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Influence of land use and landscape pattern on legacy nitrogen pollution in a typical watershed in eastern China

Catena 2025年 256卷

作者： Wang, Yucang Wu, Hao Pan, Zheqi Ma, Longdan Zhang, Yu Zhou, Jia Hu, Minpeng Cheng, Zhihan Zheng, Xin Chen, Dingjiang College of Environmental & Resource Sciences Zhejiang University Hangzhou 310058 China State Key Laboratory of Soil Pollution Control and Safety Zhejiang University Hangzhou 310058 China Ministry of Education Key Laboratory of Environment Remediation and Ecological Health Zhejiang University Hangzhou 310058 China Zhejiang Provincial Key Laboratory of Agricultural Resources and Environment Zhejiang University Hangzhou 310058 China

Legacy effects from nonpoint source nutrient pollution reduce the effectiveness of nitrogen remediation strategies in watersheds, yet spatial landscape variations and their influence on the legacy effects remain unclear. This study addressed spatial differences in legacy nitrogen pollution within the Yongan watershed in eastern China using detrended fluctuation analysis (where H > 0.5 indicates a legacy effect). Results revealed strong legacy effects for total nitrogen (TN) and nitrate nitrogen (NO₃^–-N) at the watershed outlet, with H values of 0.70 and 0.87, respectively, primarily influenced by soil nitrogen contributions (40 ± 8 %), as revealed by isotopic source apportionment. Significant spatial variation in the legacy effect was observed across different catchments, with H-index ranging from 0.42 to 0.85 for TN and from 0.58 to 0.91 for NO₃^–-N. Land use explained 90 % of this variation, predominantly driven by grasslands (48 %), impervious surfaces (16 %), and orchards (14 %). Grasslands were found to reduce legacy effects by reducing nitrogen inputs from soil and groundwater, whereas impervious surfaces reduced the legacy effect by increasing domestic wastewater contributions. Conversely, agricultural lands (orchards, paddy fields and drylands) exacerbated the legacy effect through elevated soil nitrogen contributions. Threshold values for key landscape metrics were identified that effectively mitigated the legacy effect: increasing grassland edge density (ED) to 0.16 km/km², orchard connectivity (CONNECT) to 32 %, and impervious surface aggregation (AI) to 91 %. The integration of stable isotopes and landscape data provides a robust framework for identifying dominant nitrogen sources and uncovering the spatial mechanisms underlying legacy pollution. These findings can guide landscape management strategies and support targeted interventions for nonpoint source nitrogen control at the watershed scale. © 20

关键词： Landscape indices Legacy effect Nitrogen Spatial variation Watershed nutrient pollution

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UV/H2O2 oxidation of tri(2-chloroethyl) phosphate: Intermediate products, degradation pathway and toxicity evaluation

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Journal of environmental Sciences 2020年第12期32卷 55-61页

作者： Qiuyi Ji Huan He Zhanqi Gao Xiaohan Wang Shaogui Yang Cheng Sun Shiyin Li Yong Wang Limin Zhang School of Environment Nanjing Normal UniversityNanjing 210023China State Environmental Protection Key Laboratory of Monitoring and Analysis for Organic Pollutants in Surface Water Environment Monitoring Center of JiangsuNanjing 210036China State Key Laboratory of Pollution Control and Resources Reuse School of EnvironmentNanjing UniversityNanjing 210023China School of Environment Northeast Normal UniversityChangchun 130024China

