Environmental Science: Processes & Impacts最新文献

{"title":"Kinetic multilayer models for surface chemistry in indoor environments.","authors":"Pascale S J Lakey, Manabu Shiraiwa","doi":"10.1039/d4em00549j","DOIUrl":"https://doi.org/10.1039/d4em00549j","url":null,"abstract":"<p><p>Multiphase interactions and chemical reactions at indoor surfaces are of particular importance due to their impact on air quality in indoor environments with high surface to volume ratios. Kinetic multilayer models are a powerful tool to simulate various gas-surface interactions including partitioning, diffusion and multiphase chemistry of indoor compounds by treating mass transport and chemical reactions in a number of model layers in the gas and condensed phases with a flux-based approach. We have developed a series of kinetic multilayer models that have been applied to describe multiphase chemistry and interactions indoors. They include the K2-SURF model treating the reversible adsorption of volatile organic compounds on surfaces, the KM-BL model treating diffusion through an indoor surface boundary layer, the KM-FILM model treating organic film formation by multi-layer adsorption and film growth by absorption of indoor compounds, and the KM-SUB-Skin-Clothing model treating reactions of ozone with skin lipids in skin and clothing. We also developed the effective mass accommodation coefficient that can treat surface partitioning by effectively taking into account kinetic limitations of bulk diffusion. In this study we provide detailed instructions and code annotations of these models for the model user. Example sensitivity simulations that investigate the impact of input parameters are presented to help with familiarization to the codes. The user can adapt the codes as required to model experimental and indoor field campaign measurements, can use the codes to gain insights into important reactions and processes, and can extrapolate to new conditions that may not be accessible by measurements.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" ","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142612992","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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":"Kinetics of hypochlorous acid reactions with organic and chloride-containing tropospheric aerosol†","authors":"Spiro D. Jorga, Tengyu Liu, Yutong Wang, Sumaiya Hassan, Han Huynh and Jonathan P. D. Abbatt","doi":"10.1039/D3EM00292F","DOIUrl":"10.1039/D3EM00292F","url":null,"abstract":"<p >Chlorine plays an important role in tropospheric oxidation processes, in both marine and continental environments. Although modeling studies have explored the importance of halogen chemistry, uncertainty remains in associated chemical mechanisms and fundamental kinetics parameters. Prior kinetics measurements of multiphase halogen recycling reactions have been largely performed with dilute, bulk solutions, leaving unexplored more realistic chemical systems which have high solute concentrations and are internally mixed with both halide and organic components. Here, we address the multiphase kinetics of gaseous HOCl using an aerosol flow tube and aerosol mass spectrometer to study its reactions with particulate chloride, using atmospherically relevant particle acidity, solute concentrations, and ionic strength. We also investigate the chemistry that results when biomass burning (BB) aerosol components and chloride are internally mixed. Using pH-buffered deliquesced particles, we show that the rate constant for reaction of dissolved HOCl with H<small>⁺</small> and Cl<small>⁻</small> at high relative humidity (RH) (80–85%) is within a factor of two of the literature value for bulk phase conditions. However, at lower RH values (60–70%) where the particles are considerably more concentrated, the rate constant for chloride loss from the particles is an order of magnitude higher. For pure organic compounds commonly found in biomass burning (BB) aerosol, such as coniferaldehyde, salicylic acid and furfural, an increase in the aerosol chlorine content occurs with HOCl exposure, indicating the formation of organochlorine species. Together, these independent findings explain results for internally mixed aerosol particles with both chloride and BB components present where we observed behavior consistent with both chloride loss and organochlorine formation occurring simultaneously upon HOCl exposure. Our results indicate that chlorine recycling <em>via</em> HOCl uptake by chloride-containing particles will occur in the atmosphere efficiently over a wide range of RH conditions, even when reactive organic compounds are present in the same particles as chloride. Simultaneously, formation of organochlorine compounds, which are commonly toxic, is likely occurring when reactive organic components are present.