环境科学与技术最新文献

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dilp2-Mediated Insulin Signaling Pathway Was Involved in O3-Induced Multigenerational Effects of Shortened Lifespan in Drosophila melanogasters
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2025-02-04 DOI: 10.1021/acs.est.4c04580
Nan Nan, Yuntong Liu, Zhipeng Yan, Yaru Zhang, Shiya Li, Jianqin Zhang, Guohua Qin, Nan Sang
{"title":"dilp2-Mediated Insulin Signaling Pathway Was Involved in O3-Induced Multigenerational Effects of Shortened Lifespan in Drosophila melanogasters","authors":"Nan Nan, Yuntong Liu, Zhipeng Yan, Yaru Zhang, Shiya Li, Jianqin Zhang, Guohua Qin, Nan Sang","doi":"10.1021/acs.est.4c04580","DOIUrl":"https://doi.org/10.1021/acs.est.4c04580","url":null,"abstract":"As a long-standing atmospheric pollutant, ozone (O<sub>3</sub>) exerts enduring effects on biological health. However, experimental research on its impact on organism lifespan and generational effects is limited. This study exposed three generations of fruit flies (<i>Drosophila melanogaster</i>) to O<sub>3</sub>, revealing a shortened lifespan across generations. Specifically, after O<sub>3</sub> exposure, the lifespan of the F2 generation was significantly reduced compared with F0 and F1 generations, indicating a cumulative multigenerational effect. Transcriptome analysis unveiled significant disruptions in metabolic pathways, notably the insulin signaling pathway. Subsequent qRT-PCR analysis showed elevated mRNA levels of insulin pathway-related genes (<i>dilp2</i>, <i>dilp3</i>, <i>dilp5</i>, <i>InR</i>, and <i>TOR</i>), alongside decreased expression levels of <i>FOXO</i>, <i>4E-BP</i>, and <i>Atg5</i> in flies exposed to O<sub>3</sub>. Notably, knocking down <i>dilp2</i>, rather than <i>dilp3</i>, <i>dilp5,</i> and <i>InR</i>, rescued the O<sub>3</sub>-induced lifespan shortening. Overall, O<sub>3</sub> exposure triggered activation of the dilp2-mediated InR-FOXO/TOR-4E-BP-Atg5 signaling pathway, potentially contributing to shortened lifespan with cumulative effects. This study highlights the viability of employing fruit flies as a model to evaluate the multigenerational toxicity of environmental pollutants, particularly atmospheric pollutants.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"63 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143084172","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}
引用次数: 0
Sulfidation of Magnetite for Superior Dechlorination of Trichloroethene
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2025-02-04 DOI: 10.1021/acs.est.4c07127
Ariel Nunez Garcia, Matt Lee, Lei Ding, Xiguang Liang, Chengqi Wang, Feng He, Denis M. O’Carroll
{"title":"Sulfidation of Magnetite for Superior Dechlorination of Trichloroethene","authors":"Ariel Nunez Garcia, Matt Lee, Lei Ding, Xiguang Liang, Chengqi Wang, Feng He, Denis M. O’Carroll","doi":"10.1021/acs.est.4c07127","DOIUrl":"https://doi.org/10.1021/acs.est.4c07127","url":null,"abstract":"The reported contributions of magnetite to the abiotic natural attenuation of chlorinated ethenes have generated interest in its potential for soil and groundwater remediation. In this study, we investigated the impact of the two-step sulfidation method on the physicochemical properties and reactivity of magnetite with trichloroethene (TCE). We systematically evaluated the effect of different sulfur precursors (dithionite, thiosulfate, and sulfide) and sulfur-to-iron ([S/Fe]<sub>dosed</sub>) molar ratios on the reactivity. Results were compared to those of sulfidated nZVI (S-nZVI) as a benchmark for assessing the efficacy of sulfidated magnetite (S–Fe<sub>3</sub>O<sub>4</sub>). The findings indicated limited reactivity of magnetite when sulfidated with dithionite and thiosulfate. However, sulfidation with sulfide yielded reaction rates comparable to those of S-nZVI, particularly at lower [S/Fe]<sub>dosed</sub> ratios. At higher [S/Fe]<sub>dosed</sub> ratios (&gt;0.1), sulfide-sulfidated magnetite (S–Fe<sub>3</sub>O<sub>4_S</sub>) exhibited reaction rates surpassing those of S-nZVI, with the major dechlorination product being acetylene. Nonetheless, reusability experiments demonstrated that the performance of S–Fe<sub>3</sub>O<sub>4</sub> diminished with aging. These results show that S–Fe<sub>3</sub>O<sub>4_S</sub> achieved complete transformation of TCE to acetylene, with reaction rates comparable to S-nZVI. Given its lower cost of production, engineered S–Fe<sub>3</sub>O<sub>4_S</sub> remediation systems could serve as a more affordable alternative for in situ chemical reduction of TCE with further research and development.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"133 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083987","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}
引用次数: 0
Detoxification of Carbonaceous Species for Efficient Perfluorocarbon Hydrolysis
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2025-02-04 DOI: 10.1021/acs.est.4c11326
Xiaojian Wang, Junwei Fu, Hang Zhang, Jialin Zheng, Heping Chen, Kang Liu, Lihong Jing, Xueqing Xing, Zhang Lin, Liyuan Chai, Min Liu
{"title":"Detoxification of Carbonaceous Species for Efficient Perfluorocarbon Hydrolysis","authors":"Xiaojian Wang, Junwei Fu, Hang Zhang, Jialin Zheng, Heping Chen, Kang Liu, Lihong Jing, Xueqing Xing, Zhang Lin, Liyuan Chai, Min Liu","doi":"10.1021/acs.est.4c11326","DOIUrl":"https://doi.org/10.1021/acs.est.4c11326","url":null,"abstract":"Thermocatalytic hydrolysis of perfluorocarbons (PFCs) is a promising way to reduce their emission and environmental hazards. However, hydrolysis of PFCs, such as CF<sub>4</sub>, usually suffers from a drastic activity decline during the induction period, which seriously hinders its conversion performances and practical applications. In this work, we found that the carbonaceous (*COO) species account for the activity decline during the induction period, and their detoxification could promote PFC hydrolysis at low temperature. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) shows that the poisoning signals belong to *COO species on the surface of γ-Al<sub>2</sub>O<sub>3</sub> during CF<sub>4</sub> catalytic hydrolysis. The adsorption configuration of *CFOH intermediate is the key to the formation of poisoned *COO species. By introducing Ni sites with strong *CFOH adsorption capacity into γ-Al<sub>2</sub>O<sub>3</sub>, the *CFOH at the Al active site can transfer to the adjacent Ni site to avoid the formation of poisoned *COO species, which was proved by DRIFTS and density functional theory. As a result, the optimal 0.1Ni/γ-Al<sub>2</sub>O<sub>3</sub> (10% Ni loaded γ-Al<sub>2</sub>O<sub>3</sub>) catalyst achieved 100% CF<sub>4</sub> conversion without any activity decline at 570 °C for over 300 h, much higher than that of ∼55% CF<sub>4</sub> conversion on pure γ-Al<sub>2</sub>O<sub>3</sub> at the same temperature. This work provides new insights into the detoxification of thermocatalytic PFC hydrolysis at low temperatures.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"38 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083988","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}
引用次数: 0
Correction to “Winter Polycyclic Aromatic Hydrocarbon-Bound Particulate Matter from Peri-urban North China Promotes Lung Cancer Cell Metastasis”
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2025-02-04 DOI: 10.1021/acs.est.4c13857
Huifeng Yue, Yang Yun, Rui Gao, Guangke Li, Nan Sang
