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Needle-like PVP@Ce/Zr-MOFs for the highly efficient selective of fluoride and phosphate from aqueous solution

Separation and Purification Technology 2025年 371卷

作者： Liu, Ruilai Song, Jiangyan Zhang, Ziyi Ji, Lichang Yang, Weisen Zhao, Jinyun Jian, Shaoju Hu, Jiapeng Ma, Jie Fujian Provincial Key Laboratory of Eco-Industrial Green Technology Wuyi University Key Laboratory of Green Chemical Technology of Fujian Province University Wuyishan354300 China Research Center for Environmental Functional Materials State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China College of Environment and Safety Engineering Fuzhou University Fuzhou350001 China School of Civil Engineering Kashi University Kashi844000 China

Polyvinylpyrrolidone (PVP) dispersant was added to Ce/Zr metal–organic frameworks (MOFs), forming needle-like PVP@Ce/Zr-MOFs adsorbents via the hydrothermal method. The effects of solution pH, co-existing ions, reaction temperature, and PVP dosage on the performance of fluoride and phosphate elimination from aqueous solution were examined in batch adsorption experiments. The sorption behaviors were also revealed through adsorption thermodynamic and kinetic studies. The PVP@Ce/Zr-MOFs had an outstanding selectivity over a wide pH range. In addition, they selectively adsorbed phosphate and fluoride ions co-existing with common ions in simulated and real wastewater and maintained high efficiency in the existence of other anions. The sorption procedure was depicted with the pseudo-second order model and the Langmuir model. A mechanistic analysis revealed that fluoride and phosphorus were eliminated by PVP@Ce/Zr-MOFs via exchange interaction with hydroxide ions, electrostatic interactions with charged particles on the adsorbent surface, and the formation of strong inner-sphere complexes of Zr and Ce ions with the target phosphate and fluoride ions. © 2025 Elsevier B.V.

关键词： Metal ions

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NH2-MIL-101(Fe) and cellulose nanocrystals incorporated catalytic membrane with high flux and tetrabromobisphenol A degradation performance in synergistic oxidation-filtration

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Chemical Engineering Journal 2025年 518卷

作者： Ji, Xin Wu, Zixuan Liu, Yuanhua Kou, Yingwei Li, Xiaodong Zhang, Wei-xian Deng, Zilong State Key Laboratory for Pollution Control and Resource Reuse College of Environmental Science and Engineering Shanghai Institute of Pollution Control and Ecological Security Tongji University 1239 Siping Road Shanghai 200092 China College of Civil Engineering Tongji University 1239 Siping Road Shanghai 200092 China China Shipping Environment Technology (Shanghai) Co. Ltd. Shanghai Ship and Shipping Research Institute 600 Minsheng Road Shanghai 200135 China

The key challenges in catalytic filtration membrane lie in achieving synergistic integration of high permeability, efficient oxidation performance and fouling resistance. NH2-MIL-101(Fe)-cellulose nanocrystal@PVDF (NM-C@PVDF) membranes were fabricated by one-pot phase inversion method. NM-C@PVDF (815.41 L·h⁻¹·m⁻²) had the highest pure water flux compared to other developed membranes, attributed to the rich porous structure, enhanced surface roughness and increased hydrophilicity due to the presence of grafted amino group. Although metal organic frameworks (MOFs) incorporation increased composite hydrophilicity, the retention of tetrabromobisphenol A (TBBPA) by NM-C@PVDF remained superior (44.84 %, only 2.7 % lower than C@PVDF membrane). The retention process was closely associated with hydrophobic interactions, electrostatic repulsions (negative charges between TBBPA and membranes surface) and initial adsorption of MOFs. For mitigating the trade-off effect, the peroxydisulfate (PDS) oxidation was introduced to enhance removal rate by elevating purity water flux. NM-C@PVDF (90.35 %) showed the highest TBBPA degradation rate due to the activation of PDS by free radicals and non-radicals pathways (pH = 7 and PDS of 5 mM). The susceptible atoms of TBBPA and possible reaction pathways were predicted based on density functional theory (DFT) calculations and Liquid Chromatography-Mass Spectrometry (LC-MS) analysis. The toxicity of intermediate product, simulated by Toxicity Estimation Software Tool (T.E.S.T.), gradually decreased along with the degradation process. In addition, NM-C@PVDF maintained 92.49 % efficiency for TBBPA after five degradation cycles. This work offered an innovative strategy for engineering catalytic filtration membrane and the demonstrated removal performance of bifunctional membrane may guide future developments in advanced water purification technologies.

