Journal of hazardous materials最新文献

The worldwide detection of emerging transformation products of organic micropollutants has raised accumulating concerns owing to their unknown environmental fate and undesired toxicity. This work first explored the reaction kinetics and mechanisms of the prevalent N-acetylated sulfonamides (N⁴-AcSAs, the typical sulfonamide metabolites) from wastewater disinfection to solar-irradiated receiving waters. The transformation scenarios included chlorination/bromination, photodegradation, and solar/chlorine treatment. The halogenations of two N⁴-AcSAs (N⁴-acetylated sulfadiazine, N⁴-AcSDZ; N⁴-acetylated sulfamethoxazole, N⁴-AcSMX) were pH-dependent at pH 5.0-8.0, and the reactions between the neutral forms of oxidants and anionic N⁴-AcSAs dominated the process. Furthermore, solar-based photolysis significantly eliminated N⁴-AcSAs in small water bodies with low dissolved organic carbon levels, while the indirect photolysis mediated by hydroxyl radicals and carbonate radicals contributed the most. The presence of chlorine residues in solar-irradiated wastewater effluents promoted the decay of N⁴-AcSAs, in which the generated hydroxyl radicals and ozone played a major role. Product analysis suggested the main transformation patterns of N⁴-AcSAs during the above scenarios included electrophilic attack, bond cleavage, SO₂ extrusion, hydroxylation, and rearrangement. Multiple secondary products maintained higher persistence, mobility, and toxicity to aquatic organisms than N⁴-AcSAs. Overall, the natural and engineered transformations of such micropollutants underlined the necessity of including their degradation products in future chemical management and risk assessment.

Herein, copper sulfide (CuS) was introduced to the Fenton-like (Fe(III)/H₂O₂) system for the efficient removal of phenylarsonic acid (PAA). Results of reactive oxygen and Fe/Cu species showed that CuS preferentially reacted with Fe(III) and H₂O₂ to generate Cu(I) and superoxide anion (•O₂^-). These reductive species could efficiently promote the Fe(III)/Fe(II) and Cu(II)/Cu(I) cycles, and are beneficial to the sequential Fenton reaction to generate •OH. The organoic/inorganic arsenic species detected in the CuS/Fe(III)/H₂O₂ system confirmed that PAA was oxidized by •OH to hydroxylated organoarsenic and phenolic intermediates, which were further mineralized to oxalate and formic acid. Meanwhile, the inorganic As(III)/As(V) released during PAA degradation were efficiently immobilized by CuS. The PAA removal efficiency remained as high as 92.9 % after 5 cycles of the CuS-mediated Fenton-like process. These results demonstrate an innovative method for the treatment of organoarsenic-contaminated water, and provide new insights into the enhanced Fenton-like process utilizing sulfide minerals.

Microplastics (MPs) pose significant concerns for marine ecological security due to their minuteness and ubiquity. However, comprehensive knowledge on their distribution and fate in seawater columns remains limited. This study investigated the abundances and characteristics of MPs across 3-6 water layers in the South Yellow Sea and East China Sea. Results indicate that high-abundance small MPs (< 100 µm) (average 6567 items/m³) were hidden beneath the sea-surface, predominantly fine-grained particles (< 20 µm) and high-density polymers (> 1.03 g/cm³). The total suspended MPs (5.0-834.2 µm) are estimated at 2.9-3.1 × 10¹⁷ particles, with most of them occurring in upper layers. In profiles, their distribution varied by physical properties with depth; fragment-shaped and high-density MPs increased in proportion at greater depths, contrasting with fibrous MPs. These MPs originated primarily from the Yangtze River and their winter transport was driven by the Yangtze River Dilution Water, East China Sea Coastal Current, and Yellow Sea Warm Current, resulting in their accumulation in coastal and estuarine regions. Consequently, the Yangtze River Estuary ecosystem faces substantial risks from MP pollution throughout the water column. This work unveils the prevalence of small MPs in coastal water columns and intricate interaction between their fate and hydrodynamic conditions.

