Here, we demonstrate the coupling of n-DAEO with anammox in a laboratory-scale model system to prevent nitrite accumulation. Our results suggest that a high concentration of ethane (6.9–7.9%) has acute inhibition on anammox activities, thus making the coupling process a significant challenge. By maintaining ethane concentrations within the range of 1.7–5.5%, stable ethane and ammonium oxidation, nitrate reduction, and dinitrogen gas generation without nitrite accumulation were finally achieved. After the accomplished coupling of n-DAEO with anammox, nitrate reduction rates increased by 8.1 times compared to the rate observed with n-DAEO alone. Microbial community profiling via 16S rRNA gene amplicon sequencing showed “Ca. A. nitratireducens” (6.6–12.9%) and anammox bacteria “Candidatus Kuenenia” (3.4–5.6%) were both dominant in the system, indicating they potentially form a syntrophic partnership to jointly contribute to nitrogen removal. Our findings offer insights into the cross-feeding interaction between “Ca. A. nitratireducens” and anammox bacteria in anoxic environments.
{"title":"Coupling Nitrate-Dependent Anaerobic Ethane Degradation with Anaerobic Ammonium Oxidation","authors":"Xiawei Liu, Mengxiong Wu and Jianhua Guo*, ","doi":"10.1021/acs.est.4c00488","DOIUrl":"10.1021/acs.est.4c00488","url":null,"abstract":"<p >The microbial oxidation of short-chain gaseous alkanes (SCGAs, consisting of ethane, propane, and butane) serves as an efficient sink to mitigate these gases’ emission to the atmosphere, thus reducing their negative impacts on air quality and climate. “<i>Candidatus</i> Alkanivorans nitratireducens” are recently found to mediate nitrate-dependent anaerobic ethane oxidation (n-DAEO). In natural ecosystems, anaerobic ammonium-oxidizing (anammox) bacteria may consume nitrite generated from nitrate reduction by “<i>Ca.</i> A. nitratireducens”, thereby alleviating the inhibition caused by nitrite accumulation on the metabolism of “<i>Ca.</i> A. nitratireducens”. Here, we demonstrate the coupling of n-DAEO with anammox in a laboratory-scale model system to prevent nitrite accumulation. Our results suggest that a high concentration of ethane (6.9–7.9%) has acute inhibition on anammox activities, thus making the coupling process a significant challenge. By maintaining ethane concentrations within the range of 1.7–5.5%, stable ethane and ammonium oxidation, nitrate reduction, and dinitrogen gas generation without nitrite accumulation were finally achieved. After the accomplished coupling of n-DAEO with anammox, nitrate reduction rates increased by 8.1 times compared to the rate observed with n-DAEO alone. Microbial community profiling via 16S rRNA gene amplicon sequencing showed “<i>Ca.</i> A. nitratireducens” (6.6–12.9%) and anammox bacteria “<i>Candidatus</i> Kuenenia” (3.4–5.6%) were both dominant in the system, indicating they potentially form a syntrophic partnership to jointly contribute to nitrogen removal. Our findings offer insights into the cross-feeding interaction between “<i>Ca.</i> A. nitratireducens” and anammox bacteria in anoxic environments.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141425673","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}
Zhiheng Li, Jie Chen, Linglin Xu, Ping Zhang, Haohua Ni, Wenlu Zhao, Zhiguo Fang and Huijun Liu*,
Soil antibiotic pollution profoundly influences plant growth and photosynthetic performance, yet the main disturbed processes and the underlying mechanisms remain elusive. This study explored the photosynthetic toxicity of quinolone antibiotics across three generations on rice plants and clarified the mechanisms through experimental and computational studies. Marked variations across antibiotic generations were noted in their impact on rice photosynthesis with the level of inhibition intensifying from the second to the fourth generation. Omics analyses consistently targeted the light reaction phase of photosynthesis as the primary process impacted, emphasizing the particular vulnerability of photosystem II (PS II) to the antibiotic stress, as manifested by significant interruptions in the photon-mediated electron transport and O2 production. PS II center D2 protein (psbD) was identified as the primary target of the tested antibiotics, with the fourth-generation quinolones displaying the highest binding affinity to psbD. A predictive machine learning method was constructed to pinpoint antibiotic substructures that conferred enhanced affinity. As antibiotic generations evolve, the positive contribution of the carbonyl and carboxyl groups on the 4-quinolone core ring in the affinity interaction gradually intensified. This research illuminates the photosynthetic toxicities of antibiotics across generations, offering insights for the risk assessment of antibiotics and highlighting their potential threats to carbon fixation of agroecosystems.