关键词： Cellulose nanocrystals Fe-based mental organic frameworks Membrane Peroxydisulfate Tetrabromobisphenol A

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Hormetic mechanism of sulfonamides on Aliivibrio fischeri luminescence based on a bacterial cell-cell communication

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Chemosphere 2019年 215卷 793-799页

作者： Yao, Zhifeng Wang, Dali Wu, Xiaodan Lin, Zhifen Long, Xi Liu, Ying State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China School of Environment Jinan University Guangzhou510632 China College of Marine Ecology and Environment Shanghai Ocean University Shanghai201306 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China Shanghai Key Lab of Chemical Assessment and Sustainability Shanghai China State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental Sciences Chinese Academy of Sciences China

Hormesis is a biphasic dose-response model with low-dose stimulation and high-dose inhibition. The mechanism for hormesis remains inconclusive, although it is becoming a central concept in toxicology. In this paper, the hormetic mechanism of sulfachloropyridazine (SCP) on Aliivibrio fischeri (A. fischeri) luminescence was explored by investigating into the interference of SCP with the bacterial quorum sensing (QS) communications. It was revealed that the SCP-induced hormesis on luminescence was due to its action on LitR – a key protein that connects lux and ain QS communications in A. fischeri. It was suggested SCP acted on LitR proteins to change its active forms, which subsequently induced hormetic effects on luxR (QS signal receptor) and thereby the luminescence. It is the first time that the hormetic mechanism based on bacterial QS was proposed, which provides a novel insight into the essence of the hormesis on A. fischeri luminescence. © 2018 Elsevier Ltd

关键词： Luminescence

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Quantitative analysis of PBAT microplastics and their degradation products in soil by mass spectrometry

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Eco-Environment & Health 2025年

作者： Zhuyao Hua Ya Li Xin He Fengxiao Zhu Sha Chang Jijie Kong Changyin Zhu Chao Wang Shiyin Li Huan He Cheng Gu School of Environment Nanjing Normal University Nanjing 210023 China Co-Innovation Center for the Sustainable Forestry in Southern China College of Ecology and Environment Nanjing Forestry University Nanjing 210037 China Key Laboratory of Environmental Remediation and Ecological Health of Ministry of Industry and Information Technology Jiangsu Province Ecology and Environment Protection Engineering Research Center of Groundwater Pollution Prevention and Control Jiangsu Environmental Engineering Technology Co. Ltd. Nanjing 210019 China State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Nanjing 210023 China

Global production of biodegradable plastics is increasing, but the degradation behavior of microplastics derived from these items in soil is still scarcely reported. In this study, a method for quantifying soil poly(butylene adipate-co-terephthalate) (PBAT) microplastics was developed, and their degradation behavior in three different soils was investigated. PBAT was quantified by analyzing the content of the monomer terephthalic acid (TPA) released during thermally assisted alkali hydrolysis, using liquid chromatography-mass spectrometry (LC-MS). For alkali hydrolysis, the use of capped bottle, water bath (90 °C for 30 min), and ultrasonication (100 kHz for 15 min) allowed for high-throughput sample processing in comparison to the use of round-bottom flask, reflux condenser, and stirring heating mantle. After 150 days, 10.8%–11.0% of PBAT microplastics were degraded in the acidic and neutral soils, while 17.1% were degraded in the alkaline soil, in line with the greatest lipase activity changes in the alkaline soil. This may be due to the fact that alkaline conditions favor initial depolymerization of PBAT, facilitating subsequent microbial attack. PBAT degradation products were also monitored, using solvent extraction combined with LC-MS and gas chromatography-mass spectrometry analysis. It was found that butanediol (up to 1580 μg/kg) accumulated to a higher level than TPA (about 50 μg/kg), especially in acidic and alkaline soils. Overall, this study, for the first time, precisely quantified the degradation of PBAT microplastics in soil. Further study is needed to better understand the fate of biodegradable microplastics in the soil environment and whether they will persist.

