We analyze oxidative activity of DNA due to fluorescence of chromosomes inside cells, using flow cytometry method with nanometer spatial resolution. Statistics of fluorescence is presented in histogram as frequency di...We analyze oxidative activity of DNA due to fluorescence of chromosomes inside cells, using flow cytometry method with nanometer spatial resolution. Statistics of fluorescence is presented in histogram as frequency distributions of flashes in the dependence on their intensity and in distributions of Shannon entropy, which was defined on the base of normalized distribution of information in original histogram for frequency of flashes. We show that overall sum of entropy, i.e. total entropy E , for any histogram is invariant and has identical trends of changes all values of E(r) = lnr at reduction of histogram’ rank r. This invariance reflects informational homeostasis of chromosomes activity in multi-scale networks of entropy inside all cells in various samples of blood for DNA inside neutrophils, lymphocytes, inside all leukocytes of human and inside chicken erythrocytes for various dyes, colors and various excitations of fluorescence. Informational homeostasis of oxidative activity of 3D DNA in the full set of chromosomes inside living cells exists for any Shannon-Weaver index of biodiversity of cells, at any state of health different beings. Regulation perturbations in information activity DNA provides informational adaptability and vitality of cells at homeostasis support. Noises of entropy, during regulation of informational homeostasis, depend on the states of health in real time. The main structural reconstructions of chromosomal correlations, corresponding to self-regulation of homeostasis, occur in the most large-scale networks of entropy, for rank r<32. We show that stability of homeostasis is supported by activity of all 46 chromosomes inside cells. Patterns, hidden switching and branching in sequences of averages of H?lder and central moments for noises in regulation of homeostasis define new opportunities in diagnostics of health and immunity. All people and all aerobic beings have one overall homeostatic level for countdown of information activity of DNA inside cells. We noted very bad and dangerous properties of artificial cells with other levels of informational homeostasis for all aerobic beings in foods, medical treatment and in biotechnologies.展开更多
The apparent sulfur oxidation activities of four pure thermophilic archaea, Acidianus brierleyi (JCM 8954), Metallosphaera sedula (YN 23), Acidianus manzaensis (YN 25) and Sulfolobus metallicus (YN 24) and the...The apparent sulfur oxidation activities of four pure thermophilic archaea, Acidianus brierleyi (JCM 8954), Metallosphaera sedula (YN 23), Acidianus manzaensis (YN 25) and Sulfolobus metallicus (YN 24) and their mixture in bioleaching chalcopyrite were compared, which were characterized indirectly by the evolution of the cells concentration, pH value and sulfate ions concentration in solution. The results show that the mixed culture contributed significantly to the raising of leaching rate, which suggests that the mixed culture had a higher sulfur oxidation activity than the pure culture. Meanwhile, the results also indicate that the changes of parameters characterizing the sulfur oxidation activity of thermophilic archaea are often influenced by many factors, so it is hard to reflect accurately the specific sulfur oxidation activities among the different sulfur-oxidizing microbes when bioleaching chalcopyrite at different conditions. Accordingly, an efficient method to characterize microbial sulfur oxidation activity appears to be desirable.展开更多
Precipitation is often used for the preparation of La(OH)_(3)with precipitants of liquid alkali and ammonia.To solve the problems of high cost and wastewater pollution caused by common precipitants,the active MgO synt...Precipitation is often used for the preparation of La(OH)_(3)with precipitants of liquid alkali and ammonia.To solve the problems of high cost and wastewater pollution caused by common precipitants,the active MgO synthesized by pyrolysis was used as the precipitant to prepare La(OH)_(3).The species distribution of LaCl_(3)and LaCl_(3)-MgCl_(2)mixed system solution was calculated,and the kinetic analysis of the precipi-tation process was carried out to confirm the key factors influencing the precipitation of La(OH)_(3).The results show that La(OH)_(3)with D_(50)of 5.57μm,a specific surface area of 25.70 m^(2)/g,a rod-like shape,and MgO content of 0.044 wt%,was successfully prepared by adding active MgO.The precipitation ratio of La reaches 99.92%.The La(OH)_(3)precipitation is controlled by the diffusion process.The activity of MgO has a significant influence on MgO content in the precipitate.The preparation of La(OH)_(3)by active MgO provides a potential way for an eco-friendly preparation method of rare earth.展开更多