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 10","pages":" 1645-1656"},"PeriodicalIF":5.5,"publicationDate":"2023-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10287122","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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":"Read-across-based intelligent learning: development of a global q-RASAR model for the efficient quantitative predictions of skin sensitization potential of diverse organic chemicals†","authors":"Arkaprava Banerjee and Kunal Roy","doi":"10.1039/D3EM00322A","DOIUrl":"10.1039/D3EM00322A","url":null,"abstract":"<p >Environmental chemicals and contaminants cause a wide array of harmful implications to terrestrial and aquatic life which ranges from skin sensitization to acute oral toxicity. The current study aims to assess the quantitative skin sensitization potential of a large set of industrial and environmental chemicals acting through different mechanisms using the novel quantitative Read-Across Structure–Activity Relationship (q-RASAR) approach. Based on the identified important set of structural and physicochemical features, Read-Across-based hyperparameters were optimized using the training set compounds followed by the calculation of similarity and error-based RASAR descriptors. Data fusion, further feature selection, and removal of prediction confidence outliers were performed to generate a partial least squares (PLS) q-RASAR model, followed by the application of various Machine Learning (ML) tools to check the quality of predictions. The PLS model was found to be the best among different models. A simple user-friendly Java-based software tool was developed based on the PLS model, which efficiently predicts the toxicity value(s) of query compound(s) along with their status of Applicability Domain (AD) in terms of leverage values. This model has been developed using structurally diverse compounds and is expected to predict efficiently and quantitatively the skin sensitization potential of environmental chemicals to estimate their occupational and health hazards.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 10","pages":" 1626-1644"},"PeriodicalIF":5.5,"publicationDate":"2023-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10173946","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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":"Diversity of organic components in airborne waste discharged from sewer pipe repairs†","authors":"Ana C. Morales, Christopher P. West, Brianna N. Peterson, Yoorae Noh, Andrew J. Whelton and Alexander Laskin","doi":"10.1039/D3EM00084B","DOIUrl":"10.1039/D3EM00084B","url":null,"abstract":"<p >Air-discharged waste from commonly used trenchless technologies of sewer pipe repairs is an emerging and poorly characterized source of urban pollution. This study reports on the molecular-level characterization of the atmospherically discharged aqueous-phase waste condensate samples collected at four field sites of the sewer pipe repairs. The molecular composition of organic species in these samples was investigated using reversed-phase liquid chromatography coupled with a photodiode array detector and a high-resolution mass spectrometer equipped with interchangeable atmospheric pressure photoionization and electrospray ionization sources. The waste condensate components comprise a complex mixture of organic species that can partition between gas-, aqueous-, and solid-phases when water evaporates from the air-discharged waste. Identified organic species have broad variability in molecular weight, molecular structures, and carbon oxidation state, which also varied between the waste samples. All condensates contained complex mixtures of oxidized organics, N- and S-containing organics, condensed aromatics, and their functionalized derivatives that are directly released to the atmospheric environment during installations. Furthermore, semi-volatile, low volatility, and extremely low volatility organic compounds comprise 75–85% of the total compounds identified in the waste condensates. Estimates of the component-specific viscosities suggest that upon evaporation of water waste material would form the semi-solid and solid phases. The low volatilities and high viscosities of chemical components in these waste condensates will contribute to the formation of atmospheric secondary organic aerosols and atmospheric solid nanoplastic particles. Lastly, selected components expected in the condensates were quantified and found to be present at high concentrations (1–20 mg L<small>⁻¹</small>) that may exceed regulatory limits.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 10","pages":" 1670-1683"},"PeriodicalIF":5.5,"publicationDate":"2023-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10182473","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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":"Impact of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) on secondary sludge microorganisms: removal, potential toxicity, and their implications on existing wastewater treatment regulations in Canada","authors":"Zanina Ilieva, Patricia Hania, Roxana Suehring, Kimberley Gilbride and Rania Hamza","doi":"10.1039/D3EM00202K","DOIUrl":"10.1039/D3EM00202K","url":null,"abstract":"<p >Perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) are two of the most commonly researched per- and polyfluoroalkyl substances (PFAS). Globally, many long-chain PFAS compounds including PFOS and PFOA are highly regulated and, in some countries, PFAS use in commercial products is strictly prohibited. Despite the legal regulation of these ‘forever chemicals’ under the Canadian Environmental Protection Act, PFOA and PFOS compounds are still found in high concentrations in discharges from wastewater treatment plants, both from liquid and sludge streams. Yet, their potential impact on wastewater treatment effectiveness remains poorly understood. The findings of this research show that: (1) PFOS and PFOA might be hindering the overall outcome treatment performance – calling into question the efficacy of Canada's existing wastewater treatment regulatory standard (Wastewater Systems Effluent Regulations, SOR/2012-139), and (2) specific microorganisms from the <em>Thiobacillus</em> and <em>Pseudomonas</em> genera seem capable of adsorbing PFOS and PFOA onto their cell wall and even degrading the chemicals, but it is unclear as to what extent degradation occurs. The results also raise questions whether existing wastewater regulations should be expanded to include the detection and monitoring of PFAS, as well as the establishment of a regulatory wastewater treatment plant discharge standard for PFAS that is protective of human and ecological health.