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Towards Elevated Perfluorooctanoic Acid (Pfoa) Enrichment in Water: Sequential Liquid-Liquid Extraction Pretreatment for Ion Chromatography Detection

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SSRN 2024年

作者： Yang, Yang He, Huan Chen, Yuheng Chen, Baiyang Banayan Esfahani, Ehsan Mohseni, Madjid Xu, Nan Nesterenko, Pavel N. State Key Laboratory of Urban Water Resource and Environment Shenzhen Key Laboratory of Organic Pollution Prevention and Control Harbin Institute of Technology Shenzhen518055 China Department of Chemical & Biological Engineering University of British Columbia VancouverBCV6T 1Z3 Canada Key Laboratory for Heavy Metal Pollution Control and Reutilization School of Environment and Energy Peking University Shenzhen Graduate School Shenzhen518055 China Department of Chemistry Lomonosov Moscow State University Vorob’evy Gory GSP-3 Moscow119899 Russia

The widespread detection of perfluorooctanoic acid (PFOA) in the environment has raised significant concerns. The standard PFOA analytical method relies on expensive solid-phase extraction (SPE) and liquid chromatography tandem mass spectrometry (LC-MS/MS) instruments, making routine use prohibitive. We herein proposed a cost-effective yet novel enrichment method for determining PFOA at ng/L level. This method entailed a two-step sample preparation process: firstly, PFOA was extracted and enriched using a forward-extraction under acidic conditions, followed by a backward-extraction and enrichment step utilizing alkaline water. The enriched samples were subsequently subjected to a common ion chromatography (IC). Results reveal that maintaining a forward-extraction pH below its pKa value (2.8) is essential, as protonated PFOA proves effective in enhancing the enrichment factor (EF). The challenge lied in driving PFOA from forward-extractant to aqueous backward-extractant due to the decreased hydrophobicity of deprotonated PFOA (log Kow2 = 1.0). In addition, we found that evaporating forward-extractant with alkaline backward-extractant (containing 5% methanol) reduced potential analytical uncertainties associated with PFOA evaporation and sorption. Under optimal conditions, the method achieved a detection limit of 9.2 ng/L and an impressive EF value of 719. Comparison with SPE-LC-MS/MS confirmed the proposed method as a promising alternative for PFOA determination. Although initially targeted for PFOA, the novel methodology is likely applicable to preconcentration of other poly-fluoroalkyl substances. © 2024, The Authors. All rights reserved.

关键词： Ion chromatography

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Synergistic rare-earth yttrium single atoms and copper phosphide nanoparticles for high-selectivity ammonia electrosynthesis

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Rare metals 2024年第11期43卷 5792-5801页

作者： Yi-Meng Cai Yang-Hua Li Yi Xiao Quentin Meyer Qian Sun Wan-Jing Lai Shu-Wen Zhao Jun Li Lin-Jie Zhang Han Wang Zhang Lin Jun Luo Li-Li Han School of Materials Science and Engineering Institute for New Energy Materials and Low-Carbon TechnologiesTianjin University of TechnologyTianjin 300384China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China School of Chemistry The University of New South WalesSydneyNSW 2052Australia School of Metallurgy and Environment Central South UniversityChangsha 410083China Chinese National Engineering Research Center for Control&Treatment of Heavy Metal Pollution Changsha 410083China ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaShenzhen 518110China

Electrochemical nitrate reduction to NH_(3)holds a great promise for N-upcycling in nature,while its sluggish reaction kinetics involved in both the stepwise deoxygenation and hydrogenation processes necessitates the development of bespoke catalysts with multi-site ***,we report a hybrid catalyst composed of rare-earth(RE)yttrium(Y)single atoms and copper phosphide(Cu_(3)P)nanoparticles loaded on N,P-doped carbon(Y_(SA)-Cu_(3)P/CNP)through a chelating and pyrolysis *** to a synergistic contribution of Y single atoms and Cu_(3)P nanoparticles,Y_(SA)-Cu_(3)P/CNP achieves an impressive NH_(3)Faradaic efficiency(FE)of 92%at-0.5V(***)and the highest NH_(3)yield rate of11.4 mg·h^(-1)·cm^(-2)at-0.6 V(***)in an alkaline media,which surpass most of the reported *** intricate reaction pathway has been explored by online differential electrochemical mass spectrometry(DEMS),and the synergistic effect between Y single atoms and Cu_(3)P nanoparticles has been studied by in situ synchrotron X-ray absorption ***,density-functional theory(DFT)calculations unveil that the high-efficiency nitrate reduction on Y_(SA)-Cu_(3)P/CNP is attributed to a reduced energy barrier of the rate-determining deoxygenation step coupled with the enhanced stabilization of active hydrogen favorable for the hydrogenation steps,thereby boosting the overall reaction *** addition,a prototype Zn-nitrate battery utilizing Y_(SA)-Cu_(3)P/CNP as the cathode is *** work not only elucidates the mechanism behind the enhanced catalytic performance but also paves the way for the future development of highefficiency electrocatalysts through dual-site engineering.

