Journal of environmental sciences最新文献

Beijing-Tianjin-Hebei and its surrounding areas (hereinafter referred to as “2+26” cities) are one of the most severe air pollution areas in China. The fine particulate matter (PM_2.5) and surface ozone (O₃) pollution have aroused a significant concern on the national scale. In this study, we analyzed the pollution characteristics of PM_2.5 and O₃ in “2+26” cities, and then estimated the health burden and economic loss before and after the implementation of the joint PM_2.5-O₃ control policy. During 2017–2019, PM_2.5 concentration reduced by 19% while the maximum daily 8 hr average (MDA8) O₃ stayed stable in “2+26” cities. Spatially, PM_2.5 pollution in the south-central area and O₃ pollution in the central region were more severe than anywhere else. With the reduction in PM_2.5 concentration, premature deaths from PM_2.5 decreased by 18% from 2017 to 2019. In contrast, premature deaths from O₃ increased by 5%. Noticeably, the huge potential health benefits can be gained after the implementation of a joint PM_2.5-O₃ control policy. The premature deaths attributed to PM_2.5 and O₃ would be reduced by 91.6% and 89.1%, and the avoidable economic loss would be 60.8 billion Chinese Yuan (CNY), and 68.4 billion CNY in 2035 compared with that in 2019, respectively. Therefore, it is of significance to implement the joint PM_2.5-O₃ control policy for improving public health and economic development.

Extracellular polymeric substances (EPS) are an important medium for communication and material exchange between iron-oxidizing bacteria and the external environment and could induce the iron (oxyhydr) oxides production which reduced arsenic (As) availability. The main component of EPS secreted by iron-oxidizing bacteria (Ochrobactrum EEELCW01) was composed of polysaccharides (150.76-165.33 mg/g DW) followed by considerably smaller amounts of proteins (12.98–16.12 mg/g DW). Low concentrations of As (100 or 500 µmol/L) promoted the amount of EPS secretion. FTIR results showed that EPS was composed of polysaccharides, proteins, and a miniscule amount of nucleic acids. The functional groups including -COOH, -OH, -NH, -C=O, and -C-O played an important role in the adsorption of As. XPS results showed that As was bound to EPS in the form of As³⁺. With increasing As concentration, the proportion of As³⁺ adsorbed on EPS increased. Ferrihydrite with a weak crystalline state was only produced in the system at 6 hr during the mineralization process of Ochrobactrum sp. At day 8, the minerals were composed of goethite, galena, and siderite. With the increasing mineralization time, the main mineral phases were transformed from weakly crystalline hydrous iron ore into higher crystallinity siderite (FeCO₃) or goethite (α-FeOOH), and the specific surface area and active sites of minerals were reduced. It can be seen from the distribution of As elements that As is preferentially adsorbed on the edges of iron minerals. This study is potential to understand the biomineralization mechanism of iron-oxidizing bacteria and As remediation in the environment.

Due to significant differences in biotic and abiotic properties of soils compared to those of sediments, the predicted underlying microbe-mediated mechanisms of soil carbon emissions in response to warming may not be applicable for estimating similar emissions from inland water sediments. We addressed this issue by incubating different types of sediments, (including lake, small river, and pond sediments) collected from 36 sites across the Yangtze River basin, under short-term experimental warming to explore the effects of climate warming on sediment carbon emission and the underlying microbe-mediated mechanisms. Our results indicated that under climate warming CO₂ emissions were affected more than CH₄ emissions, and that pond sediments may yield a greater relative contribution of CO₂ to total carbon emissions than lake and river sediments. Warming-induced CO₂ and CH₄ increases involve different microbe-mediated mechanisms; Warming-induced sediment CO₂ emissions were predicted to be directly positively driven by microbial community network modularity, which was significantly negatively affected by the quality and quantity of organic carbon and warming-induced variations in dissolved oxygen, Conversely, warming-induced sediment CH₄ emissions were predicted to be directly positively driven by microbial community network complexity, which was significantly negatively affected by warming-induced variations in pH. Our findings suggest that biotic and abiotic drivers for sediment CO₂ and CH₄ emissions in response to climate warming should be considered separately when predicting sediment organic carbon decomposition dynamics resulting from climate change.