Silicosis represents a form of interstitial lung disease induced by the inhalation of silica particles in production environments. A key pathological characteristic of silica-induced pulmonary fibrosis is its localized tissue heterogeneity, which presents significant challenges in analyzing transcriptomic data due to the loss of important spatial context. To address this, we integrate spatial gene expression data with single-cell analyses and achieve a detailed mapping of cell types within and surrounding fibrotic regions, revealing significant shifts in cell populations in normal and diseased states. Additionally, we explore cell interactions within fibrotic zones using ligand-receptor mapping, deepening our understanding of cellular dynamics in these areas. We identify a subset of fibroblasts, termed Inmt fibroblasts, that play a suppressive role in the fibrotic microenvironment. Validating our findings through a comprehensive suite of bioinformatics, histological, and cell culture studies highlights the role of monocyte-derived macrophages in shifting Inmt fibroblast populations into profibrotic Grem1 fibroblast, potentially disrupting lung homeostasis in response to external challenges. Hence, the spatially detailed deconvolution offered by our research markedly advances the comprehension of cell dynamics and environmental interactions pivotal in the development of pulmonary fibrosis.

While the impact of human activities on organic matter pollution is recognized, how these impacts vary seasonally in the Changjiang Delta needs further investigation. This study addresses this gap by investigating seasonal variations in organic matter sources and ecological responses to human activities in Changjiang Delta sediments. Total organic carbon (TOC), total nitrogen (TN), and carbon (δ¹³C) and nitrogen (δ¹⁵N) isotopic compositions of surface sediments collected from the Taipu River and Dalian Lake wetland were analyzed. Both water bodies exhibited similar seasonal trends for TOC and TN, with the Taipu River containing an average of 0.46% and 0.03% higher concentrations of TOC and TN, respectively, compared to Dalian Lake. Additionally, the organic index (OI) and organic nitrogen (ON) index were elevated in both water bodies during the wet season. Sediments from Dalian Lake remained uncontaminated to moderately contaminated, while those from the Taipu River were generally classified as moderately to heavily contaminated. Stable isotope analysis identified terrestrial C₃ plants (averaging 25.5%), C₄ plants (averaging 16.0%), and municipal wastewater (averaging 16.0%) as the main contributors to organic matter in the sediments. These findings suggest that terrestrial plant material and municipal wastewater are key targets for managing organic matter contamination in the Changjiang Delta. Implementing strategic land-use planning and targeted interventions to minimize these inputs can significantly improve water quality and ecosystem health.

Microplastics (MPs) have unique toxicokinetic (TK) processes that differ from those of soluble pollutants. This study investigated the ingestion, migration, accumulation, and clearance of environmental aging MPs in the Japanese swamp shrimp (Macrobrachium nipponense). The concentrations of plastic additives and personal care products adsorbed onto MPs in natural river water were determined, and TK models for MPs and MPs-loaded pollutants were developed. Results showed that the formation of surface biofilms and alterations in the distribution of MPs in waters caused by environmental aging affect MPs bioavailability, which is mainly related to the feeding habits of shrimp. The decrease in MPs particle size caused by biological digestion and the increase in the number of oxygen-containing functional groups caused by environmental aging affect the TK process of MPs. The TK model of MPs-loaded pollutants revealed the cleaning effect of shrimp on pollutants adsorbed onto MPs during swallowing and spitting MPs. This cleaning effect significantly increases the bioavailability of MPs-associated pollutants in aquatic environments. This study provides a new perspective for understanding the interactions between environmental MPs and their associated pollutants in aquatic ecosystems.

Efficient degradation of haloacetic acids (HAAs) is crucial due to their potential risks. This study firstly proposed vacuum ultraviolet - activated peroxymonosulfate (VUV/PMS) to remove HAAs (i.e., monochloroacetic acid (MCAA), monobromoacetic acid (MBAA), dichloroacetic acid (DCAA), etc). VUV/PMS achieved 99.51 % MCAA and 63.29 % TOC removal within 10 min. Electron paramagnetic resonance (EPR), quenching and probe experiments demonstrated that •OH was responsible for MCAA degradation. MCAA degradation followed pathways of dehalogenation (major) and decarboxylation (minor). VUV/PMS showed application potential under various reaction parameters. Broad spectrum of VUV/PMS on various HAAs was further explored. Chlorinated HAAs (Cl-HAAs) were primarily degraded by oxidation reactions, while brominated HAAs (Br-HAAs) by direct VUV photolysis. The density functional theory-based calculations (DFT) revealed that reaction rates of HAAs correlated with the highest occupied molecular orbital (HOMO) and energy gap (ΔE), indicating that HAAs degradation depends on their chemical structures. The Fukui function (f⁰ values) and bond length showed vulnerability of the halogen atom in Cl-HAAs and C-Br bond in Br-HAAs. Overall, this study provides an in-depth perspective on the oxidation performance and mechanism of HAAs using VUV/PMS. It not only demonstrates a green and efficient method but also inspires new strategies for HAAs remediation.

