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A review on the transformation of birnessite in the environment:Implication for the stabilization of heavy metals

Journal of Environmental Sciences 2024年第5期139卷 496-515页

作者： Miao Shi Qingzhu Li Qingwei Wang Xuelei Yan Bensheng Li Linhai Feng Chao Wu Rongrong Qiu Hongkai Zhang Zhihui Yang Weichun Yang Qi Liao Liyuan Chai School of Metallurgy and Environment Central South UniversityChangsha 410083China National Engineering Research Centre for Control and Treatment ofHeavy Metal Pollution Central South UniversityChangsha 410083China Water Pollution Control Technology Key Lab of Hunan Province Changsha 410083China

Birnessite is ubiquitous in the natural environment where heavy metals are retained and easily *** surface properties and structure of birnessite change with the changes in external environmental conditions,which also affects the fate of heavy *** the effect and mechanism of the birnessite phase transition process on heavy metals is the key to taking effective measures to prevent and control heavy metal ***,the four transformation pathways of birnessite are summarized first in this ***,the relationship between transformation pathways and environmental conditions is *** relevant environmental conditions include abiotic(e.g.,co-existing ions,pH,oxygen pressure,temperature,electric field,light,aging,pressure)and biotic factors(e.g.,microorganisms,biomolecules).The phase transformation is achieved by the key intermediate of Mn(Ⅲ)through interlayer-condensation,folding,neutralizationdisproportionation,and dissolution-recrystallization *** AOS(average oxidation state)of Mn and interlayer spacing are closely correlated with the phase transformation of *** but not least,the mechanisms of heavy metals immobilization in the transformation process of birnessite are summed *** involve isomorphous substitution,redox,complexation,hydration/dehydration,*** transformation of birnessite and its implication on heavy metals will be helpful for understanding and predicting the behavior of heavy metals and the crucial phase of manganese oxides/hydroxides in natural and engineered environments.

关键词： Birnessite Transformation Heavy metals Pathways Mechanism

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The determinants of effective defluorination by the LiAl-LDHs

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Journal of Environmental Sciences 2023年第4期126卷 153-162页

作者： Kaizhong Li Hui Liu Shuimei Li Qingzhu Li Shengtu Li Qingwei Wang School of Metallurgy and Environment Central South UniversityChangsha 410083China Chinese National Engineering Research Center for Control&Treatment of Heavy Metal Pollution Changsha 410083China Water Pollution Control Technology Key Lab of Hunan Province Changsha 410004China

Millions of people in poor areas are still under the threat of fluoride *** to effectively separate fluorine in water is an important step to reduce the ecological *** this paper,we performed a systematic DFT calculation focused on the defluorination behavior between the LiAl-and *** results indicated that the LiAl-LDHs exhibited high chemical activity before the defluorination,because of the better electronic *** the defluorination,the LiAl-LDHs with adsorbed-F–were also more stable than the *** addition,the existence of coordination covalent bond for the adsorbed-F–attached to the LiAl-LDHs was *** is an important reason for the high defluorination efficiency by the *** addition,a series of weak interaction,including hydrogen bond and van der Waals interaction were also ***,a LiAl-LDHs with excellent fluoride removal properties were synthesized well by simple hydrothermal *** results showed that our synthesized LiAl-LDHs with the capacity of 156.09 mg/g,could be effectively defluorinated in ***,it surpasses most materials and has potential applications.

关键词： Efficient Defluorination water treatment LDHs DFT

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CuInS2/ZnS QDs-based fluorescent probe for detection of Cu2+

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Progress in Natural Science:Materials International 2023年第4期33卷 495-500页

作者： Haiyan Kang Hongchao Geng Sisi Shi Zhongxian Song Yuting Dong Xiaole Yan Chaohai Wang Yanli Mao Qingyun Cai Henan Province Key Laboratory of Water Pollution Control and Rehabilitation Technology Henan University of Urban Construction State Key Laboratory of Chemo/Biosensing and Chemometrics College of Chemistry and Chemical Engineering Hunan University

High concentrations of Cu2+exceeding what the required level for the cellular process can changes the properties of protein, affects the normal function of the body, but also affect the body's metabolism, so that the body's immunity appears to decline. Detection of Cu2+is important for the environmental monitoring. Here, a fluorescence probe that uses heavy metal-free and properties-superior CuInS2/ZnS was proposed for detection of Cu2+. The fluorescence intensity of CuInS2/ZnS quantum dots（QDs） decreased obviously after Cu2+were added,and the intensity with the concentration of Cu2+showed excellent linear relation within the scope of 0–50 μM, the LOD down to 0.45 μM, a possible detection mechanism was analyzed. The QDs was further applied to the detection of Cu2+in drinking water, manifesting the foreground of the current strategy.