{"title":"Quinolone Antibiotics Inhibit the Rice Photosynthesis by Targeting Photosystem II Center Protein: Generational Differences and Mechanistic Insights","authors":"Zhiheng Li, Jie Chen, Linglin Xu, Ping Zhang, Haohua Ni, Wenlu Zhao, Zhiguo Fang and Huijun Liu*, ","doi":"10.1021/acs.est.4c01866","DOIUrl":"10.1021/acs.est.4c01866","url":null,"abstract":"<p >Soil antibiotic pollution profoundly influences plant growth and photosynthetic performance, yet the main disturbed processes and the underlying mechanisms remain elusive. This study explored the photosynthetic toxicity of quinolone antibiotics across three generations on rice plants and clarified the mechanisms through experimental and computational studies. Marked variations across antibiotic generations were noted in their impact on rice photosynthesis with the level of inhibition intensifying from the second to the fourth generation. Omics analyses consistently targeted the light reaction phase of photosynthesis as the primary process impacted, emphasizing the particular vulnerability of photosystem II (PS II) to the antibiotic stress, as manifested by significant interruptions in the photon-mediated electron transport and O<sub>2</sub> production. PS II center D2 protein (psbD) was identified as the primary target of the tested antibiotics, with the fourth-generation quinolones displaying the highest binding affinity to psbD. A predictive machine learning method was constructed to pinpoint antibiotic substructures that conferred enhanced affinity. As antibiotic generations evolve, the positive contribution of the carbonyl and carboxyl groups on the 4-quinolone core ring in the affinity interaction gradually intensified. This research illuminates the photosynthetic toxicities of antibiotics across generations, offering insights for the risk assessment of antibiotics and highlighting their potential threats to carbon fixation of agroecosystems.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141425681","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}
Clara Ganhör, Lukas Mayr, Julia Zolles, Marion Almeder, Matin Kazemi, Markus Mandl, Christian Wechselberger, Dave Bandke, Sarah Theiner, Christian Doppler*, Andreas Schweikert, Marina Müller, Špela Puh, Michaela Kotnik, Rupert Langer, Gunda Koellensperger and David Bernhard,
Aluminum (Al) is the most abundant metal in the earth’s crust, and humans are exposed to Al through sources like food, cosmetics, and medication. So far, no comprehensive data on the Al distribution between and within human tissues were reported. We measured Al concentrations in 24 different tissue types of 8 autopsied patients using ICP–MS/MS (inductively coupled plasma–tandem mass spectrometry) under cleanroom conditions and found surprisingly high concentrations in both the upper and inferior lobes of the lung and hilar lymph nodes. Al/Si ratios in lung and hilar lymph node samples of 12 additional patients were similar to the ratios reported in urban fine dust. Histological analyses using lumogallion staining showed Al in lung erythrocytes and macrophages, indicating the uptake of airborne Al in the bloodstream. Furthermore, Al was continuously found in PM2.5 and PM10 fine dust particles over 7 years in Upper Austria, Austria. According to our findings, air pollution needs to be reconsidered as a major Al source for humans and the environment.
Little is known about the distribution of aluminum within humans. In this study, human lung tissues revealed surprisingly high Al concentrations, identifying airborne Al as a potentially underestimated source of human Al.
