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Hydroxyl radical production by abiotic oxidation of pyrite under estuarine conditions:The effects of aging,seawater anions and illumination

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Journal of Environmental Sciences 2024年第1期135卷 715-727页

作者： Ruixue Liu Yinshun Dai Yucheng Feng Shiwen Sun Xiaodong Zhang Chunjiang An Shan Zhao Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong UniversityQingdao 266237China Department of Building Civil and Environmental EngineeringConcordia UniversityMontrealQC H3G 1M8Canada

Pyrite is widely distributed in estuarine sediments as an inexpensive natural Fenton-like reagent,however,the mechanism on the hydroxyl radical(HO^(·))production by pyrite under estuarine environmental conditions is still poorly understood.The batch experiments were performed to investigate the effects of estuarine conditions including aging(in air,in water),seawater anions(Cl^(-),Br^(-)and HCO_(3)^(-))and light on the HO^(·)production by pyrite oxidation.The one-electron transfer dominated the process from O_(2) to HO^(·)induced by oxidation of pyrite.The Fe(oxyhydr)oxide coatings on the surface of pyrite aged in air and water consumed hydrogen peroxide while mediating the electron transfer,and the combined effect of the two resulted in a suppression of HO^(·)production in the early stage of aging and a promotion of HO^(·)production in the later stage of aging.Corrosion of the surface oxide layers by aggressive anions was the main reason for the inhibition of HO^(·)production by Cl^(-)and Br^(-),and the generation of Cl^(·)and Br^(·)may also play a role in the scavenging of HO^(·).HCO_(3)^(-)increased the average rate of HO^(·)production through surface-CO_(2) complexes formed by adsorption on the surface of pyrite.The significant enhancement of HO^(·)production under light was attributed to the formation of photoelectrons induced by photochemical reactions on pyrite and its surface oxide layers.These findings provide new insights into the environmental chemical behavior of pyrite in the estuary and enrich the understanding of natural remediation of estuarine environments.

关键词： Hydroxyl radical Pyrite oxidation Aging anions Irradiation

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Theoretical investigation of excited dipole bound states of alkali-containing diatomic anions

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Chinese Physics B 2024年第5期33卷 389-393页

作者：连艺肖利丹边丽丽徐海峰闫冰 Institute of Atomic and Molecular Physics Jilin UniversityChangchun 130012China

Information about electronic excited states of molecular anions plays an important role in investigating electron attachment and detachment processes.Here we present a high-level theoretical study of the electronic structures of 12 alkali-metal-containing diatomic anions MX-(MX = LiH,LiF,LiCl,NaF,NaCl,NaBr,RbCl,KCl,KBr,RbI,KI and CsI).The equation-of-motion electron-attachment coupled-cluster singles and doubles(EOM-EA-CCSD) method is used to calculate the electron binding energies(EBEs) of 10 electronic excited states of each of the 12 molecule anions.With addition of different s-/p-/d-type diffusion functions in the basis set,we have identified possible excited dipole bound states(DBSs) of each anion.With the investigation of EBEs on the 12 MXs with dipole moment(DM) up to 12.1 D,we evaluate the dependence of the number of anionic excited DBSs on molecular DM.The results indicate that there are at least two or three DBSs of anions with a molecular DM larger than 7 D and a molecule with DM > 10 D can sustain a π-DBS of the anion.Our study has some implications for the excited DBS electronic states of alkali-metal-containing diatomic molecules.

关键词： anions dipole bound states alkali-metal-containing diatomic molecules

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Enhancement of catalytic activity for hydrogenation of nitroaromatic by anionic metal-organic framework

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Chinese Chemical Letters 2024年第3期35卷 144-148页

作者： Qi Wu Anyang Li Ruibo He Yaxi Wu Lei Hou Guoping Yang Wenyan Zhang Yao-Yu Wang Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education College of Chemistry&Materials ScienceNorthwest UniversityXi'an 710127China

