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Effects of two transition metal sulfate salts on secondary organic aerosol formation in toluene/NO

Biwu CHU, Jiming HAO, Junhua LI, Hideto TAKEKAWA, Kun WANG, Jingkun JIANG

《环境科学与工程前沿(英文)》 2013年 第7卷 第1期   页码 1-9 doi: 10.1007/s11783-012-0476-x

摘要: Aerosol phase reactions play a very important role on secondary organic aerosol (SOA) formation, and metal-containing aerosols are important components in the atmosphere. In this study, we tested the effects of two transition metal sulfate salts, manganese sulfate (MnSO ) and zinc sulfate (ZnSO ), on the photochemical reactions of a toluene/NO photooxidation system in a 2 m smog chamber. By comparing photochemical reaction products of experiments with and without transition metal sulfate seed aerosols, we evaluated the effects of transition metal sulfate seed aerosols on toluene consumption, NO conversion and the formation of ozone and SOA. MnSO and ZnSO seed aerosols were found to have similar effects on photochemical reactions, both enhance the SOA production, while showing negligible effects on the gas phase compounds. These observations are consistent when varying metal sulfate aerosol concentrations. This is attributed to the catalytic effects of MnSO and ZnSO seed aerosols which may enhance the formation of condensable semivolatile compounds. Their subsequent partitioning into the aerosol phase leads to the observed SOA formation enhancement.

关键词: manganese sulfate     zinc sulfate     seed aerosols     toluene photooxidation     secondary organic aerosol    

Zero-valent manganese nanoparticles coupled with different strong oxidants for thallium removal from

Keke Li, Huosheng Li, Tangfu Xiao, Gaosheng Zhang, Aiping Liang, Ping Zhang, Lianhua Lin, Zexin Chen, Xinyu Cao, Jianyou Long

《环境科学与工程前沿(英文)》 2020年 第14卷 第2期 doi: 10.1007/s11783-019-1213-5

摘要: • Nano zero-valent manganese (nZVMn, Mn0) is synthesized via borohydrides reduction. • Mn0 combined with persulfate/hypochlorite is effective for Tl removal at pH 6-12. • Mn0 can activate persulfate to form hydroxyl and sulfate radicals. • Oxidation-induced precipitation and surface complexation contribute to Tl removal. • Combined Mn0-oxidants process is promising in the environmental field. Nano zero-valent manganese (nZVMn, Mn0) was prepared through a borohydride reduction method and coupled with different oxidants (persulfate (S2O82−), hypochlorite (ClO−), or hydrogen peroxide (H2O2)) to remove thallium (Tl) from wastewater. The surface of Mn0 was readily oxidized to form a core-shell composite (MnOx@Mn0), which consists of Mn0 as the inner core and MnOx (MnO, Mn2O3, and Mn3O4) as the outer layer. When Mn0 was added alone, effective Tl(I) removal was achieved at high pH levels (>12). The Mn0-H2O2 system was only effective in Tl(I) removal at high pH (>12), while the Mn0-S2O82− or Mn0-ClO− system had excellent Tl(I) removal (>96%) over a broad pH range (4–12). The Mn0-S2O82− oxidation system provided the best resistance to interference from an external organic matrix. The isotherm of Tl(I) removal through the Mn0-S2O82− system followed the Freundlich model. The Mn0 nanomaterials can activate persulfate to produce sulfate radicals and hydroxyl radicals. Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy suggested that oxidation-induced precipitation, surface adsorption, and electrostatic attraction are the main mechanisms for Tl(I) removal resulting from the combination of Mn0 and oxidants. Mn0 coupled with S2O82−/ClO− is a novel and effective technique for Tl(I) removal, and its application in other fields is worthy of further investigation.

