It is well known that atoms of the same element in different valence states show very different chemical behaviors.Calcium is a typical divalent metal,sharing or losing both of its valence electrons when forming compo...It is well known that atoms of the same element in different valence states show very different chemical behaviors.Calcium is a typical divalent metal,sharing or losing both of its valence electrons when forming compounds.Attempts have been made to synthesize compounds of monovalent calcium ions for decades,but with very little success(e.g.,in clusters).Pressure can result in substantial changes in the properties of atoms and chemical bonding,creating an extensive variety of unique materials with special valence states.In this study,using the ab initio evolutionary algorithm USPEX,we search for stable calcium-chlorine(Ca-Cl)system compounds at pressures up to 100 GPa.Besides the expected compound CaCl_(2),we predict three new compounds with monovalent Ca to be stable at high pressures,namely,CaCl,Ca_(5)Cl_(6),and Ca_(3)Cl_(4).According to our calculations,CaCl is stable at pressures above 18 GPa and is predicted to undergo a transition from nonmagnetic Fm-3m-CaCl to ferromagnetic Pm-3m-CaCl at 40 GPa.Ca_(5)Cl_(6)and Ca_(3)Cl_(4)are stable at pressures above 37 and 73 GPa,with space groups P-1 and R-3,respectively.Following these predictions,we successfully synthesized Pm-3m-CaCl in laser-heated diamond anvil cell experiments.The emergence of the unusual valence state at high pressures reveals exciting opportunities for creating entirely new materials in sufficiently large quantities for a variety of potential applications.展开更多
Nano zero valent iron particles (nZVI) are popular the last few years because of the numerous applications in remediation of a wide range of pollutants in contaminated soils and aquifers. The nZVI particles can be 10 ...Nano zero valent iron particles (nZVI) are popular the last few years because of the numerous applications in remediation of a wide range of pollutants in contaminated soils and aquifers. The nZVI particles can be 10 - 1000 times more reactive than granular or micro-scale ZVI particles due to the small particle size, large specific surface area and high reactivity. An alternative green synthesis procedure was used for the production of nano zero valent iron particles (nZVI) using green tea (GT) extract, which is characterized by its high antioxidant content. Polyphenols in green tea extract possess double role in the synthesis of nZVI, because they not only reduce ferric cations, but also protect nZVI from oxidation and agglomeration as capping agents. The objective of current study was to simulate ata laboratory scale the attachment of GT-nZVI particles on soil material and study the effectiveness of attached nanoparticles for removing hexavalent chromium (Cr(VI)) from contaminated groundwater flowing through the porous soil bed. Column tests were carried out with various flowrates in order to examine the effect of contact time between the attached on porous medium nZVI and the flow-through solution on Cr(VI) reduction. After the completion of column tests the soil material in each column was split in 5 vertical sections, which were further subjected to chemical analyses and leaching tests. According to the results of the study increasing the contact time favors the reduction and removal of Cr(VI) from the aqueous phase. The reductive precipitation of Cr can be described as a reaction that follows a pseudo-first order kinetic law, with rate constant equal to k = 0.0243 ± 0.0011 min-1. Leaching tests indicated that precipitated chromium is not soluble. In the examined soil material, the total amount of precipitated Cr was found to range between 280 and 890 mg/(kg soil), while soluble Cr was less than 1.4 mg/kg and most probably it was due to the presence of residual Cr(VI) solution in the porosity of soil.展开更多
Microscale zero valent iron(mFe^(0))is one of the most potential water pollution remediation materials,but the effective utilization ability of electrons released by mFe^(0)in the reduction of hexavalent chromium(Cr(V...Microscale zero valent iron(mFe^(0))is one of the most potential water pollution remediation materials,but the effective utilization ability of electrons released by mFe^(0)in the reduction of hexavalent chromium(Cr(VI))is not satisfactory.Here,we find the microscale iron-copper(m Fe/Cu)bimetals coated with copper on the surface of mFe^(0)can significantly improve the effective utilization of electrons released by mFe^(0).Electrochemical analysis displays that copper plating on the surface of m Fe/Cu can promote the release the electrons from mFe^(0)and reduce the impedance of mFe^(0).Spin-polarized density functional theory(DFT)calculation reveals that Cu on the surface of m Fe/Cu bimetals promotes the release of electrons from mFe^(0)and reduces the adsorption energy of Fe to Cr.As the electron transporter,moreover,Cu can always attract Cr to the hollow position near itself of the Fe surface,which could promote the effective utilization of electrons released by Fe.Effective utilization ability of electrons in m Fe/Cu system is 12.5 times higher than that in mFe^(0)system.Our findings provide another basis for the efficient reduction of Cr(VI)by m Fe/Cu bimetals,which could promote the application and popularization of m Fe/Cu bimetals.展开更多
Solid phase reactions of Cr（Ⅵ） with Fe（0） were investigated with spherical-aberration-corrected scanning transmission electron microscopy（Cs-STEM） integrated with X-ray energy-dispersive spectroscopy（XEDS）. N...Solid phase reactions of Cr（Ⅵ） with Fe（0） were investigated with spherical-aberration-corrected scanning transmission electron microscopy（Cs-STEM） integrated with X-ray energy-dispersive spectroscopy（XEDS）. Near-atomic resolution elemental mappings of Cr（Ⅵ）–Fe（0） reactions were acquired. Experimental results show that rate and extent of Cr（Ⅵ） encapsulation are strongly dependent on the initial concentration of Cr（Ⅵ） in solution. Low Cr loading in nZⅥ（〈1.0 wt%） promotes the electrochemical oxidation and continuous corrosion of n ZⅥ while high Cr loading（〉1.0 wt%） can quickly shut down the Cr uptake. With the progress of iron oxidation and dissolution, elements of Cr and O counter-diffuse into the nanoparticles and accumulate in the core region at low levels of Cr（Ⅵ）（e.g., 〈 10 mg/L）. Whereas the reacted n ZⅥ is quickly coated with a newly-formed layer of 2–4 nm in the presence of concentrated Cr（Ⅵ）（e.g., 〉 100 mg/L）. The passivation structure is stable over a wide range of pH unless pH is low enough to dissolve the passivation layer. X-ray photoelectron spectroscopy（XPS） depth profiling reconfirms that the composition of the newly-formed surface layer consists of Fe（Ⅲ）–Cr（Ⅲ）（oxy）hydroxides with Cr（Ⅵ） adsorbed on the outside surface. The insoluble and insulating Fe（Ⅲ）–Cr（Ⅲ）（oxy）hydroxide layer can completely cover the n ZⅥ surface above the critical Cr loading and shield the electron transfer. Thus, the fast passivation of nZⅥ in high Cr（Ⅵ） solution is detrimental to the performance of nZⅥ for Cr（Ⅵ） treatment and remediation.展开更多