Nitroaromatic hydrogenation catalysis without precious metals remains a longstanding challenge.The rate of electron transfer is the crucial factor affecting hydrogenation catalysis.Herein,an ionic Cd-based metal-organic framework(I-Cd-MOF)exhibiting a unique structure with one-dimensional(1D)opening nanochannels and good electron transfer ability was synthesized for catalyzing hydrogenation of 4-nitrophenol(4-NP).The catalytic activity of the unique I-Cd-MOF without noble metals is detected,which is higher than most reported noble metal catalysts.Remarkably,the reaction rate of I-Cd-MOF(4.28 min^(-1))is about 47.6 times higher than that of the Cd-based neutral MOF(N-Cd-MOF)with the similar crystalline structure.Liquid chromatograph mass spectrometer(LC-MS)and theoretical results demonstrate that 4-NP and five intermediates are stabilized in the channels of I-Cd-MOF,which increases the possibility of contact with H^*and H_(2)g enerated at the Cd sites.The I-Cd-MOF was extended to other nitroaromatic hydrogenation catalysis,which still displays excellent activity.More importantly,the I-MOF@Filter membrane was successfully constructed for continuous hydrogenation catalytic reactions,which maintains a high catalytic performance after 7 cycles of recycling without washing.This work fills in the application of the I-MOFs in hydrogenation catalytic reactions and provides an effective way for the rapid and green degradation of nitroaromatic compounds.

关键词： anions Metal-organic frameworks Catalysis Electron transfer Hydrogen production

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anions Distorting Triggering Ferroelectricity in a Molecular Crystal

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Chinese Journal of Chemistry 2022年第18期40卷 2226-2231页

作者： Si-Yu Ye Jing-Yuan Liu Liang Tong Yan-Ning Wang Min Wan Abraham Mensah Xiao-Fan Jiang Jun-Yi Li Li-Zhuang Chen School of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiangJiangsu212003 China College of Chemistry Key Laboratory of Theoretical&Computational Photochemistry of Ministry of EducationBeijing Normal UniversityBeijing100875 China

Recently,molecular ferroelectrics have attracted more and more attention due to their structural diversity,low cost of manufacture,and environmental-friendly processing.However,most of the design strategies for molecular ferroelectrics have focused on the selection and modification of cations,and the use of anions has been rarely reported.Here,introducing distorted[CuBr_(4)]^(2-) tetrahedra,we obtained a high curie temperature(T_(c))ferroelectric,[cyclopentylammonium]_(2)CuBr_(4),with a T_(c) as high as 393 K,and exceeding commercial and most of reported molecular ferroelectric BaTiO_(3)(393 K).Variable-temperature hysteresis loop shows the nonlinear P-E loop of the crystal under a wide temperature range.Variable-temperature single-crystal X-ray diffraction revealed that the Aizu expression can be written as mmmFmm2.In short,this work will inspire more creative strategies by exploiting the tunability of the anion module.

关键词： Molecular ferroelastic anions Design strategy Organic-inorganic hybrid composites Phase transitions

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The role of hydrated anions in hydration lubrication

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Nano Research 2023年第1期16卷 1096-1100页

作者： Zibo Li Qian Liu Qiang Li Mingdong Dong Key Laboratory of Colloid and Interface Chemistry of the Ministry of Education School of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China Interdisciplinary Nanoscience Center(iNANO) Aarhus UniversityAarhus C DK-8000Denmark

Hydration lubrication has long been invoked to account for the ultralow sliding friction between charged surfaces in aqueous environments,but still not well understood at molecular-level.Herein,we explored the lubrication effect of hydrated halogen anions on positively charged surface at the atomic scale by using three-dimensional atomic force microscopy and friction force microscopy.Atomically resolved three-dimensional imaging revealed that the anion layer was topped by a few hydration layers.The mechanical properties of the hydration layers were found mainly dependent on the concentration of electrolyte solutions and independent of the species of hydrated anions.Atomic-scale friction experiments showed that the hydration friction coefficient and friction dissipation at low concentrations were orders of magnitude lower than that at high concentrations and in pure water.Superlubricity can be achieved in low concentration electrolyte solution.These results indicated that the changes of electrolyte solution concentrations led to different adsorption state of anions on the positively charged surface which gave rise to the difference of the friction behaviors.The findings in this study reveal the role of hydrated anions in hydration lubrication and provide deep insights into the origins of hydration lubrication.