{"title":"Correction to “Winter Polycyclic Aromatic Hydrocarbon-Bound Particulate Matter from Peri-urban North China Promotes Lung Cancer Cell Metastasis”","authors":"Huifeng Yue, Yang Yun, Rui Gao, Guangke Li, Nan Sang","doi":"10.1021/acs.est.4c13857","DOIUrl":"https://doi.org/10.1021/acs.est.4c13857","url":null,"abstract":"We recently found that the incorrect representative images were used in Figure 3. The error affects only the presentation of representative images and not the underlying calculations. None of the conclusions of the work is affected. The wound healing assay of 0.3 μg/mL PM<sub>10</sub> at 24 h and 10 μg/mL PM<sub>2.5</sub> and PM<sub>10</sub> at 24 h in Figure 3A and the transwell image panels of the 3 and 10 μg/mL PM<sub>2.5</sub> groups in Figure 3B have been corrected in the version of Figure 3 presented here. Figure 3. Effects of winter PM on A549 cell migration and invasion. (A) Effect of winter PM on A549 cell migration determined by a wound healing assay (200× magnification). A549 cells were treated with winter PM at various concentrations (0, 0.1, 0.3, 1, 3, and 10 μg/mL) for different times (0, 6, 12, and 24 h), and the micrographs show representative images of cell migration. (B) Effect of winter PM on A549 cell invasion as detected by the cell invasion assay (400× magnification). A549 cells were incubated with winter PM at various concentrations (0, 0.1, 0.3, 1, 3, and 10 μg/mL) for 24 h; subsequently, the invasive ability was evaluated using the cell invasion assay. The top section includes micrographs of the representative images of cell migration under different treatment conditions, and the bottom panel shows the calculation of the mean number of invasive cells in each group. For PM<sub>2.5</sub>, *<i>p</i> &lt; 0.05 and **<i>p</i> &lt; 0.01 vs the control group; for PM<sub>10</sub>, <sup>#</sup><i>p</i> &lt; 0.05 vs the control group. This article has not yet been cited by other publications.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"76 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083989","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}
引用次数: 0
Interception History Drives Colloid Transport Variance in Porous Media
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2025-02-03 DOI: 10.1021/acs.est.4c06509
Sabrina N. Volponi, Bashar M. Al-Zghoul, Giovanni Porta, Diogo Bolster, William P. Johnson
{"title":"Interception History Drives Colloid Transport Variance in Porous Media","authors":"Sabrina N. Volponi, Bashar M. Al-Zghoul, Giovanni Porta, Diogo Bolster, William P. Johnson","doi":"10.1021/acs.est.4c06509","DOIUrl":"https://doi.org/10.1021/acs.est.4c06509","url":null,"abstract":"Colloid transport in porous media is traditionally predicted using the principle of constant fractional removal for each grain passed, such that concentrations decrease exponentially with transport distance. This approach successfully describes transport when repulsive barriers to attachment are absent. However, repulsive barriers characterize environmental contexts wherein attachment upon grain interception is inhibited, causing colloid concentrations to decay nonexponentially with distance from the source and thwarting prediction. The pervasiveness of these nonexponential trends across wide-ranging experiments suggests that a fundamental process is at play. Here, we propose a paradigm shift by considering constant fractional loss with each interception rather than with each grain passed. We show that by recognizing the history of grain interceptions, a pathway is revealed toward a simple and predictive framework in which nonexponential trends emerge. This shift in perspective offers the possibility of colloid transport prediction in settings that were previously infeasible using classic filtration theory, with potential applications in contexts ranging from environmental (e.g., groundwater aquifer protection) to biomedical (e.g., drug delivery).","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"61 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083990","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}
引用次数: 0
Atomic Hydrogen in Hydrogenolysis: Converting and Detoxifying Carbon-Heteroatom Bonds via Paired Electrolysis
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2025-02-03 DOI: 10.1021/acs.est.4c11680
