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Thiol/Nitrogen Functionalized Fe3o4@Zif-8-Dmtd by One-Pot Post Coordination Modulation for Efficient and Rapid Removal of Trace Heavy Metals from Drinking Water

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SSRN 2022年

作者： Zhang, Yu Zheng, Hong Zhang, Pengyi Zuo, Qi Zhang, Baichao Ren, Xueying Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral Materials School of Materials Science and Technology China University of Geosciences Beijing100083 China State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China

The deep purification of trace heavy metals in drinking water is of great significance and has received considerable attention worldwide. The thiol/nitrogen functionalized magnetic ZIF-8 adsorbent (Fe3O4@ZIF-8-DMTD) using a novel one-pot post coordination modulation method at room temperature could effectively adsorb trace heavy metals from drinking water through cooperating with the abundant functional groups and surface charges. The negative surface charges promoted the rapid accumulation of trace heavy metals on the surface of the adsorbent, meanwhile, the abundant thiol/nitrogen sites contributed to their adsorption, thus the adsorption rate and adsorption capacity of trace heavy metals were greatly improved. For trace Pb(Ⅱ) (150 ppb), the effluent concentration could meet the World Health Organization (WHO) standard (≤ 10 ppb) within 10 s after adsorption by Fe3O4@ZIF-8-DMTD, and the cumulative adsorption capacity that meets WHO standard was 12.11 mg/g. Fe3O4@ZIF-8-DMTD also showed high stability in a broad pH range and excellent adsorption performance in a wide low concentration range. The effluent concentration still could meet the WHO standard when the initial Pb(Ⅱ) concentration was 11.70 ppm, and the corresponding adsorption capacity reached 35.00 mg/g. Moreover, the capture experiments for multiple heavy metals that coexisted in tap water showed that the effluent concentrations of Hg(Ⅱ), Pb(Ⅱ), Cu(Ⅱ), Cd(Ⅱ), Cr(Ⅲ) could be lower than the allowable limits in a few minutes. The adsorbent could also be easily recovered using magnets and regenerated by thiourea solution, which showed great application potential for the purification of trace heavy metals in drinking water. © 2022, The Authors. All rights reserved.

关键词： Adsorption

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Ice-Covered Lakes: Dom Composition, Migration Patterns, and Ion Distribution During Freeze-Thaw Processes

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SSRN 2023年

作者： Feng, Weiying Deng, Yuxin Yang, Fang Li, Tingting Wang, Fu Zhang, Qi Yao, Haipeng Liao, Haiqing School of Materials Science and Engineering Beihang University Beijing100191 China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences Beijing100012 China State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China School of Electronic Engineering Beijing University of Posts and Telecommunications Beijing100876 China

During the freeze-thaw processes of ice-covered lakes, DOM undergoes enrichment, dispersion, and filtration;however, mechanisms underlying these processes and their impacts on lake pollution processes remain unclear. Therefore, this study investigates the distribution of DOM components and elucidate the impact of ice-layer sieving on its mechanisms in sub-ice water and sediments. Study found: Sedimentary DOM is primarily composed of four categories of fluorescent substances, namely tryptophan-like, tyrosine-like, terrigenous, and endogenous humic-like. The first two components together constitute over 60% of total, primarily originating from biogenic endogenous processes such as phytoplankton and bacterial activity. Functional groups in sedimentary DOM contain phosphorus- or sulfur-based groups. However, in the urban lake, exhibited a higher abundance of alcohol and phenol groups compared with the macrophytic lake, which can generate –OH, methyl, and methylene groups. During the freezing process, fluorescence intensity of humic-like and tryptophan-like in water DOM exhibited an increasing trend, while fluorescence intensity of tyrosine-like showed a decreasing trend. This indicates that ice has an enriching and concentrating effect on tyrosine-like substances. Our findings suggest that ice layer melting exhibits material selectivity, providing a theoretical basis for endogenous pollution control and ecological restoration in ice-covered lakes. © 2023, The Authors. All rights reserved.