An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide (GO) at -0.8 V, which shows unique electrocatalytic activity toward tetracycline (TTC) det...An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide (GO) at -0.8 V, which shows unique electrocatalytic activity toward tetracycline (TTC) detection compared to the ERGO-12v (GO applied to a negative potential of-1.2 V), GO, chemically reduced GO (CRGO)-modified glassy carbon electrode (GC) and bare GC electrodes. The redox peaks of TTC on an ERGO-0.8v-modifled glass carbon electrode (GC/ERGO-0.8v) were within 0-0.5 V in a pH 3.0 buffer solution with the oxidation peak current correlating well with TTC concentration over a wide range from 0.1 to 160 mg/L Physical characterizations with Fourier transform infrared (FT-IR), Raman, and X-ray photoelectron spectroscopies (XPS) demonstrated that the oxygen-containing functional groups on GO diminished after the electrochemical reduction at -0.8 V, yet still existed in large amounts, and the defect density changed as new sp2 domains were formed. These changes demonstrated that this adjustment in the number of oxygen-containing groups might be the main factor affecting the electrocatalytic behavior of ERGO. Additionally, the defect density and sp2 domains also exert a profound influence on this behavior. A possible mechanism for the TTC redox reaction at the GC/ERGO-0.8v electrode is also presented. This work suggests that the electrochemical reduction is an effective method to establish new catalytic activities of GO by setting appropriate parameters.展开更多
Bioleaching of sulfide minerals by bacteria, mainly Thiobacillus ferrooxidans(T.f.) and Thiobacillus thiooxidans, plays an important role in hydrometallurgy because of its economic and environmental attractions. The s...Bioleaching of sulfide minerals by bacteria, mainly Thiobacillus ferrooxidans(T.f.) and Thiobacillus thiooxidans, plays an important role in hydrometallurgy because of its economic and environmental attractions. The surveys of production process and the bacterial oxidation activity in the heap bioleaching were investigated. The results show that pH value is high, bacteria biomass and ferric concentration are low, generation time (above 7.13 h) is long in leachate, and less bacteria are adsorbed on the ores. The bacteria in the leachate exposing on the surface and connecting with mineral, have much faster oxidation rate of Fe(Ⅱ) and shorter generation time, compared with those which are in the reservoir for a long time. There is diversity for oxidation activity of Fe(Ⅱ), while there is no diversity for oxidation of sulfur. So it is advisable to add sulfuric acid to degrade pH value to 2.0, add nutrients and shorten recycling time of leachate, so as to enhance bacteria concentration of leachate and the leaching efficiency.展开更多
For the first time,Au nanoparticles on graphene oxide(GO-AuNPs) were successfully fabricated without applying any additional reductants,just by the redox reaction between AuCl_4^(-1) and GO.Their structure was cha...For the first time,Au nanoparticles on graphene oxide(GO-AuNPs) were successfully fabricated without applying any additional reductants,just by the redox reaction between AuCl_4^(-1) and GO.Their structure was characterized by transmission electron microscopy and X-ray powder diffraction.The results show that flower-like AuNPs were successfully dispersed on GO surface.Importantly,they showed a high catalytic activity for the Suzuki-Miyaura coupling reaction in an aqueous medium.展开更多
Nanowire-shaped α-Mo O3 was synthesized on a large scale by hydrothermal route.Nanocrystalline α-Mo2 C phase was obtained by the carburization of α-Mo O3 nanowires with urea as a carbon source precursor.The phase p...Nanowire-shaped α-Mo O3 was synthesized on a large scale by hydrothermal route.Nanocrystalline α-Mo2 C phase was obtained by the carburization of α-Mo O3 nanowires with urea as a carbon source precursor.The phase purity and crystalline size of the synthesized materials were ascertained by using powder X-ray diffraction.The shape and morphology of synthesized materials were characterized by field-emission scanning electron microscopy(FE-SEM) and high resolution transmission electron microscopy(HR-TEM).The electrocatalytic activity of α-Mo2 C for I-/I3^-redox couple was investigated by the cyclic voltammetry.The synthesized α-Mo2 C was subsequently applied as counter electrode in dye-sensitized solar cells to replace the expensive platinum.展开更多
