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

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

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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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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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Characteristics of copper removal and ion release during copper biosorption by Stenotrophomonas maltophilia in presence of benzo[a]pyrene

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Journal of Central South University 2013年第10期20卷 2796-2805页

作者：田云叶锦韶尹华彭辉李取生白洁琼谢丹平 Department of Environmental Engineering Key Laboratory of Water/Soil Toxic Pollutants Control and Bioremediation of Guangdong Higher Education InstitutesJinan University College of Environment and Energy Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters of Ministry of EducationSouth China University of Technology Key Lab of Water and Air Pollution Control of Guangdong Province

The ability of Stenotrophomonas maltophilia was demonstrated to selectively remove Cu2+from Cu(NO3)2 solution under the circumstance that 1 mg/L benzo[a]pyrene(BaP) was either present or not. The removal ratios of 2 and 10 mg/L Cu2+by 0.25 g/L biosorbent are up to 80% and 49% at 10 min, respectively. The biosorption includes ion exchange, NO3 reduction, ion release, and cell oxidation by Cu2+. BaP does not significantly affect Cu2+removal and ion release. Although 2 mg/L Cu2+increases the release of PO4 3, K+, NH4 +and Ca2+, 10 mg/L Cu2+has strong oxidation on cell, and then decreases NO3 reduction and hinders the release of K+, NH4 +and Ca2+. Exogenous cations inhibit the Cu2+biosorption, while additional anions increase the removal ratios of 10 mg/L Cu2+from 52% to 88%.

关键词： biosorption copper benzo[a]pyrene Stenotrophomonas maltophilia

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Carbon-mediated iron valence state transformation for deep aluminum removal toward battery-grade FePO4 recycling

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Separation and Purification technology 2025年 371卷

作者： Feng, Yufa Yang, Liming Yang, Guang Ren, Wei Yi, Genping Wang, Huijie Yu, Haoxuan Xie, Yaohui Zhang, Fen Xue, Shimao Shi, Hui Shao, Penghui Luo, Xubiao School of Chemistry and Chemical Engineering Nanchang University Nanchang330031 China National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization Nanchang Hangkong University Nanchang330063 China School of Life Sciences Key Laboratory of Jiangxi Province for Functional Biology and Pollution Control in Red Soil Regions Jinggangshan University Ji'an343009 China Biomass Molecular Engineering Center and Department of Materials Science and Engineering School of Materials and Chemistry Architecture Anhui Agricultural University Hefei230036 China State Key Lab of Urban Water Resource and Environment School of Civil and Environmental Engineering Harbin Institute of Technology Shenzhen Shenzhen518055 China

A key challenge in the closed-loop recycling of spent lithium iron phosphate is the difficulty in removing aluminum during the regeneration of battery-grade iron phosphate. Our study demonstrates that the carbon-mediated reduction of iron to its ferrous state facilitates the efficient removal of aluminum under controlled pH conditions. The carbon-mediated transfer of electrons from sulfite to Fe3+ and complete reduction to Fe2+, resulting in 99.4 % removal of aluminum in the pH-regulated precipitation de-alumination process. The purified iron phosphate solution is oxidatively precipitated to produce iron phosphate with an Al content as low as 0.00175 %. In-situ Raman, electron paramagnetic resonance (EPR), and the open circuit potential method confirm the formation of low-potential carbon-sulfite complexes and their role in accelerating electron transfer. A life cycle analysis shows that the process reduces energy consumption by 28.72 % and greenhouse gas emissions by 29.47 % while improving profit by nearly 369 % compared to conventional hydrometallurgical processes. The high-efficiency, clean technology proposed in this study for regenerating low-aluminum battery-grade iron phosphate will significantly contribute to the sustainable development of the lithium iron phosphate battery industry. © 2025

关键词： Paramagnetic resonance

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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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