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Leaching kinetics of fluorine during the aluminum removal from spent Li-ion battery cathode materials

Journal of environmental sciences 2024年第4期138卷 312-325页

作者： Shengjie Li Jianxin Zhu research center for eco-environmental sciences Chinese Academy of SciencesBeijing 100085China University of Chinese Academy of sciences Beijing 100049China

The high content of aluminum(Al)impurity in the recycled cathode powder seriously affects the extraction efficiency of Nickel,Cobalt,Manganese,and Lithium resources and the actual commercial value of recycled materials,so Al removal is crucially important to conform to the industrial standard of spent Li-ion battery cathode materials.In this work,we systematically investigated the leaching process and optimum conditions associated with Al removal from the cathode powder materials collected in a wet cathode-powder peeling and recycling production line of spent Li-ion batteries(LIBs).Moreover,we specifically studied the leaching of fluorine(F)synergistically happened along with the removal process of Al,which was not concerned about in other studies,but one of the key factors affecting pollution prevention in the recovery process.The mechanism of the whole process including the leaching of Al and F from the cathode powder was indicated by using NMR,FTIR,and XPS,and a defluoridation process was preliminarily investigated in this study.The leaching kinetics of Al could be successfully described by the shrinking core model,controlled by the diffusion process and the activation energy was 11.14 kJ/mol.While,the leaching of F was attributed to the dissolution of LiPF6and decomposition of PVDF,and the kinetics associated was described by Avrami model.The interaction of Al and F is advantageous to realize the defluoridation to some degree.It is expected that our investigation will provide theoretical support for the large-scale recycling of spent LIBs.

关键词： Al removal F leaching Cathode powder Heating alkali leaching Leaching kinetics

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Field-based evidence for the enrichment of intrinsic antibiotic resistome stimulated by plant-derived fertilizer in agricultural soil

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Journal of environmental sciences 2024年第1期135卷 728-740页

作者： Shihai Liu Ziming Han Dong Zhu Xiao Luan Liujie Deng Liping Dong Min Yang Yu Zhang State Key Laboratory of environmental Aquatic Chemistry Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China State Key Laboratory of Urban and Regional ecology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China State environmental Protection Engineering center for Harmless Treatment and Resource Utilization of Antibiotic Residues Khorgos 835007China University of Chinese Academy of sciences Beijing 100049China

Animal manures have been demonstrated to enhance antibiotic resistance in agricultural soils.However,little is known about the effects of plant-derived fertilizer on soil antibiotic resistome.Herein,metagenomic sequencing was used to investigate the effects of a plantderived fertilizer processed from sugarcane and beet on soil antibiotic resistance genes(ARGs)in a soybean field along crop growth stages.ARG profiles in the soils amended by plant-derived fertilizer were compared with those in the soils amended by chicken manure.The abundance and diversity of total ARGs in the soils amended by plant-derived fertilizer were significantly(P<0.05)elevated at the sprout stage,to a level comparable to that in the manured soils.Whereas,unlike chicken manure mainly introducing manure-borne ARGs to soil,the plant-derived fertilizer was indicated to mainly enrich multidrug resistance genes in soil by nourishing indigenous bacteria.ARGs with abundances in amended soils significantly(P<0.05)higher than in unamended soils at the sprout stage of soybean were considered as enriched ARGs.Decrease in the abundance of the enriched ARGs was observed in both the amended soils from the sprout to the harvest.Network analysis further identified Proteobacteria and Bacteroidetes as the primary bacterial taxa involved in the temporal variation of the enriched ARGs in the soils amended by plant-derived fertilizer,while in manured soils were Firmicutes and Actinobacteria.As revealed by multivariate statistical analyses,variation of the enriched ARGs in the soils amended by plant-derived fertilizer was majorly attributed to the response of co-occurred bacteria to depleting nutrients,which was different from the failed establishment of manure-borne bacteria in the manured soils.Our study provided field-based evidence that plant-derived fertilizer stimulated the intrinsic antibiotic resistome,and proposed attention to the un-perceived risk since some clinically relevant ARGs originate and evolve from natural resistome.