关键词： Lakes

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Enhanced Daytime Atmospheric Mercury in the Marine Boundary Layer in the South Oceans

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SSRN 2023年

作者： Tang, Yi Wu, Qingru Wang, Shuxiao Zhang, Min Zhang, Yanxu Qiao, Fangli State Key Joint Laboratory of Environmental Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing100084 China First Institute of Oceanography Key Laboratory of Marine Sciences and Numerical Modelling Ministry of Natural Resources Qingdao266061 China Joint International Research Laboratory of Atmospheric and Earth System Sciences School of Atmospheric Sciences Nanjing University Nanjing210023 China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental Science Beijing100012 China

Understanding the spatial and temporal variations of atmospheric mercury (Hg) in the marine boundary layer could advances our knowledge on ocean evasion of Hg. Here, we conducted continuous measurement of total gaseous mercury (TGM) in the marine boundary layer along a round-the-world cruise from August 2017 to May 2018, with the maximum and minimum observed in Southern Indian Ocean (1.29±0.22 ng m-3) and Southern Atlantic Ocean (0.61±0.28 ng m-3), respectively. Enhanced TGM was observed during the daytime with the diurnal amplitude difference reaching its maximum in the range of 0.30-0.37 ng m-3 in Southern Indian Ocean and Southern Ocean. The positive correlation between TGM (R2=0.68-0.92) and hourly solar radiation in each ocean suggested the daytime enhanced TGM was probably driven by Hg photoreduction in seawater after excluding the influence of other meteorological factors. The diurnal amplitude of TGM in the marine boundary layer is impacted by the microbial productivity and the ratio of ultraviolet radiation. Our study highlights that ocean acts as a net TGM source during the daytime in the South Hemisphere and aqueous photoreduction process may play an important role in the biogeochemical cycling of Hg. © 2023, The Authors. All rights reserved.

关键词： Atmospheric boundary layer

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The Co-Removal of Pcdd/Fs by Scr System in a Full-Scale Municipal Solid Waste Incinerator: Transformation and Decomposition Mechanism

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SSRN 2022年

作者： Wang, Pengju Yan, Feng Xie, Feng Cai, Jianjun Shen, Xuehua Wei, Xuankun Huang, Junbin Li, Zhongzheng Zhong, Rigang Zhang, Zuotai School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control Southern University of Science and Technology Shenzhen518055 China Key Laboratory of Municipal Solid Waste Recycling Technology and Management of Shenzhen City Shenzhen518055 China Shenzhen Energy Environment Co. LTD Shenzhen518055 China

Polychlorinated dibenzo-p-dioxins and furans (PCDD/Fs) generated from municipal solid waste (MSW) incineration are considered as the key pollutants, which could pose serious risk to environment and ecology. This study comprehensively investigated the effect of selective catalytic reduction (SCR) system on PCDD/Fs removal, phase distributions, and migration-transformation characteristics of 17 congeners in a full-scale MSW incinerator. The three flue gas samples and two fly ash samples were separately collected for PCDD/Fs analyzing. The results showed that the SCR system reduced the I-TEQ concentrations of PCDD/Fs from 0.135 to 0.010 ng I-TEQ Nm -3 with a remarkable toxicity removal efficiency of 92.6%, through oxidation decomposition over V2O5 -WO3 /TiO2 catalysts and chlorination process of low-chlorinated congeners. In addition, the de novo synthesis observed along the flue between SCR system and stack regenerated unexpected PCDD/Fs, which might enhance the PCDD/Fs emission level. This study verified the three pathways of SCR system on PCDD/Fs removal and inspired operating suggestions of SCR system, i.e., keeping SCR system operated in stable and consistent conditions, regularly replacing V2O5 -WO3 /TiO2 catalysts, and timely cleaning the dusts and inlet materials of SCR system, which would be beneficial to achieving the ultra-low emission of PCDD/Fs in full-scale MSW incinerator. © 2022, The Authors. All rights reserved.