Tri(2-chloroethyl) phosphate(TCEP) with the initial concentration of 5 mg/L was degraded by UV/H2O2 oxidation process. The removal rate of TCEP in the UV/H2O2 system was 89.1% with the production of Cl-and PO4^3- of 0.23 and 0.64 mg/L. The removal rate of total organic carbon of the reaction was 48.8% and the pH reached 3.3 after the reaction. The oxidative degradation process of TCEP in the UV/H2O2 system obeyed the first order kinetic reaction with the apparent rate constant of 0.0025 min^-1( R^2 = 0.9788). The intermediate products were isolated and identified by gas chromatography-mass spectrometer. The addition reaction of HO · and H2O and the oxidation reaction with H2O2 were found during the degradation pathway of 5 mg/L TCEP in the UV/H2O2 system. For the first time, environment risk was estimated via the "ecological structure activity relationships" program and acute and chronic toxicity changes of intermediate products were pointed out. The luminescence inhibition rate of photobacterium was used to evaluate the acute toxicity of intermediate products. The results showed that the toxicity of the intermediate products increased with the increase of reaction time, which may be due to the production of chlorine compounds. Some measures should be introduced to the UV/H2O2 system to remove the highly toxic Cl-containing compounds, such as a nanofiltration or reverse osmosis unit.

关键词： Tri(2-chloroethyl)phosphate(TCEP) UV/H2O2 Mechanisms Toxicity evaluation

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Influencing factors and prediction of ambient Peroxyacetyl nitrate concentration in Beijing,China

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Journal of environmental Sciences 2019年第3期31卷 189-197页

作者： Boya Zhang Bu Zhao Peng Zuo Zhi Huang Jianbo Zhang State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University School of Environment Tsinghua University

Peroxyacyl nitrates(PANs) are important secondary pollutants in ground-level *** prediction of atmospheric pollutant concentrations is crucial to guide effective precautions for before and during specific pollution events. In this study, four models based on the back-propagation(BP) artificial neural network(ANN) and multiple linear regression(MLR) methods were used to predict the hourly average PAN concentrations at Peking University, Beijing, in 2014. The model inputs were atmospheric pollutant data and meteorological parameters. Model 3 using a BP-ANN based on the original variables achieved the best prediction results among the four models, with a correlation coefficient(R) of 0.7089, mean bias error of -0.0043 ppb, mean absolute error of 0.4836?ppb, root mean squared error of 0.5320?ppb, and Willmott's index of agreement of 0.8214. Based on a comparison of the performance indices of the MLR and BP-ANN models, we concluded that the BP-ANN model was able to capture the highly non-linear relationships between PAN concentration and the conventional atmospheric pollutant and meteorological parameters,providing more accurate results than the traditional MLR models did, with a markedly higher goodness of R. The selected meteorological and atmospheric pollutant parameters described a sufficient amount of PAN variation, and thus provided satisfactory prediction results. More specifically, the BP-ANN model performed very well for capturing the variation pattern when PAN concentrations were low. The findings of this study address some of the existing knowledge gaps in this research field and provide a theoretical basis for future regional air pollution control.

关键词： Artificial neural network Conventional atmospheric pollutants Meteorological parameters Concentration prediction Multiple linear regression

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Metagenomic Insights into the Influence of Thallium Spill on Sediment Microbial Community

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SSRN 2022年

作者： Chen, Sili Chen, Xiuli Wang, Ji Pan, Chaoyi Feng, Lishi Xie, Shuguang Guangzhou510655 China State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University Beijing100871 China

Thallium (Tl) is an extremely toxic metal. The release of Tl into the natural environment can pose a potential threat to organisms. In addition, there has been no report on how sudden Tl spill influences the structure and function of the microbial community. This study explored the response of river sediment microbiome to a Tl spill. Residual T1 in the sediment significantly decreased bacterial community diversity. The increase in the abundance of Bacteroidetes in all Tl- impacted sediments suggested the advantage of Bacteroidetes to resist Tl pressure. After T1 spill, increase in both metal resistance genes (MRGs) and antibiotic resistance genes (ARGs) was observed in Tl-impacted sediments. The abundance of MRGs and ARGs was significantly correlated with sediment Tl concentration, implying the positive effect of Tl contamination on the proliferation of these resistance genes. Procrustes analysis suggested a significant congruence between profiles of MRGs and bacterial communities. Through LEfSe and co-occurrence network analysis, Trichococcus, Polaromonas, and Arenimonas were identified to be tolerant and resistant to Tl pollution. This study added new insights into the effect of Tl spill on microbial community and highlighted the role of heavy metal spill in the increase of both heavy metal and antibiotic resistance genes. © 2022, The Authors. All rights reserved.

