Science of the Total Environment最新文献

{"title":"Mechanistic insights into adsorption-desorption of PFOA on biochars: Effects of biomass feedstock and pyrolysis temperature, and implication of desorption hysteresis.","authors":"Tongshuai Wang, Jingqi Wu, Tao Hu, Congcong Wang, Shijia Li, Zhixiong Li, Jiawei Chen","doi":"10.1016/j.scitotenv.2024.177668","DOIUrl":"10.1016/j.scitotenv.2024.177668","url":null,"abstract":"<p><p>Adsorptive removal of the emerging organic pollutant perfluorooctanoic acid (PFOA) from contaminated water using biochar is a promising cost-effective approach. To determine the stability of PFOA adsorption on biochar, the thermodynamic analysis of the adsorption-desorption behavior is essential. This study comprehensively investigated the adsorption and desorption of PFOA on biochars derived from maple sawdust, peanut shells and corn stalks, pyrolyzed at peak temperatures of 400, 600 and 800 °C. The findings indicated that the micropore volume of the biochars was key to PFOA adsorption, with peanut shell biochar produced at 800 °C showing the highest adsorption capacity of 16.75 mg/g, attributed to its larger micropore volume (0.22 m³/g). Thermodynamic analysis showed that the negative values of ∆G⁰ of PFOA adsorption ranged from -2.24 to -5.38 kJ/mol, confirmed that the process was spontaneous and involved physical pore-filling. However, the close similarity between the adsorption and desorption isotherms, coupled with a low hysteresis coefficient, clarified that the PFOA adsorption was unstable and prone to desorption. The thermodynamic insights from this study highlighted that lignin-rich biochar produced at high temperature with high micropore content was very favorable for the effective adsorptive removal of PFOA, while the long-term adsorption stability should not be overlooked in the remediation applications.</p>","PeriodicalId":422,"journal":{"name":"Science of the Total Environment","volume":" ","pages":"177668"},"PeriodicalIF":8.2,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685615","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}

{"title":"Polycyclic aromatics-derived benzene carboxylic acids (BPCAs) as a fast predictor of the genotoxicity of combustion particles.","authors":"Chuxin Yao, Jiao Tang, Yangzhi Mo, Guangcai Zhong, Xiaofei Geng, Xin Yi, Qianyu Zhang, Jun Li, Huimin Ma, Shizhen Zhao, Gan Zhang","doi":"10.1016/j.scitotenv.2024.177632","DOIUrl":"10.1016/j.scitotenv.2024.177632","url":null,"abstract":"<p><p>Polycyclic aromatic compounds (PAC) are common toxics in combustion particles. Numerous studies on health effects of PAC mixtures focused on limited compounds. It's still challenging to quantify complex PAC mixtures in combustion particles. Recently, benzene polycarboxylic acids (BPCAs) method, which involves conversion of PAC mixtures into a few BPCAs, has been used to quantify complex PAC mixtures in particles. In this study, in vitro biossays were used to evaluate the toxicity of extractable organic matter (EOM) in combustion particles. Analysis with Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) identified ~1000 molecules, mostly aromatics (84.47 ± 5.32 %), that positively associate with the EOM toxicity (p < 0.05). We further employed BPCAs method to quantify PAC mixtures in the EOM of combustion particles, and observed the toxicity (especially genotoxicity) of EOM linearly increases with the abundance of PAC mixtures (r²: 0.68-0.89, p < 0.05), as it is shown by a data set referring to all source types including biomass burning, coal combustion and vehicle exhaust. The genotoxicity of PAC mixtures in EOM of combustion particles was estimated to be 10-13 times that of benzo[a]pyrene at the same mass concentration. Target analysis of 48 PAC was carried out, but a weaker relationship is found for the toxicity of EOM and the abundance of 48 PAC. Taken together, we suggest PAC-derived BPCAs as a fast predictor of the genotoxicity of combustion particles, which could be promising in routine monitoring of PAC pollution in the air.</p>","PeriodicalId":422,"journal":{"name":"Science of the Total Environment","volume":" ","pages":"177632"},"PeriodicalIF":8.2,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685621","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}