关键词： CuInS2/ZnS QDs Fluorescence probe Detection Cu2+

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The role of doped-Mn on enhancing arsenic removal by MgAl-LDHs

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Journal of Environmental Sciences 2022年第10期34卷 125-134页

作者： Kaizhong Li Hui Liu Qingzhu Li Wenming Yao LanyanWu Shuimei Li Qingwei Wang School of Metallurgy and Environment Central South UniversityChangsha 410083China Chinese National Engineering Research Center for Control&Treatment of Heavy Metal Pollution Changsha 410083China Water Pollution Control Technology Key Lab of Hunan Province Changsha 410004China

To meet the challenges posed by global arsenic water contamination, the Mg Al Mn-LDHs with extraordinary efficiency of arsenate removal was developed. In order to clarify the enhancement effect of the doped-Mn on the arsenate removal performance of the LDHs, the cluster models of the Mg Al Mn-LDHs and Mg Al-LDHs were established and calculated by using density functional theory(DFT). The results shown that the doped-Mn can significantly change the electronic structure of the LDHs and improve its chemical activity. Compared with the Mg Al-LDHs that without the doped-Mn, the HOMO-LUMO gap was smaller after doping. In addition, the-OH and Al on the laminates were also activated to improve the adsorption property of the LDHs. Besides, the doped-Mn existed as a novel active site. On the other hand, the Mg Al Mn-LDHs with the doped-Mn, the increased of the binding energy, as well as the decreased of the ion exchange energy of interlayer Cl^(-), making the ability to arsenate removal had been considerably elevated than the Mg Al-LDHs. Furthermore, there is an obvious coordination covalent bond between arsenate and the laminates of the Mg Al MnLDHs that with the doped-Mn.

关键词： Mechanism Arsenate removal Mn LDHs DFT

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Mechanisms of Pb(Ⅱ) coprecipitation with natrojarosite and its behavior during acid dissolution

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Journal of Environmental Sciences 2022年第12期34卷 128-137页

作者： Meiqing Shi Xiaobo Min Chen Tian Taixu Hao Sijie Zhu Yun Ge Qingwei Wang Xu Yan Zhang Lin Institute of Environmental Engineering School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083China Chinese National Engineering Research Center for Control&Treatment of Heavy Metal Pollution Changsha 410083China Water Pollution Control Technology Key Lab of Hunan Province Changsha 410004China

Lead(Pb) coprecipitation with jarosite is common in natural and engineered environments,such as acid mine drainage(AMD) sites and hydrometallurgical industry. Despite the high relevance for environmental impact, few studies have examined the exact interaction of Pb with jarosite and the dissolution behavior of each phase. In the present work, we demonstrate that Pb mainly interacts with jarosite in four modes, namely incorporation, occlusion,physically mixing, and chemically mixing. For comparison, the four modes of Pb-bearing natrojarosite were synthesized and characterized separately. Batch dissolution experiments were undertaken on these synthetic Pb-bearing natrojarosites under pH_(2) to simulate the AMD environments. The introduction of Pb decreases the final Fe releasing efficiency of jarosite-type compounds from 18.18% to 3.45%-5.01%, showing a remarkable inhibition of their dissolution. For Pb releasing behavior, PbSO_(4) dissolves in preference to Pb-substituted natrojarosite, i.e.,(Na, Pb)-jarosite, which primarily results in the sharp increase of Pb releasing concentration(> 40 mg/L). PbSO_(4) occlusion by jarosite-type compounds can significantly reduce the release of Pb. The results of this study could provide useful information regarding Fe and Pb cycling in acidic natural and engineered environments.

关键词： Pb-bearing natrojarosite Interaction mechanism Acid dissolution Releasing behavior

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Synthesis and electrochemical behavior of monolayer-Ti_(3)C_(2)T_(x) for capacitive deionization

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Journal of Central South University 2022年第2期29卷 359-372页

作者： MIN Xiao-bo LIU Fan-song WANG Yun-yan YAN Yi-qi WANG Hai-ying School of Metallurgy and Environment Central South UniversityChangsha 410083China Chinese National Engineering Research Center for Control&Treatment of Heavy Metal Pollution Changsha 410083China Water Pollution Control Technology Key Lab of Hunan Province Changsha 410083China