To confirm sub-regular solution model valid for predicting the activity of component in binary oxide systems, seven systems in the whole concentration and twelve systems presenting saturation concentration have been s...To confirm sub-regular solution model valid for predicting the activity of component in binary oxide systems, seven systems in the whole concentration and twelve systems presenting saturation concentration have been studied. The total average relative errors of component 1 and 2 are 3.2 % and 4.1% respectively by application of the sub-regular solution model into the systems within the whole concentration. However, the total average relative errors are 16 % and 1088 % in the systems presenting saturation concentration. The results show that sub-regular solu- tion model is not good for predicting the systems presenting saturation concentration, especially for the systems con- taining acidic or neutral oxide. The reason may be that the influence of the two types of oxide on the configuration is greater in binary oxide systems. These oxides can be present in the form of complex anion partly, Si-O, Al-O, Ti-O and so on, for example (SiO4)4-. That is contrary to sub-regular solution model which is supposed that the oxide systems consist of cation and O2-. But compared with regular solution model and quasi-regular solution model, sub- regular solution model is closer to the characteristics of actual solution and the calculated results are superior.展开更多
6-Substituted 5,8-O-dimethyl-1,4-naphthoquinones(6-DMNQ),the promising anticancer scaffolds,were selectively generated by oxidative demethylation of 2-substituted 1,4,5,8-tetramethoxynaphthalenes with CAN in EtOAc/H...6-Substituted 5,8-O-dimethyl-1,4-naphthoquinones(6-DMNQ),the promising anticancer scaffolds,were selectively generated by oxidative demethylation of 2-substituted 1,4,5,8-tetramethoxynaphthalenes with CAN in EtOAc/H2O in comparatively high yields.An interesting finding was that apart from the reported electron-withdrawing effects of substituents on position 2 of naphthalene ring,regioselective synthesis of 6-DMNQ was largely dependent on the steric effects in CAN-mediated oxidation.The selective cytotoxicities of 6-DMNQ from the in vitro cell-based assays were exhibited between the cancer cells and normal cells.Moreover,most of sulfur-containing 6-DMNQ derivatives displayed better anticancer activities than the corresponding oxygen-containing ones,which could provide an available strategy for the design of 6-DMNQ derivatives as potential anticancer agents.展开更多
The catalytic activity of Perovskite-type mixed oxides (LaCoO3, PrCoO3 and SmCoO3) for the reduction of cyclohexanone to cyclohexanol with 2-propanol (Meerwein-PonndorfVerley reduction) has been studied. The data have...The catalytic activity of Perovskite-type mixed oxides (LaCoO3, PrCoO3 and SmCoO3) for the reduction of cyclohexanone to cyclohexanol with 2-propanol (Meerwein-PonndorfVerley reduction) has been studied. The data have been correlated with the surface electron donor properties of these mixed oxides展开更多
Diradical polycyclic hydrocarbons(PHs)have unique open-shell structures and interesting physical prop-erties.However,owing to high reactivity of unpaired electrons,such open-shell organic diradicaloids are usually les...Diradical polycyclic hydrocarbons(PHs)have unique open-shell structures and interesting physical prop-erties.However,owing to high reactivity of unpaired electrons,such open-shell organic diradicaloids are usually less stable than closed-shell systems,limiting their practical applications.In this study,we report P=O-attaching of diradical PHs as a new strategy to enhance their stability while maintaining diradi-cal properties.Three P=O-attached PHs containing the indeno[1,2-b]fluorene,fluoreno[3,2-b]fluorene and indeno[2,1-b]fluoreneπ-skeletons,respectively,were designed and synthesized.As theoretically and ex-perimentally proved,two of them have the relatively large diradical characters and open-shell singlet diradical nature.In comparison to their all-carbon analogues,the attached electron-withdrawing P=O groups endow them with much lower LUMO/HOMO energy levels but preserved magnetic activities and physical properties,such as thermally accessible triplet species and multi-redox ability.Moreover,the P=O groups effectively decrease their oxidation activities and thereby lead to their remarkably excellent ambient stabilities.Thus,this P=O-attaching strategy will be applicable to other diradical PH systems and may promote the generation of stable organic diradicaloids for radical chemistry and materials.展开更多