关键词： Rare-earth single atom Cu_(3)P nanoparticle Synergistic electrocatalysis Nitrate reduction reaction Zn-nitrate battery

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Towards elevated perfluorooctanoic acid (PFOA) enrichment in water: Sequential liquid-liquid extraction pretreatment for ion chromatography detection

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Chemosphere 2024年 358卷 142227页

作者： Yang, Yang He, Huan Chen, Yuheng Chen, Baiyang Esfahani, Ehsan Banayan Mohseni, Madjid Xu, Nan Nesterenko, Pavel 518055 China Department of Chemical & Biological Engineering University of British Columbia Vancouver BCV6T 1Z3 Canada Key Laboratory for Heavy Metal Pollution Control and Reutilization School of Environment and Energy Peking University Shenzhen Graduate School Shenzhen518055 China Department of Chemistry Lomonosov Moscow State University Vorob'evy Gory GSP-3 Moscow119899 Russia

The widespread detection of perfluorooctanoic acid (PFOA) in the environment has raised significant concerns. The standard PFOA analytical method relies on expensive solid-phase extraction (SPE) and liquid chromatography tandem mass spectrometry (LC-MS/MS) instruments, making routine use prohibitive. We herein proposed a cost-effective yet novel enrichment method for determining PFOA at ng L−1 level. This method entailed a two-step sample preparation process: firstly, PFOA was extracted and enriched using a forward-extraction under acidic conditions, followed by a backward-extraction and enrichment step utilizing alkaline water. The enriched samples were subsequently subjected to a common ion chromatography (IC). Results reveal that maintaining a forward-extraction pH below its pKa value (2.8) is essential, as protonated PFOA proves effective in enhancing the enrichment factor (EF). The challenge lied in driving PFOA from forward-extractant to aqueous backward-extractant due to the decreased hydrophobicity of deprotonated PFOA (log Kow2 = 1.0). In addition, we found that evaporating forward-extractant with alkaline backward-extractant (containing 5% methanol) reduced potential analytical uncertainties associated with PFOA evaporation and sorption. Under optimal conditions, the method achieved a detection limit of 9.2 ng L−1 and an impressive EF value of 719. Comparison with SPE-LC-MS/MS confirmed the proposed method as a promising alternative for PFOA determination. Although initially targeted for PFOA, the novel methodology is likely applicable to preconcentration of other poly-fluoroalkyl substances. © 2024 Elsevier Ltd

关键词： Ion chromatography

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Molecular characterization of transformation and halogenation of natural organic matter during the UV/chlorine AOP using FT-ICR mass spectrometry

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Journal of Environmental Sciences 2021年第4期33卷 24-36页

作者： Xiaoxue Ruan Yingying Xiang Chii Shang Shuangshuang Cheng Jingfu Liu Zhineng Hao Xin Yang School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation TechnologySun Yat-sen UniversityGuangzhou 510275China Department of Civil and Environmental Engineering The Hong Kong University of Science and TechnologyHong KongChina Hong Kong Branch of Chinese National Engineering Research Center for Control&Treatment of Heavy Metal Pollution The Hong Kong University of Science and TechnologyHong KongChina State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