Qiancheng Wang, Jianqiao Xu, Shuai Wu, Mu Wang, Xingyun Zhuang, Guofang Tian, Fu Xu, Jianyun Liu, Gong Zhang, Jinghong Li
{"title":"Atomic Hydrogen in Hydrogenolysis: Converting and Detoxifying Carbon-Heteroatom Bonds via Paired Electrolysis","authors":"Qiancheng Wang, Jianqiao Xu, Shuai Wu, Mu Wang, Xingyun Zhuang, Guofang Tian, Fu Xu, Jianyun Liu, Gong Zhang, Jinghong Li","doi":"10.1021/acs.est.4c11680","DOIUrl":"https://doi.org/10.1021/acs.est.4c11680","url":null,"abstract":"The presence of carbon-heteroatom bonds (C–N, C–O, and C–S) significantly enhances the stability and toxicity of pollutants. Hydroxyl radicals (<sup>•</sup>OH)-mediated electrochemical processes show promise; however, the bond energies associated with carbon-heteroatom bonds exceed 200 kJ/mol, which constrains the effectiveness of oxidative degradation and detoxification. We have developed a paired electrolysis process coupling hydrogen atom (H<sup>*</sup>) generation at the cathode with <sup>•</sup>OH production at the anode. The involvement of H<sup>*</sup> and <sup>•</sup>OH in this system was first confirmed by using methylene blue (MB) as an electrochemical probe. When applied to the degradation of glyphosate (GP), which contains C–N bonds, the paired electrolysis process achieved removal efficiencies for COD, TOC, and toxicity that were twice those of individual oxidation processes. The degradation kinetics also exhibited performance that was double that of individual oxidation processes. Mass spectrometry and theoretical calculations confirmed that hydrogenolysis of H<sup>*</sup> effectively attacks high-energy C–N bonds, thereby circumventing the rate-limiting steps associated with standalone <sup>•</sup>OH oxidation, enhancing pollutant degradation and reducing toxicity. When applied to pollutants containing C–O and C–S bonds, the paired electrolysis process demonstrated improvements in COD, TOC, and toxicity removal of approximately 30%, 10%, and 20%, respectively, showcasing its multifunctionality and scalability. Seven days of practical wastewater experiments further validated the effectiveness and durability of this technology.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"12 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083991","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}
引用次数: 0
The Influence of Wildfire Smoke on Ambient PM2.5 Chemical Species Concentrations in the Contiguous US
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2025-02-03 DOI: 10.1021/acs.est.4c09011
Emma Krasovich Southworth, Minghao Qiu, Carlos F. Gould, Ayako Kawano, Jeff Wen, Sam Heft-Neal, Kara Kilpatrick Voss, Alandra Lopez, Scott Fendorf, Jennifer Anne Burney, Marshall Burke
{"title":"The Influence of Wildfire Smoke on Ambient PM2.5 Chemical Species Concentrations in the Contiguous US","authors":"Emma Krasovich Southworth, Minghao Qiu, Carlos F. Gould, Ayako Kawano, Jeff Wen, Sam Heft-Neal, Kara Kilpatrick Voss, Alandra Lopez, Scott Fendorf, Jennifer Anne Burney, Marshall Burke","doi":"10.1021/acs.est.4c09011","DOIUrl":"https://doi.org/10.1021/acs.est.4c09011","url":null,"abstract":"Wildfires significantly contribute to ambient air pollution, yet our understanding of how wildfire smoke influences specific chemicals and their resulting concentration in smoke remains incomplete. We combine 15 years of daily species-specific PM<sub>2.5</sub> concentrations from 700 air pollution monitors with satellite-derived ambient wildfire smoke PM<sub>2.5</sub>, and use a panel regression to estimate wildfire smoke’s contribution to the concentrations of 27 different chemical species in PM<sub>2.5</sub>. Wildfire smoke drives detectable increases in the concentration of 25 out of the 27 species with the largest increases observed for organic carbon, elemental carbon, and potassium. We find that smoke originating from wildfires that burned structures had higher concentrations of