The process of preparing anodic oxide film containing active sites and electroless nickel plating on highly active rare earth magnesium alloy was developed.The formation mechanism of electroless nickel plating on acti...The process of preparing anodic oxide film containing active sites and electroless nickel plating on highly active rare earth magnesium alloy was developed.The formation mechanism of electroless nickel plating on active anodic oxide film and the structure and properties of the composite coating were studied by several surface and electrochemical techniques.The results showed that Ag nanograins with an average size of 10 nm were embedded into the anodic oxide film with pores of 0.1−2μm.Ag nanoparticles provided a catalytic site for the deposition of Ni-B alloy,and the Ni crystal nucleus was first grown in horizontal mode and then in cylindrical mode.The corrosion potential of the composite coating increased by 1.37 V and the corrosion current reduced two orders of magnitude due to the subsequent deposition of Ni-P alloy.The high corrosion resistance was attributed to the misaligning of these micro defects in the three different layers and the amorphous structure of the Ni-P alloy in the outer layer.These findings provide a new idea for electroless nickel plating on anodic oxide film.展开更多
Polycrystalline SnO2 fine powder consisting of nano-particles (SnO2-NP), SnO2 nano-sheets (SnO2-NS), and SnO2 containing both nano-rods and nano-particles (SnO2-NR+NP) were prepared and used for CO oxidation. S...Polycrystalline SnO2 fine powder consisting of nano-particles (SnO2-NP), SnO2 nano-sheets (SnO2-NS), and SnO2 containing both nano-rods and nano-particles (SnO2-NR+NP) were prepared and used for CO oxidation. SnO2-NS possesses a mesoporous structure and has a higher surface area, larger pore volume, and more active species than SnO2-NP, and shows improved activity. In contrast, although SnO2-NR+NP has only a slightly higher surface area and pore volume, and slightly more active surface oxygen species than SnO2-NP, it has more exposed active (110) facets, which is the reason for its improved oxidation activity. Water vapor has only a reversible and weak influence on SnO2-NS, therefore it is a potential catalyst for emission control processes.展开更多
Rechargeable Na-O2 batteries have attracted significant attention as energy storage devices owing to their theoretically high energy storage capacity and the natural abundance of sodium. However, practical application...Rechargeable Na-O2 batteries have attracted significant attention as energy storage devices owing to their theoretically high energy storage capacity and the natural abundance of sodium. However, practical applications of this type of battery still suffer from low specific capability, poor cycle sta- bility, instable electrolytes, and unstable polymer binders. Herein, we report a facile method of synthesizing binder free and flexible cathodes with C0304 nanowire arrays vertically grown onto carbon textiles. When employed as a cathode for Na-O2 batteries, this cathode exhibits superior performance, including a reduction of charge overpotential, high specific capacity (4687 mAh/g), and cycle stability up to 62 cycles. These enhanced performance can be attributed to the synergistic effect of the porosity and catalytic activity of the C0304 nanowire catalyst.展开更多
Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization met...Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization method. Through transmission electron microscopy, powder X-ray di raction, and X-ray photoelectron spectroscopy, the role of the carbon supports for the catalytic performances of Pd/C catalysts was examined in selective hydrogenation of acetylene. The results indicate that Pd/AC exhibited higher activity and selectivity than Pd/GO and Pd/rGO in the gas phase selective hydrogenation of acetylene. Thermal and chemical treatment of AC supports also have some effect on the catalytic performance of Pd/AC catalysts. The differences in the activity and selectivity of various Pd/C catalysts were partly attributed to the metal-support interaction.展开更多
The effects of chloride anion (Cl-) (up to 1.0 mol/L) on the decolorization of a model compound,azo dye Acid Orange 7 (AO7),by sulfate radical (SO4-) based-peroxydisulfate (PS) or peroxymonosulfate (PMS) o...The effects of chloride anion (Cl-) (up to 1.0 mol/L) on the decolorization of a model compound,azo dye Acid Orange 7 (AO7),by sulfate radical (SO4-) based-peroxydisulfate (PS) or peroxymonosulfate (PMS) oxidation under various activated conditions (UV 254 nm /PS,Thermal (70°C/PS,UV 254 nm /PMS,Co 2+ /PMS) were investigated.Methanol and NH4 + were used as quenching reagents to determine the contributions of active chlorine species (dichloride radical (Cl2-.) and hypochlorous acid (HClO)).The results indicated that the effects of Cl- on the reaction mechanism were different under various activated conditions.For UV/PS and Thermal/PS,the inhibition tendency