关键词： Organic fertilizer Intrinsic antibiotic resistance Indigenous bacteria Metagenomic sequencing

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Characteristics and sources of peroxyacetyl nitrate(PAN)in the rural North China Plain:Results from1-year continuous observations

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Journal of environmental sciences 2024年第4期138卷 719-731页

作者： Xin Liu Xiaowei He Chenglong Zhang Yifei Song Shuyang Xie Chengtang Liu Pengfei Liu Yuanyuan Zhang Yujing Mu Junfeng Liu research center for eco-environmental sciences Chinese Academy of SciencesBeijing 100085China University of Chinese Academy of sciences Beijing 100049China

Peroxyacetyl nitrate(PAN)is an important photochemical pollutant in the troposphere,whereas long-term measurements are scarce in rural areas in North China Plain(NCP),resulting in unclear seasonal variations and sources of PAN in rural NCP.In this study,we conducted a 1-year observation of PAN during 2021-2022 at the rural NCP site.The average concentrations of PAN were 1.10,0.75,0.65,and 0.88 ppbv in spring,summer,autumn,and winter,respectively,with a 1-year average of 0.81±0.60 ppbv.Calculations indicate that the loss of PAN through thermal decomposition in summer accounts for 43.2% of the total formed PAN,which is an important reason for the low concentration of PAN in summer.We speculate that since the correlation between PAN and O_(3) in winter is significantly lower than that in other seasons,the observed regional transport of PAN cannot be ignored in winter.Through budget analysis,regional transport accounted for 12.8% and 55.9% of the observed PAN on the spring and winter pollution days,respectively,which showed that regional transport played key roles during the photochemical pollution of the rural NCP in winter.The potential source contribution function revealed that the transported PAN mainly comes from southern Hebei in spring.In winter,the transported PAN was mainly from Langfang,Hengshui,and southern Beijing.Our findings may aid in understanding PAN variations in different seasons in rural areas and highlight the impact of regional transport on the PAN budget.

关键词： Photochemical pollution Peroxyacetyl nitrate(PAN) Seasonal variations Regional transport Rural area

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Chronic administration of triclosan leads to liver fibrosis through hepcidin-ferroportin axis-mediated iron overload

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Journal of environmental sciences 2024年第3期137卷 144-154页

作者： Jing Liu Lecong Zhang Fang Xu Ping Zhang Yang Song College of eco-environmental Engineering Guizhou Minzu UniversityGuiyang 550025China The Institute of Karst Wetland ecology Guizhou Minzu UniversityGuiyang 550025China State Key Laboratory of environmental Chemistry and ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

Triclosan(TCS)has been manufactured as an antibacterial compound for half a century.Currently,it is widely used in various personal care products;however,its potential adverse effects raise a lot of attention.Here,we create a long-term oral administration mouse model and identify the corresponding hepatotoxicity of TCS.We discover that daily intragastric administration of 10 mg/kg TCS to mice for 12 weeks results in severe hepatic fibrosis.Further study displays that hepatic iron increased 18%,23%and 29%upon oral TCS treatment for4,8 and 12 weeks,respectively.Accompanied by hepatic iron variation,splenic and duodenal iron are increased,which indicates systemic iron disorder.Not only excessive iron accumulated in the liver,abnormal hepatic malondialdehyde,prostaglandin synthase 2 and glutathione peroxidase 4 are pointed to ferroptosis.Additional study uncovers that hepcidin expression increases 7%,10%,4%in serum and 2.4-,4.8-,and 2.3-fold on transcriptional levels upon TCS exposure for 4,8 and 12 weeks,individually.Taken together,the mice in the TCS-treated group show disordered systemic iron homeostasis via the upregulated hepatic hepcidin-ferroportin axis.Meanwhile,both hepatic iron overload(systemic level)and hepatocyte ferroptosis(cellular level)are accused of TCS-induced liver fibrosis.Ferriprox■,an iron scavenger,significantly ameliorates TCS-induced liver fibrosis.In summary,this study confirms the impact of TCS on liver fibrosis;a critical signal pathway is also displayed.The significance of the current study is to prompt us to reevaluate the“pros and cons”of TCS applications.