copper, lead, zinc, and nickel relative to smoke from fires that did not burn structures. Wildfire smoke is responsible for an increasing share of ambient concentrations of multiple species, some of which are particularly harmful to health. Using a risk assessment approach, we find that wildfire-induced enhancement of carcinogenic species concentrations could cause increases in population cancer risk, but these increases are very small relative to other environmental risks. We demonstrate how combining ground-monitored and satellite-derived data can be used to measure wildfire smoke’s influence on chemical concentrations and estimate population exposures at large scales.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"62 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143084173","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}
引用次数: 0
Emerging PFAS Exposure Is More Potent in Altering Childhood Lipid Levels Mediated by Mitochondrial DNA Copy Number
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2025-02-03 DOI: 10.1021/acs.est.4c13095
Peiwei Xu, Min Nian, Jie Xiang, Xinhan Zhang, Ping Cheng, Dandan Xu, Yuan Chen, Xiaofeng Wang, Zhijian Chen, Xiaoming Lou, Mingliang Fang
{"title":"Emerging PFAS Exposure Is More Potent in Altering Childhood Lipid Levels Mediated by Mitochondrial DNA Copy Number","authors":"Peiwei Xu, Min Nian, Jie Xiang, Xinhan Zhang, Ping Cheng, Dandan Xu, Yuan Chen, Xiaofeng Wang, Zhijian Chen, Xiaoming Lou, Mingliang Fang","doi":"10.1021/acs.est.4c13095","DOIUrl":"https://doi.org/10.1021/acs.est.4c13095","url":null,"abstract":"Per- and polyfluoroalkyl substances (PFAS) pose potential health risks to lipid metabolism, but the effects of emerging PFAS alternatives, particularly in children, remain unclear. This cross-sectional study investigated the association between emerging PFAS exposure and lipid levels in 294 Chinese children aged 7–10 years, analyzing blood samples for 14 PFAS and lipid profiles, including triglycerides (TG), total cholesterol (TC), high-density lipoprotein (HDL), low-density lipoprotein (LDL), apolipoprotein A1 (ApoA1), and apolipoprotein B (ApoB). Exposure to 6:2 Cl-PFESA, PFO4DA, and PFO5DoDA was associated with higher TC, TG, and LDL levels, with PFO4DA increasing the TC by 1.7% and PFO5DoDA increasing the TG by 10.7%. Weighted quantile sum (WQS) regression showed mixed PFAS exposure positively associated with TG (0.08, 95% CI: 0.007, 0.153). PFO4DA had the highest weight for TC (0.468), TG (0.327), LDL (0.57), ApoA1 (0.243), and ApoB (0.466), while PFMOAA had the highest weight for HDL (0.332). Bayesian Kernel Machine Regression (BKMR) analysis confirmed positive associations between the PFAS mixture and TC, TG, LDL, and ApoA1. Mediation analysis revealed that mtDNAcn significantly mediated PFAS exposure’s effect on TG levels, explaining 27.2–74.2% of the total effect. These findings highlight the need for regulatory action to address the emerging PFAS risks.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"5 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143076957","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}
引用次数: 0
Unexpectedly High Levels of H2O2 Drive Sulfate Formation over the Residual Layer in Beijing
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2025-02-02 DOI: 10.1021/acs.est.4c09004
Pengfei Liu, Shuyuan Jia, Shuying Li, Pengkun Ma, Yongjing Ma, Yuan Liu, Zhiheng Liao, Yonghong Wang, Biwu Chu, Qingxin Ma, Jiannong Quan, Yujing Mu, Hong He