关键词: Nano zero-valent manganese     Thallium     Adsorption     Oxidation     Sulfate radical     Hydroxyl radical    

Effects of natural zeolite and sulfate ions on the mechanical properties and microstructure of plastic

《结构与土木工程前沿(英文)》 2022年 第16卷 第1期   页码 86-98 doi: 10.1007/s11709-021-0793-x

摘要: One of the strategic materials used in earth-fill embankment dams and in modifying and preventing groundwater flow is plastic concrete (PlC). PlC is comprised of aggregates, water, cement, and bentonite. Natural zeolite (NZ) is a relatively abundant mineral resource and in this research, the microstructure, unconfined strength, triaxial behavior, and permeability of PlC made with 0%, 10%, 15%, 20%, and 25% replacement of cement by NZ were studied. Specimens of PIC-NZ were subjected to confined conditions and three different confining pressures of 200, 350, and 500 kPa were used to investigate their mechanical behavior and permeability. To study the effect of sulfate ions on the properties of PlC-NZ specimens, the specimens were cured in one of two different environments: normal condition and in the presence of sulfate ions. Results showed that increasing the zeolite content decreases the unconfined strength, elastic modulus, and peak strength of PlC-NZ specimens at the early ages of curing. However, at the later ages, increasing the zeolite content increases unconfined strength as well as the peak strength and elastic modulus. Specimens cured in the presence of sulfate ions indicated lower permeability, higher unconfined strength, elastic modulus, and peak strength due to having lower porosity.

关键词: plastic concrete     sulfate resistance     natural zeolite     triaxial compression test     SEM     permeability    

A time−space porosity computational model for concrete under sulfate attack

《结构与土木工程前沿(英文)》 doi: 10.1007/s11709-023-0985-7

摘要: The deterioration of the microscopic pore structure of concrete under external sulfate attack (ESA) is a primary cause of degradation. Nevertheless, little effort has been invested in exploring the temporal and spatial development of the porosity of concrete under ESA. This study proposes a mechanical–chemical model to simulate the spatiotemporal distribution of the porosity. A relationship between the corrosion damage and amount of ettringite is proposed based on the theory of volume expansion. In addition, the expansion strain at the macro-scale is obtained using a stress analysis model of composite concentric sphere elements and the micromechanical mean-field approach. Finally, considering the influence of corrosion damage and cement hydration on the diffusion of sulfate ions, the expansion deformation and porosity space−time distribution are obtained using the finite difference method. The results demonstrate that the expansion strains calculated using the suggested model agree well with previously reported experimental results. Moreover, the tricalcium aluminate concentration, initial elastic modulus of cement paste, corrosion damage, and continuous hydration of cement significantly affect concrete under ESA. The proposed model can forecast and assess the porosity of concrete covers and provide a credible approach for determining the residual life of concrete structures under ESA.

关键词: expansion deformation     porosity     internal expansion stress     external sulfate attack     mechanical–chemical coupling model    

Effects of humic acid and surfactants on the aggregation kinetics of manganese dioxide colloids

Xiaoliu HUANGFU,Yaan WANG,Yongze LIU,Xixin LU,Xiang ZHANG,Haijun CHENG,Jin JIANG,Jun MA

《环境科学与工程前沿(英文)》 2015年 第9卷 第1期   页码 105-111 doi: 10.1007/s11783-014-0726-1

摘要: The aggregation of common manganese dioxide (MnO ) colloids has great impact on their surface reactivity and therefore on their fates as well as associated natural and synthetic contaminants in engineered (e.g. water treatment) and natural aquatic environments. Nevertheless, little is known about the aggregation kinetics of MnO colloids and the effect of humic acid (HA) and surfactants on these. In this study, the early stage aggregation kinetics of MnO nanoparticles in NaNO and Ca(NO ) solutions in the presence of HA and surfactants (i.e., sodium dodecyl sulfate (SDS), and polyvinylpyrrolidone (PVP)) were modeled through time-resolved dynamic light scattering. In the presence of HA, MnO colloids were significantly stabilized with a critical coagulation concentration (CCC) of ~300 mmol·L NaNO and 4 mmol·L Ca(NO ) . Electrophoretic mobility (EPM) measurements confirmed that steric hindrance may be primarily responsible for increasing colloidal stability in the presence of HA. Moreover, the molecular and/or chemical properties of HA might impact its stabilizing efficiency. In the case of PVP, only a slight increase of aggregation kinetics was observed, due to steric reactions originating from adsorbed layers of PVP on the MnO surface. Consequently, higher CCC values were obtained in the presence of PVP. However, there was a negligible reduction in MnO colloidal stability in the presence of 20 mg·L SDS.