UV/chlorine process,as an emerging advanced oxidation process(AOP),was effective for removing micro-pollutants via various reactive radicals,but it also led to the changes of natural organic matter(NOM)and formation of disinfection byproducts(DBPs).By using negative ion electrospray ionization coupled with Fourier transform ion cyclotron resonance mass spectrometry(ESI FT-ICR MS),the transformation of Suwannee River NOM(SRNOM)and the formation of chlorinated DBPs(Cl-DBPs)in the UV/chlorine AOP and subsequent post-chlorination were tracked and compared with dark *** comparison to dark chlorination,the involvement of Cl O·,Cl·,and HO·in the UV/chlorine AOP promoted the transformation of NOM by removing the compounds owning higher aromaticity(AI mod)value and DBE(double-bond equivalence)/C ratio and causing the decrease in the proportion of aromatic ***,more compounds which contained only C,H,O,N atoms(CHON)were observed after the UV/chlorine AOP compared with dark chlorination via photolysis of organic chloramines or radical reactions.A total of 833 compounds contained C,H,O,Cl atoms(CHOCl)were observed after the UV/chlorine AOP,higher than 789 CHOCl compounds in dark chlorination,and one-chlorine-containing components were the dominant *** different products from chlorine substitution reactions(SR)and addition reactions(AR)suggested that SR often occurred in the precursors owning higher H/C ratio and AR often occurred in the precursors owning higher ***-chlorination further caused the cleavages of NOM structures into small molecular weight compounds,removed CHON compounds and enhanced the formation of *** results provide information about NOM transformation and Cl-DBPs formation at molecular levels in the UV/chlorine AOP.

关键词： UV/chlorine AOP Disinfection byproducts(DBPs) Natural organic matter(NOM) FT-ICR MS Water treatment

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Exploration of the bio-availability and the risk thresholds of cadmium and arsenic in contaminated paddy soils

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Heliyon 2024年第24期10卷 e40910页

作者： Guan, Di Ji, Xionghui Liu, Saihua Chen, Shan Xie, Yunhe Wu, Jiamei The Key Laboratory of Agro-Environment in Midstream of Yangtze Plain Ministry of Agriculture The Key Laboratory of Prevention Control and Remediation of Soil Heavy Metal Pollution in Hunan Province Institute of Agro-Environment and Ecology Hunan Academy of Agricultural Sciences Changsha 410125 China

Cadmium (Cd) and arsenic (As) contamination risk in paddy soils has raised global concern. In order to scientifically and objectively evaluate the bioavailability of soil Cd, As and the risk of Cd or As threshold in contaminated farmland, this study was conducted to investigate different types of extractants for their potential extraction efficiency of Cd and As. Soils from two different parent materials in Hunan, Yueyang and Yiyang, typical double-cropping rice production areas in the south of China, were used as test soils. The extraction capabilities of 10 extractants (ultrapure water, 0.1 mol/L HCl, 1.0 mol/L NH₄OAc, CaCl₂-DTPA, 0.01 mol/L CaCl₂, 0.1 mol/L CaCl₂, 0.5 mol/L NaH₂PO₄, 0.05 mol/L NaHCO₃, 0.1 mol/L NaNO₃, 0.1 mol/L HNO₃), were compared for their extraction capabilities of soil available Cd and As. Meanwhile, the content of Cd and As in plants issues and grains of rice was monitored during harvest, and the Cd, As content correlation between extracted forms and rice was analyzed. The results showed that the HCl, CaCl₂, HNO₃, and CaCl₂-DTPA solutions exhibited high extraction efficiency for Cd (42.2–88.4 %);for As, NaH₂PO₄, HCl, and HNO₃ have the extraction efficiency (0.85–23.4 %). The concentration of Cd extracted by 0.01 mol/L CaCl₂ was significantly positively correlated with Cd levels in rice. The potential risk extraction threshold of CaCl₂ in sandy loam soil was 0.178 mg/kg, while it was 0.312 mg/kg in clay soil. The concentration of As extracted by CaCl₂-DTPA and 0.05 mol/L NaHCO₃ in clay soil was significantly positively correlated with As levels in rice, the potential risk extraction thresholds were 0.115 mol/L and 0.106 mg/kg, respectively. These investigations indicated that the heavy metals extraction methods by 0.01 mol/L CaCl₂

关键词： Arsenic Bioavailability Cadmium Extraction efficiency Farmland soil Rice Risk threshold

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Vertical Distribution, Accumulation, and Characteristics of Microplastics in Mangrove Sediment in China

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SSRN 2022年

作者： Yu, Lingyun Li, Ruili Chai, Minwei Li, Bing Key Laboratory for Heavy Metal Pollution Control and Reutilization School of Environment and Energy Peking University Shenzhen Graduate School Shenzhen518055 China Water Research Center Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen518055 China