关键词： hydration lubrication hydration structures anions friction three-dimensional atomic force microscopy(3D-AFM)

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Trace Analysis of anions in Perfluorodecalin by Green Liquid-Liquid Extraction Combined with Ion Chromatography

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Journal of Analysis and Testing 2022年第3期6卷 346-351页

作者： Sheng Liu Jian Xu Yu Lu Yong Huang Zhi-Wen Fang Mei Lv Li-Tao Wang The Technical Center of Zibo Customs Zibo 255031China Suzhou Jieshitong Medical Equipment Co. Ltd.Suzhou 215000China School of Pharmacy Jining Medical UniversityJining 272000China Jining Medical University No.669Xueyuan RoadRizhao 276800China

Perfluoronaphthenes,with inert chemical and biological properties and ability to dissolve large amounts of oxygen,have received the most attention in medical applications.However,the excessive anion contained may cause some side effects.Herein,liquid-liquid extraction technique with shaking and ultrasonic extraction was used for the trace analysis of five anions(F^(-),Cl^(-),NO_(3)^(-),PO_(4)^(3-),SO_(4)^(2-))in perfluorodecalin using water as green extractant.The optimum pretreatment technology and ion chromatography detection conditions were established.Good linearity was observed in each concentration range,and the linear correlation coefficient(R^(2))was better than 0.997.The limits of detection(S/N=3)of five anions from perfluorodecalin were 3.2,5.5,14.2,23.2 and 29.5μg/L,respectively.The established method with high sensitivity and accuracy has been successfully appliedfor the determination of five anions in three perfluorodecalin products,which provides a basis for further development of green detection and quality standard formulation in perfluorodecalin and other fluorocarbon solvents.

关键词： Perfluorodecalin Trace analysis anions Liquid-liquid extraction Ion chromatography

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Effect of electrolyte anions on the cycle life of a polymer electrode in aqueous batteries

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eScience 2022年第1期2卷 110-115页

作者： Ye Zhang Lihong Zhao Yanliang Liang Xiaojun Wang Yan Yao Department of Electrical and Computer Engineering Materials Science and Engineering ProgramUniversity of HoustonHoustonTX77204USA Texas Center for Superconductivity at the University of Houston HoustonTX77204USA

Redox polymers are a class of high-capacity, low-cost electrode materials for electrochemical energy storage, butthe mechanisms governing their cycling stability are not well understood. Here we investigate the effect of anionson the longevity of a p-dopable polymer through comparing two aqueous zinc-based electrolytes. Galvanostaticcycling studies reveal the polymer has better capacity retention in the presence of triflate anions than that withsulfate anions. Based on electrode microstructural analysis and evolution profiles of the cell stacking pressure, theorigin of capacity decay is ascribed to mechanical fractures induced by volume change of the polymer activematerials during repeated cycling. The volume change of the polymer with the triflate anion is 61% less than thatwith the sulfate anion, resulting in fewer cracks in the electrodes. The difference is related to the different anionsolvation structures—the triflate anion has fewer solvated water molecules compared with the sulfate anion,leading to smaller volume expansion. This work highlights that anions with low solvation degree are preferablefor long-term cycling.

关键词： Aqueous batteries Polymer electrode anions Volume chang

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Turn-on fluorescence detection of specific inorganic anions by Zr(Ⅳ)-MOF with amino-functional group

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钨科技(英文) 2023年第2期5卷 217-224页

作者： Jing Dong Shi-Qing Wang Xiao-Yu Zhang Zi-Qing Huang Xiu-Du Zhang Wei-Yin Sun Coordination Chemistry Institute State Key Laboratory of Coordination ChemistrySchool of Chemistry and Chemical EngineeringNanjing National Laboratory of MicrostructuresCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210023China Scientific Research Institute Nanjing Tech UniversityNanjing 211816China College of Chemistry and Materials Science Key Laboratory of Functional Molecular Solids Ministry of EducationAnhui Laboratory of Molecule-Based MaterialsAnhui Key Laboratory of Functional Molecular SolidsAnhui Normal UniversityWuhu 241002China