{"title":"Mobilization of grassland soil arsenic stores due to agronomic management.","authors":"Wanqi Jia, Coalain McCreanor, Manus Carey, Jonathan Holland, Caroline Meharg, Andrew A Meharg","doi":"10.1016/j.scitotenv.2024.177702","DOIUrl":"10.1016/j.scitotenv.2024.177702","url":null,"abstract":"<p><p>The fate of arsenic in mineral soil stores over time is poorly understood. Here we examined arsenic loss over five decades from a managed grassland soil profile through analysing archived material from a long-term slurry (LTS) experiment at Hillsborough, Northern Ireland. A randomized block experiment was established in 1970 where a perennial ryegrass sward was seeded onto the site and subjected to control (no fertilization) and fertilization treatments using conventional (i.e. at farmers recommended application rate) mineral NPK fertilizer, and pig and cow slurry treatments. Soil (0-5, 5-10 and 10-15 cm), slurry applied, and sward off-take was archived each year. A mass-balance calculation found that control soils lost no arsenic down the 15 cm depth soil profile, the NPK treatment had a 10 % loss, while cow slurry caused 25 % loss, and a 35 % loss was observed for pig slurry. For treatments with arsenic loss, removal was linear over the 50 years of study in 2 out of the 3 blocks, with the 3rd block showing little or no change. Principal Component Analysis (PCA) found that arsenic was most positively associated with soil magnesium, manganese and nickel, while negatively associated with pH, organic carbon, phosphorus and silicon. Laser ablation - inductively coupled plasma - mass spectrometry (LA-ICP-MS) of soil found that arsenic association with lead mineralogy could potentially explain why there was a gradient in arsenic loss across the experimental plots. Slurry and atmospheric inputs, and sward off-take had little impact on the soil arsenic mass-balance. The findings suggest that leaching loss down the soil profile was the mechanism of loss of arsenic. The applicability of the LTS experimental site arsenic findings to other soils is discussed, as is the implication for the global biogeochemical cycling of those soils.</p>","PeriodicalId":422,"journal":{"name":"Science of the Total Environment","volume":" ","pages":"177702"},"PeriodicalIF":8.2,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142692428","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}

{"title":"Methane degassing in global river reservoirs and its impacts on carbon budgets and sustainable water management.","authors":"Yanlai Zhou, Hanbing Xu, Tianyu Xia, Lihua Xiong, Li-Chiu Chang, Fi-John Chang, Chong-Yu Xu","doi":"10.1016/j.scitotenv.2024.177623","DOIUrl":"10.1016/j.scitotenv.2024.177623","url":null,"abstract":"<p><p>Degassing methane (CH₄) through reservoir water compromises hydroelectricity's presumed low-carbon status, which has emerged as a critical hotspot for global carbon dynamics. However, a comprehensive understanding of the involved pathways remains elusive, hindering the accurate estimation of global reservoirs' carbon budget (emission-to-burial ratio). This study presents a holistic upscaling approach to assess methane degassing in global river reservoirs and its impacts on carbon budgets. Firstly, a machine learning model is utilized to characterize the contributions of climate and human factors to annual water residence time. Secondly, the stepwise multiple linear regression method is used to calculate CH₄ degassing emissions for each reservoir. Finally, to systematically tackle all sources of uncertainty, separate uncertainty analyses are implemented for the estimates of degassing emissions, areal emissions, and organic carbon burial. Analyzing 30-year data from 6695 reservoirs worldwide, our assessment considers water residence time, temperature, catchment area, and reservoir size. Findings indicate that water releases contribute significantly to global CO₂ emissions from reservoirs, elevating the carbon budget by 20 % from 2.02 to 2.18 TgC/year, underscoring the previously underestimated significance of CH₄ degassing in shaping the carbon cycle impact of river reservoirs. We propose a redefined threshold for low carbon credits, suggesting that reservoirs with power densities exceeding 6.1 MW/km², instead of the conventional 4 MW/km², should qualify. This study underscores the need for sustainable water management and reshaping the carbon dynamics associated with hydroelectricity. Future research can advocate Artificial Intelligence (AI) techniques to enhance water management and mitigate carbon emissions by multi-objectively optimizing reservoir operations.</p>","PeriodicalId":422,"journal":{"name":"Science of the Total Environment","volume":" ","pages":"177623"},"PeriodicalIF":8.2,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694999","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}