关键词： PBAT Microplastics Soil Quantification Metabolite

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Occurrence, sources and Risk Assessment of Pyrethroid Insecticides in Surface Water and Tap Water from Taihu Lake, China

SSRN

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SSRN 2022年

作者： Wang, Rui Zhang, Shengwei Xiao, Kaiyan Cai, Minghong Liu, Hongling Ministry of Natural Resources Key Laboratory for Polar Science Polar Research Institute of China 451 Jinqiao Road Shanghai 200136 China School of Oceanography Shanghai Jiao Tong University 1954 Huashan Road Shanghai 200030 China Antarctic Great Wall Ecology National Observation and Research Station Polar Research Institute of China 1000 Xuelong Road Shanghai 201209 China State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Nanjing210023 China State Key Laboratory of Water Environment Simulation School of Environment Beijing Normal University Beijing100875 China Department of Municipal and Environmental Engineering School of Civil Engineering Beijing Jiaotong University Beijing100044 China

Pyrethroid insecticides are among the most widely used insecticides worldwide and pose a serious threat to human health and the environment. In this study, we applied high-throughput organic analysis testing combined with high-volume solid-phase extraction (Hi-throat/Hi-volume SPE) to investigate the occurrence of 11 pyrethroid insecticides in lake water (n=37), tributary river water (n=15), and tap water (n=6) in the Taihu Lake Basin. Permethrin was determined to be the major contributing pyrethroid insecticide (100%). The concentrations of pyrethroid insecticides from different areas of the lake were as follows: southern (S023–S26, mean 2,331 ng/L) > eastern (S01–S04 and S32–S37, mean 1,664 ng/L) > western (S17–S22 and S28–S31, mean 1,459 ng/L) > northern (S05–S16, mean 821.1 ng/L). The results of the principal component analysis with multiple linear regression indicated that landscape maintenance, agricultural cultivation, and livestock breeding were the main sources of pyrethroid insecticides in the Taihu Lake surface water. Runoff input plays an important role in the accumulation of pyrethroid insecticides in Taihu Lake, and surrounding rivers contribute 2,292 kg of pyrethroid insecticides to Taihu Lake annually. The risk assessment results indicate that pyrethroid insecticides present a high risk to both the ecological environment and surrounding human populations and must be taken seriously. Further, the use of pyrethroid insecticides in the Yangtze River Delta region needs to be controlled. This is the first study in China to report the residue levels in water sources and tap water. © 2022, The Authors. All rights reserved.

关键词： Risk assessment

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Foliar spraying of different size SiO 2 nanoparticles affected phenanthrene accumulation in amaranth ( Amaranthus tricolor L.): A metabolomics insight

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Pedosphere 2024年

作者： Yue CAI Lirong PU Lianzhou SHEN Xinghao WANG Zhaoyue SUN Guodong FANG Dongmei ZHOU Yunjiang YU Juan GAO Institute of Soil Science Chinese Academy of Sciences Nanjing 210008 (China) University of Chinese Academy of Sciences-Nanjing College Nanjing 211135 (China) State Environmental Protection Key Laboratory of Environmental Health Risk Assessment South China Institute of Environmental Science Ministry of Ecology and Environment Guangzhou 510655 (China) State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Nanjing 210023 (China)

Silica nanoparticles (nSiO 2 ) have attracted considerable attention in agricultural practices. However, their effects on polycyclic aromatic hydrocarbon (PAH) accumulation in plants remain largely unknown. Thus, this issue was tracked here with a 30-d pot experiment with foliar spraying different sizes of nSiO 2 (100 mg L -1 , 10 mL) on Amaranthus tricolor L. (amaranth). Results showed that 30 nm and 100 nm nSiO 2 increased phenanthrene (PHE) contents in amaranth leaves by 242% ± 88.4% and 158% ± 29.6%, respectively, which was more significant than 2 µm particles (96.0% ± 29.2%). Metabolomics indicated that compared to nSiO 2 , 2 µm SiO 2 more significantly boosted oxidative defense in amaranth leaves, enhanced cell membrane fluidity, and upregulated amino acid metabolism, glycolysis, and gluconeogenesis. In addition, the upregulation of discriminating metabolites was the most significant in 2 µm SiO 2 -treatment, followed by 100 nm and 30 nm. This is mainly because nSiO 2 promoted amaranth growth and decreased average PHE content per unit biomass, namely “dilute effect”. Thus, slighter metabolic disturbances were observed in 30 nm and 100 nm SiO 2 -treated group. The present study revealed the possibility of PAHs accumulation enhancement in vegetables with nSiO 2 foliar spayed. The results of this study provide theoretical guidance regarding to particle size selection for the safe agricultural application of nSiO 2 in PAHs-contaminated areas.