关键词： Triclosan Iron metabolism Hepcidin Hepatotoxicity Liver fibrosis

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Transcriptomic analysis reveals the effects of maternal exposure to bisphenol AF on hypothalamic development in male neonatal mice

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Journal of environmental sciences 2024年第7期141卷 304-313页

作者： Lin Lv Yuanyuan Li Xuanyue Chen Zhanfen Qin State Key Laboratory of environmental Chemistry and ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of sciences Beijing 100049China

Fragmented data suggest that bisphenol AF(BPAF),a chemical widely used in a variety of products,might have potential impacts on the hypothalamus.Here,we employed male neonatal mice following maternal exposure to explore the effects of low-dose BPAF on hypothalamic development by RNA-sequencing.We found that maternal exposure to approximately 50μg/(kg·day)BPAF from postanal day(PND)0 to PND 15 altered the hypothalamic transcriptome,primarily involving the pathways and genes associated with extracellular matrix(ECM)and intercellular adhesion,neuroendocrine regulation,and neurological processes.Further RNA analysis confirmed the changes in the expression levels of concerned genes.Importantly,we further revealed that low-dose BPAF posed a stimulatory impact on pro-opiomelanocortin(POMC)neurons in the arcuate nucleus of the hypothalamus and induced the browning of inguinal white adipose tissue.All findings indicate that developmental exposure to low-dose BPAF could interfere with hypothalamic development and thereby lead to alterations in the metabolism.Interestingly,5000μg/(kg·day)BPAF caused slighter,non-significant or even inverse alterations than the low dose of 50μg/(kg·day),displaying a dose-independent effect.Further observations suggest that the the dose-independent effects of BPAF might be associated with oxidative stress and inflammatory responses caused by the high dose.Overall,our study highlights a risk of low-dose BPAF to human neuroendocrine regulation and metabolism.

关键词： Bisphenol AF Hypothalamus Transcriptomic alteration Pro-opiomelanocortin(POMC)neurons White adipose tissue browning

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Developing a novel quantitative parameter for characterizing spatial distribution of fish following exposure to chemicals and wastewater:Behavioral Gini coefficient

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Journal of environmental sciences 2024年第7期141卷 129-138页

作者： Xuanyue Chen Yuanyuan Li Zhanfen Qin State Key Laboratory of environmental Chemistry and ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of sciences Beijing 100049China

While the spatial distribution pattern of fish is increasingly used for toxicological test o chemicals or wastewater,no ideal parameter is available for quantitative assessment of spa tial distribution,especially uneven distribution with multiple hotspots.Here,to develop a quantitative assessment parameter for spatial distribution,the zebrafish were exposed to ethanol,pentylenetetrazole(PTZ),paraquat dichloride(paraquat)and wastewater,followed by a behavioral test in a narrow tank.Behavioral data was acquired and analyzed by id Tracker and MATLAB.By comparing the effects of all treatments on behavior parameters we confirmed that the spatial distribution was more easily altered rather than general loco motor parameters,e.g.0.7-70 mg/L PTZ and 5-20 mg/L paraquat being effective for altering spatial distribution but having little effects on general locomotor parameters.Based on the heatmap,i.e.,the cumulative proportion of grids and that of frequency in grids,we calcu lated the behavioral Gini coefficient(G_(b))for quantitative assessment of fish spatial distri bution.The Gini coefficient ranged from zero to 1,with larger values meaning poorer even ness of spatial distribution.Of note,G_(b)showed smaller coefficient of variations(CV)with3%-19%between replicate tanks in all treatments than the highest frequency(4%-79%),dis playing well robustness.Especially,G_(b)addressed the challenge of the complicated heatmap with multiple hotspots.Overall,the behavioral Gini coefficient we established is an idea parameter to quantitatively assess spatial distribution of fish shoal,which is expected to be applied in toxicity testing for chemicals and wastewater and automatic quality monitoring for surface water and aquaculture water.