An open-label, multicenter study was conducted to describe the safety of the 13-valent pneumococcal conjugate vaccine (PCV13) in 1049 individuals aged ≥68 years, who had previously been immunized with the unconjugate...An open-label, multicenter study was conducted to describe the safety of the 13-valent pneumococcal conjugate vaccine (PCV13) in 1049 individuals aged ≥68 years, who had previously been immunized with the unconjugated 23-valent pneumococcal polysaccharide vaccine (PPSV23). In addition, the safety profile of PCV13 in this study was compared, in a post-hoc descriptive analysis, to that observed in other elderly populations, who had received PCV13 or PPSV23 as part of other completed studies. Local (56.6%) and systemic reactions (58.4%) were very common, but were mainly mild, and of short duration (mean: 1.3 - 4.6 days). There were no related serious adverse events (AEs) within 1 month after PCV13. 123 days after PCV13 and 94 days after a nonstudy influenza vaccine, a case of transient Guillain-Barré syndrome occurred, which the investigator assessed as possibly related to the vaccination. Reactogenicity observed in this study population was generally similar to that of other elderly study populations with PPSV23-preimmunized adults, and with PPSV23-naive adults. Reactogenicity was less common in this study than that observed in PPSV23-preimmunized adults who were revaccinated with PPSV23 rather than a subsequent dose of PCV13. There were no related serious AEs reported after PCV13 and PPSV23 in these comparator studies. Conclusion: PCV13 may be administered safely to older adults previously immunized with PPSV23. (ClinicalTrials. gov Identifier: NCT00500266)展开更多
Excess phosphorus from non-point pollution sources is one of the key factors causing eutrophication in many lakes in China,so finding a cost-effective method to remove phosphorus from non-point pollution sources is ve...Excess phosphorus from non-point pollution sources is one of the key factors causing eutrophication in many lakes in China,so finding a cost-effective method to remove phosphorus from non-point pollution sources is very important for the health of the aqueous environment. Graphene was selected to support nanoscale zero-valent iron（nZVI）for phosphorus removal from synthetic rainwater runoff in this article. Compared with nZVI supported on other porous materials,graphene-supported nZVI（G-nZVI） could remove phosphorus more efficiently. The amount of nZVI in G-nZVI was an important factor in the removal of phosphorus by G-nZVI,and G-nZVI with 20 wt.% nZVI（20% G-nZVI）could remove phosphorus most efficiently. The nZVI was very stable and could disperse very well on graphene,as characterized by transmission electron microscopy（TEM） and scanning electron microscopy（SEM）. X-ray photoelectron spectroscopy（XPS）,Fourier Transform infrared spectroscopy（FT-IR） and Raman spectroscopy were used to elucidate the reaction process,and the results indicated that Fe-O-P was formed after phosphorus was adsorbed by G-nZVI. The results obtained from X-ray diffraction（XRD） indicated that the reaction product between nZVI supported on graphene and phosphorus was Fe3（PO4）2·8H2O（Vivianite）. It was confirmed that the specific reaction mechanism for the removal of phosphorus with nZVI or G-nZVI was mainly due to chemical reaction between nZVI and phosphorus.展开更多
Laboratory studies were conducted to find out the efficacy of uniquely prepared zero valent iron impregnated silica in transforming xenobiotic chlorophenols namely 4-chlorophenol, 2,4-dichlorophenol and 2,4,6-trichlor...Laboratory studies were conducted to find out the efficacy of uniquely prepared zero valent iron impregnated silica in transforming xenobiotic chlorophenols namely 4-chlorophenol, 2,4-dichlorophenol and 2,4,6-trichlorophenol. Continuous mode column experiments were performed to investigate the transformation of chlorophenols by varying pH, column height, flow rate and initial chlorophenol concentration. Reusability study of the zero valent iron impregnated silica was studied as well as the morphological changes and the chemical composition of the catalyst medium were also investigated. Dechlorination kinetic studies were conducted and the order of dechlorination of chlorophenols was found to be 2,4,6-trichlorophenol 〉 2,4-dichlorophenol 〉 4-chlorophenol. The optimum pH, column height and flow rate were found to be 7, 20 cm and 0.75 L/hr respectively for all chlorophenols in the reaction duration of 4 hr. Intermediates formed during dechlorination study were identified by gas chromatography-mass spectroscopy analysis. This method was applied to real pulp and paper wastewater and was found satisfactory.展开更多
Zero valent iron （ZVI） is expected to help create an enhanced anaerobic environment that might improve the performance of anaerobic treatment. Based on this idea, a novel ZVI packed upflow anaerobic sludge blanket ...Zero valent iron （ZVI） is expected to help create an enhanced anaerobic environment that might improve the performance of anaerobic treatment. Based on this idea, a novel ZVI packed upflow anaerobic sludge blanket （ZVI-UASB） reactor was developed to treat azo dye wastewater with variable influent quality. The results showed that the reactor was less influenced by increases of Reactive Brilliant Red X-3B concentration from 50 to 1000 mg/L and chemical oxygen demand （COD） from 1000 to 7000 mg/L in the feed than a reference UASB reactor without the ZVI. The ZVI decreased oxidation-reduction potential in the reactor by about 80 mV. Iron ion dissolution from the ZVI could buffer acidity in the reactor, the amount of which was related to the COD concentration. Fluorescence in situ hybridization test showed the abundance of methanogens in the sludge of the ZVI-UASB reactor was significantly greater than that of the reference one. Denaturing gradient gel electrophoresis showed that the ZVI increased the diversity of microbial strains responsible for high efficiency.展开更多
Risk associated with heavy metals in soil has been received widespread attention.In this study,a porous biochar supported nanoscale zero-valent iron(BC-nZVI)was applied to immobilize cadmium(Cd)and lead(Pb)in clayey s...Risk associated with heavy metals in soil has been received widespread attention.In this study,a porous biochar supported nanoscale zero-valent iron(BC-nZVI)was applied to immobilize cadmium(Cd)and lead(Pb)in clayey soil.Experiment results indicated that the immobilization of Cd or Pb by BC-nZVI process was better than that of BC or nZVI process,and about 80%of heavy metals immobilization was obtained in BC-nZVI process.Addition of BC-nZVI could increase soil pH and organic matter(SOM).Cd or Pb immobilization was inhibited with coexisting organic compound 2,4-dichlorophenol(2,4-DCP),but 2,4-DCP could be removed in a simultaneous manner with Cd or Pb immobilization at low concentration levels.Simultaneous immobilization of Cd and Pb was achieved in BC-nZVI process,and both Cd and Pb availability significantly decreased.Stable Cd species inculding Cd(OH)_(2),CdCO_(3)and CdO were formed,whereas stable Pb species such as PbCO_(3),PbO and Pb(OH)_(2)were produced with BC-nZVI treatment.Simultaneous immobilization mechanism of Cd and Pb in soil by BC-nZVI was thereby proposed.This study well demonstrates that BC-nZVI has been emerged as a potential technology for the remediation of multiple heavy metals in soil.展开更多
Reductive immobilization of radioactive pertechnetate(99TcO4^-) in simulated groundwater was studied by prepared carboxymethyl cellulose(CMC) and starch stabilized zero valent iron nanoparticles(nZVI),and long-term re...Reductive immobilization of radioactive pertechnetate(99TcO4^-) in simulated groundwater was studied by prepared carboxymethyl cellulose(CMC) and starch stabilized zero valent iron nanoparticles(nZVI),and long-term remobilization of reduced Tc was also evaluated under anoxic and oxic conditions.The stabilized nZVI can effectively reduce soluble 99Tc(Ⅶ) to insoluble 99 Tc(Ⅳ),and they can be easily delivered into a contaminated groundwater zone and facilitate in situ remediation.In this study,CMCstabilized nZVI showed higher reactivity than that using starch as the stabilizer.Batch experiments indicated that more than 99% of 99 Tc(Ⅶ)(CO=12 mg/mL) was reduced and removed from groundwater by CMC-stabilized nZVI with a CMC content of 0.2%(w/w) at a broad pH of 5-8.X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS) analyses further confirmed that 99Tc(Ⅶ)O4^-transformed into 99Tc(Ⅳ)O2(s).The presence of bicarbonate exhibited insignificant effect on Tc immobilization,while humic acid(HA) inhibited reaction mainly due to retardation on electron transfer and formation of Tc(IV)-HA complexes.More interesting,the immobilized Tc(Ⅳ) remained insoluble even after 120 d under anoxic condition,while only^21 % was remobilized when exposed to air.Therefore,biomacromolecules stabilized nZVI nanoparticles could be a viable alternative for in situ remediation of radioactive contamination in groundwater.展开更多
