{"title":"Submarine Groundwater Discharge Acts as a Significant Vector for Coastal Organophosphate Esters: Joint Evidence from Pollution Surveys and Radionuclide Analysis","authors":"Li Zhang,Xiang Li,Xinhui He,Xuemin Feng,Bochao Xu,Shuo Yu,Luqi Zhang,Lu Lu,Qinglong Liang,Kaiyuan Guo,Zhenming Zheng","doi":"10.1021/acs.est.6c11341","DOIUrl":"https://doi.org/10.1021/acs.est.6c11341","url":null,"abstract":"Organophosphate esters (OPEs) are ubiquitous marine contaminants that raise global concern. While surface inputs are well-studied, the role of subsurface transport remains poorly constrained. Submarine groundwater discharge (SGD) drives seawater-groundwater interactions, yet its impact on OPEs behavior remains overlooked. This study comprehensively investigates the distribution, transport property and sources of OPEs from coastal groundwater to seawater in the Beibu Gulf, China. No statistically significant difference in Σ19OPEs levels was found between groundwater and tidal flat porewater, while both matrices exhibited significantly higher levels than seawater. The high compositional similarity, strong correlations (p < 0.01) and PCA overlap of OPEs in different waters, as well as their shared source profiles indicated the transport potential of OPEs from groundwater to seawater. Multiple statistical modeling integrating OPEs, environmental factors and DOM components reveals the land-to-sea transport pathways and biogeochemical processes of OPEs via SGD. Furthermore, radon isotope analysis verified the presence of SGD, offering evidence for SGD-mediated OPE transport. For the first time, this work integrates pollutant investigation, multiple statistical analysis, and radionuclide tracing, to identify SGD as a previously underestimated vector of coastal OPEs and elucidates its potential transport mechanisms, providing crucial support for integrated land-sea management and risk assessment.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"231 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210885","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}
环境科学与技术Pub Date : 2026-10-19DOI: 10.1021/acs.est.6c04712
Christopher J. Howick
{"title":"Correspondence on “Legacy and Emerging Plasticizers and Stabilizers in PVC Floorings and Implications for Recycling”","authors":"Christopher J. Howick","doi":"10.1021/acs.est.6c04712","DOIUrl":"https://doi.org/10.1021/acs.est.6c04712","url":null,"abstract":"","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"62 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221660","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":"Aqueous Carbonyl-Amino Aggregation Drives Atmospheric Nitrogen-Containing Oligomer Formation in China Haze","authors":"Binyu Xiao,Chenlong Liang,Gehui Wang,Rongjie Li,Luyao Chen,Zheng Li,Haoyang Wang,Can Wu,Jingjing Meng,Yunfei Wu,Renjian Zhang","doi":"10.1021/acs.est.6c09940","DOIUrl":"https://doi.org/10.1021/acs.est.6c09940","url":null,"abstract":"Nitrogen-containing organic compounds (NOCs) are ubiquitous in the troposphere and contribute to the reactive nitrogen cycle and aerosol light absorption, yet their formation mechanisms remain unclear, especially in polluted regions. Here, we characterized NOCs in PM2.5 during winter haze in the North China Plain (NCP), with a comparison to those in the Sichuan Basin (ScB). Reduced-nitrogen NOCs (Re-NOCs) accounted for 40% of organics detected in the ESI+ mode, highlighting their importance within atmospheric NOCs. Compared to dry haze (DH) in NCP, high-molecular-weight (HMW, m/z > 250) Re-NOCs in humid haze (HH) were enhanced, which positively correlated with NH+4 and the mass ratio of aqueous-phase secondary organic aerosols to total water-soluble organic aerosols, along with increases in aliphatic chain length and molecular unsaturation, indicating carbonyl-amino-driven oligomerization and cyclization. Aliphatic Re-NOCs dominated the Re-NOCs during HH, together with strong correlations of a typical NOC oligomer (C8H13N3O2) with water-soluble organic nitrogen and HMW Re-NOCs, further suggesting oligomerization as a key formation pathway for NOCs. We found that stronger aerosol acidity and higher temperature favored oligomerization of Re-NOCs compared to cyclization, resulting in enhanced C8H13N3O2 in ScB relative to that in NCP. Our work revealed oligomerization as a critical mechanism shaping the NOC composition, particularly HMW species.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"55 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210883","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}
环境科学与技术Pub Date : 2026-10-19DOI: 10.1021/acs.est.6c13970
Ruifeng Zhang,Yong Jie Li,Chak K. Chan
{"title":"Photochemical Interactions of Nitrate Photolysis and Photosensitization of BBOA: Enhanced HONO Production and the Formation of Nitrophenols","authors":"Ruifeng Zhang,Yong Jie Li,Chak K. Chan","doi":"10.1021/acs.est.6c13970","DOIUrl":"https://doi.org/10.1021/acs.est.6c13970","url":null,"abstract":"Renoxification of nitrate to reactive nitrogen species (RNS) can sustain atmospheric oxidant production. Because nitrate and light-absorbing brown carbon can coexist in biomass burning (BB) plumes, their photochemical interaction may alter RNS cycling. Furthermore, nitration of phenols in biomass burning organic aerosol (BBOA) can form nitrophenols, potentially increasing the warming effect of aged BBOA. Yet the mechanisms of renoxification and nitration in irradiated nitrate-BBOA mixtures remain poorly understood. We experimentally investigate these coupled processes over a wide range of fir-wood BBOA concentrations during