关键词： Organic pollutants

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Uptake of Polycyclic Aromatic Hydrocarbons (Pahs) from Pah–Contaminated Soils to Carrots and Chinese Cabbages Under the Greenhouse and Field Conditions

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SSRN 2024年

作者： Cao, Chun Wu, Yu-Yao Lv, Zhen-Ying Wang, Ji-Wei Wang, Chen-Wen Wang, Jun-Jian Chen, Huan College of Geography and Environmental Science Northwest Normal University Gansu Lanzhou730070 China Key Laboratory of Resource Environment and Sustainable Development of Oasis Gansu Lanzhou730070 China Northwest Institute of Eco-Environment and Resources Chinese Academy of Sciences Lanzhou730000 China University of Chinese Academy of Sciences Beijing100049 China Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control School of Environmental Science and Engineering Southern University of Science and Technology Shenzhen518055 China State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control School of Environmental Science and Engineering Southern University of Science and Technology Shenzhen518055 China Department of Environmental Engineering and Earth Science Clemson University South Carolina29634 United States

Polycyclic aromatic hydrocarbons (PAHs) with the properties of structural stability, semi–volatility, and hydrophobicity are toxic and persistent in environments;thus, their transport and fate in agroecosystems is essential for reducing PAH accumulation in the edible parts of crops. Here, we cultivated cabbages (Brassica pekinensis L.) and carrots (Daucus carota L.) in PAH–contaminated soils under the greenhouse and field conditions. After harvesting, we observed a 9.5–46% reduction in soil ∑PAH concentrations. There were 37% of bioconcentration factors (BCFbs) > 1 and 93% of translocation factors (TFab) > 1, while low–molecular–weight (LMW) PAHs had higher BCFbs than high–molecular–weight (HMW) PAHs. The PAH concentrations showed significant and positive correlations among soils, the belowground parts, and the aboveground parts. The toxicity equivalent concentration (TEQBaP) followed the order of cabbage (greenhouse) > cabbage (field) > carrot (greenhouse) > carrot (field), suggesting potentially higher health risks in cabbage relative to carrot and vegetables under the greenhouse relative to field condition. Our study suggested growing carrots under field conditions as a management strategy for reducing the risks of vegetables grown in PAH–contaminated soils. © 2024, The Authors. All rights reserved.

关键词： Health risks

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Facile Green Preparation of Single- and Two-Component Modified Activated Carbon Fibers for Efficient Trace Heavy Metals Removal from Drinking Water

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SSRN 2022年

作者： Zuo, Qi Zheng, Hong Zhang, Pengyi Zhang, Yu Zhang, Jiejing Zhang, Baichao Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral Materials School of Materials Science and Technology China University of Geosciences Beijing100083 China State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China

Trace heavy metals exist in drinking water, having great adverse effects on human health and making it a huge challenge to remove. Herein, novel materials have been prepared by a simple and green method using single- (polydopamine (PDA) or 2,3-dimercaptopropanesulfonic sodium (DMPS)) (PDA-OACF or DMPS-OACF) and two-component (PDA and DMPS) (DMPS-PDA-OACF) functionalized activated carbon fibers pretreated by hydrogen peroxide for the removal of trace heavy metals. The as-prepared DMPS-OACF (7.5,20) under DMPS addition of 7.5 mg and sonication time of 20 min retained large specific surface area, micro-mesoporous structure and rich functional groups and showed better adsorption performance for trace lead and mercury. It also exhibited wide applicable ranges of pH (3.50-10.50) and concentration (50-1136 ppb), rapid adsorption kinetics, and excellently selective removal performance for trace lead. The maximum lead adsorption capacity reached 16.03 mg/g when the effluent lead concentration met World Health Organization (WHO) standard and the adsorbent can be regenerated by EDTA solution. The fitting results of adsorption kinetics and isotherm models revealed that the lead adsorption process was multi-site adsorption on heterogeneous surfaces and chemical adsorption. The excellent adsorption properties for trace heavy metals were attributed that the sulfur/oxygen/nitrogen-containing functional groups boosted diffusion and adsorption by electrostatic attraction and coordination, suggesting that DMPS-OACF (7.5,20) has great application potential in the removal of trace heavy metals. © 2022, The Authors. All rights reserved.