Nitrobenzene has been considered as a significant groundwater contaminant due to its wide usage in explosives, insecticides, herbicides, pharmaceuticals and dyes. Nitrobenzene is of environmental concern because of it...Nitrobenzene has been considered as a significant groundwater contaminant due to its wide usage in explosives, insecticides, herbicides, pharmaceuticals and dyes. Nitrobenzene is of environmental concern because of its toxicity. In the presence of zero-valent iron （ZVI）, reduction of the nitro group is the dominant transformation process for nitrobenzene. A series of experiments were carried out to investigate the kinetics of nitrobenzene reduction by ZVI and the effects of pH and ZVI particle size on nitrobenzene removal in groundwater. The results indicated that nitrobenzene could be reduced to aniline by ZVI; the reduction of nitrobenzene by ZVI followed a pseudo first-order kinetics; the observed nitrobenzene reduction rate constant （k obs ） was 0.0006 min^-1 and the half-life of nitrobenzene （t 1/2 ） was 115.5 min; the mass balance achieved 87.5% for nitrobenzene reduction by the 1 mm ZVI particle and the final removal efficiency was 80.98%. In addition, the pH and ZVI particle size were found to exhibit significant influences on the nitrobenzene reduction. The observed nitrobenzene reduction rate constant linearly decreased with increase pH and the data fitted on polynomial regression equation for the observed nitrobenzene reduction rate constant and ZVI particle size. Therefore, use of ZVI based permeable reactive barrier technology to remedy nitrobenzene contaminated groundwater was feasible.展开更多
In this study, a novel nanoscale zero-valent iron（n ZVI） composite material was successfully synthesized using a low-cost natural clay, ＂Hangjin 2~#clay＂（HJ clay） as the support and tested for the decolorization...In this study, a novel nanoscale zero-valent iron（n ZVI） composite material was successfully synthesized using a low-cost natural clay, ＂Hangjin 2~#clay＂（HJ clay） as the support and tested for the decolorization of the azo dye Methyl Orange（MO） in aqueous solution by n ZVI particles. According to the characterization and MO decolorization experiments, the sample with 5：1 HJ clay-supported n ZVI（HJ/n ZVI） mass ratio（HJ-n ZVI5） showed the best dispersion and reactivity and the highest MO decolorization efficiency. With the same equivalent Fe0 dosage, the HJ-n ZVI1 and HJ-n ZVI5 samples demonstrated a synergetic effect for the decolorization of MO： their decolorization efficiencies were much higher than that achieved by physical mixing of HJ clay and n ZVIs, or the sum of HJ clay and n ZVIs alone. The synergetic effect was primarily due to the improved dispersion and more effective utilization of the n ZVI particles on/in the composite materials. Higher decolorization efficiency of MO was obtained at larger HJ-n ZVI dosage, higher temperature and under N2 atmosphere, while the MO initial concentration and p H were negatively correlated to the efficiency. HJ clay not only works as a carrier for n ZVI nanoparticles, but also contributes to the decolorization through an ＂adsorption-enhanced reduction＂ mechanism. The high efficiency of HJ-n ZVI for decontamination gives it great potential for use in a variety of remediation applications.展开更多
Experiments were conducted to investigate the behavior of the sequential system of intensified zero-valent iron process(IZVI) and anaerobic filter and biological aerated filter(AF/BAF) reactors for advanced treatment ...Experiments were conducted to investigate the behavior of the sequential system of intensified zero-valent iron process(IZVI) and anaerobic filter and biological aerated filter(AF/BAF) reactors for advanced treatment of biologically pretreated coking wastewater. Particular attention was paid to the performance of the integrated system for the removal of chemical oxygen demand(COD), ammonia nitrogen(NH3-N) and total nitrogen(TN). The average removal efficiencies of COD, NH3-N and TN were 76.28%, 96.76% and 59.97%, with the average effluent mass concentrations of 56, 0.53 and 18.83 mg/L, respectively, reaching the first grade of the national discharge standard. Moreover, the results of gas chromatography/mass spectrum(GC/MS) and gel permeation chromatography(GPC) analysis demonstrated that the refractory organic compounds with high relative molecular mass were partly removed in IZVI process by the function of oxidation-reduction, flocculation and adsorption which could also enhance the biodegradability of the system effluent. The removal efficiencies of NH3-N and TN were achieved mainly in the subsequent AF/BAF reactors by nitrification and denitrification. Overall, the results obtained show that the application of IZVI in combination with AF/BAF is a promising technology for advanced treatment of biologically pretreated coking wastewater.展开更多
In this study, bimetallic nanoscale zero-valent iron particles（nZVI）, including copper/nanoscale zero-valent iron particles（Cu/nZVI） and nickel/nanoscale zero-valent iron particles（Ni/nZVI）, were synthesized by ...In this study, bimetallic nanoscale zero-valent iron particles（nZVI）, including copper/nanoscale zero-valent iron particles（Cu/nZVI） and nickel/nanoscale zero-valent iron particles（Ni/nZVI）, were synthesized by one-step liquid-phase reduction and applied for oxytetracycline（OTC） removal. The effects of contact time and initial p H on the removal efficiency were studied. The as-prepared nanoscale particles were characterized by scanning electron microscopy（SEM）, energy dispersive spectroscopy（EDS） and X-ray diffraction（XRD）. Finally, the degradation mechanisms of OTC utilizing the as-prepared nanoparticles were investigated by using X-ray photoelectron spectroscopy（XPS） and mass spectrometry（MS）. Cu/n ZVI presented remarkable ability for OTC degradation and removed71.44% of OTC（100 mg/L） in 4 hr, while only 62.34% and 31.05% of OTC was degraded by Ni/nZVI and nZVI respectively. XPS and MS analysis suggested that OTC was broken down to form small molecules by ·OH radicals generated from the corrosion of Fe0. Cu/nZVI and Ni/n ZVI have been proved to have potential as materials for application in OTC removal because of their significant degradation ability toward OTC.展开更多
Zero-valent iron（ZⅥ） was loaded on expanded graphite（EG） to produce a composite material（EG-ZⅥ） for efficient removal of hexavalent chromium（Cr（Ⅵ））. EG and EG-ZⅥ were characterized by X-ray diffraction（...Zero-valent iron（ZⅥ） was loaded on expanded graphite（EG） to produce a composite material（EG-ZⅥ） for efficient removal of hexavalent chromium（Cr（Ⅵ））. EG and EG-ZⅥ were characterized by X-ray diffraction（XRD）, scanning electron microscopy（SEM）,Fourier-transform infrared（FTIR） spectroscopy and Brunauer–Emmett–Teller（BET） analysis. EG-ZⅥ had a high specific surface area and contained sub-micron sized particles of zero-valent iron. Batch experiments were employed to evaluate the Cr（Ⅵ） removal performance. The results showed that the Cr（Ⅵ） removal rate was 98.80% for EG-ZⅥ,which was higher than that for both EG（10.00%） and ZⅥ（29.80%）. Furthermore, the removal rate of Cr（Ⅵ） by EG-ZⅥ showed little dependence on solution p H within a p H range of 1–9.Even at pH 11, a Cr（Ⅵ） removal rate of 62.44% was obtained after reaction for 1 hr. EG-ZⅥ could enhance the removal of Cr（Ⅵ） via chemical reduction and physical adsorption,respectively. X-ray photoelectron spectroscopy（XPS） was used to analyze the mechanisms of Cr（Ⅵ） removal, which indicated that the ZⅥ loaded on the surface was oxidized, and the removed Cr（Ⅵ） was immobilized via the formation of Cr（III） hydroxide and Cr（III）–Fe（III）hydroxide/oxyhydroxide on the surface of EG-ZⅥ.展开更多