As an anticonvulsant, oxcarbazepine (OXC) has attracted considerable attention for its potential threat to aquatic organisms. Density functional theory has been used to study the mechanisms and kinetics of OXC degradation initiated by OH radicals in aqueous environment. A total of fourteen OH-addition pathways were investigated, and the addition to the C8 position of the right benzene ring was the most vulnerable pathway, resulting in the intermediate IM8. The H-abstraction reactions initiated by OH radicals were also explored, where the extraction site of the methylene group (C14) on the seven-member carbon heterocyclic ring was found to be the optimal path. The calculations show that the total rate constant of OXC with OH radicals is 9.47 × 10⁹ (mol/L)⁻¹sec⁻¹, and the half-life time is 7.32 s at 298 K with the [·OH] of 10⁻¹¹ mol/L. Moreover, the branch ratio values revealed that OH-addition (89.58%) shows more advantageous than H-abstraction (10.42%). To further understand the potential eco-toxicity of OXC and its transformation products to aquatic organisms, acute toxicity and chronic toxicity were evaluated using ECOSAR software. The toxicity assessment revealed that most degradation products such as OXC-2OH, OXC-4OH, OXC-1O-1OOH, and OXC-1OH' are innoxious to fish and daphnia. Conversely, green algae are more sensitive to these compounds. This study can provide an extensive investigation into the degradation of OXC by OH radicals and enrich the understanding of the aquatic oxidation processes of pharmaceuticals and personal care products (PPCPs).

Sediment core is the recorder of polycyclic aromatic hydrocarbon (PAH) pollutions and the associated sedimentary organic matter (SOM), acting as crucial supports for pollution control and environmental management. Here, the sedimentary records of PAHs and SOM in the past century in Lake Taihu, China, were reconstructed from a 50-cm sediment core. On the one hand, the presence of PAHs ranged from 8.99 to 199.2 ng/g. Vertically, PAHs declined with the depth increased, and the sedimentation history of PAHs was divided into two stages with a discontinuity at 20 cm depth. In composition, PAHs in the sediment core were dominated by three-ring PAHs (44.6% ± 9.1%, mean ± standard deviation), and were followed by four-ring (27.0% ± 3.3%), and five-ring (12.1% ± 4.0%) PAHs. In toxicity assessment, the sedimentary records of benzo[a]pyrene-based toxic equivalency were well described by an exponential model with R-square of 0.95, and the environmental background toxic value was identified as 1.62 ng/g. On the other hand, different components of SOM were successfully identified by n-alkane markers (p < 0.01) and the variations of SOM were well explained (84.6%). A discontinuity of SOM was recognized at 22 cm depth. Association study showed that the sedimentary PAHs were associated with both anthropogenic and biogenic SOM (p < 0.05) with explained variances for most individual PAHs of 60%. It indicated the vertical distributions of PAHs were driven by sedimentary SOM. Therefore, environmental processes such as biogenic factors should attract more attentions as well as PAH emissions to reduce the impacts of PAHs.

Despite coastal mudflats serving as essential ecological zones interconnecting terrestrial/freshwater and marine systems, little is known about the profiles of antibiotic resistance genes (ARGs) in this area. In this study, characteristics of typical ARGs, involving both intracellular (iARGs) and extracellular ARGs (eARGs) at different physical states, were explored in over 1000 km of coastal mudflats in Eastern China. Results indicated the presence of iARGs and eARGs at states of both freely present or attached by particles. The abundance of eARGs was significantly higher than that of iARGs (87.3% vs 12.7%), and their dominance was more significant than those in other habitats (52.7%-76.3%). ARG abundance, especially for eARGs, showed an increasing trend (p < 0.05) from southern (Nantong) to northern (Lianyungang) coastal mudflats. Higher salinity facilitated the transformation from iARGs to eARGs, and smaller soil particle size was conducive to the persistence of eARGs in northern coastal mudflats. This study addresses the neglected function of coastal mudflats as eARGs reservoirs.