关键词: humic acid     surfactant     aggregation kinetics     drinking water     manganese dioxide colloids    

Tripotassium citrate monohydrate derived carbon nanosheets as a competent assistant to manganese dioxide

《化学科学与工程前沿(英文)》 2022年 第16卷 第3期   页码 420-432 doi: 10.1007/s11705-021-2065-7

摘要: Production cost, capacitance, and electrode materials safety are the key factors to be concerned about for supercapacitors. In this work, a type of carbon nanosheets was produced through the carbonization of tripotassium citrate monohydrate and nitric acidification. Subsequently, a well-designed manganese dioxide/carbon nanosheets composite was synthesized through hydrothermal treating. The carbon nanosheets served as the substrate for growing the manganese dioxide, regulating its distribution, and preventing it from inhomogeneous dimensions and severe agglomeration. Many manganese dioxide nanosheets grew vertically on the numerous functional groups generated on the surface of the carbon nanosheets during acidification. The synergistic combination of carbon nanosheets and manganese dioxide tailors the electrochemical performance of the composite, which benefits from the excellent conductivity and stability of carbon nanosheets. The carbon nanosheets derived from tripotassium citrate monohydrate are conducive to the remarkable performance of manganese dioxide/carbon nanosheets electrode. Finally, an asymmetric supercapacitor with active carbon as the cathode and manganese dioxide/carbon nanosheets as the anode was assembled, achieving an outstanding energy density of 54.68 Wh·kg–1 and remarkable power density of 6399.2 W·kg–1 superior to conventional lead-acid batteries. After 10000 charge-discharge cycles, the device retained 75.3% of the initial capacitance, showing good cycle stability. Two assembled asymmetric supercapacitors in series charged for 3 min could power a yellow light emitting diode with an operating voltage of 2 V for 2 min. This study may provide valuable insights for applying carbon materials and manganese dioxide in the energy storage field.

关键词: carbon nanosheets     manganese dioxide     asymmetric supercapacitors     energy density     power density    

Catalytic activity of manganese oxide supported on alumina in the synthesis of quinoxalines

Rekha M., H. Kathyayini, N. Nagaraju

《化学科学与工程前沿(英文)》 2013年 第7卷 第4期   页码 415-421 doi: 10.1007/s11705-013-1360-3

摘要: Two catalysts, alumina and manganese oxide supported on alumina, have been prepared by calcination and precipitation-impregnation methods, respectively. The catalysts are characterised by the following techniques: Brunner-Emmett-Teller-N adsorption-desorption for surface area, temperature programmed desorption of NH and -butyl amine back titration methods for surface acidity, powder X-ray diffraction for textural properties, and Fourier transform infrared spectroscopy for the anionic radicals. The catalytic activity has been determined under heterogeneous conditions in the condensation reaction between -phenylenediamine and benzil. The product purity is checked by thin-layer chromatography and melting point. The products are also analysed by LC-MS and H-NMR techniques. The yields of the products have been found to be good and catalysts exhibited excellent recyclability. The effect of changing the reaction parameters such as temperature, reaction time, amount of the catalyst, nature of solvent and molar ratio of reactants on the yield of the product has been studied. The surface acidity of the catalysts plays an important role in activating the reaction.

关键词: alumina     manganese oxide deposited on alumina     quinoxaline synthesis    

Coextraction of vanadium and manganese from high-manganese containing vanadium wastewater by a solvent

Zishuai Liu, Yimin Zhang, Zilin Dai, Jing Huang, Cong Liu

《化学科学与工程前沿(英文)》 2020年 第14卷 第5期   页码 902-912 doi: 10.1007/s11705-019-1887-z

摘要: High-manganese containing vanadium wastewater (HMVW) is commonly produced during the vanadium extraction process from vanadium titano-magnetite. HMVW cannot be reused and discharged directly, and is harmful to the environment and affect product quality due to heavy metals in the wastewater. The wastewater is usually treated by lime neutralization, but valuable metals (especially V and Mn) cannot be recovered. In this study, an efficient and environmentally friendly method was developed to recover valuable metals by using a solvent extraction-precipitation process. In the solvent extraction process, 98.15% of vanadium was recovered, and the V O product, with a purity of 98.60%, was obtained under optimal conditions. For the precipitation process, 91.05% of manganese was recovered as MnCO which meets the III grade standard of HG/T 2836-2011. Thermodynamic simulation analysis indicated that MnCO was selectively precipitated at pH 6.5 while Mg and Ca could hardly be precipitated. The results of X-ray diffraction and scanning electron microscopy demonstrated that the obtained V O and MnCO displayed a good degree of crystallinity. The treated wastewater can be returned for leaching, and resources (V and Mn) in the wastewater were utilized efficiently in an environmentally friendly way. Therefore, this study provides a novel method for the coextraction of V and Mn from HMVW.