The importance of enhancing sludge dewaterability is increasing due to the considerable impact of excess sludge volume on disposal costs and on overall sludge management. This study presents an innovative approach to ...The importance of enhancing sludge dewaterability is increasing due to the considerable impact of excess sludge volume on disposal costs and on overall sludge management. This study presents an innovative approach to enhance dewaterability of anaerobic digestate（AD） harvested from a wastewater treatment plant. The combination of zero valent iron（ZVI, 0–4.0 g/g total solids（TS）） and hydrogen peroxide（HP, 0–90 mg/g TS） under pH 3.0 significantly enhanced the AD dewaterability. The largest enhancement of AD dewaterability was achieved at 18 mg HP/g TS and 2.0 g ZVI/g TS, with the capillary suction time reduced by up to 90%. Economic analysis suggested that the proposed HP and ZVI treatment has more economic benefits in comparison with the classical Fenton reaction process. The destruction of extracellular polymeric substances and cells as well as the decrease of particle size were supposed to contribute to the enhanced AD dewaterability by HP ＋ ZVI conditioning.展开更多
Toxicity studies considering both the bare and stabilized forms of zero valent iron nanoparticles（nZVI） could be timely, given that ecological risks identified are minimized through modification or with substitution...Toxicity studies considering both the bare and stabilized forms of zero valent iron nanoparticles（nZVI） could be timely, given that ecological risks identified are minimized through modification or with substitution of approaches in the synthesis, development and environmental application of the nanoparticles before succeeding to volume production.This review is focused on the fate, transport and toxicological implications of the bare nZVI and surface modified particles used for environmental applications.展开更多
While manganese-based cathodes have been intensively studied for zinc-ion batteries(ZIBs),the limited rate capability and cycle life have always been a difficult problem to be solved.Here,we report a mixed valent mang...While manganese-based cathodes have been intensively studied for zinc-ion batteries(ZIBs),the limited rate capability and cycle life have always been a difficult problem to be solved.Here,we report a mixed valent manganese oxide(MnOx)cathode with superior electrochemical performance,which exhibits a high specific capacity of 450 mA h/g at 0.2 C and a satisfactory specific capacity of 158.3 mA h/g at a high rate of 5 C.The mixed cathode system reduces the charge transfer resistance,and show good surface stability and adsorption properties,so it is beneficial for the storage of Zn^(2+).Meanwhile,coaxial fiber ZIBs(CFZIBs)with splendid flexibility are assembled utilizing the elaborately prepared cathode material.The CFZIBs achieve a reversible capacity of 255.8 m A h/g and the capacity retention rate is as high as 80%after 1000 bending deformations.This study provides new opportunities for designing ZIBs with high performance and high flexibility.展开更多
Some problems including low treatment capacity,agglomeration and clogging phenomena,and short working life,limit the application of pre-treatment methods involving zero-valent iron （ZVI）.In this article,ZVI was froz...Some problems including low treatment capacity,agglomeration and clogging phenomena,and short working life,limit the application of pre-treatment methods involving zero-valent iron （ZVI）.In this article,ZVI was frozen in an amorphous state through a melt-spinning technique,and the decolorization effect of amorphous ZVI on Acid Orange II solution was investigated under varied conditions of experimental variables such as reaction temperature,ribbon dosage,and initial pH.Batch experiments suggested that the decolorization rate was enhanced with the increase of reaction temperature and ribbon dosage,but decreased with increasing initial solution pH.Kinetic analyses indicated that the decolorization process followed a first order exponential kinetic model,and the surface-normalized decolorization rate could reach 2.09 L/（m^2 ·min） at room temperature,which was about ten times larger than any previously reported under similar conditions.Recycling experiments also proved that the ribbons could be reused at least four times without obvious decay of decolorization rate and efficiency.This study suggests a tremendous application potential for amorphous ZVI in remediation of groundwater or wastewater contaminated with azo dyes.展开更多
Sulfide-modified nanoscale zero-valent iron(S-nZVI) is a promising material for removal of organic pollutants from water, but S-nZVI nanoparticles(NPs) easily agglomerate and have poor contact with organic contaminant...Sulfide-modified nanoscale zero-valent iron(S-nZVI) is a promising material for removal of organic pollutants from water, but S-nZVI nanoparticles(NPs) easily agglomerate and have poor contact with organic contaminants.Herein, we propose a new S-nZVI/graphene aerogel(S-nZVI/GA) composite which exhibits superior removal capability for trichloroethylene(TCE) from water.Three-dimensional porous graphene aerogel(GA) can improve the efficiency of electron transport, enhance the adsorption of organic pollutants and restrain the agglomeration of the core-shell S-nZVI NPs.The TCE removal rates of Fe S, nZVI, GA and S-nZVI were 27.8%, 42%, 63% and 75% in 2 hr, respectively.Furthermore, TCE was completely removed within 50 min by S-nZVI/GA.The TCE removal rate increased with increasing p H and temperature, and TCE removal followed the pseudo-first-order kinetic model.The results demonstrate the great potential of S-nZVI/GA composite as a low-cost,easily separated and superior monolithic adsorbent for removal of organic pollutants.展开更多
基金supported by the National Science Foundation of China(Grant Nos.92263101,12174200,21627802,51722209,and 21273206)the Science Challenge Project(Grant No.TZ2016001)+2 种基金the Key Research Project of Higher Education(Grant Nos.15A140016 and 2010GGJS-110)the National Key R&D Program of China(Grant No.YS2018YFA070119)supported by the Russian Science Foundation(Grant No.24-43-00162)。
文摘It is well known that atoms of the same element in different valence states show very different chemical behaviors.Calcium is a typical divalent metal,sharing or losing both of its valence electrons when forming compounds.Attempts have been made to synthesize compounds of monovalent calcium ions for decades,but with very little success(e.g.,in clusters).Pressure can result in substantial changes in the properties of atoms and chemical bonding,creating an extensive variety of unique materials with special valence states.In this study,using the ab initio evolutionary algorithm USPEX,we search for stable calcium-chlorine(Ca-Cl)system compounds at pressures up to 100 GPa.Besides the expected compound CaCl_(2),we predict three new compounds with monovalent Ca to be stable at high pressures,namely,CaCl,Ca_(5)Cl_(6),and Ca_(3)Cl_(4).According to our calculations,CaCl is stable at pressures above 18 GPa and is predicted to undergo a transition from nonmagnetic Fm-3m-CaCl to ferromagnetic Pm-3m-CaCl at 40 GPa.Ca_(5)Cl_(6)and Ca_(3)Cl_(4)are stable at pressures above 37 and 73 GPa,with space groups P-1 and R-3,respectively.Following these predictions,we successfully synthesized Pm-3m-CaCl in laser-heated diamond anvil cell experiments.The emergence of the unusual valence state at high pressures reveals exciting opportunities for creating entirely new materials in sufficiently large quantities for a variety of potential applications.