MXene materials have got great attention from researchers of environmental treatment for the great electrochemical ***-Ti_(3)C_(2)T_(x)(T_(x) is the surface terminal groups such as-O,-OH and/or-F species),as a typical structural MXene,always shows better chemical-physical characteristics than multilayer-Ti_(3)C_(2)T_(x).Thus,we prepared monolayer-Ti_(3)C_(2)T_(x) electrode by HF etching method and absolute ethyl alcohol intercalationdelamination treatment for capacitive deionization(CDI).The prepared monolay-Ti_(3)C_(2)T_(x) shows a higher specific surface area(235.6 m^(2)/g)and a thinner thickness(0.8 nm).Moreover,a series of systematic investigation demonstrated that monolayer-Ti_(3)C_(2)T_(x) has obvious promotional phenomenon on electrochemical properties(e.g.,mass specific capacitance increased from 52.1 F/g to 144.7 F/g).The NaCl adsorption capacity of monolayer-Ti_(3)C_(2)T_(x),is 30.7 mg/g in 1000 mg/L NaCl solution at 1.2 *** concluded that the electro-sorption mechanism could be expressed as double electric layer and monolayer coverage by a good fitting of Langmuir isotherms and the pseudo-second-order kinetics *** work would provide a new strategy for the application of monolayer-Ti_(3)C_(2)T_(x) material in wastewater treatment in the future.

关键词： monolayer-Ti_(3)C_(2)T_(x) capacitive deionization NaCl electro-sorption mechanism MXene materials

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Facet-controlled LiMn_(2)O_(4)/C as Deionization Electrode with Enhanced Stability and High Desalination Performance

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Nano-Micro Letters 2022年第11期14卷 75-86页

作者： Yuxin Jiang Liyuan Chai Dehe Zhang Fangping Ouyang Xiangyuan Zhou Sikpaam IAlhassan Sailin Liu Yingjie He Lvji Yan Haiying Wang Wenchao Zhang School of Metallurgy and Environment Central South UniversityChangsha 410083People’s Republic of China Chinese National Engineering Research Center for Control and Treatment of Heavy Metal Pollution Changsha 410083People’s Republic of China Water Pollution Control Technology Key Lab of Hunan Province Changsha 410083People’s Republic of China School of Physics and Electronics Hunan Key Laboratory for Super-Microstructure and Ultrafast Processand Hunan Key Laboratory of Nanophotonics and DevicesCentral South UniversityChangsha 410083People’s Republic of China State Key Laboratory of Powder Metallurgy and Powder Metallurgy Research InstituteCentral South UniversityChangsha 410083People’s Republic of China School of Chemical Engineering and Advanced Materials Faculty of SciencesEngineering and TechnologyThe University of AdelaideAdelaide 5005Australia

Battery materials as emerging capacitive deionization electrodes for desalination have better salt removal capacities than traditional carbon-based ***_(2)O_(4),a widely used cathode mate-rial,is difficult to utilize as a deionization electrode due to its structural instability upon cycling and Mn dissolution in aqueous-based ***,a facile and low-cost ball-milling routine was proposed to prepare a LiMn_(2)O_(4)material with highly exposed(111)*** prepared electrode exhibited relatively low dissolution of Mn during cycling,which shows its long cycle *** the hybrid capacitive deionization system,the LiMn_(2)O_(4)/C electrode delivered a high desalination capacity of 117.3 mg g^(−1) without obvious capacity decay at a voltage of 1.0 V with a 20 mM initial salt *** addition,the exposed(111)facets significantly alleviated Mn ion dissolution,which also enhanced the structural steadiness.

关键词： Deionization electrode Desalination Lithium-ion battery

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Application and mechanism of Fenton-like iron-based functional materials for arsenite removal

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Transactions of Nonferrous Metals Society of China 2022年第12期32卷 4139-4155页

作者： Qing-wei WANG Xue-lei YAN Mei-juan MA Ben-sheng LI Zong-run LI Qing-zhu LI School of Metallurgy and Environment Central South UniversityChangsha 410083China National Engineering Research Centre for Control and Treatment of Heavy Metal Pollution Central South UniversityChangsha 410083China Water Pollution Control Technology Key Lab of Hunan Province Changsha 410004China

Between the two major arsenic-containing salts in natural water, arsenite(As(Ⅲ)) is far more harmful to human and the environment than arsenate(As(V)) due to its high toxicity and transportability. Therefore, preoxidation of As(Ⅲ) to As(V) is considered to be an effective means to reduce the toxicity of arsenic and to promote the removal efficiency of arsenic. Due to their high catalytic activity and arsenic affinity, iron-based functional materials can quickly oxidize As(Ⅲ) to As(V) in heterogeneous Fenton-like systems, and then remove As(V) from water through adsorption and surface coprecipitation. In this review, the effects of different iron-based functional materials such as zero-valent iron and iron(hydroxy) oxides on arsenic removal are compared, and the catalytic oxidation mechanism of As(Ⅲ) in heterogeneous Fenton process is further clarified. Finally, the main challenges and opportunities faced by iron-based As(Ⅲ) oxidation functional materials are prospected.