关键词： Zebrafish Behavioral test Spatial distribution Behavioral Gini coefficient

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Less pressure contributes to gravity-driven membrane ultrafiltration with greater performance:Enhanced driving efficiency and reduced disinfection by-products formation potential

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Journal of environmental sciences 2024年第3期137卷 407-419页

作者： Xiaoting Wu Yufei Li Zhaoyang Su Long Tian Muhammad Saboor Siddique Wenzheng Yu Colleges of Forestry Northeast Forestry UniversityHarbin 150040China State Key Laboratory of environmental Aquatic Chemistry Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

Gravity-driven membrane(GDM)systems have been well developed previously;however,impacts of driving(i.e.,transmembrane)pressure on their performance received little attention,which may infuence GDM performance.In this study,we evaluated 4 GDM systems via altering the transmembrane pressure from 50 mbar to 150 mbar with 2 groups,treating surface water in Beijing,China.Results showed that less driving pressure was more favorable.Specifically,compared to groups(150 mbar),groups under a pressure of 50 mbar were found to have greater normalized permeability and lower total resistance.During the whole operation period,the quality of effuents was gradually improved.For example,the removal efficiency of UV254was significantly improved;particularly,under low driving pressure,the removal efficiency of UV254in PES GDM system increased by 11.91%,as compared to the corresponding system under high driving pressure.This observation was consistent with the reduction on disinfection by-products(DBPs)formation potential;groups under 50 mbar achieved better DBPs potential control,indicating the advantages of lower driving pressure.Biofilms were analyzed and responsible for these differences,and distinct distributions of bacteria communities of two GDM systems under 50 and 150 mbar may be responsible for various humic-like substances removal efficiency.Overall,GDM systems under less pressure should be considered and expected to provide suggestions on the design of GDM systems in real applications.

关键词： Ultrafiltration Gravity driven operation Membrane fouling Biofilms Disinfection by-products

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Understanding the initial use stage of cement mortar lining in drinking water distribution systems:Silicon and aluminum as stability indicators

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Journal of environmental sciences 2024年第1期135卷 495-505页

作者： Qiaozhi Liu Yuan Zhuang Guiwei Li Yao Zhang Marc A.Edwards Baoyou Shi Key Laboratory of Drinking Water science and Technology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of sciences Beijing 100049China Civil and environmental Engineering Virginia TechBlacksburgVA 24061USA

The cement mortar lining(CML)of commonly used ductile iron pipes can severely deteriorate the drinking water quality at the initial stage of use,but the behavioral characteristics of different elements release from the CML in this stage is still unclear.In this study,dynamic immersion experiments with new cement mortar lined ductile iron pipe reactors were conducted under different feed water hardness and alkalinity conditions.The results showed that the release of alkaline substances from the CML at the initial stage of use could strongly influence the pH of water,which consequently greatly impacted the release/precipitation behaviors of calcium,aluminum and silicon.The pH and aluminum concentration of the effluent water could reach 11.5 and 700μg/L within 24 hr of hydraulic retention time,respectively,under conditions of relatively lower hardness and alkalinity.Due to the pH elevation,calcium carbonate precipitation could occur even at much lower feed water alkalinity.Whereas the aluminum and silicon could keep release from the CML in soluble form at different hardness and alkalinity levels,and their release rate depended on the amount of calcium carbonate precipitation.Thus,aluminum and silicon were more suitable as indicators of the corrosion intensity at the initial stage of CML use rather than the traditional calcium carbonate precipitation potential.Appropriate feed water hardness and alkalinity levels for mitigating the initial intense corrosion of CML were proposed:hardness>40 mg/L(CaCO_(3)),alkalinity>100 mg/L(CaCO_(3)).