文摘Nano zero valent iron particles (nZVI) are popular the last few years because of the numerous applications in remediation of a wide range of pollutants in contaminated soils and aquifers. The nZVI particles can be 10 - 1000 times more reactive than granular or micro-scale ZVI particles due to the small particle size, large specific surface area and high reactivity. An alternative green synthesis procedure was used for the production of nano zero valent iron particles (nZVI) using green tea (GT) extract, which is characterized by its high antioxidant content. Polyphenols in green tea extract possess double role in the synthesis of nZVI, because they not only reduce ferric cations, but also protect nZVI from oxidation and agglomeration as capping agents. The objective of current study was to simulate ata laboratory scale the attachment of GT-nZVI particles on soil material and study the effectiveness of attached nanoparticles for removing hexavalent chromium (Cr(VI)) from contaminated groundwater flowing through the porous soil bed. Column tests were carried out with various flowrates in order to examine the effect of contact time between the attached on porous medium nZVI and the flow-through solution on Cr(VI) reduction. After the completion of column tests the soil material in each column was split in 5 vertical sections, which were further subjected to chemical analyses and leaching tests. According to the results of the study increasing the contact time favors the reduction and removal of Cr(VI) from the aqueous phase. The reductive precipitation of Cr can be described as a reaction that follows a pseudo-first order kinetic law, with rate constant equal to k = 0.0243 ± 0.0011 min-1. Leaching tests indicated that precipitated chromium is not soluble. In the examined soil material, the total amount of precipitated Cr was found to range between 280 and 890 mg/(kg soil), while soluble Cr was less than 1.4 mg/kg and most probably it was due to the presence of residual Cr(VI) solution in the porosity of soil.
基金the financial support from Fundamental Research Funds for the Central Universities(Southwest Minzu University,No.U2021124)the Startup Foundation of Chengdu University of Information Technology(No.KYTZ202013)+1 种基金National Natural Science Foundation of China(No.21808146)China Postdoctoral Science Foundation(No.2018M643479)。
文摘Microscale zero valent iron(mFe^(0))is one of the most potential water pollution remediation materials,but the effective utilization ability of electrons released by mFe^(0)in the reduction of hexavalent chromium(Cr(VI))is not satisfactory.Here,we find the microscale iron-copper(m Fe/Cu)bimetals coated with copper on the surface of mFe^(0)can significantly improve the effective utilization of electrons released by mFe^(0).Electrochemical analysis displays that copper plating on the surface of m Fe/Cu can promote the release the electrons from mFe^(0)and reduce the impedance of mFe^(0).Spin-polarized density functional theory(DFT)calculation reveals that Cu on the surface of m Fe/Cu bimetals promotes the release of electrons from mFe^(0)and reduces the adsorption energy of Fe to Cr.As the electron transporter,moreover,Cu can always attract Cr to the hollow position near itself of the Fe surface,which could promote the effective utilization of electrons released by Fe.Effective utilization ability of electrons in m Fe/Cu system is 12.5 times higher than that in mFe^(0)system.Our findings provide another basis for the efficient reduction of Cr(VI)by m Fe/Cu bimetals,which could promote the application and popularization of m Fe/Cu bimetals.
基金supported by the National Natural Science Foundation of China(Nos.21677107,51578398)the Fundamental Research Funds for the Central Universities(No.0400219363)
文摘Solid phase reactions of Cr（Ⅵ） with Fe（0） were investigated with spherical-aberration-corrected scanning transmission electron microscopy（Cs-STEM） integrated with X-ray energy-dispersive spectroscopy（XEDS）. Near-atomic resolution elemental mappings of Cr（Ⅵ）–Fe（0） reactions were acquired. Experimental results show that rate and extent of Cr（Ⅵ） encapsulation are strongly dependent on the initial concentration of Cr（Ⅵ） in solution. Low Cr loading in nZⅥ（〈1.0 wt%） promotes the electrochemical oxidation and continuous corrosion of n ZⅥ while high Cr loading（〉1.0 wt%） can quickly shut down the Cr uptake. With the progress of iron oxidation and dissolution, elements of Cr and O counter-diffuse into the nanoparticles and accumulate in the core region at low levels of Cr（Ⅵ）（e.g., 〈 10 mg/L）. Whereas the reacted n ZⅥ is quickly coated with a newly-formed layer of 2–4 nm in the presence of concentrated Cr（Ⅵ）（e.g., 〉 100 mg/L）. The passivation structure is stable over a wide range of pH unless pH is low enough to dissolve the passivation layer. X-ray photoelectron spectroscopy（XPS） depth profiling reconfirms that the composition of the newly-formed surface layer consists of Fe（Ⅲ）–Cr（Ⅲ）（oxy）hydroxides with Cr（Ⅵ） adsorbed on the outside surface. The insoluble and insulating Fe（Ⅲ）–Cr（Ⅲ）（oxy）hydroxide layer can completely cover the n ZⅥ surface above the critical Cr loading and shield the electron transfer. Thus, the fast passivation of nZⅥ in high Cr（Ⅵ） solution is detrimental to the performance of nZⅥ for Cr（Ⅵ） treatment and remediation.