关键词： Fenton-like reaction iron-based functional materials catalytic oxidation arsenic removal

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Mechanistic insights to sorptive removal of four sulfonamide antibiotics from water using magnetite-functionalized biochar

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Biochar 2023年第1期5卷 1377-1388页

作者： Shanshan Bai Yaolu Zhou Mingrong Qian Jun Xia Zhiqiang Sun Yujiao Wang Xiaochen Huang Shishu Zhu Key Laboratory of Pollution Exposure and Health Intervention of Zhejiang Province Interdisciplinary Research AcademyZhejiang Shuren UniversityHangzhou 310015People’s Republic of China State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090People’s Republic of China State Key Lab of Biocontrol Guangdong Provincial Key Laboratory of Plant ResourcesSchool of AgricultureShenzhen Campus of Sun Yat-Sen UniversityShenzhen 518107People’s Republic of China The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationSchool of Environment and EnergySouth China University of TechnologyGuangzhou 510006People’s Republic of China

Magnetite-functionalized biochar(MBC)is a promising engineered material for remediation of antibiotic-contaminated ***,sorption mechanisms of ionizable organic compounds such as sulfonamide antibiotics(SAs)on MBC are still *** study employed four representative SAs including sulfamethazine(SMT),sulfamerazine(SMR),sulfadiazine(SDZ),and sulfamethoxazole(SMX),to compare the difference in sorption on *** showed that the sorption capacities and affinities of the four SAs varied with their substituents,hydrophobic properties,and dissociation constants(pKa).Synergistic effect during co-pyrolysis with Fe^(3+)enhanced the sorption performance of MBC towards SAs compared to original *** methods confirmed structural changes of MBC such as the variance in oxygen-containing groups and defective/graphitized *** of modeling pH-dependent sorption revealed that H-bonding orπ-bond assisted H-bonding determined the sorption affinities and capacities of *** particular,the SAs with lower pKa were thermodynamically favorable to form H-bonding with MBC via proton exchange with water *** calculation results quantified the contributions of H-bonding strengths and found that the energies of H-bonding were correlated with affinities of ***,contributions of oxygencontaining groups instead of minerals dominated the H-bonding *** insights from this study can be valuable in exploring engineered BC composites for practical application in field remediation.

关键词： Biochar Antibiotics Sorption capacity Synergistic effect Quantum calculation

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Occurrence and Effects of Microplastics in Lake Ecosystems: Particular Focus on Migration in water and Food Chains

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Reviews of Environmental Contamination and Toxicology 2023年第1期261卷 1-22页

作者： Yin, Lingshi Du, Li Wen, Xiaofeng Huang, Danlian Xiao, Ruihao Wang, Zeyu Su, Hongyu Huang, Jiali Wang, Guangfu Tao, Jiaxi Kang, Yuantai College of Environmental Science and Engineering Hunan University Changsha China Key Laboratory of Environmental Biology and Pollution Control (Hunan University) Ministry of Education Changsha China School of Hydraulic Engineering Changsha University of Science and Technology Changsha China Key Laboratory of Dongting Lake Aquatic Eco-Environmental Control and Restoration of Hunan Province Changsha China Key Laboratory of Water-Sediment Sciences and Water Disaster Prevention of Hunan Province Changsha China

Microplastics have become a research hotspot in the environmental field owing to their persistence and complex ecological effects. Although microplastics have attracted public attention only recently, the microplastic pollution in lake, a unique water system characterized by their irreplaceable ecological value and special hydrodynamic conditions, were increasingly documented, calling for a summary of the most recent advance in this research area. Therefore, the sampling and analysis methods, occurrence, sources, and ecological effects of microplastics in lakes were summarized in this review. Various types of plastics are produced and used in large quantities for different purposes, resulting in microplastic pollution being widespread in lakes worldwide, albeit with different levels and characteristics. Microplastics constantly migrate and transform in lake ecosystems, exerting impacts on ecological, including pollution diffusion and biological toxicity. This review focused on the migration of microplastics in water and food chains, which is a different perspective than that considered in previously published reviews. This review also discussed the limitations of existing studies and made recommendations. Future research directions should include the following: 1) improving the baseline database of microplastic pollution in lakes; (2) unifying the sampling and laboratory analysis methods; (3) exploring the quantitative analysis methods of the sources, transportation, and fate of microplastics; (4) considering more factors to explore the effects of microplastics on lake ecosystems.

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