关键词：

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Emerging pollutants–part i: Occurrence, fate and transport

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Water Environment Research 2018年第10期90卷 1301-1322页

作者： Zhao, Yanting Ye, Lin Zhang, Xu-Xiang State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Nanjing210023 China

The presence of emerging pollutants (EPs) in water poses a potentially new and serious challenge on human health. Here, we reviewed the relevant literatures published in 2017, summarized the occurrence, environmental fate, transport and impacts of EPs in the environment, and analyzed the environmental toxicity of personal care products (PPCPs), endocrine disrupting chemicals (EDCs), antibiotics and antibiotic resistance genes (ARGs), nanoparticles (NPs) and nanomaterials (NMs). This — review mainly focused on the occurrence surveys on surface water and the associations between exposure to EPs and toxicity of testing organisms. The control strategies and regulation for EPs based on the screening and monitoring methods were also discussed. Future efforts should be made to establish a comprehensive framework to study the adverse effects of EPs on organisms and new policies and legislations should be developed to control the release of hazardous EPs to the environment. © 2018 Water Environment Federation.

关键词： Toxicity

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controlling Nucleophilic Emerging Organic Contaminants (Eocs) Using an Inorganic Oxidizing Coagulant (Ioc) Based on the Synergistic Oxidation-Induced Coagulation Mechanisms

SSRN

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SSRN 2024年

作者： Wang, Lili Xu, Weiying Xu, Zhenghe Zhu, Yuanji Song, Yan Wang, Dongsheng Xin, Xiaodong Jia, Ruibao Xu, Xing School of Water Conservancy and Environment University of Jinan No. 336 Nanxinzhuang Western Road Shandong Jinan250022 China Key Laboratory of Drinking Water Science and Technology Research Center for Eco-Environmental Science Chinese Academy of Science No. 18 Shuangqing Road Beijing100085 China Economic & Technology Research Institute of State Grid Shandong Electric Power Company No. 111 Weishi Road Shandong Jinan250021 China Shandong Province City Water Supply and Drainage Water Quality Monitoring Center No 5111 Aoti Middle Road Shandong Jinan250013 China Department of Environmental Engineering College of Environmental & Resource Sciences Zhejiang University No 866 Yuhangtang Road Zhejiang Hangzhou310013 China Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and Engineering Shandong University Shandong Qingdao266237 China Shandong Jianzhu University China

Coagulation is not effective in treatment of emerging organic contaminants (EOCs) contaminated water and wastewater, and many researches focus on the hybrid technologies. In this study, a multifunctional inorganic oxidizing coagulant (IOC) was developed by a simple alkaline co-polymerization method to increase the efficiency and feasibility of coagulation in elimination of low molecular weight (MW) organic compounds, which were demonstrated by eight kinds of representative EOCs. The IOC present exceptional removal capabilities for hydrophilic with low logKow and nucleophilic (high NI) EOCs, like sulfamethazine (SMZ), tetracycline (TC), and ciprofloxacin (CIP), achieving removal efficiencies of 45-95%. The dynamic coagulation investigation conducted through continuous monitor on floc formation and growth demonstrated that large floc played minor role in EOCs removal. Instead, an obvious positive correlation between removal efficiency (REOCs) and floc growth rate (Sfloc), which was associated with the reactivity of EOCs with coagulant, was observed. Combined with the electron paramagnetic resonance (EPR) and ultra-high-performance liquid chromatography high-resolution mass spectrometry (UHPLC-HRMS) results, an innovative coagulation mechanism for EOCs abatement by IOC, namely oxidation-induced coagulation was proposed. Oxidizing agent in IOC promoted the formation of activate intermediates through nonradical pathway, which were more prone to complexation with aluminum than their original condition. Comparatively, traditional charge neutralization, adsorption and sweeping mechanisms involved in the aluminum sulfate (AS) and poly-aluminum chloride (PACl) coagulation systems, which generally lead to large but invalid flocs, turned out to inapplicable to EOCs removals. This study provides a novel strategy and inorganic coagulant for EOCs-contained water and wastewater treatments based on the oxidation-induced complexation mechanism, which was demonstrated to be a promisin

关键词： Aluminum chloride

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Efficient Treatment of the Sweet Potato Starch Wastewater by Enhanced Flocculation–Coagulation of Environmentally Benign Materials