文摘An open-label, multicenter study was conducted to describe the safety of the 13-valent pneumococcal conjugate vaccine (PCV13) in 1049 individuals aged ≥68 years, who had previously been immunized with the unconjugated 23-valent pneumococcal polysaccharide vaccine (PPSV23). In addition, the safety profile of PCV13 in this study was compared, in a post-hoc descriptive analysis, to that observed in other elderly populations, who had received PCV13 or PPSV23 as part of other completed studies. Local (56.6%) and systemic reactions (58.4%) were very common, but were mainly mild, and of short duration (mean: 1.3 - 4.6 days). There were no related serious adverse events (AEs) within 1 month after PCV13. 123 days after PCV13 and 94 days after a nonstudy influenza vaccine, a case of transient Guillain-Barré syndrome occurred, which the investigator assessed as possibly related to the vaccination. Reactogenicity observed in this study population was generally similar to that of other elderly study populations with PPSV23-preimmunized adults, and with PPSV23-naive adults. Reactogenicity was less common in this study than that observed in PPSV23-preimmunized adults who were revaccinated with PPSV23 rather than a subsequent dose of PCV13. There were no related serious AEs reported after PCV13 and PPSV23 in these comparator studies. Conclusion: PCV13 may be administered safely to older adults previously immunized with PPSV23. (ClinicalTrials. gov Identifier: NCT00500266)
基金supported by the Major Science and Technology Programs for Water Pollution Control and Management of China (Nos.2011ZX07301-002 and 2012ZX07205-001)
文摘Excess phosphorus from non-point pollution sources is one of the key factors causing eutrophication in many lakes in China,so finding a cost-effective method to remove phosphorus from non-point pollution sources is very important for the health of the aqueous environment. Graphene was selected to support nanoscale zero-valent iron（nZVI）for phosphorus removal from synthetic rainwater runoff in this article. Compared with nZVI supported on other porous materials,graphene-supported nZVI（G-nZVI） could remove phosphorus more efficiently. The amount of nZVI in G-nZVI was an important factor in the removal of phosphorus by G-nZVI,and G-nZVI with 20 wt.% nZVI（20% G-nZVI）could remove phosphorus most efficiently. The nZVI was very stable and could disperse very well on graphene,as characterized by transmission electron microscopy（TEM） and scanning electron microscopy（SEM）. X-ray photoelectron spectroscopy（XPS）,Fourier Transform infrared spectroscopy（FT-IR） and Raman spectroscopy were used to elucidate the reaction process,and the results indicated that Fe-O-P was formed after phosphorus was adsorbed by G-nZVI. The results obtained from X-ray diffraction（XRD） indicated that the reaction product between nZVI supported on graphene and phosphorus was Fe3（PO4）2·8H2O（Vivianite）. It was confirmed that the specific reaction mechanism for the removal of phosphorus with nZVI or G-nZVI was mainly due to chemical reaction between nZVI and phosphorus.
文摘Laboratory studies were conducted to find out the efficacy of uniquely prepared zero valent iron impregnated silica in transforming xenobiotic chlorophenols namely 4-chlorophenol, 2,4-dichlorophenol and 2,4,6-trichlorophenol. Continuous mode column experiments were performed to investigate the transformation of chlorophenols by varying pH, column height, flow rate and initial chlorophenol concentration. Reusability study of the zero valent iron impregnated silica was studied as well as the morphological changes and the chemical composition of the catalyst medium were also investigated. Dechlorination kinetic studies were conducted and the order of dechlorination of chlorophenols was found to be 2,4,6-trichlorophenol 〉 2,4-dichlorophenol 〉 4-chlorophenol. The optimum pH, column height and flow rate were found to be 7, 20 cm and 0.75 L/hr respectively for all chlorophenols in the reaction duration of 4 hr. Intermediates formed during dechlorination study were identified by gas chromatography-mass spectroscopy analysis. This method was applied to real pulp and paper wastewater and was found satisfactory.
基金supported by the National Basic Research Program of China (No. 2007CB407302)the Natural Science Foundation of China (No. 21177015)+2 种基金the New Century Excellent Talent Program of the Ministry of Education of China (No. NCET-10-028)the Fundamental Research Funds for the Central Universities of China (No.DUT11ZD108)the Program for Changjiang Scholars and Innovative Research Team at the University of China(No. IRT0813)
文摘Zero valent iron （ZVI） is expected to help create an enhanced anaerobic environment that might improve the performance of anaerobic treatment. Based on this idea, a novel ZVI packed upflow anaerobic sludge blanket （ZVI-UASB） reactor was developed to treat azo dye wastewater with variable influent quality. The results showed that the reactor was less influenced by increases of Reactive Brilliant Red X-3B concentration from 50 to 1000 mg/L and chemical oxygen demand （COD） from 1000 to 7000 mg/L in the feed than a reference UASB reactor without the ZVI. The ZVI decreased oxidation-reduction potential in the reactor by about 80 mV. Iron ion dissolution from the ZVI could buffer acidity in the reactor, the amount of which was related to the COD concentration. Fluorescence in situ hybridization test showed the abundance of methanogens in the sludge of the ZVI-UASB reactor was significantly greater than that of the reference one. Denaturing gradient gel electrophoresis showed that the ZVI increased the diversity of microbial strains responsible for high efficiency.
基金supported by the Special project in key areas of Guangdong Province Ordinary Universities (No. 2020ZDZX1003)the Guangdong Provincial Key R&D Programme (No. 2020B1111350002)+4 种基金the Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme (2018)the research project and development plan for key areas of Guangdong Province (No. 2020B0202080002)the Project of Educational Commission of Guangdong Province of China (No. 2019KTSCX067)the Guangdong Provincial Special Fund for Modern Agriculture Industry Technology Innovation Teams (No. 2019KJ140)the National Natural Science Foundation of China (No. 21407155).
文摘Risk associated with heavy metals in soil has been received widespread attention.In this study,a porous biochar supported nanoscale zero-valent iron(BC-nZVI)was applied to immobilize cadmium(Cd)and lead(Pb)in clayey soil.Experiment results indicated that the immobilization of Cd or Pb by BC-nZVI process was better than that of BC or nZVI process,and about 80%of heavy metals immobilization was obtained in BC-nZVI process.Addition of BC-nZVI could increase soil pH and organic matter(SOM).Cd or Pb immobilization was inhibited with coexisting organic compound 2,4-dichlorophenol(2,4-DCP),but 2,4-DCP could be removed in a simultaneous manner with Cd or Pb immobilization at low concentration levels.Simultaneous immobilization of Cd and Pb was achieved in BC-nZVI process,and both Cd and Pb availability significantly decreased.Stable Cd species inculding Cd(OH)_(2),CdCO_(3)and CdO were formed,whereas stable Pb species such as PbCO_(3),PbO and Pb(OH)_(2)were produced with BC-nZVI treatment.Simultaneous immobilization mechanism of Cd and Pb in soil by BC-nZVI was thereby proposed.This study well demonstrates that BC-nZVI has been emerged as a potential technology for the remediation of multiple heavy metals in soil.