关键词： Hazardous materials spills

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Filtration performance of biofilm membrane bioreactor: Fouling control by threshold flux operation

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Chemosphere 2024年 362卷 142458页

作者： Zhang, Wenxiang Liang, Wenzhong Jin, Jiarou Meng, Shujuan He, Ziqiang Ali, Muhammad Saikaly, Pascal E. Guangzhou511458 China State Environmental Protection Key Laboratory of Water Environmental Simulation and Pollution Control South China Institute of Environmental Sciences Ministry of Ecology and Environment of the People's Republic of China Guangzhou510655 China School of Materials Science and Engineering Beihang University Beijing100191 China Key Laboratory of Electromechanical Equipment Safety in Western Complex Environment for State Market Regulation Chongqing Special Equipment Inspection and Research Institute Chongqing401121 China Department of Civil Structural & Environmental Engineering Trinity College Dublin The University of Dublin Dublin 2 Ireland Thuwal23955-6900 Saudi Arabia

Membrane fouling is the major factor that restricts the furtherly widespread use of membrane bioreactor (MBR). As a new generation of MBR, biofilm membrane bioreactor (BF-MBR) demonstrates high treatment efficiency and low sludge growth rate, however the filtration performance improvement and membrane fouling control are still the challenges for its further development. This work investigated the filtration performance using resistance in series model and membrane fouling control via threshold flux for BF-MBR. At first, the flux behavior and filtration resistance under various operating conditions, including agitation speed, membrane and TMP, were explored by resistance in series model. Because of the desirable anti-fouling capacity, UP100 and UP030 had the high threshold flux (100 and 90 L m−2 h−1) and low irreversible fouling resistance (1 and 1.3 × 10−10 m-1). Higher shear stress produced by higher agitation speed could reduce membrane fouling, while greatly promote the threshold flux (138 L m−2 h−1) and membrane cleaning efficiency (96%). Moreover, increasing shear stress or selecting membrane with large pore size could decrease the fouling rate and raise the threshold flux. As for TMP, high TMP reduced the removal rate for organic and nutrient, and enhanced the irreversible fouling. Besides, the aerobic-BF-MBR (101 L m−2 h−1 and 1.3 × 10−10 m-1) with lower foulant concentration had a better filtration performance than anoxic-BF-MBR (90 L m−2 h−1 and 1.5 × 10−10 m-1). Additionally, the long-term tests with 10 cycles were conducted to evaluate the industrial application value of BF-MBR (45–58 L m−2 h−1). This work provides the technical support for sustainable filtration performance of BF-MBR. © 2024 Elsevier Ltd

关键词： Bioreactors

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Ionic-Liquid-Assisted Synthesis of N, F, and P Codoped Fenc/Hss on Hollow Carbon Nanospheres for Li–S Batteries

SSRN

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SSRN 2024年

作者： Li, Guanglei Zhu, Zhenye Chen, Shengmin Yue, Yapeng Li, Gefeng Zhou, Liang Zhu, Rongshu Yan, Zhenghong School of Materials Science and Engineering Harbin Institute of Technology Shenzhen Graduate School Shenzhen518055 China State Key Laboratory of Urban Water Resource and Environment Shenzhen Key Laboratory of Organic Pollution Prevention and Control School of Civil and Environmental Engineering Harbin Institute of Technology Shenzhen Shenzhen518055 China