{"title":"Unexpectedly High Levels of H2O2 Drive Sulfate Formation over the Residual Layer in Beijing","authors":"Pengfei Liu, Shuyuan Jia, Shuying Li, Pengkun Ma, Yongjing Ma, Yuan Liu, Zhiheng Liao, Yonghong Wang, Biwu Chu, Qingxin Ma, Jiannong Quan, Yujing Mu, Hong He","doi":"10.1021/acs.est.4c09004","DOIUrl":"https://doi.org/10.1021/acs.est.4c09004","url":null,"abstract":"Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) plays a key role in atmospheric chemistry, but knowledge of its variation, sources, and impact on sulfate formation remains incomplete, especially in the urban boundary layer aloft. Here, we conducted a field campaign with measurements of H<sub>2</sub>O<sub>2</sub> and related species at a tower-based site (∼528 m above the ground surface) of Beijing in spring of 2022. The observed hourly H<sub>2</sub>O<sub>2</sub> concentration reached up to 21.2 ppbv with an average value of 3.4 ± 3.7 ppbv during the entire observation period, which was higher than values from previous observations throughout the world. The H<sub>2</sub>O<sub>2</sub> budget revealed that the two known sources (self-reaction of HO<sub>2</sub> radicals and ozonolysis of alkenes) could not account for the significant formation of H<sub>2</sub>O<sub>2</sub>, leading to a considerable unknown source strength (∼0.14–0.53 ppbv h<sup>–1</sup>) of H<sub>2</sub>O<sub>2</sub> at noon and after sunset. Based on the levoglucosan signal, distribution of fire points, and backward trajectories, biomass burning emissions from the southwest of Beijing (e.g., North China Plain) were found to contribute greatly to H<sub>2</sub>O<sub>2</sub> formation. Besides, photochemical aging of PM<sub>2.5</sub> might also have a potential impact on H<sub>2</sub>O<sub>2</sub> production at noon. The unexpectedly high concentrations of H<sub>2</sub>O<sub>2</sub> aloft made a vital contribution to sulfate production (0.2–1.1 μg m<sup>–3</sup> h<sup>–1</sup>), which could be transported to the ground surface during the turbulent mixing. Our findings provide an improved understanding of the H<sub>2</sub>O<sub>2</sub> chemistry in the boundary layer aloft in a megacity, as well as its impact on sulfate formation.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"12 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143076961","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}
引用次数: 0
Global Atmospheric Composition Effects from Marine Isoprene Emissions
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2025-02-02 DOI: 10.1021/acs.est.4c10657
Wentai Zhang, James Weber, Alex T. Archibald, Nathan Luke Abraham, Dennis Booge, Mingxi Yang, Dasa Gu
{"title":"Global Atmospheric Composition Effects from Marine Isoprene Emissions","authors":"Wentai Zhang, James Weber, Alex T. Archibald, Nathan Luke Abraham, Dennis Booge, Mingxi Yang, Dasa Gu","doi":"10.1021/acs.est.4c10657","DOIUrl":"https://doi.org/10.1021/acs.est.4c10657","url":null,"abstract":"Isoprene emissions, primarily of biogenic origin, play an important role in atmospheric chemistry and climate. However, the atmospheric implications of marine isoprene emissions remain underexplored due to sparse in situ measurements and the intricate mechanisms governing isoprene in the upper ocean. This study uses 20 years of MODIS satellite observations to upscale isoprene production and loss rates derived from laboratory experiments, enabling global modeling of aqueous isoprene concentrations and emissions. Earth system model simulations with integrated marine isoprene emissions demonstrate substantial alterations in atmospheric composition over global oceanic regions. Our investigation uncovers diurnal variations in the vertical profiles of atmospheric isoprene, indicating that surface isoprene can ascend to the mid-to-upper troposphere, where nitrogen monoxide (NO) influences isoprene epoxydiol (IEPOX) production differently over selected oceanic and terrestrial regions. These findings pave the way for future studies on the role of marine isoprene in climate models and advance our understanding of its broader implications for atmospheric chemistry under a changing climate.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"22 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143076962","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}
引用次数: 0
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