基金partially supported by the National Natural Science Foundation of China(No.41230638)a grant from the USDA AAES 2015 Hatch and Multistate funding program
文摘Reductive immobilization of radioactive pertechnetate(99TcO4^-) in simulated groundwater was studied by prepared carboxymethyl cellulose(CMC) and starch stabilized zero valent iron nanoparticles(nZVI),and long-term remobilization of reduced Tc was also evaluated under anoxic and oxic conditions.The stabilized nZVI can effectively reduce soluble 99Tc(Ⅶ) to insoluble 99 Tc(Ⅳ),and they can be easily delivered into a contaminated groundwater zone and facilitate in situ remediation.In this study,CMCstabilized nZVI showed higher reactivity than that using starch as the stabilizer.Batch experiments indicated that more than 99% of 99 Tc(Ⅶ)(CO=12 mg/mL) was reduced and removed from groundwater by CMC-stabilized nZVI with a CMC content of 0.2%(w/w) at a broad pH of 5-8.X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS) analyses further confirmed that 99Tc(Ⅶ)O4^-transformed into 99Tc(Ⅳ)O2(s).The presence of bicarbonate exhibited insignificant effect on Tc immobilization,while humic acid(HA) inhibited reaction mainly due to retardation on electron transfer and formation of Tc(IV)-HA complexes.More interesting,the immobilized Tc(Ⅳ) remained insoluble even after 120 d under anoxic condition,while only^21 % was remobilized when exposed to air.Therefore,biomacromolecules stabilized nZVI nanoparticles could be a viable alternative for in situ remediation of radioactive contamination in groundwater.
基金supported by the National High Technology Research and Development Program(863) of China(No.2007AA06A410)the Water Pollution Control and Management Project(No.2008ZX07207-007-05)the National Natural Science Foundation of China(No.40802055)
文摘Nitrobenzene has been considered as a significant groundwater contaminant due to its wide usage in explosives, insecticides, herbicides, pharmaceuticals and dyes. Nitrobenzene is of environmental concern because of its toxicity. In the presence of zero-valent iron （ZVI）, reduction of the nitro group is the dominant transformation process for nitrobenzene. A series of experiments were carried out to investigate the kinetics of nitrobenzene reduction by ZVI and the effects of pH and ZVI particle size on nitrobenzene removal in groundwater. The results indicated that nitrobenzene could be reduced to aniline by ZVI; the reduction of nitrobenzene by ZVI followed a pseudo first-order kinetics; the observed nitrobenzene reduction rate constant （k obs ） was 0.0006 min^-1 and the half-life of nitrobenzene （t 1/2 ） was 115.5 min; the mass balance achieved 87.5% for nitrobenzene reduction by the 1 mm ZVI particle and the final removal efficiency was 80.98%. In addition, the pH and ZVI particle size were found to exhibit significant influences on the nitrobenzene reduction. The observed nitrobenzene reduction rate constant linearly decreased with increase pH and the data fitted on polynomial regression equation for the observed nitrobenzene reduction rate constant and ZVI particle size. Therefore, use of ZVI based permeable reactive barrier technology to remedy nitrobenzene contaminated groundwater was feasible.
基金support provided by the National Key Technology R&D Program(no.2012BAJ21B04)the financial support from the China Scholarship Council(CSC)for one year as a visiting scholar at Stevens Institute of Technology
文摘In this study, a novel nanoscale zero-valent iron（n ZVI） composite material was successfully synthesized using a low-cost natural clay, ＂Hangjin 2~#clay＂（HJ clay） as the support and tested for the decolorization of the azo dye Methyl Orange（MO） in aqueous solution by n ZVI particles. According to the characterization and MO decolorization experiments, the sample with 5：1 HJ clay-supported n ZVI（HJ/n ZVI） mass ratio（HJ-n ZVI5） showed the best dispersion and reactivity and the highest MO decolorization efficiency. With the same equivalent Fe0 dosage, the HJ-n ZVI1 and HJ-n ZVI5 samples demonstrated a synergetic effect for the decolorization of MO： their decolorization efficiencies were much higher than that achieved by physical mixing of HJ clay and n ZVIs, or the sum of HJ clay and n ZVIs alone. The synergetic effect was primarily due to the improved dispersion and more effective utilization of the n ZVI particles on/in the composite materials. Higher decolorization efficiency of MO was obtained at larger HJ-n ZVI dosage, higher temperature and under N2 atmosphere, while the MO initial concentration and p H were negatively correlated to the efficiency. HJ clay not only works as a carrier for n ZVI nanoparticles, but also contributes to the decolorization through an ＂adsorption-enhanced reduction＂ mechanism. The high efficiency of HJ-n ZVI for decontamination gives it great potential for use in a variety of remediation applications.
基金Project(2006BAJ04A)suppprted by the National Sci-Tech Support Plan,China
文摘Experiments were conducted to investigate the behavior of the sequential system of intensified zero-valent iron process(IZVI) and anaerobic filter and biological aerated filter(AF/BAF) reactors for advanced treatment of biologically pretreated coking wastewater. Particular attention was paid to the performance of the integrated system for the removal of chemical oxygen demand(COD), ammonia nitrogen(NH3-N) and total nitrogen(TN). The average removal efficiencies of COD, NH3-N and TN were 76.28%, 96.76% and 59.97%, with the average effluent mass concentrations of 56, 0.53 and 18.83 mg/L, respectively, reaching the first grade of the national discharge standard. Moreover, the results of gas chromatography/mass spectrum(GC/MS) and gel permeation chromatography(GPC) analysis demonstrated that the refractory organic compounds with high relative molecular mass were partly removed in IZVI process by the function of oxidation-reduction, flocculation and adsorption which could also enhance the biodegradability of the system effluent. The removal efficiencies of NH3-N and TN were achieved mainly in the subsequent AF/BAF reactors by nitrification and denitrification. Overall, the results obtained show that the application of IZVI in combination with AF/BAF is a promising technology for advanced treatment of biologically pretreated coking wastewater.
基金supported by grants from Tai Shan Scholar Foundation(No.ts 201511003)
文摘In this study, bimetallic nanoscale zero-valent iron particles（nZVI）, including copper/nanoscale zero-valent iron particles（Cu/nZVI） and nickel/nanoscale zero-valent iron particles（Ni/nZVI）, were synthesized by one-step liquid-phase reduction and applied for oxytetracycline（OTC） removal. The effects of contact time and initial p H on the removal efficiency were studied. The as-prepared nanoscale particles were characterized by scanning electron microscopy（SEM）, energy dispersive spectroscopy（EDS） and X-ray diffraction（XRD）. Finally, the degradation mechanisms of OTC utilizing the as-prepared nanoparticles were investigated by using X-ray photoelectron spectroscopy（XPS） and mass spectrometry（MS）. Cu/n ZVI presented remarkable ability for OTC degradation and removed71.44% of OTC（100 mg/L） in 4 hr, while only 62.34% and 31.05% of OTC was degraded by Ni/nZVI and nZVI respectively. XPS and MS analysis suggested that OTC was broken down to form small molecules by ·OH radicals generated from the corrosion of Fe0. Cu/nZVI and Ni/n ZVI have been proved to have potential as materials for application in OTC removal because of their significant degradation ability toward OTC.