关键词: high-manganese containing vanadium wastewater     solvent extraction     carbonate precipitation     vanadium titano-magnetite     valuable metal recovery    

Biological conversion pathways of sulfate reduction ammonium oxidation in anammox consortia

Zhen Bi, Deqing Wanyan, Xiang Li, Yong Huang

《环境科学与工程前沿(英文)》 2020年 第14卷 第3期 doi: 10.1007/s11783-019-1217-1

摘要: The SRAO phenomena tended to occur only under certain conditions. High amount of biomass and non-anaerobic condition is requirement for SRAO. Anammox bacteria cannot oxidize ammonium with sulfate as electron acceptor. AOB and AnAOB are mainly responsible for ammonium conversion. Heterotrophic sulfate reduction mainly contributed to sulfate conversion. For over two decades, sulfate reduction with ammonium oxidation (SRAO) had been reported from laboratory experiments. SRAO was considered an autotrophic process mediated by anammox bacteria, in which ammonium as electron donor was oxidized by the electron acceptor sulfate. This process had been attributed to observed transformations of nitrogenous and sulfurous compounds in natural environments. Results obtained differed largely for the conversion mole ratios (ammonium/sulfate), and even the intermediate and final products of sulfate reduction. Thus, the hypothesis of biological conversion pathways of ammonium and sulfate in anammox consortia is implausible. In this study, continuous reactor experiments (with working volume of 3.8L) and batch tests were conducted under normal anaerobic (0.2≤DO<0.5 mg/L) / strict anaerobic (DO<0.2 mg/L) conditions with different biomass proportions to verify the SRAO phenomena and identify possible pathways behind substrate conversion. Key findings were that SRAO occurred only in cases of high amounts of inoculant biomass under normal anaerobic condition, while absent under strict anaerobic conditions for same anammox consortia. Mass balance and stoichiometry were checked based on experimental results and the thermodynamics proposed by previous studies were critically discussed. Thus anammox bacteria do not possess the ability to oxidize ammonium with sulfate as electron acceptor and the assumed SRAO could, in fact, be a combination of aerobic ammonium oxidation, anammox and heterotrophic sulfate reduction processes.

关键词: Anammox bacteria     Autotrophic     Biological conversion     Sulfate reducing ammonium oxidation (SRAO)    

The role of manganese oxides in the activation of peroxymonosulfate (PMS)

Jianzhi Huang, Huichun Zhang

《环境科学与工程前沿(英文)》 2019年 第13卷 第5期 doi: 10.1007/s11783-019-1158-8

摘要: Manganese oxides (MnOx) have been demonstrated to be effective materials to activate Oxone (i.e., PMS) to degrade various contaminants. However, the contribution of direct oxidation by MnOx to the total contaminant degradation under acidic conditions was often neglected in the published work, which has resulted in different and even conflicting interpretations of the reaction mechanisms. Here, the role of MnOx (as both oxidants and catalysts) in the activation of Oxone was briefly discussed. The findings offered new insights into the reaction mechanisms in PMS-MnOx and provided a more accurate approach to examine contaminant degradation for water/wastewater treatment.

关键词: Peroxymonosulfate     Manganese oxides     Catalyst     Oxidant    

Multivalent manganese oxides with high electrocatalytic activity for oxygen reduction reaction

Xiangfeng Peng, Zhenhai Wang, Zhao Wang, Yunxiang Pan

《化学科学与工程前沿(英文)》 2018年 第12卷 第4期   页码 790-797 doi: 10.1007/s11705-018-1706-y

摘要: A noble-metal-free catalyst based on both Mn O and MnO was prepared by using the dielectric barrier discharge technique at moderate temperature. The prepared catalyst shows a higher electrocatalytic activity towards the oxygen reduction reaction than the catalyst prepared by using the traditional calcination process. The enhanced activity could be due to the coexistence of manganese ions with different valences, the higher oxygen adsorption capacity, and the suppressed aggregation of the catalyst nanoparticles at moderate temperature. The present work would open a new way to prepare low-cost and noble-metal-free catalysts at moderate temperature for more efficient electrocatalysis.