{"title":"Applications of geographically weighted machine learning models for predicting soil heavy metal concentrations across mining sites.","authors":"Hyemin Jeong, Younghun Lee, Byeongwon Lee, Euisoo Jung, Jai-Young Lee, Sangchul Lee","doi":"10.1016/j.scitotenv.2024.177667","DOIUrl":"10.1016/j.scitotenv.2024.177667","url":null,"abstract":"<p><p>The accurate prediction of soil heavy metal contamination is crucial for the effective environmental management of abandoned mining areas. However, conventional machine learning models (CMLMs) often fail to account for the spatial heterogeneity of soil contamination, which limits their predictive accuracy. This study evaluated the performance of geographically weighted machine learning models (GWMLMs) in predicting soil Cd and Pb concentrations in abandoned mines in the Republic of Korea. We compared two GWMLMs (Geographically Weighted Random Forest and Geographically Weighted Extreme Gradient Boosting) with four CMLMs (Random Forest, Gradient Boosting, Light Gradient Boosting, and extreme Gradient Boosting). The data used in this study included soil samples from six abandoned mining sites with various geographical and soil input variables. The results showed that the GWMLMs consistently outperformed the CMLMs in predicting heavy metal contamination. For Cd predictions, GWMLMs exhibited on average 0.02 lower root mean square error and mean absolute error values, with a 0.26 increase in R² values compared to CMLMs. Similarly, for Pb predictions, the GWMLMs showed 0.18 and 0.13 lower root mean square error and mean absolute error values, respectively, and a 0.17 increase in R² relative to the CMLMs. The findings demonstrate the usefulness of GWMLMs for predicting the spatial distribution of soil heavy metals. SHapley Additive exPlanations analysis exhibited elevation and distance from abandoned mining sites as the most influential factors in predicting both Cd and Pb concentrations. This study highlights the value of GWMLMs that incorporate spatial heterogeneity into CMLMs for enhancing prediction accuracy and providing crucial insights for environmental management in mining-impacted regions.</p>","PeriodicalId":422,"journal":{"name":"Science of the Total Environment","volume":" ","pages":"177667"},"PeriodicalIF":8.2,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142695056","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}

{"title":"The denitrification ability and nitrogen metabolism pathway of aerobic denitrifier Marinobacter alkaliphilus SBY-1 under low C/N ratios.","authors":"Chao Pan, Yang-Guo Zhao, Progress Mupindu, Shuxue Zhao","doi":"10.1016/j.scitotenv.2024.177651","DOIUrl":"10.1016/j.scitotenv.2024.177651","url":null,"abstract":"<p><p>Mariculture tail water is characterized as the low C/N ratios and thus blocks the conventional heterotrophic denitrification process due to insufficient carbon source. Therefore, oligotrophic marine bacteria with heterotrophic nitrification and aerobic denitrification (HN-AD) are urgently required to bioaugment aerobic biological filter. In this study, Marinobacter alkaliphilus SBY-1 was isolated and confirmed optimal nitrate removal capacity at a rate of 716 mg/L·d without ammonia production or nitrite accumulation under initial nitrate concentration of 800 mg/L, pH 7, salinity 20 ‰, sodium acetate as the carbon source, and low C/N ratios of 3.6. SBY-1 also demonstrated heterotrophic nitrification capability with a maximum ammonia removal rate reaching 69.21 % when ammonia was used as the nitrogen source. The enzymes involved in the HN-AD process including ammonia monooxygenase (AMO), nitrate reductase (NR), and nitrite reductase (NIR) were all detected in SBY-1 with superior activity observed for NR and NIR. Additionally, analysis of EPS and auto-aggregation revealed that SBY-1 exhibited excellent auto-aggregation ability under high influent nitrogen concentration conditions, making it more suitable for biofilm formation and further application in biofilm-based denitrification process. Genome analysis identified genes associated with Nar, Nap, Nas, Nir, Nif, Nrt, Nrf, Nor, Nos which confirmed that SBY-1 possessed a complete HN-AD pathway for nitrogen metabolism. The predicted nitrogen metabolism pathway of SBY-1 was NO₃^--N → NO₂^--N → NO→N₂O → N₂. These findings provide new insights into the efficient removal of nitrate by SBY-1 under lower C/N conditions.</p>","PeriodicalId":422,"journal":{"name":"Science of the Total Environment","volume":" ","pages":"177651"},"PeriodicalIF":8.2,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142695173","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}