基金supported by the National Key Research and Development Program of China(No.2017YFD0801503)the Fundamental Research Funds for the Central Universities(No.PYVZ1703)the Higher Education and High-quality and World-class Universities(PY201606)
文摘Zero-valent iron（ZⅥ） was loaded on expanded graphite（EG） to produce a composite material（EG-ZⅥ） for efficient removal of hexavalent chromium（Cr（Ⅵ））. EG and EG-ZⅥ were characterized by X-ray diffraction（XRD）, scanning electron microscopy（SEM）,Fourier-transform infrared（FTIR） spectroscopy and Brunauer–Emmett–Teller（BET） analysis. EG-ZⅥ had a high specific surface area and contained sub-micron sized particles of zero-valent iron. Batch experiments were employed to evaluate the Cr（Ⅵ） removal performance. The results showed that the Cr（Ⅵ） removal rate was 98.80% for EG-ZⅥ,which was higher than that for both EG（10.00%） and ZⅥ（29.80%）. Furthermore, the removal rate of Cr（Ⅵ） by EG-ZⅥ showed little dependence on solution p H within a p H range of 1–9.Even at pH 11, a Cr（Ⅵ） removal rate of 62.44% was obtained after reaction for 1 hr. EG-ZⅥ could enhance the removal of Cr（Ⅵ） via chemical reduction and physical adsorption,respectively. X-ray photoelectron spectroscopy（XPS） was used to analyze the mechanisms of Cr（Ⅵ） removal, which indicated that the ZⅥ loaded on the surface was oxidized, and the removed Cr（Ⅵ） was immobilized via the formation of Cr（III） hydroxide and Cr（III）–Fe（III）hydroxide/oxyhydroxide on the surface of EG-ZⅥ.
基金the Australian Research Council Discovery Early Career Researcher Award(No.DE160100667)the Australian Research Council Discovery Project(No.DP170102812)+1 种基金the Philanthropic Grant for Early Career Engineering Researcher(No.GE12015)the postdoctoral fellowship support from the Japan Society for the Promotion of Science(JSPS)(No.268245)
文摘The importance of enhancing sludge dewaterability is increasing due to the considerable impact of excess sludge volume on disposal costs and on overall sludge management. This study presents an innovative approach to enhance dewaterability of anaerobic digestate（AD） harvested from a wastewater treatment plant. The combination of zero valent iron（ZVI, 0–4.0 g/g total solids（TS）） and hydrogen peroxide（HP, 0–90 mg/g TS） under pH 3.0 significantly enhanced the AD dewaterability. The largest enhancement of AD dewaterability was achieved at 18 mg HP/g TS and 2.0 g ZVI/g TS, with the capillary suction time reduced by up to 90%. Economic analysis suggested that the proposed HP and ZVI treatment has more economic benefits in comparison with the classical Fenton reaction process. The destruction of extracellular polymeric substances and cells as well as the decrease of particle size were supposed to contribute to the enhanced AD dewaterability by HP ＋ ZVI conditioning.
文摘Toxicity studies considering both the bare and stabilized forms of zero valent iron nanoparticles（nZVI） could be timely, given that ecological risks identified are minimized through modification or with substitution of approaches in the synthesis, development and environmental application of the nanoparticles before succeeding to volume production.This review is focused on the fate, transport and toxicological implications of the bare nZVI and surface modified particles used for environmental applications.
基金National Natural Science Foundation of China with Grant No.21905304Natural Science Foundation of Shandong Province(No.ZR2019BEM031)+1 种基金the Fundamental Research Funds for the Central Universities(Nos.18CX02158A,05Y18030020 and 19CX05001A)the support from the Western University-Soochow University Center for Synchrotron Radiation Research。
文摘While manganese-based cathodes have been intensively studied for zinc-ion batteries(ZIBs),the limited rate capability and cycle life have always been a difficult problem to be solved.Here,we report a mixed valent manganese oxide(MnOx)cathode with superior electrochemical performance,which exhibits a high specific capacity of 450 mA h/g at 0.2 C and a satisfactory specific capacity of 158.3 mA h/g at a high rate of 5 C.The mixed cathode system reduces the charge transfer resistance,and show good surface stability and adsorption properties,so it is beneficial for the storage of Zn^(2+).Meanwhile,coaxial fiber ZIBs(CFZIBs)with splendid flexibility are assembled utilizing the elaborately prepared cathode material.The CFZIBs achieve a reversible capacity of 255.8 m A h/g and the capacity retention rate is as high as 80%after 1000 bending deformations.This study provides new opportunities for designing ZIBs with high performance and high flexibility.
基金the financial support from the Ministry of Science and Technology of China(No. 2011CB606301)the National Natural Science Foundation of China (No. 50825402,51101156)
文摘Some problems including low treatment capacity,agglomeration and clogging phenomena,and short working life,limit the application of pre-treatment methods involving zero-valent iron （ZVI）.In this article,ZVI was frozen in an amorphous state through a melt-spinning technique,and the decolorization effect of amorphous ZVI on Acid Orange II solution was investigated under varied conditions of experimental variables such as reaction temperature,ribbon dosage,and initial pH.Batch experiments suggested that the decolorization rate was enhanced with the increase of reaction temperature and ribbon dosage,but decreased with increasing initial solution pH.Kinetic analyses indicated that the decolorization process followed a first order exponential kinetic model,and the surface-normalized decolorization rate could reach 2.09 L/（m^2 ·min） at room temperature,which was about ten times larger than any previously reported under similar conditions.Recycling experiments also proved that the ribbons could be reused at least four times without obvious decay of decolorization rate and efficiency.This study suggests a tremendous application potential for amorphous ZVI in remediation of groundwater or wastewater contaminated with azo dyes.
基金financially supported by the National Natural Science Foundation of China (No.51408101)the Key Research and Development (R&D) Program from the Department of Science and Technology of Sichuan Province (No.2018FZ0011).
文摘Sulfide-modified nanoscale zero-valent iron(S-nZVI) is a promising material for removal of organic pollutants from water, but S-nZVI nanoparticles(NPs) easily agglomerate and have poor contact with organic contaminants.Herein, we propose a new S-nZVI/graphene aerogel(S-nZVI/GA) composite which exhibits superior removal capability for trichloroethylene(TCE) from water.Three-dimensional porous graphene aerogel(GA) can improve the efficiency of electron transport, enhance the adsorption of organic pollutants and restrain the agglomeration of the core-shell S-nZVI NPs.The TCE removal rates of Fe S, nZVI, GA and S-nZVI were 27.8%, 42%, 63% and 75% in 2 hr, respectively.Furthermore, TCE was completely removed within 50 min by S-nZVI/GA.The TCE removal rate increased with increasing p H and temperature, and TCE removal followed the pseudo-first-order kinetic model.The results demonstrate the great potential of S-nZVI/GA composite as a low-cost,easily separated and superior monolithic adsorbent for removal of organic pollutants.