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 10","pages":" 1604-1614"},"PeriodicalIF":5.5,"publicationDate":"2023-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10167999","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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":"Maternal hair segments reveal metal(loid) levels over the course of pregnancy: a preliminary study in Southern China†","authors":"Bingqing Liu, Fengshan Cai, Bin Tang, Jialu Li, Xiao Yan, Dongwei Du, Jing Zheng, Mingzhong Ren and Yunjiang Yu","doi":"10.1039/D3EM00279A","DOIUrl":"10.1039/D3EM00279A","url":null,"abstract":"<p >Characterization of metal(loid) variation during pregnancy and identification of the affecting factors are important for assessing pregnancy exposures in epidemiological studies. In this study, maternal hair was collected in three segments (each 3 cm) from pregnant women in Guangzhou, China. Ten metal(loid)s, including six essential trace metal(loid)s and four toxic trace metal(loid)s, were analyzed to investigate the levels of various metal(loid)s during pregnancy and the factors that influence them. Strong pairwise correlations were observed between manganese (Mn), cobalt (Co), and vanadium (V), between selenium (Se), arsenic (As), and antimony (Sb), and between cadmium (Cd) and lead (Pb). All metal(loid)s except for Se, Mn, and Co showed strong correlations among the three hair segments, and most of the metal(loid)s had good reproducibility, with intraclass correlation coefficients (ICCs) ranging from 0.510 to 0.931, except for As (ICC = 0.334), Mn (ICC = 0.231), and Co (ICC = 0.235). Zn levels decreased, while Sb increased, in maternal hair during pregnancy. Maternal sociodemographic characteristics and dietary intake affected metal(loid) levels in maternal hair. These results provide foundational data for using maternal hair segmental analysis to evaluate exposure variation to metal(loid)s during pregnancy and the potential factors associated with them.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 10","pages":" 1684-1693"},"PeriodicalIF":5.5,"publicationDate":"2023-08-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10598223","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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":"Biomonitoring, exposure routes and risk assessment of chlorinated paraffins in humans: a mini-review†","authors":"Hanyu Liao, Xue Li, Yuanyuan Zhou, Yinyin Wu, Yifei Cao, Jun Yang and Jianyun Zhang","doi":"10.1039/D3EM00235G","DOIUrl":"10.1039/D3EM00235G","url":null,"abstract":"<p >Chlorinated paraffins (CPs), which were conventionally classified into short- (SCCPs), medium- (MCCPs) and long- (LCCPs) chain CPs, have received growing attention due to their wide usage and extensive detection in environmental samples and biota. The number of studies regarding the biomonitoring of CPs in human beings increased rapidly and their health risk gained great concern. This review summarized their occurrence and homologue patterns in human matrices including blood/serum, placenta, cord serum and breast milk. As the production and usage of SCCPs was progressively banned after being listed in Annex A of the Stockholm Convention, the production of MCCPs and LCCPs was stimulated. Accordingly, the ratio of MCCPs/SCCPs in human samples has increased rapidly in the last 5 years. The current understanding of exposure routes and risk assessments of CPs was also reviewed. Oral dietary intake is the most predominant source of daily CP intake, but dust ingestion, inhalation and dermal exposure is also nonnegligible, especially for MCCPs and LCCPs. Furthermore, the reported upper bound of the estimated daily intakes (EDIs) in various risk assessment studies was close to or exceeded the tolerable daily intakes (TDIs). Considering the bioaccumulation and long-lasting exposure of CPs, their health impacts on humans and the ecosystem required continuous monitoring and evaluation.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 10","pages":" 1588-1603"},"PeriodicalIF":5.5,"publicationDate":"2023-08-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10120319","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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":"Combining predictive and analytical methods to elucidate pharmaceutical biotransformation in activated sludge†","authors":"Leo Trostel, Claudia Coll, Kathrin Fenner and Jasmin Hafner","doi":"10.1039/D3EM00161J","DOIUrl":"https://doi.org/10.1039/D3EM00161J","url":null,"abstract":"<p >While man-made chemicals in the environment are ubiquitous and a potential threat to human health and ecosystem integrity, the environmental fate of chemical contaminants such as pharmaceuticals is often poorly understood. Biodegradation processes driven by microbial communities convert chemicals into transformation products (TPs) that may themselves have adverse ecological effects. The detection of TPs formed during biodegradation has been continuously improved thanks to the development of TP prediction algorithms and analytical workflows. Here, we contribute to this advance by (i) reviewing past applications of TP identification workflows, (ii) applying