{"title":"Improving fecal bacteria estimation using machine learning and explainable AI in four major rivers, South Korea.","authors":"SungMin Suh, JunGi Moon, Sangjin Jung, JongCheol Pyo","doi":"10.1016/j.scitotenv.2024.177459","DOIUrl":"10.1016/j.scitotenv.2024.177459","url":null,"abstract":"<p><p>This study addresses the critical public health issue of fecal coliform contamination in the four major rivers in South Korea (Han, Nakdong, Geum, and Yeongsan rivers) by applying advanced machine learning (ML) algorithms combined with Explainable Artificial Intelligence to enhance both prediction accuracy and interpretability. Both traditional and machine learning models often face challenges in accurately estimating fecal coliform levels due to the complexity of environmental variables and data limitations. To address this limitation, we employed two tree-based models (i.e., random forest [RF] and extreme gradient boost [XGBoost]), and two neural network models (i.e., deep neural network and convolutional neural network [CNN]). we employed the use of Shapley Additive Explanations (SHAP) to facilitate a more comprehensive understanding of the influence exerted by each variable on the model's predictions. Based on a comprehensive dataset collected from the National Institute of Environmental Research covering 16 water quality parameters and meteorological data from 2014 to 2022, our study improved the accuracy of fecal coliform estimation using XGBoost and CNN models. The optimal result was obtained using XGBoost, which had a validation Nash-Sutcliffe efficiency of 0.597 in the Han River. In addition, this study provides insights into the significant factors influencing fecal coliform concentrations across different river environments using the SHAP model. The results indicated that the XGBoost model provided superior estimation accuracy and explanations for the contributions of variables. The SHAP results provided the precise contribution of each water quality variable that affected the fecal estimation results using the XGBoost model. The study facilitates an improved understanding of the relationship between water quality variables and fecal coliform contamination mechanisms in the four major rivers in South Korea.</p>","PeriodicalId":422,"journal":{"name":"Science of the Total Environment","volume":" ","pages":"177459"},"PeriodicalIF":8.2,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142611264","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}

{"title":"The Keap1-Nrf2/ARE signaling pathway regulates redox balance and apoptosis in the small yellow croaker (Larimichthys polyactis) under hypoxic stress.","authors":"Jingqian Wang, Li Wang, Yang Liu, Congcong Hou, Qingping Xie, Daojun Tang, Feng Liu, Bao Lou, Junquan Zhu","doi":"10.1016/j.scitotenv.2024.177396","DOIUrl":"10.1016/j.scitotenv.2024.177396","url":null,"abstract":"<p><p>Hypoxic stress can result in redox imbalance and apoptosis in teleostean fishes; however, the precise molecular mechanisms underlying this process, including its regulation by the key signaling pathway Kelch-like ECH-associated protein 1 (Keap1)-nuclear factor erythroid 2 related factor (Nrf2)/antioxidant response element (ARE), remain elusive. Therefore, in this study, we chose the Keap1-Nrf2/ARE signaling pathway as the entry point and a combination of in vivo (target organ liver) and in vitro (small yellow croaker fry [SYCF] cell line) experiments to investigate the molecular mechanism by which Larimichthys polyactis (L. polyactis) adapts to hypoxic stress by regulating redox balance and apoptosis. As our previous study found that hypoxic stress could lead to redox imbalance and apoptosis in L. polyactis. First, we observed significant alterations in the expression of key genes Lpkeap1, Lpnrf2, Lpho-1, and Lpnqo1 within the Keap1-Nrf2/ARE signaling pathway in both liver tissue and SYCF cells of L. polyactis under hypoxic stress, indicating activation of this pathway in response to hypoxia. Subsequently, we elucidated the mechanism by which hypoxia activates this pathway, that is, hypoxia weakened the interaction between LpNrf2 and LpKeap1, promoting the nuclear translocation of LpNrf2 and enhancing its binding activity to ARE, thereby activating the transcription of target genes. Furthermore, we found that significant changes occurred in the redox balance and apoptosis-related indicators after LpNrf2 knockdown and exposure to hypoxic stress for 24 h in SYCF cells, indicating that this pathway can regulate redox balance and apoptosis regulation under hypoxic stress in L. polyactis. Additionally, we used DNA affinity purification sequencing (DAP-seq) to identify the ARE sequence (ATGATTTAGC) that bound to LpNrf2 and its target genes. Finally, we conducted a combined analysis of DAP-seq and RNA-seq to identify six key target genes involved in the process: haeme oxygenase-1 (Ho-1), B-cell lymphoma-2 (Bcl2), pituitary homeobox 2 isoform X1 (Pitx2), aquaporin-4 isoform X1 (Aqp4), stress-induced phosphoprotein 1-like isoform X1 (Stip1), and guanine nucleotide-binding protein G (i) subunit alpha-2-like (Gnai2). In summary, hypoxic stress induced by weakening LpNrf2 and LpKeap1 interaction promoted LpNrf2 nuclear entry and enhanced its binding activity to ARE, thereby activating the transcription of multiple target genes to regulate redox balance and apoptosis. The research results not only help deepen our understanding of the adaptive mechanisms of L. polyactis and even marine fish to hypoxic stress and its survival strategies but also provide new ideas and potential targets for breeding new hypoxia-tolerant strains.</p>","PeriodicalId":422,"journal":{"name":"Science of the Total Environment","volume":" ","pages":"177396"},"PeriodicalIF":8.2,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142611441","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}