Reservoirs have been served as the major source of drinking water for dozens of years. The water quality safety of large and medium reservoirs increasingly becomes the focus of public concern. Field test has proved that water-lifting and aeration system (WLAS) is a piece of effective equipment for in situ control and improvement of water quality. However, its intrinsic bioremediation mechanism, especially for nitrogen removal, still lacks in-depth investigation. Hence, the dynamic changes in water quality parameters, carbon source metabolism, species compositions and co-occurrence patterns of microbial communities were systematically studied in Jinpen Reservoir within a whole WLAS running cycle. The WLAS operation could efficiently reduce organic carbon (19.77%), nitrogen (21.55%) and phosphorus (65.60%), respectively. Biolog analysis revealed that the microbial metabolic capacities were enhanced via WLAS operation, especially in bottom water. High-throughput sequencing demonstrated that WLAS operation altered the diversity and distributions of microbial communities in the source water. The most dominant genus accountable for aerobic denitrification was identified as Dechloromonas. Furthermore, network analysis revealed that microorganisms interacted more closely through WLAS operation. Oxidation-reduction potential (ORP) and total nitrogen (TN) were regarded as the two main physicochemical parameters influencing microbial community structures, as confirmed by redundancy analysis (RDA) and Mantel test. Overall, the results will provide a scientific basis and an effective way for strengthening the in-situ bioremediation of micro-polluted source water.

The excessive accumulation of potentially toxic metals (Pb and Cd) in coastal wetlands is among the main factors threatening wetland ecosystems. However, the effects of water table depth (WTD) on the risk and binding mechanisms of potentially toxic metals in sediments remain unclear. Here, sediments from different WTD obtained from a typical coastal wetland were evaluated using a newly developed strategy based on chemical extraction methods coupled with high-resolution spectroscopy. Our findings indicated that the WTD of the coastal wetland fluctuates frequently and the average enrichment factor for Pb was categorized as minor, whereas Cd enrichment was categorized as moderate. High-resolution spectroscopy techniques also demonstrated that organic functional groups and partly inorganic compounds (e.g., Fe-O/Si-O) played a vital role in the binding of Pb and Cd to surface sediments. Additionally, mineral components rather than organic groups were mainly bound to these metals in the bottom sediments. Collectively, our findings provide key insights into the potential health effects and binding characteristics of potentially toxic metals in sediments, as well as their dynamic behavior under varying sediment depths at a microscale.

Urea oxidation reaction (UOR) provides a method for hydrogen production besides wastewater treatment, but the current limited catalytic activity has prevented the application. Herein, we develop a novel H₂O₂ treatment strategy for tailoring the surface oxygen ligand of NiFe-layered double hydroxides (NiFe-LDH). The sample after H₂O₂ treatment (NiFeO-LDH) shows significant enhancement on UOR efficiency, with the potential of 1.37 V (RHE) to reach a current density of 10 mA/cm². The boost is attributed to the richness adsorption O ligand on NiFeO-LDH as revealed by XPS and Raman analysis. DFT calculation indicates formation of two possible types of oxygen ligands: adsorbed oxygen on the surface and exposed from hydroxyl group, lowered the desorption energy of CO₂ product, which lead to the lowered onset potential. This strategy is further extended to NiFe-LDH nano sheet on Ni foam to reach a higher current density of 440 mA/cm² of UOR at 1.8 V (RHE). The facile surface O ligand manipulation is also expected to give chance to many other electro-catalytic oxidations.

This study investigated the enhancement effects of dissolved carbonates on the peroxymonosulfate-based advanced oxidation process with CuS as a catalyst. It was found that the added CO₃²⁻ increased both the catalytic activity and the stability of the catalyst. Under optimized reaction conditions in the presence of CO₃²⁻, the degradation removal of 4-methylphenol (4-MP) within 2 min reached 100%, and this was maintained in consecutive multi-cycle experiments. The degradation rate constant of 4-MP was 2.159 min⁻¹, being 685% greater than that in the absence of CO₃²⁻ (0.315 min⁻¹). The comparison of dominated active species and 4-MP degradation pathways in both CO₃²⁻-free and CO₃²⁻-containing systems suggested that more CO₃•⁻/¹O₂ was produced in the case of CO₃²⁻deducing an electron transfer medium, which tending to react with electron-rich moieties. Meanwhile, Characterization by X-ray photoelectron spectroscopic and cyclic voltammetry measurement verified CO₃²⁻ enabled the effective reduction of Cu²⁺ to Cu⁺. By investigating the degradation of 11 phenolics with different substituents, the dependence of degradation kinetic rate constant of the phenolics on their chemical structures indicated that there was a good linear relationship between the Hammett constants σ_p of the aromatic phenolics and the logarithm of k in the CO₃²⁻-containing system. This work provides a new strategy for efficient removal of electron-rich moieties under the driving of carbonate being widely present in actual water bodies.