The spread of opportunistic pathogens (OPs) and antibiotic resistance genes (ARGs) through drinking water has already caused serious human health issues. There is also an urgent need to know the effects of perfluorooctanoic acid (PFOA) on OPs with different ARGs in drinking water. Our results suggested that PFOA accumulation and release from the pipelines induced its concentration in pipelines effluents increase from 0.03 ± 0.01 μg/L to 0.70 ± 0.01 μg/L after 6 months accumulation. The PFOA also promoted the growth of Hyphomicrobium, Microbacterium, and Bradyrhizobium. In addition, PFOA accumulation and release from the pipelines enhanced the metabolism and tricarboxylic acid (TCA) cycle processes, resulting in more extracellular polymeric substances (EPS) production. Due to EPS protection, Pseudomonas aeruginosa and Legionella pneumophila increased to (7.20 ± 0.09) × 10⁴ gene copies/mL, and (8.85 ± 0.11) × 10² gene copies/mL, respectively. Moreover, PFOA also enhanced the transfer potential of different ARGs, including emrB, mdtB, mdtC, mexF, and macB. The main bacterial community composition and the main OPs positively correlated with the main ARGs and mobile genetic elements (MGE)-ARGs significantly. Therefore, PFOA promoted the propagation of OPs with different ARGs. These results are meaningful for controlling the microbial risk caused by the OPs with ARGs and MGE-ARGs in drinking water.

Fluoride (F¯) contamination in groundwater in India has gained global attention due to human health hazards. India's hydrogeological heterogeneity, spatio-temporal variability of F¯, and health hazards due to geogenic and geo-environmental control pose unique challenges. Addressing these with only a single region-specific study is not possible. Therefore, this study provides an in-depth, holistic analysis of pan India F¯ contamination, controlling factors, and health hazards using a coupled advanced geostatistical and geospatial approach. Alarming F¯ contaminations are identified in Rajasthan, Telangana, Western Andhra Pradesh, Eastern Karnataka, Parts of Haryana, Gujarat, Madhya Pradesh, Tamil Nadu, Uttar Pradesh, Jharkhand, Bihar, and Chhattisgarh. Probabilistic health-risk evaluation using hot-spot, showed similar spatio-temporal distribution of F¯ contamination. The hazard quotient (HQ) for high F¯ shows more adversity to children than adults. Nationally, 8.65 % and 7.10 % of pre- and post-monsoon sites exceed the recommended safe limit of 1.50 mg/L. The highest average F¯ concentration is in Rajasthan. Very high-risk skeletal fluorosis is possible at around ≤ 2 %, whereas dental caries due to deficiency in F¯ concentration is approximately 40 %. A decisive hierarchy of lithology, geomorphology, soils, and lineaments control are identified on F¯ contamination. Climatic conditions are pivotal in governing all these controlling variables. Thus, in arid/semi-arid dry western regions, F¯ contamination is much higher than in the humid areas. Integration of strengths, weaknesses, opportunities, and threats (SWOT) analysis with the results can aid policymakers and government authorities in achieving sustainable remedial measures for future adaptability.

Advanced oxidation processes are a desirable technology for treatment of contaminants of emerging concern. Nevertheless, conventional advanced oxidation of organophosphorus compounds releases inorganic phosphate, posing downstream concerns related to eutrophication. For this reason, we evaluated the ultraviolet light-activated calcium peroxide (UV/CaO₂) system for effective treatment of organophosphorus compounds and concurrent capture of the mineralization products, phosphate. The degradation mechanisms, reaction kinetics, and mineralizations were assessed to determine the overall efficiency and performance of the UV/CaO₂ process. Knowledge gaps related to photocatalysis in the UV/CaO₂ system were not only addressed, but also leveraged to identify unique advantages for removal of organophosphorus compounds and their degradation products. Experimental results confirmed that the UV/CaO₂ system effectively mineralized organophosphorus compounds and recovered inorganic phosphate; additionally, collaborative carbon fixation performance of the system reveals the potential of carbon utilization. These outcomes were facilitated by the alkaline environment generated by CaO₂. The recovered solids contained most of the phosphorus and carbon from the parent compounds. Ultimately, these findings provide transformative, new insights into the development and application of advanced oxidation processes that prevent downstream concerns related to mineralization products, especially inorganic phosphorus and carbon.