关键词： Cement mortar lining Hardness Alkalinity Elemental release Drinking water supply

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Context‑dependent antioxidant defense system(ADS)‑based stress memory in response to recurrent environmental challenges in congeneric invasive species

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Marine Life science & Technology 2024年第2期6卷 315-330页

作者： Hanxi Li Xuena Huang Aibin Zhan research center for eco-environmental sciences Chinese Academy of SciencesBeijing 100085China University of Chinese Academy of sciences Beijing 100049China

Marine ecosystems are facing escalating environmental fluctuations owing to climate change and human activities,imposing pressures on marine species.To withstand recurring environmental challenges,marine organisms,especially benthic species lacking behavioral choices to select optimal habitats,have to utilize well-established strategies such as the antioxidant defense system(ADS)to ensure their survival.Therefore,understanding of the mechanisms governing the ADS-based response is essential for gaining insights into adaptive strategies for managing environmental challenges.Here we conducted a com-parative analysis of the physiological and transcriptional responses based on the ADS during two rounds of'hypersalinity-recovery'challenges in two model congeneric invasive ascidians,Ciona robusta and C.savignyi.Our results demonstrated that C.savignyi exhibited higher tolerance and resistance to salinity stresses at the physiological level,while C.robusta demonstrated heightened responses at the transcriptional level.We observed distinct transcriptional responses,particularly in the utilization of two superoxide dismutase(SOD)isoforms.Both Ciona species developed physiological stress memory with elevated total SOD(T-SOD)and glutathione(GSH)responses,while only C.robusta demonstrated transcriptional stress memory.The regulatory distinctions within the Nrf2-Keap1 signalling pathway likely explain the formation disparity of transcriptional stress memory between both Ciona species.These findings support the'context-dependent stress memory hypothesis',emphasizing the emergence of species-specific stress memory at diverse regulatory levels in response to recurrent environmental challenges.Our results enhance our understanding of the mechanisms of environmental challenge manage-ment in marine species,particularly those related to the ADS.

关键词： Antioxidant defense Ascidian Biological invasion environmental stress Stress memory

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In-situ sludge reduction based on Mn^(2+)-catalytic ozonation conditioning:Feasibility study and microbial mechanisms

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Journal of environmental sciences 2024年第1期135卷 185-197页

作者： Haozhe Huang Tingting Wei Hui Wang Bing Xue Sisi Chen Xiankai Wang Haibin Wu Bin Dong Zuxin Xu College of environmental science and Engineering Tongji UniversityShanghai 200092China YANGTZE eco-Environment Engineering research center China Three Gorges CorporationBeijing 100038China

To improve the sludge conditioning efficiency without increasing the ozone dose,an in-situ sludge reduction process based on Mn^(2+)-catalytic ozonation conditioning was proposed.Using ozone conditioning alone as a control,a lab-scale sequencing batch reactor coupled with ozonated sludge recycle was evaluated for its operating performance at an ozone dose of 75 mg O_(3)/g VSS and 1.5 mmol/L Mn^(2+)addition.The results showed a 39.4%reduction in MLSS and an observed sludge yield of 0.236 kg MLSS/kg COD for the O_(3)+Mn^(2+)group compared to the O_(3)group (15.3%and 0.292 kg MLSS/kg COD),accompanied by better COD,NH_(4)^(+)-N,TN and TP removal,improved effluent SS and limited impact on excess sludge properties.Subsequently,activity tests,BIOLOG eco microplates and 16S rRNA sequencing were applied to elucidate the changing mechanisms of Mn^(2+)-catalytic ozonation related to microbial action:(1) Dehydrogenase activity reached a higher peak.(2) Microbial utilization of total carbon sources had an elevated effect,up to approximately 18%,and metabolic levels of six carbon sources were also increased,especially for sugars and amino acids most pronounced.(3) The abundance of Defluviicoccus under the phylum Proteobacteria was enhanced to 12.0%and dominated in the sludge,they had strong hydrolytic activity and metabolic capacity.Denitrifying bacteria of the genus Ferruginibacter also showed an abundance of 7.6%,they contributed to the solubilization and reduction of sludge biomass.These results could guide researchers to further reduce ozonation conditioning costs,improve sludge management and provide theoretical support.

关键词： Activated sludge In-situ reduction Catalytic ozonation conditioning Dehydrogenase activity Carbon source utilization Microbial community

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