关键词: oxygen reduction reaction     manganese oxides     mixed valences of manganese     oxygen adsorption     dielectric barrier discharge    

Chemical composition and formation mechanisms in the cathode-electrolyte interface layer of lithium manganese

Sahithya REDDIVARI, Christian LASTOSKIE, Ruofei WU, Junliang ZHANG

《能源前沿(英文)》 2017年 第11卷 第3期   页码 365-373 doi: 10.1007/s11708-017-0500-8

摘要: Lithium manganese oxide (LiMn O ) is a principal cathode material for high power and high energy density electrochemical storage on account of its low cost, non-toxicity, and ease of preparation relative to other cathode materials. However, there are well-documented problems with capacity fade of lithium ion batteries containing LiMn O . Experimental observations indicate that the manganese content of the electrolyte increases as an electrochemical cell containing LiMn O ages, suggesting that active material loss by dissolution of divalent manganese from the LiMn O surface is the primary reason for reduced cell life in LiMn O batteries. To improve the retention of manganese in the active material, it is key to understand the reactions that occur at the cathode surface. Although a thin layer of electrolyte decomposition products is known to form at the cathode surface, the speciation and reaction mechanisms of Mn in this interface layer are not yet well understood. To bridge this knowledge gap, reactive force field (ReaxFF) based molecular dynamics was applied to investigate the reactions occurring at the LiMn O cathode surface and the mechanisms that lead to manganese dissolution. The ReaxFFMD simulations reveal that the cathode-electrolyte interface layer is composed of oxidation products of electrolyte solvent molecules including aldehydes, esters, alcohols, polycarbonates, and organic radicals. The oxidation reaction pathways for the electrolyte solvent molecules involve the formation of surface hydroxyl species that react with exposed manganese atoms on the cathode surface. The presence of hydrogen fluoride (HF) induces formation of inorganic metal fluorides and surface hydroxyl species. Reaction products predicted by ReaxFF-based MD are in agreement with experimentally identified cathode-electrolyte interface compounds. An overall cathode-electrolyte interface reaction scheme is proposed based on the molecular simulation results.

关键词: lithium manganese oxide batteries     reactive force field (ReaxFF)     cathode-electrolyte interface layer     molecular dynamics    

The solubility of cefquinome sulfate in pure and mixed solvents

Rongbao Qi,Jingkang Wang,Junxiao Ye,Hongxun Hao,Ying Bao

《化学科学与工程前沿(英文)》 2016年 第10卷 第2期   页码 245-254 doi: 10.1007/s11705-016-1569-z

摘要: Solid-liquid equilibrium data of cefquinome sulfate is important to develop industrial crystallization processes for cefquinome sulfate. The solubilities of cefquinome sulfate in five pure solvents (methanol, ethanol, ethylene glycol, acetic acid and water) from 277.15 to 305.15 K and in a binary acetone-water solvent from 278.15 to 293.15 K were measured at atmospheric pressure. The pure-solvent solubility data was correlated to the modified Apelblat and Van’t Hoff equations whereas the mixed-solvent system data was correlated to the modified Apelblat, Van’t Hoff, CNIBS/R-K and Jouyban-Acree models. It was found that the solubilities of cefquinome sulfate in all tested solvents decreased with the increasing of temperature. In addition, the thermodynamic properties of the dissolution processes, including standard Gibbs free energy, enthalpy and entropy changes, were calculated using the Van’t Hoff equation. It was found that the dissolution of cefquinome sulfate is exothermic.