The severe shuttle effect and slow redox kinetics of polysulfides are major obstacles to the practical application of lithium sulfur batteries. In this study, we proposed a method for synthesizing hollow carbon nanospheres supported by iron single-atom catalysts using [HMIM] PF6 ionic liquid (IL) as a promoter. Metal single atoms are embedded in carbon nanospheres to mitigateshuttle effects and enhance the bidirectional redox kinetics of sulfur. The incorporation of iron sites is beneficial for the reduction reaction of polysulfides, and the addition of ionic liquids not only increases the porosity of the catalyst but also enhances the loading of iron atoms. The sulfur cathode with metal single atom pairs exhibited an ultra-high capacity retention rate of 94% after 150 cycles at 0.2C. Even under a high sulfur load of 6.58 mg cm-2 and a current density of 0.2 C, an ideal areal capacity of 4.64 mAh cm-2 can still be maintained. Impressively, the assembled button cell battery achieved a high discharge capacity of 1451 mAh g-1 and maintained 867.9 mAh g-1 after 150 cycles at 0.2 C. This work provides new insights into designing loaded single-atom catalysts for application in lithium sulfur batteries. © 2024, The Authors. All rights reserved.

关键词： Lithium sulfur batteries

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Hydrogen Spillover Induced PtCo/CoOx Interfaces with Enhanced Catalytic Activity for CO Oxidation at Low Temperatures in Humid Conditions

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Small 2024年第22期20卷 2309181-2309181页

作者： Lin, Jiajin Zhao, Shuaiqi Yang, Jin Huang, Wei-Hsiang Chen, Chi-Liang Chen, Tingyu Zhao, Yun Chen, Guangxu Qiu, Yongcai Gu, Lin School of Environment and Energy State Key Laboratory of Luminescent Materials and Devices Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control South China University of Technology Guangzhou510000 China School of Chemistry and Chemical Engineering Wuhan Textile University Wuhan430200 China National Synchrotron Radiation Research Center Hsinchu30076 Taiwan Hsinchu30076 Taiwan Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and Devices Laboratory of Advanced Materials and Electron Microscopy Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing100190 China

The development of catalysts with abundant active interfaces for superior low-temperature catalytic CO oxidation is critical to meet increasingly rigorous emission requirements, yet still challenging. Herein, this work reports a PtCo/CoOx/Al2O3 catalyst with PtCo clusters and enriched Pt─O─Co interfaces induced by hydrogen spillover from the Pt sites and self-oxidation process in air, exhibiting excellent performance for CO oxidation at low temperatures and humid conditions. The combination of structural characterizations and in situ Fourier transform infrared spectroscopy reveals that the PtCo cluster effectively prevents CO saturation/poisoning on the Pt surface. Additionally, the presence of Pt─O─Co interfaces in the PtCo/CoOx/Al2O3 catalyst provides a significant number of active sites for oxygen activation and ─OH formation. This facilitates efficient generation of CO2 at ambient temperature by coupling with nearby adsorbed CO molecules, resulting in superior low-temperature activity and long-term stability for CO oxidation under humid conditions. This work provides a facile route toward rationalizing the design of catalysts with more active interfaces for superior low-temperature CO oxidation under humid conditions for practical applications. © 2023 Wiley-VCH GmbH.

关键词： Binary alloys

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Preparation and characterization of colorful graphene oxide papers and flexible N-doping graphene papers for supercapacitor and capacitive deionization

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Carbon Energy 2020年第4期2卷 656-674页

作者： Hao Zhang Aiyang Li Ying Yuan Yuquan Wei Di Zheng Zhuning Geng Haichuan Zhang Guanghe Li Fang Zhang School of Environment and State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijingChina National Engineering Laboratory for Site Remediation Technologies BeijingChina Chinese Research Academy of Environmental Sciences BeijingChina Beijing Key Laboratory of Biodiversity and Organic Farming College of Resources and Environmental SciencesChina Agricultural UniversityBeijingChina

An efficient method that utilizes simple techniques,easy operation,and low-cost production to create flexible graphene-based materials is a worthy practical challenge.A rapid strategy for preparing flexible,functional graphene oxide(GO)is introduced using GO-ethanol dispersion *** filtration process is highly efficient and drying time is significantly reduced by employing ethanol as solvent,due to the fact that ethanol is a volatile *** GO papers can be harvested with ultralarge size(700 cm2),color variety,and writable *** reduction,N-doped graphene(NDG)papers still maintain good foldability with improved electric conductivity and porous *** used as an electrode for a supercapacitor,the flexible NDG paper device demonstrates good electrochemical performance even with size expansion and extreme double ***,this NDG paper capacitor device shows a good electrosorption performance for capacitive deionization of sulfate and chromate in groundwater *** flexible GO and NDG papers promise potential to facilitate the production of graphene-based materials for practical applications in energy and environmental related fields.