an updated workflow for TP prediction to 42 pharmaceuticals in biodegradation experiments with activated sludge, and (iii) benchmarking 5 different pathway prediction models, comprising 4 prediction models trained on different datasets provided by enviPath, and the state-of-the-art EAWAG pathway prediction system. Using the updated workflow, we could tentatively identify 79 transformation products for 31 pharmaceutical compounds. Compared to previous works, we have further automatized several steps that were previously performed by hand. By benchmarking the enviPath prediction system on experimental data, we demonstrate the usefulness of the pathway prediction tool to generate suspect lists for screening, and we propose new avenues to improve their accuracy. Moreover, we provide a well-documented workflow that can be (i) readily applied to detect transformation products in activated sludge and (ii) potentially extended to other environmental studies.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 8","pages":" 1322-1336"},"PeriodicalIF":5.5,"publicationDate":"2023-08-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2023/em/d3em00161j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3984792","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}

{"title":"Spatiotemporal patterns in differences between the 137Cs concentrations of forest and stream litters: effect of leaching†","authors":"Masaru Sakai, Mitsuru Ohira and Takashi Gomi","doi":"10.1039/D3EM00236E","DOIUrl":"https://doi.org/10.1039/D3EM00236E","url":null,"abstract":"<p >Forest–stream ecotones possess prominent detritus-based food webs, and <small>¹³⁷</small>Cs-contaminated litter can influence the contamination levels of animals inhabiting such ecosystems. The effects of leaching on contaminated litter induce greater absolute differences between the <small>¹³⁷</small>Cs concentrations of forest and stream litter in more contaminated sites. Because <small>¹³⁷</small>Cs concentrations in litter can be attenuated temporally, spatiotemporal patterns in the differences in <small>¹³⁷</small>Cs concentrations between forest and stream litter may vary depending on both the amount of <small>¹³⁷</small>Cs deposition and the passage of time. To test this hypothesis, we sampled coniferous needle and broad-leaved deciduous litter in forests and streams at seven forested headwater sites affected by the Fukushima nuclear accident 3.24 and 11.24 years after the accident. We found that <small>¹³⁷</small>Cs concentrations in the two litter types were one order of magnitude lower 11.24 years after the accident than 3.24 years afterwards. The absolute difference in <small>¹³⁷</small>Cs activity concentrations of litter between forest and stream ecosystems was higher at more contaminated sites both 3.24 and 11.24 years after the accident. The spatiotemporal changes in litter contamination provide insight into <small>¹³⁷</small>Cs dynamics and complex transfer in the detritus-based food webs of forest–stream ecotones.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 8","pages":" 1385-1390"},"PeriodicalIF":5.5,"publicationDate":"2023-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3927388","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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":"Analytical methodologies for oxidized organic compounds in the atmosphere†","authors":"Aleksi Tiusanen, Jose Ruiz-Jimenez, Kari Hartonen and Susanne K. Wiedmer","doi":"10.1039/D3EM00163F","DOIUrl":"https://doi.org/10.1039/D3EM00163F","url":null,"abstract":"<p >Oxidized compounds in the atmosphere can occur as emitted primary compounds or as secondary products when volatile emitted precursors react with various oxidants. Due to the presence of polar functional groups, their vapor pressures decrease, and they condense onto small particles. Thereby, they have an effect on climate change by the formation of clouds and scattering solar radiation. The particles and oxidized compounds themselves can cause serious health problems when inhaled. Therefore, it is of utmost importance to study oxidized compounds in the atmosphere. Much ongoing research is focused on the discovery of new oxidized substances and on the evaluation of their sources and factors influencing their formation. Monitoring biogenic and anthropogenic primary oxidized compounds or secondary oxidized products in chamber experiments or field campaigns is common. New discoveries have been reported, including various oxidized compounds and a new group of compounds called highly oxidized organic molecules (HOMs). Analytics of HOMs are mainly focused on chromatography and high-resolution mass spectrometry employing chemical ionization for identifying and quantifying compounds at low concentrations. Oxidized compounds can also be monitored by spectrophotometric methods in which the determinations of total amounts are based on functional groups. This review highlights recent findings on oxidized organic compounds in the atmosphere and analytical methodologies used for their detection and quantification. The discussion includes gas and liquid chromatographic methods, sampling, extraction, concentration, and derivatization procedures involved, as well as mass spectrometric and spectrophotometric methods.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 8","pages":" 1263-1287"},"PeriodicalIF":5.5,"publicationDate":"2023-07-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2023/em/d3em00163f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3984787","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}