{"title":"Toxicological effects of bisphenol F on growth, antioxidant response, ultrastructure, and microbial properties of the submerged macrophyte Ceratophyllum demersum L.","authors":"Gui Yu, Jie Wang, Hongkuan Cheng, Xingzhang Luo, Shoubing Wang, Zheng Zheng","doi":"10.1016/j.scitotenv.2024.177481","DOIUrl":"10.1016/j.scitotenv.2024.177481","url":null,"abstract":"<p><p>Alternative chemicals to bisphenol A (BPA), such as bisphenol F (BPF), have been detected in aquatic environments worldwide and can potentially exert negative effects on aquatic organisms. To evaluate the toxic effects of the exposure of BPF on submerged macrophytes and biofilms, Ceratophyllum demersum L. (C. demersum) was exposed to different concentrations of BPF (1, 5, 10, and 20 mg L^-1). In general, the growth of C. demersum was inhibited, and the chlorophyll content of C. demersum noticeably decreased at high concentrations of BPF (20 mg L^-1). In addition, different concentrations of exposure to BPF induced a certain degree of oxidative stress, as evidenced by increased the activities of superoxide dismutase, catalase, and peroxidase, as well as increased malondialdehyde concentrations. Furthermore, the scanning electron microscopy results and high-throughput sequencing analysis showed the diversity and structure of the microbial community were altered on the leaf biofilms in the presence of BPF. In addition, the leaf cells of C. demersum showed some damage and variation of organelles and membranes when examined by transmission electron microscopy. The current study is the first to assess the effects of BPF on the physiological and biochemical of C. demersum, these results suggest the understanding of how submerged macrophyte and leaf biofilms respond to environmental stress induced by BPF.</p>","PeriodicalId":422,"journal":{"name":"Science of the Total Environment","volume":" ","pages":"177481"},"PeriodicalIF":8.2,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142611468","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}

{"title":"Variations of chloride depletion and its impacts on ozone formation: Case study of a coastal area in Shanghai.","authors":"Yusen Duan, Yan Liu, Kun Zhang, Li Li, Juntao Huo, Jia Chen, Qingyan Fu, Zongjiang Gao, Guangli Xiu, Tingting Hu","doi":"10.1016/j.scitotenv.2024.176899","DOIUrl":"10.1016/j.scitotenv.2024.176899","url":null,"abstract":"<p><p>Chlorine plays a critical role in atmospheric chemistry. Marine chloride depletion, as a significant source of atmospheric chlorine, impacts coastal acid deposition, atmospheric oxidizing capacity, and global climate. Based on continuous monitoring data of PM_2.5 water soluble ions, criteria pollutants, and meteorological data at Chongming Dongtan supersite from 2019 to 2022, variations in chloride depletion and related impact factors were analyzed. Using trajectory analysis via Concentration Weighted Trajectory (CWT) method, the main source regions contributing to chloride depletion were identified. The influence of meteorological conditions on chloride depletion was examined, and the contribution of typical chloride depletion processes to ozone was analyzed using the community atmospheric chemistry box model Chemistry As A Box model Application/Module Efficiently Calculating the Chemistry of the Atmosphere (CAABA/MECCA). Results show that chloride depletion increases in summer and decreases in winter. Chloride depletion reaches to peak around noon and gradually decreases after 6 p.m. CWT analysis reveals that airflows predominantly originate from ocean during periods of chloride depletion. As a large coastal port, shipping NO_x emissions produce abundant N₂O₅ through oxidation processes. The liquid-phase reactions of N₂O₅ with sea-salt aerosol via liquid-phase reactions result in chloride depletion. Chlorine depletion follows the same trend as O₃ and temperature, while showing an inverse trend with NO₂, N₂O₅, NO₃, and pH. Modelling results indicate that oceanic chlorine depletion contributes approximately 8 ppb, 0.1 ppt, and 18 ppt to the enhancement of O₃, OH, and HO₂ concentrations. Therefore, attention should be paid to the contribution of ship emissions through chloride depletion mechanisms to O₃ pollution in coastal port cities. Chloride depletion serves as a typical indicator of the impact of chloride circulation on coastal ozone.</p>","PeriodicalId":422,"journal":{"name":"Science of the Total Environment","volume":" ","pages":"176899"},"PeriodicalIF":8.2,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142611484","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}