关键词： Adsorption

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High-Performance Iron-Doped Molybdenum Disulfide Photocatalysts Enhance Peroxymonosulfate Activation for Water Decontamination

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SSRN 2022年

作者： Li, Zhongxu Dong, Shuangshi Sun, Meng Ministry of Education Jilin University Jilin Changchun130021 China Jilin Provincial Key Laboratory of Water Resources and Environment Jilin University Jilin Changchun130021 China Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China

Although Fe-based catalysts for peroxymonosulfate (PMS) activation for environmental remediation are effective, the poor regeneration of ferric (Fe (III)) to ferrous ions (Fe (II)) in conventional Fe-based catalysts compromises the durability of PMS activation. Given this, an iron-doped molybdenum disulfide MoS2 (Fe-MoS2) catalyst was prepared via a one-step hydrothermal method, and it was demonstrated to sustain PMS activation for removing tetracycline hydrochloride (TCH) from aqueous solution under visible-light irradiation. The as-prepared Fe-MoS2 catalysts feature dual metallic active sites of Fe and Mo atoms to enhance photoelectrons production from MoS2 for Fe (II) regeneration, thereby preventing iron leakage. Moreover, the Fe-MoS2 catalysts exhibited good recyclability, enabling multiple cycles of TCH degradation in the presence of PMS under the irradiation of visible-light. In addition, we confirmed that the generated radicals (SO4•−, O2•−, and •OH) and non-radical species (1O2 and h+) were responsible for TCH degradation. We also determined critical intermediates during TCH degradation and proposed TCH degradation pathways. This study develops a high-performance Fe-doped MoS2 photocatalyst for PMS activation and paves the way for leveraging dual metallic sites on catalysts for enhancing water purification. © 2022, The Authors. All rights reserved.

关键词： Molybdenum compounds

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Evidence of sewage discharge on the coalescence mechanism of aquatic microbial communities during high amplitude hydrological periods

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Science of the Total environment 2025年 959卷 178223页

作者： Kou, Xin Huang, Shier Bian, Rui Tang, Qingwen Wang, Hui Liu, Song Wang, Li Qi, Weixiao Cao, Xiaofeng Lan, Huachun Liu, Huijuan Qu, Jiuhui Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China Center for Ecological Civilization Tsinghua University Beijing100084 China Center of Tsinghua Think Tanks Tsinghua University Beijing100084 China School of Environment Northeast Normal University Changchun130117 China Co. Ltd. Zunyi564501 China Chishui River Middle Basin Watershed ecosystem Observation and Research Station of Guizhou Province Zunyi564501 China

Microbial community coalescence is a ubiquitous ecological process in various ecosystems. However, limited research has addressed the effects of the coalescence on microbial ecological processes and network structure, particularly in the context of sewage discharge during high amplitude hydrological periods. Employing 16S rRNA sequencing and species source tracking analysis, we investigated the coalescence pattern of bacterioplankton in the Chishui river and sewage across various hydrological periods. The results demonstrated that the downstream bacterioplankton mainly originated from the upstream water body, and the sewage discharge from the wastewater treatment plants (WWTPs) had less impact on the downstream bacterioplankton. In the low-water period, the bacterioplankton community showed significant coalescence, and the specialist species and functional taxa gathered in the downstream. Bacterioplankton displayed distinct ecological succession patterns after community coalescence, with notable variations in the abundance of dominant group. Bacterioplankton community assembly was dominated by stochastic processes in river and the sewage over different hydrological periods. The ecological networks exhibited the highest complexity in the high-water period, whereas their stability was most pronounced in the low-water period. Species diversity, as opposed to functional and phylogenetic diversity, might be a more accurate indicator to predict changes in microbial network structure. Our findings will provide new perspectives on the mechanisms of aquatic microbial community coalescence in natural environments. © 2024 Elsevier B.V.