{"title":"Airborne Aluminum as an Underestimated Source of Human Exposure: Quantification of Aluminum in 24 Human Tissue Types Reveals High Aluminum Concentrations in Lung and Hilar Lymph Node Tissues","authors":"Clara Ganhör, Lukas Mayr, Julia Zolles, Marion Almeder, Matin Kazemi, Markus Mandl, Christian Wechselberger, Dave Bandke, Sarah Theiner, Christian Doppler*, Andreas Schweikert, Marina Müller, Špela Puh, Michaela Kotnik, Rupert Langer, Gunda Koellensperger and David Bernhard, ","doi":"10.1021/acs.est.4c01910","DOIUrl":"10.1021/acs.est.4c01910","url":null,"abstract":"<p >Aluminum (Al) is the most abundant metal in the earth’s crust, and humans are exposed to Al through sources like food, cosmetics, and medication. So far, no comprehensive data on the Al distribution between and within human tissues were reported. We measured Al concentrations in 24 different tissue types of 8 autopsied patients using ICP–MS/MS (inductively coupled plasma–tandem mass spectrometry) under cleanroom conditions and found surprisingly high concentrations in both the upper and inferior lobes of the lung and hilar lymph nodes. Al/Si ratios in lung and hilar lymph node samples of 12 additional patients were similar to the ratios reported in urban fine dust. Histological analyses using lumogallion staining showed Al in lung erythrocytes and macrophages, indicating the uptake of airborne Al in the bloodstream. Furthermore, Al was continuously found in PM<sub>2.5</sub> and PM<sub>10</sub> fine dust particles over 7 years in Upper Austria, Austria. According to our findings, air pollution needs to be reconsidered as a major Al source for humans and the environment.</p><p >Little is known about the distribution of aluminum within humans. In this study, human lung tissues revealed surprisingly high Al concentrations, identifying airborne Al as a potentially underestimated source of human Al.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.est.4c01910","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141416589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Colin A. Cooke*, Kira M. Holland, Craig A. Emmerton, Paul E. Drevnick, Alison S. Criscitiello and Brandi Newton,
Mountaintop removal coal mining is a source of downstream pollution. Here, we show that mountaintop removal coal mining also pollutes ecosystems downwind. We sampled regional snowpack near the end of winter along a transect of sites located 3–60 km downwind of coal mining in the Elk River valley of British Columbia, Canada. Vast quantities of polycyclic aromatic compounds (PACs), a toxic class of organic contaminants, are emitted and transported atmospherically far from emission sources. Summed PAC (ΣPAC) snowpack concentrations ranged from 29–94,866 ng/L. Snowpack ΣPAC loads, which account for variable snowpack depth, ranged from <10 μg/m2 at sites >50 km southeast of the mines to >1000 μg/m2 at sites in the Elk River valley near mining operations, with one site >15,000 μg/m2. Outside of the Elk River valley, snowpack ΣPAC loads exhibited a clear spatial pattern decreasing away from the mines. The compositional fingerprint of this PAC pollution matches closely with Elk River valley coal. Beyond our study region, modeling results suggest a depositional footprint extending across western Canada and the northwestern United States. These findings carry important implications for receiving ecosystems and for communities located close to mountaintop removal coal mines exposed to air pollution elevated in PACs.
Snowpack samples from across the southern Canadian Rockies reveal widespread polycyclic aromatic compound pollution sourced from mountaintop removal coal mining.
{"title":"Mountaintop Removal Coal Mining Contaminates Snowpack across a Broad Region","authors":"Colin A. Cooke*, Kira M. Holland, Craig A. Emmerton, Paul E. Drevnick, Alison S. Criscitiello and Brandi Newton, ","doi":"10.1021/acs.est.4c02596","DOIUrl":"10.1021/acs.est.4c02596","url":null,"abstract":"<p >Mountaintop removal coal mining is a source of downstream pollution. Here, we show that mountaintop removal coal mining also pollutes ecosystems downwind. We sampled regional snowpack near the end of winter along a transect of sites located 3–60 km downwind of coal mining in the Elk River valley of British Columbia, Canada. Vast quantities of polycyclic aromatic compounds (PACs), a toxic class of organic contaminants, are emitted and transported atmospherically far from emission sources. Summed PAC (ΣPAC) snowpack concentrations ranged from 29–94,866 ng/L. Snowpack ΣPAC loads, which account for variable snowpack depth, ranged from <10 μg/m<sup>2</sup> at