关键词: cefquinome sulfate     solubility     thermodynamic properties    

Effects of metal ions on the morphology of calcium sulfate hemihydrate whiskers by hydrothermal method

Tianjie Liu, Hao Fan, Yanxia Xu, Xingfu Song, Jianguo Yu

《化学科学与工程前沿(英文)》 2017年 第11卷 第4期   页码 545-553 doi: 10.1007/s11705-017-1665-8

摘要: The effects of Na , Mg , Al and Fe ion concentrations on the crystal morphology of calcium sulfate hemihydrate whiskers formed via a hydrothermal method have been studied. In the presence of Al concentrations higher than 1×10 mol/L the whiskers were significantly shorter and thicker and the presence of Mg and Fe resulted in shorter whiskers. The presence of Na did not affect the morphology of the whiskers. Through elemental analysis, it was determined that Mg and Al were selectively adsorbed on the surfaces of the crystals, whereas Fe underwent a hydrolysis reaction to form a brown precipitate which decreased the ion concentration in the solution. These results indicate that in raw materials used for the industrial preparation of calcium sulfate whiskers, Al and Fe should be removed and the Mg concentration should be less than 8 × 10 mol/L in order to obtain pure whiskers with high aspect ratios.

关键词: metal ions     morphology     calcium sulfate hemihydrate whiskers     hydrothermal method     selective adsorption    

PICRUSt2 functionally predicts organic compounds degradation and sulfate reduction pathways in an acidogenic

《环境科学与工程前沿(英文)》 doi: 10.1007/s11783-021-1481-8

摘要:

For comprehensive insights into the influences of sulfate on performance, microbial community and metabolic pathways in the acidification phase of a two-phase anaerobic system, a laboratory-scale acidogenic bioreactor was continuously operated to treat wastewater with elevated sulfate concentrations from 2000 to 14000 mg/L.

关键词: Acidogenic phase reactor     High-sulfate wastewater     Sulfate reduction     Acidogenic fermentation     PICRUSt2    

标题 作者 时间 类型 操作

Effects of two transition metal sulfate salts on secondary organic aerosol formation in toluene/NO

Biwu CHU, Jiming HAO, Junhua LI, Hideto TAKEKAWA, Kun WANG, Jingkun JIANG

期刊论文

Zero-valent manganese nanoparticles coupled with different strong oxidants for thallium removal from

Keke Li, Huosheng Li, Tangfu Xiao, Gaosheng Zhang, Aiping Liang, Ping Zhang, Lianhua Lin, Zexin Chen, Xinyu Cao, Jianyou Long

期刊论文

Effects of natural zeolite and sulfate ions on the mechanical properties and microstructure of plastic

期刊论文

A time−space porosity computational model for concrete under sulfate attack

期刊论文

Effects of humic acid and surfactants on the aggregation kinetics of manganese dioxide colloids

Xiaoliu HUANGFU,Yaan WANG,Yongze LIU,Xixin LU,Xiang ZHANG,Haijun CHENG,Jin JIANG,Jun MA

期刊论文

Tripotassium citrate monohydrate derived carbon nanosheets as a competent assistant to manganese dioxide

期刊论文

Catalytic activity of manganese oxide supported on alumina in the synthesis of quinoxalines

Rekha M., H. Kathyayini, N. Nagaraju

期刊论文

Coextraction of vanadium and manganese from high-manganese containing vanadium wastewater by a solvent

Zishuai Liu, Yimin Zhang, Zilin Dai, Jing Huang, Cong Liu

期刊论文

Biological conversion pathways of sulfate reduction ammonium oxidation in anammox consortia

Zhen Bi, Deqing Wanyan, Xiang Li, Yong Huang

期刊论文

The role of manganese oxides in the activation of peroxymonosulfate (PMS)

Jianzhi Huang, Huichun Zhang

期刊论文

Multivalent manganese oxides with high electrocatalytic activity for oxygen reduction reaction

Xiangfeng Peng, Zhenhai Wang, Zhao Wang, Yunxiang Pan

期刊论文

Chemical composition and formation mechanisms in the cathode-electrolyte interface layer of lithium manganese

Sahithya REDDIVARI, Christian LASTOSKIE, Ruofei WU, Junliang ZHANG

期刊论文

The solubility of cefquinome sulfate in pure and mixed solvents

Rongbao Qi,Jingkang Wang,Junxiao Ye,Hongxun Hao,Ying Bao

期刊论文

Effects of metal ions on the morphology of calcium sulfate hemihydrate whiskers by hydrothermal method

Tianjie Liu, Hao Fan, Yanxia Xu, Xingfu Song, Jianguo Yu

期刊论文

PICRUSt2 functionally predicts organic compounds degradation and sulfate reduction pathways in an acidogenic

期刊论文