关键词： Anthropogenic

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A single-atom Fe–N 2 embedded in nitrogen-doped porous carbon as a bifunctional photocatalyst for efficient removal of marine petroleum pollutants

Environmental Functional Materials

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environmental Functional Materials 2023年第1期2卷 66-75页

作者： Xin Li Yuwen Chen Zhiyue Zhao Yizhe Huang Ke Zhu Sitong Feng Shaojuan Luo Lei Wang Kai Yan Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology School of Environmental Science and Engineering Sun Yat-sen University Guangzhou 510275 PR China School of Chemical Engineering and Light Industry Guangdong University of Technology Guangzhou 510006 PR China School of Materials and Environmental Engineering Institute of Urban Ecology and Environment Technology Shenzhen Polytechnic Shenzhen PR China

Petroleum and its refined products enter the marine environment during the extraction process, causing serious pollution. Herein, a bifunctional Fe–N 2 single-atom embedded in nitrogen-doped porous carbon photocatalyst (FC) was fabricated for the efficient removal of marine petroleum pollutants. The combination of highly dispersed Fe–N 2 active sites, large surface area, high porosity, and good conductivity results in excellent photocatalytic activities. The FC catalyst exhibited a 96.7% degradation rate in the oxidative removal of bisphenol A (BPA) and a 63.4% reduction of Cr(VI) within 1 h, whereas the reaction equilibrium rate constants of 0.0132 min −1 and 0.0505 min −1 were reached, respectively. FC with good stability and reusability could reach 88.3% and 53.5% removal rate of BPA and Cr(VI) after 5 cycles. Radical quenching experiments and electron spin resonance (ESR) confirmed that ‧OH and e − were the most driving active species for photo-oxidation and reduction, respectively. Besides, the FC catalyst was applied to an actual seawater system and the simulation results showed a good removal rate (82.7% of BPA and 50.9% of Cr(VI) within 1 h). The BPA oxidation pathway in the system was proposed and the toxicity of each intermediate was accessed. This work offers a new way to construct single-atom functionalized carbon-based catalysts for marine pollution control.

关键词： Fe–N 2 single-atom Photocatalysis Redox reaction Marine petroleum pollutants

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Impacts of emissions and meteorological changes on China’s ozone pollution in the warm seasons of 2013 and 2017

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Frontiers of environmental Science & Engineering 2019年第5期13卷 129-137页

作者： Dian Ding Jia Xing Shuxiao Wang Xing Chang Jiming Hao State Key Joint Laboratory of Environmental Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing 100084China

We have quantified the impacts of anthropogenic emissions reductions caused by the Air pollution control Action Plan and changes in meteorological fields between 2013 and 2017 on the warm-season O3 concentration in China using a regional 3D chemical transport model. We found that the impact on daily maximum eight-hour (MDA8) O3 concentration by the meteorological variation that mostly increased O3 was greater than that from emission reduction, which decreased O3. Specifically, the control measures implemented since 2013 in China have reduced SO2, NOx, PM2.5, and VOC emissions by 33%, 25%, 30%, and 4% in 2017, while NH3 emissions have increased by 7%. The changes in anthropogenic emissions lowered MDA8 O3 by 0.4–3.7 ppb (0.8%–7.6%, varying by region and month), although MDA8 O3 was increased slightly in some urban areas (i.e. North China) at the beginning/end of warm seasons. Relative to 2013, the average 2 m temperature in 2017 shows increments in North, North-east, East, and South China (0.34℃–0.83℃) and decreases in Central China (0.24℃). The average solar radiation shows increments in North, North-east, and South China (7.0–9.7 w/m2) and decreases in Central, South-west, and North-west China (4.7–10.3 w/m2). The meteorological differences significantly change MDA8 O3 by -3.5–8.5 ppb (-8.2%–18.8%) with large temporal variations. The average MDA8 O3 was slightly increased in North, North-east, East, and South China. The response surface model suggests that the O3 formation regime transfers from NOx-saturated in April to NOx-limited in July on average in China.

关键词： O3 pollution Meteorological influences Emission reduction NOx VOC

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