sites >50 km southeast of the mines to >1000 μg/m<sup>2</sup> at sites in the Elk River valley near mining operations, with one site >15,000 μg/m<sup>2</sup>. Outside of the Elk River valley, snowpack ΣPAC loads exhibited a clear spatial pattern decreasing away from the mines. The compositional fingerprint of this PAC pollution matches closely with Elk River valley coal. Beyond our study region, modeling results suggest a depositional footprint extending across western Canada and the northwestern United States. These findings carry important implications for receiving ecosystems and for communities located close to mountaintop removal coal mines exposed to air pollution elevated in PACs.</p><p >Snowpack samples from across the southern Canadian Rockies reveal widespread polycyclic aromatic compound pollution sourced from mountaintop removal coal mining.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.est.4c02596","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141416594","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yujie Zhuang, Xin Liu, Jinhui Zhou, Hu Sheng and Zengwei Yuan*,
Excessive anthropogenic phosphorus (P) emissions put constant pressure on aquatic ecosystems. This pressure can be quantified as the freshwater eutrophication potential (FEP) by linking P emissions, P fate in environmental compartments, and the potentially disappeared fraction of species due to increase of P concentrations in freshwater. However, previous fate modeling on global and regional scales is mainly based on the eight-direction algorithm without distinguishing pollution sources. The algorithm fails to characterize the fate paths of point-source emissions via subsurface pipelines and wastewater treatment infrastructure, and exhibits suboptimal performance in accounting for multidirectional paths caused by river bifurcations, especially in flat terrains. Here we aim to improve the fate modeling by incorporating various fate paths and addressing multidirectional scenarios. We also update the P estimates by complementing potential untreated point-source emissions (PSu). The improved method is examined in a rapidly urbanizing area in Taihu Lake Basin, China in 2017 at a spatial resolution of 100 m × 100 m. Results show that the contribution of PSu on FEP (62.6%) is greater than that on P emissions (58.5%). The FEP is more spatially widely distributed with the improved fate modeling, facilitating targeted regulatory strategies tailored to local conditions.
过量的人为磷(P)排放给水生生态系统带来了持续的压力。这种压力可以量化为淡水富营养化潜能值(FEP),将磷排放、磷在环境分区中的归宿以及因淡水中磷浓度增加而可能消失的物种数量联系起来。然而,以往在全球和区域范围内进行的最终结果建模主要基于八方向算法,而没有区分污染源。该算法无法描述通过地下管道和污水处理基础设施的点源排放的归宿路径,而且在考虑河流分叉造成的多方向路径方面表现不佳,尤其是在平坦地形中。在此,我们旨在通过纳入各种归宿路径和处理多向情景来改进归宿模型。我们还通过补充潜在的未处理点源排放(PSu)来更新 P 估算值。结果表明,PSu 对 FEP 的贡献(62.6%)大于对 P 排放的贡献(58.5%)。在改进了归宿模拟后,FEP 的空间分布更加广泛,有利于因地制宜地制定有针对性的监管策略。
{"title":"Multidirectional Fate Path Model to Connect Phosphorus Emissions with Freshwater Eutrophication Potential","authors":"Yujie Zhuang, Xin Liu, Jinhui Zhou, Hu Sheng and Zengwei Yuan*, ","doi":"10.1021/acs.est.4c01205","DOIUrl":"10.1021/acs.est.4c01205","url":null,"abstract":"<p >Excessive anthropogenic phosphorus (P) emissions put constant pressure on aquatic ecosystems. This pressure can be quantified as the freshwater eutrophication potential (FEP) by linking P emissions, P fate in environmental compartments, and the potentially disappeared fraction of species due to increase of P concentrations in freshwater. However, previous fate modeling on global and regional scales is mainly based on the eight-direction algorithm without distinguishing pollution sources. The algorithm fails to characterize the fate paths of point-source emissions via subsurface pipelines and wastewater treatment infrastructure, and exhibits suboptimal performance in accounting for multidirectional paths caused by river bifurcations, especially in flat terrains. Here we aim to improve the fate modeling by incorporating various fate paths and addressing multidirectional scenarios. We also update the P estimates by complementing potential untreated point-source emissions (PSu). The improved method is examined in a rapidly urbanizing area in Taihu Lake Basin, China in 2017 at a spatial resolution of 100 m × 100 m. Results show that the contribution of PSu on FEP (62.6%) is greater than that on P emissions (58.5%). The FEP is more spatially widely distributed with the improved fate modeling, facilitating targeted regulatory strategies tailored to local conditions.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141430730","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}