Inorganic anions such as phosphates and carbonates are essential in the natural system and it is important for the detec-tion of such species.In this work,the fluorescence sensing capacity of Zr(IV)framework with an amino-functional group,namely UiO-66-NH_(2),towards specific inorganic anions was investigated in aqueous media.The results revealed that the fluorescence emission intensity of UiO-66-NH2 could be strongly enhanced by phosphate and carbonate anions including HPO_(4)^(2-),H_(2)PO_(4)^(-),PO_(4)^(3-),P_(2)O_(7)^(4-),HCO_(3)^(-)and CO_(3)^(2-),implying its sensing capacity towards phosphate and carbonate anions.Furthermore,fluorescence titration experiments exhibit that the emission intensity enhancement ratio depends linearly on the concentration of anions,suggesting the possibility of quantitative detection of these anions.Further studies suggest that the sensing of UiO-66-NH,towards HPO_(4)^(2-)/PO_(4)^(3-)/P_(2)O_(4)^(-)/HCO_(3)^(-)/CO_(2)-could be ascribed to the collapse of the framework,while that for H_(2)PO_(4)-could be attributed to the adsorption of H,PO4-by UiO-66-NH2 with hydrogen bonding interactions between H,PO4-and the amino group of UiO-66-NH_(2) supported by the different fluorescence response of UiO-66 and UiO-66-NH,towards the anions.

关键词： Zr(IV)framework UiO-66-NH_(2) anions Sensing Turn-on fluorescence

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Effect of amendments on the leaching behavior of alkaline anions and metal ions in bauxite residue

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Journal of Environmental Sciences 2019年第11期31卷 74-81页

作者： Tao Tian Jinaju Zhou Feng Zhu Yuzhen Ye Ying Guo William Hartley Shengguo Xue School of Metallurgy and Environment Central South University Changsha 410083 China Crop and Environment Sciences Department Harper Adams University Newport Shropshire TF10 8NB UK

A column leaching experiment was used to investigate the efficacy of amendments on their ability to remove alkaline anions and metal ions from bauxite residue leachates.Treatments included,simulated acid rain (AR),phosphogypsum + vermicompost (PVC),phosphogypsum + vermicompost + simulated acid rain (PVA),and biosolids + microorganisms (BSM) together with controls (CK).Results indicated that amendment could effectively reduce the leachate pH and EC values,neutralize OH-,CO32-,HCO3-,and water soluble alkali,and suppress arsenic (As) content.Correlation analysis revealed significant linear correlations with pH and concentrations of OH-,CO32-,HCO3-,water-soluble alkali,and metal ions.BSM treatment showed optimum results with neutralizing anions (OH-,CO32-,and HCO3-),water soluble alkali,and removal of metal ions (Al,As,B,Mo,V,and Na),which was attributed to neutralization from the generation of small molecular organic acids and organic matter during microbial metabolism.BSM treatment reduced alkaline anions and metal ions based on neutralization reactions in bauxite residue leachate,which reduced the potential pollution effects from leachates on the soil surrounding bauxite residue disposal areas.

关键词： Bauxite residue leachate Amendments Alkaline anions Metal ions

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Impact of anions on the heavy metals release from marine sediments

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Journal of Environmental Sciences 2006年第6期18卷 1216-1220页

作者： ZHONG Ai-ping GUO Shu-hai LI Feng-mei LI Gang JIANG Ke-xu Institute of Applied Ecology Chinese Academy of Sciences Shenyang 110016 China Graduate School of Chinese Academy of Sciences Beijing 100039 China Institute of Environmental Science Huludao 125000 China

Marine sediments from Lianshan Bay in Huludao, China, were studied in laboratory. A series of simulated experiments were carried out to investigate the influences of three kinds of anions CL^-, SO4^2- and HCO3^- on the release ofCd, Pb, Cu and Zn from the sediments. The results showed that the sequences about the impact of the three anions were Cl^-〉HCO3^-〉SO4^2＋. The release potential of heavy metals in the presence of each anions was in the following order： Cd≥Cu 〉Zn≈Pb. The correlations were positive between CI content and the quantity of Cd released from the marine sediment, whereas there was no significant relationship between CI content and amount of Cu and Zn released. For SO4^2- and HCO3^-, the release of the heavy metals from marine sediments was not obvious.

关键词： marine sediments anions heavy metals release

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