aqueous nitrate photolysis (10 mM) under acidic conditions using H2SO4. At low BBOA concentration (TOCBBOA/NO3– ≤ 0.0036 mg L–1/mg L–1), the steady-state production rate of HONO (Pss_HONO) increased as BBOA concentration increased, reaching a maximum enhancement factor of 1.8 driven primarily by triplet-mediated photosensitized reduction of NO2 to HONO. At higher BBOA concentration (TOCBBOA/NO3– > 0.0036 mg L–1/mg L–1), Pss_HONO progressively decreased and was nearly fully suppressed at TOCBBOA/NO3– = 0.7 mg L–1/mg L–1. This inhibition is attributed to reactions of aqueous HNO2/NO2 with phenols, accompanied by formation of nitrophenols. These findings point to a potentially overlooked daytime HONO source and an atmospheric source of nitrophenols, a key class of BrC chromophores, via photochemical interactions between nitrate photolysis and photosensitization of BBOA.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"1 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210889","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}
环境科学与技术Pub Date : 2026-10-19DOI: 10.1021/acs.est.6c12069
Xinkai Wang,Yiyi Li,Qifan Liu,Yongcheng Li,Li Li,Ling Ruan,Wei Liu,Yufeng Gong,Yuhe He
{"title":"OH-Initiated Heterogeneous Reactions of Novel Organophosphate Esters: Insights into Oxidation Chemistry and Atmospheric Persistence","authors":"Xinkai Wang,Yiyi Li,Qifan Liu,Yongcheng Li,Li Li,Ling Ruan,Wei Liu,Yufeng Gong,Yuhe He","doi":"10.1021/acs.est.6c12069","DOIUrl":"https://doi.org/10.1021/acs.est.6c12069","url":null,"abstract":"Novel organophosphate esters (OPEs), formed through chemical transformation of commercial antioxidants, are emerging contaminants with widespread environmental occurrence and potential health effects. Despite their widespread detection, the atmospheric reactivity, persistence, and transformation of novel OPEs remain unknown. Here, the heterogeneous OH oxidation of two surface-bound novel OPEs [tris(2,4-ditert-butylphenyl) phosphate (TDtBPP) and triisodecyl phosphate (TiDeP)] was explored by investigating the reaction kinetics and chemical mechanisms. The measured heterogeneous rate constants for TDtBPP and TiDeP were (2.81 ± 0.12) × 10–12 and (1.99 ± 0.16) × 10–12 cm3 molecules–1 s–1, respectively, equivalent to atmospheric lifetimes of up to 6.3 and 9.0 days. These lifetimes are significantly longer than previously predicted values (<1 day), suggesting that they are much more persistent in air than predicted. Based on UPLC-HRMS measurements, 22 transformation products from the heterogeneous reactions were identified for the first time. Analysis of atmospheric particle samples from two megacities in China identified four TDtBPP transformation products, demonstrating that the oxidation chemistry can occur under genuine environmental conditions. In-silico hazard screening further indicated that many transformation products may be more bioaccumulative and more toxic than the parent novel OPEs. The results not only provide new insights into the atmospheric persistence of novel OPEs but also underscore the significance of considering atmospheric transformation in the risk assessment of these emerging contaminants.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"12 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221661","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}
环境科学与技术Pub Date : 2026-10-18DOI: 10.1021/acs.est.6c07700
David Haaf,Michael McGlade,Athena A. Nghiem,Duyen Thi Vu,Tobias Steinert,Viet Hung Pham,Linh Khanh Bui,Thanh Ngoc Tong,Duong Du Bui,Andrea Stenke,Michael Berg,Lenny H. E. Winkel
{"title":"Modeled\u0000Groundwater Decline is Associated with Lower\u0000Arsenic Concentrations in Hanoi","authors":"David Haaf,Michael McGlade,Athena A. Nghiem,Duyen Thi Vu,Tobias Steinert,Viet Hung Pham,Linh Khanh Bui,Thanh Ngoc Tong,Duong Du Bui,Andrea Stenke,Michael Berg,Lenny H. E. Winkel","doi":"10.1021/acs.est.6c07700","DOIUrl":"https://doi.org/10.1021/acs.est.6c07700","url":null,"abstract":"Abstract Elevated arsenic concentrations in groundwater pose health risks. Geogenic arsenic contamination is driven by biogeochemical mobilization and groundwater dynamics. Intensive pumping can initially exacerbate contamination by drawing arsenic or mobilizing organic matter into aquifers, but over longer time scales may also promote dilution and flushing in some settings. To better understand the mechanisms controlling arsenic concentrations, we examined changes over two decades in Hanoi (Vietnam), a hotspot of geogenic arsenic contamination and groundwater pumping. Arsenic concentrations from 470 wells sampled in the year 2000 were compared with 434 wells sampled in the same area in 2013 and 2023. Median concentrations declined from 14 to 8 μg/L between 2000 and 2023, while mean concentrations and the proportion of high-arsenic wells (&gt;100 μg/L) remained similar. Using hydrochemical and groundwater-level data, CatBoost models combined with SHAP analysis assessed changes in predictor importance. In 2000, arsenic was more strongly associated with redox predictors, whereas groundwater-level predictors became more important in 2023. Within wells used to evaluate groundwater-level change (n = 251), larger decadal declines were associated with lower arsenic concentrations (median = 31 μg/L) than wells without declines (median = 120 μg/L). We hypothesize a decadal mechanism shift, from redox to hydrological controls, particularly driving arsenic declines.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"37 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209895","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}