Mangroves in tropical and subtropical regions worldwide have been recognized as important sinks for microplastics (MPs). However, most current studies have focused on surface sediments, and in China, the vertical distribution and characteristics of MPs in mangrove sediments remain poorly understood. In this study, sediment cores of 100 cm depth were taken from six representative mangroves in China to investigate MPs via chronological analysis. Futian was found to have the highest abundance of MPs (0–3,123 n/kg), followed by Zhanjiang, Dongzhaigang, Yunxiao, Dongfang, and Fangchenggang. The earliest MPs occurring in mangroves were dated to 1955, and the abundance of MPs increased exponentially from bottom to surface sediments. MPs were mainly characterized by white color, were fiber-shaped, 1,000–5,000 μm in size, and of polypropylene/polyethylene polymer types. Furthermore, the MPs in the urban mangrove also showed a higher diversity of color. The results showed that the MP stocks in the urbanized city Futian mangrove reached 1,828 mg/m 3 , an order of magnitude higher than in other areas (251±180 mg/m 3 ), contributing to 0.0057% of the carbon storage of the sediment. The abundance of MPs in mangrove sediments are expected to increase by 2.38–9.54 times by 2030, and therefore deserve further attention. © 2022, The Authors. All rights reserved.

关键词： Tropics

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Synthesis of high-performance arsenic-specific adsorption microspheres using iron-magnesium modified chitosan

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Applied Surface Science 2025年 706卷

作者： Tan, Jie Nan, Fangming Chen, Donghui Xiang, Lu Li, Xiaoting Han, Qingwen Zhan, Wei Hubei Province Engineering Research Center for Control and Treatment of Heavy Metal Pollution College of Resources and Environmental Science South-Central Minzu University Wuhan430074 China Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education Wuhan430074 China Hubei Three Gorges Laboratory Yichang443007 China

Chitosan (CS) is widely recognized for its excellent gelling properties;however, its application in heavy metal removal is often limited by the scarcity of active adsorption sites. In this study, CS was employed as a matrix material to fabricate gel beads (Fe/Mg-CS) through cross-linking with Fe3+ and Mg2+ thereby enhancing its adsorption capacity for As(V). The Fe/Mg-CS adsorbent was thoroughly characterized, and its adsorption performance was evaluated under optimized conditions. The optimal dosage of Fe/Mg-CS was determined to be 0.06 g/L, with effective adsorption observed within a pH range of 3–7. Kinetic analysis revealed that the adsorption process followed a pseudo-second-order model, suggesting that the adsorption mechanism primarily involves complexation reactions between hydroxyl groups and As(Ⅴ). Isotherm studies indicated that the Langmuir model provided the best fit, with a maximum adsorption capacity of 147.49 mg/g. Compared to conventional powdered adsorbents, Fe/Mg-CS offers several advantages, including straightforward synthesis, ease of recycling, and high efficiency. These properties make Fe/Mg-CS a promising candidate for the remediation of As(V)-contaminated groundwater, providing a sustainable and effective solution for future water purification applications. © 2025 Elsevier B.V.

关键词： Groundwater pollution

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Microplastics in Food Legumes Production Areas Affect Soil Physicochemical Properties and Bacterial Community are Dependent on Their Types

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SSRN 2024年

作者： La, Yuepeng Zhang, Li Zhao, Nan Ye, Huike Zeng, Qiang Zhao, Lijie Wang, Zhengjun Lin, Dasong Wang, Ruigang Innovation Team of Remediation for Heavy Metal Contaminated Farmlands Agro-Environmental Protection Institute Ministry of Agriculture and Rural Affairs Tianjin300191 China National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in South China Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management Institute of Eco-environmental and Soil Sciences Guangdong Academy of Sciences Guangzhou510650 China

Microplastics (MPs) pose a threat to farmland soil quality and crop safety. MPs exist widely in food legumes farmland soil due to the extensive use of agricultural film and organic fertilizer, but their distribution characteristics and their impact on soil environment have not been reported. The abundance and characteristics for MPs, soil physical and chemical properties, and bacterial community composition were investigated in 76 soil samples in five provinces in northern China. The results showed that the abundance of MPs ranged from 1600 to 36200 items/kg. MPs in soil were mostly fibrous, less than 0.2 mm, and white. Rayon, polyester and polyethylene were the main types of MPs, which exerted an important influence on soil physicochemical properties and bacterial composition. Polyethylene significantly decreased soil silt content and increased the soil nitrate nitrogen content (p © 2024, The Authors. All rights reserved.