SSRN

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SSRN 2022年

作者： Zhang, Yalan Li, Meng Zhang, Guihai Liu, Wei Xu, Jinying Tian, Yuansong Wang, Yinfeng Xie, Xingyue Peng, Zhiqi Li, Aimin Zhang, Ru Wu, Daishe Xie, Xianchuan Key Laboratory of Poyang Lake Environment and Resource Utilization Ministry of Education School of Resource and Environment Nanchang University Nanchang330031 China State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Nanjing210023 China Wireline Product Operation ZTE Corporation Nanjing210023 China Nanjing University Yancheng Academy of Environment Protection Technology and Engineering Nanjing210023 China Jiangxi Nanxin Environmental Protection Technology Co. LTD Jiujiang City of Jiangxi Province 330300 China School of Materials and Chemical Engineering Pingxiang University Pingxiang337000 China

Sweet potato starch wastewater from rural areas of China is in urgent need of a new efficient and environmental-friendly method for proper treatment, because it contains high-concentration organic pollutants, with a great impact on water quality, and also most of it is treated in a distributed manner. In this study, bentonite was selected from four kinds of clay minerals (i.e. kaolin, zeolite, attapulgite and bentonite) as coagulant aids, and chitosan-modified bentonite combined with polyglutamic acid was used for enhanced coagulation treatment for starch wastewater. Among them, bentonite can adsorb soluble pollutants in starch wastewater, chitosan modification can enhance the coagulation effect, and the flocculant of polyglutamic acid is conducive to the removal of particulate matter through bridging effects. The combination of the three can effectively and deeply remove pollutants in starch wastewater. Under the optimal conditions, the removal rates of chemical oxygen demand , total nitrogen, total phosphorus and turbidity can reach 86.2%, 80.3%, 52.3% and 98.2%, respectively, which are far higher than that of the vast majority of coagulants currently reported. Density functional theory calculation has showed that the electrostatic potential around aluminum in bentonite of 14.248 *** -1 is more conducive to the adsorption of negatively charged organic pollutants, and that bentonite has lower adsorption energy ( -1.43 eV) than chitosan and polyglutamic acid, thereby resulting in higher adsorption affinity of bentonite. Mechanistic studies confirmed that the coagulation mechanism includes electrical neutralization and the promotion of efficient collision of clay particles to form flocs . © 2022, The Authors. All rights reserved.

关键词： Flocculation

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Zif-Derived Non-Bonding Co/Zn Coordinated Hollow Carbon Nitride for Enhanced Removal of Antibiotic Contaminants by Perxymonosulfate Activation: Performance and Mechanism

SSRN

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SSRN 2022年

作者： Sun, Yongjun Li, Xi Wang, Shiwen Chen, Pei Xu, Baokang Zhang, Xiao Xu, Yanhua Yu, Yang Zheng, Huaili Yu, Peng Zhou, Ru School of Environmental Science and Engineering Nanjing Tech University Nanjing211816 China Key Laboratory of Industrial Pollution Control and Resource Reuse of Jiangsu Province College of Environmental Engineering Xuzhou University of Technology Xuzhou221000 China College of Safety Science and Engineering Nanjing Tech University Nanjing211816 China Graduate School at Shenzhen Tsinghua University Shenzhen518055 China Key laboratory of the Three Gorges Reservoir Region's Eco-Environment State Ministry of Education Chongqing University Chongqing400045 China College of Urban Construction Nanjing Tech University Nanjing211816 China

Co-Zn-N-C catalyst (MCZC) with neighboring Co and Zn pairs anchored on hollow carbon nitride was constructed by the direct etching of zeolitic imidazolate frameworks (ZIFs) assembled with Co and Zn. Adequate characterizations and density functional theory (DFT) studies confirmed the successful construction of non-bonding Co and Zn pairs with enhanced electron transfer on Co sites by adjacent Zn sites. Based on the synergy of adjacent Co and Zn atom pairs, the MCZC/Perxymosulfate (PMS) system achieved 99.6% Tetracycline (TC) degradation in 24 min with a mineralization rate of 55.8% and PMS decomposition efficiency of 73.1%. DFT calculation based on the Fukui index identified the sites susceptible to attack by the active species. TC degradation pathways could be inferred, and reduced toxicity of intermediates was observed. This work provides new insights into the design of MOF-derived bimetallic catalysts and the importance of the interaction between adjacent metal active sites to catalytic performance. © 2022, The Authors. All rights reserved.

关键词： Chemical activation

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