关键词： colorful graphene oxide energy storage flexible graphene paper N-doped graphene supercapacitor

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Mechanistic insights into the leaching and environmental safety of arsenic in ceramsite prepared from fly ash

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Chemosphere 2023年 344卷 140292页

作者： Song, Bing Liu, Zequan Li, Chengming Zhou, Shiji Yang, Linjun Chen, Zhiliang Song, Min Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education School of Energy and Environment Southeast University Jiangsu Nanjing210096 China State Key Laboratory of Coal Mine Disaster Dynamics and Control Chongqing University Chongqing400044 China Department of Environmental Science College of Environment and Ecology Chongqing University Chongqing400045 China Jiangsu Province Engineering Research Center of Soil and Groundwater Pollution Prevention and Control Jiangsu Nanjing210036 China

Utilizing fly ash to prepare ceramsite is a promising way to immobilize heavy metals and recycle industrial solid waste. However, traditional preparation method of fly ash ceramsite has the disadvantages of large ignition loss. Therefore, the present study applied the pressure molding method to enhance solid content and improve the strength of ceramsite. The optimal preparation conditions of ceramsite were suggested as preheating at 450 °C for 25 min followed by sintering at 1050 °C for 30 min. Under such conditions, ceramsite with high compressive strength of 10.8 Mpa, bulk density of 878 kg m−3, and 1-h water absorption of 18.5% was fabricated, in compliance with Chinese standard (GB/T 1743.1–2010). The arsenic leaching concentration from the resulting product was considerably lower than Chinese standard (GB 5085.3–2007). Moreover, arsenic volatilization during ceramsite calcination was insignificant, and the vast majority of arsenic remained in resulting ceramsite. A geochemical speciation model developed for the multiple component system in ceramsite suggested that FeAsO4, Ca5(OH) (AsO4)3, and hydrous ferric oxide adsorption are the primary mechanisms retaining arsenic in ceramsite. Additionally, based on density functional theory calculations and biotoxicity test, the binding site of arsenic atom on mineral components and the environmental safety of ceramsite was determined and evaluated. © 2023

关键词： Heavy metals

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Activation Rate-Dependent Reconstruction of Co-Mofs for Efficient Coooh Conversion in Oxygen Evolution Reaction

SSRN

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SSRN 2025年

作者： Feng, Youlei Jia, Jinzhi Zou, Zehua Lin, Youxiu Zheng, Xuan Lai, Wenqiang Chen, Xiaoping Wang, Qingxiang Xu, Cailing Fujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology Fujian Provincial Key Laboratory of Pollution Monitoring and Control College of Chemistry Chemical Engineering and Environment Minnan Normal University Zhangzhou363000 China State Key Laboratory of Applied Organic Chemistry Laboratory of Special Function Materials and Structure Design of the Ministry of Education College of Chemistry and Chemical Engineering Lanzhou University Lanzhou730000 China

The oxygen evolution reaction (OER) is a critical component in the fields of aqueous electrocatalysis, of which the real active species always need to be activated under the electrochemical conditions. However, the activation rate is frequently overlooked, critically associated with the reconstruction efficiency at the initial stage of OER. Herein, three analogous Co-MOFs were observed to exhibit different activation rates, involving with the triggering of reconstruction, the dissociation of organic ligands and the losing of Co nodes. The expedited activation rate can significantly enhance the conversion efficiency from Co-MOFs to CoOOH species, thereby improving the utilization of Co element. These findings focused on the activation rate are expected to help understand the fundamental principles of electrocatalyst reconstruction. © 2025, The Authors. All rights reserved.

关键词： Activation energy

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