关键词： Soils

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Size-Based Separation of Fine Mineral Particles Using Inertial Microfluidics: A Case of Jarosite and Anglesite

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SSRN 2024年

作者： Liu, Xiaoyun Li, Jiawei Zhang, Wenchao Wang, Yunyan Min, Xiaobo Yang, Zhihui Shi, Meiqing Wang, Qingwei Yan, Xu Chai, Liyuan School of Metallurgy and Environment Central South University Changsha410083 China State Key Laboratory of Advanced Metallurgy for Non-ferrous Metals Changsha410083 China Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution Changsha410083 China Institute of Environmental Science and Engineering

Many metal phases in industrial hazardous waste coexist as fine mineral particles (FMPs, with particle sizes of 0.01 μm-20 μm) in a physical mixture, making conventional methods unable to achieve separation. Advanced microfluidics has demonstrated its potential in the separation of FMPs, as exemplified by jarosite and anglesite. Our study innovatively proposed an inertial microfluidic method for the separation of FMPs by force difference in curved microchannels, thus produced two distinct migration behaviors and subsequent separation. In addition, the computational fluid dynamics (CFD) simulation model was constructed to predict and analyze the migration behavior and separation trend of FMPs through flow field simulation and particle trajectory tracking. The results indicated that 2.1 μm and 3.6 μm small particles migrated to the outer outlet of the microchannel due to the dominant Dean vortex force, while 7.2 μm and 9.4 μm large particles migrated to the inner outlet relying on inertial focusing. At a flow rate of 1.2 mL/min, the separation efficiency of 3.6 μm jarosite and 9.4 μm anglesite has achieved a leap from 0% to 60.7%. This discovery provided feasibility and insights into the application of microfluidic technology for particle separation, and offered enormous potential for practical iron residue treatment. © 2024, The Authors. All rights reserved.

关键词： Vortex flow

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Microwave-Enhanced Tea Polyphenol Reduction of Natural Iron Minerals and Effective Immobilization of Hexavalent Chromium in Soil

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SSRN 2024年

作者： Tu, Yuliang Wang, Jianle Huang, Yanfeng Deng, Hong Liu, Xueming Lin, Zhang Chai, Liyuan School of Environment and Energy Key Laboratory of Pollution C0ontrol and Ecosystem Restoration in Industry Clusters Ministry of Education South China University of Technology Guangzhou510006 China Institute of Environmental Engineering School of Metallurgy and Environment China Chinese National Engineering Research Center for Control and Treatment of Heavy Metal Pollution Central South University Changsha410083 China

Remediation of hexavalent chromium (Cr(VI)) contaminated soil has become a global challenge, not only because of the carcinogenicity and high toxicity of Cr(VI), but also because the remediation of chromium contaminated soils is often affected by the complexity of different external factors. Tea polyphenols (TP), as an eco-friendly material, can not only reduce hexavalent chromium in the soil, but also efficiently reduce Fe(III) in the soil, and further promote the reduction and immobilization of soil Cr(VI). In this study, a new cost-effective, sustainable and efficient soil remediation strategy was proposed to enhance the detoxification efficiency and long-term stability of Cr(VI) by utilizing TP to complex and reduce iron minerals in the soil with the aid of microwave (MW). Microwave-assisted TP (0.5 wt% TP+MW (700 W, 10 min)) enhanced the removal of Cr(VI) from iron-enriched soil from 70.49% to 99.94% as compared to TP (0.5 wt%) reduction alone. SEM-EDS, XRD, FTIR and XPS studies indicated that the increase in Cr(VI) removal efficiency by tea polyphenols was attributed to the accelerated reduction and fixation of Cr(VI) by tea polyphenols promoting the reduction of soil iron minerals and the conversion of Cr stabilized on the mineral surface to Cr2O3 and FeCr2O4 under MW irradiation. TP can directly complex and reduce solid-phase Fe minerals leading to a significant increase in the Fe(II) content, which is further enhanced by MW irradiation by the formation of a stable chromite. In addition, the toxic leaching concentration of Cr(VI) in soil remained below 0.05 mg·L-1 after 360 days of immobilization of microwave-assisted tea polyphenol-treated soils placed in the atmosphere. The technology offers an effective alternative for remediation Thus, the technology provides an effective alternative for The technology offers an effective alternative for remediation of soil Cr(VI). © 2024, The Authors. All rights reserved.

关键词： Soils

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