became more clear as the Cl- concentration increased,probably due to the reaction between Cl- and SO4-.and the generation of Cl2-.or HClO.For UV/PMS,Cl- did not exhibit inhibition when the concentration was below 0.1 mol/L.As Cl- concentration reached to 1.0 mol/L,the decolorization rate of AO7 was,however,accelerated,possibly because PMS directly reacts with Cl- to form HClO.For Co2+ /PMS,Cl- exhibited a significant inhibiting effect even at low concentration ( 0.01 mol/L).When Cl- concentration exceeded 0.1 mol/L,the activation of PMS by Co 2+ was almost completely inhibited.Under this condition,HClO maybe played a major role in decolorization of AO7.The results implicated that chloride ion is an important factor in SO4-.-based degradation of organic contamination in chloride-containing water.展开更多
The high-energy lithium/sulfur(Li/S) battery has become a very popular topic of research in recent years due to its high theoretical capacity of 1672 m Ah/g. However, the polysulfide shuttle effect remains of great co...The high-energy lithium/sulfur(Li/S) battery has become a very popular topic of research in recent years due to its high theoretical capacity of 1672 m Ah/g. However, the polysulfide shuttle effect remains of great concern with a great number of publications dedicated to its mitigation. In this contribution, a three-dimensional(3D) reduced graphene oxide/activated carbon(RGO/AC) film, synthesized by a simple hydrothermal method and convenient mechanical pressing, is sandwiched between the separator and the sulfur-based cathode, acting as a functional interlayer to capture and trap polysulfide species. Consequently, the Li/S cell with this interlayer shows an impressive initial discharge capacity of 1078 m Ah/g and a reversible capacity of 655 m Ah/g even after 100 cycles. The RGO/AC interlayer impedes the movement of polysulfide while providing unimpeded channels for lithium ion mass transfer. Therefore, the RGO/AC interlayer with a well-designed structure represents strong potential for high-performance Li/S batteries.展开更多
The microstructural evolution and oxidation resistance of multi-walled carbon nanotubes (MWCNTs) by di- rectly heating silicon powder and MWCNTs in a coke bed from 1000 to 1500 ~C are investigated with the aid of X-...The microstructural evolution and oxidation resistance of multi-walled carbon nanotubes (MWCNTs) by di- rectly heating silicon powder and MWCNTs in a coke bed from 1000 to 1500 ~C are investigated with the aid of X-ray diffraction (XRD), scanning electron microscopy (SEM), high resolution transmission electron microscopy (HRTEM) and thermogravimetry-differential scanning calorimetry (TG-DSC). The results showed that the morphology and microstructure of MWCNTs did not change much after being treated from 1000 ~C to 1200 ~C. An obvious SiC coating was formed on the surface of MWCNTs from 1300 to 1400 ~C. Up to 1500 ~C, nearly all the MWCNTs transformed into SiC nanowires. The oxidation resistance of the treated MWCNTs was improved compared with as-received ones. Non-isothermal kinetics showed that the oxidation activation energy of the treated MWCNTs reached 208 kJ/mol, much higher than 264 k J/tool of as-received ones.展开更多
MnO_x-CeO_2 catalysts were synthesized to investigate the active sites for NO oxidation by varying the calcination temperature. XRD and TEM results showed that cubic CeO_2 and amorphous MnO_x existed in MnO_x-CeO_2 ca...MnO_x-CeO_2 catalysts were synthesized to investigate the active sites for NO oxidation by varying the calcination temperature. XRD and TEM results showed that cubic CeO_2 and amorphous MnO_x existed in MnO_x-CeO_2 catalysts. High temperature calcination caused the sintering of amorphous MnO_x and transforming to bulk crystalline Mn_2O_3, H_2-TPR and XPS results suggested the valence of Mn in MnO_x-CeO_2 was higher than pure MnO_x, and decreased with the increasing calcination temperature, The turnover frequency(TOF) was calculated based on the initial reducibility according to H_2-TPR quantitation and kinetic study. The TOF results indicated that the initial reducibility of amorphous MnO_x with high valence manganese ions was equivalent to the active sites for NO oxidation. It can be inferred that the amorphous MnO_x plays a key role in low-temperature NO oxidation.展开更多
The wastewater discharged from tanneries lack biodegradability due to the presence of recalcitrant compounds at significant concentration. The focal theme of the present investigation was to use chemo-autotrophic acti...The wastewater discharged from tanneries lack biodegradability due to the presence of recalcitrant compounds at significant concentration. The focal theme of the present investigation was to use chemo-autotrophic activated carbon oxidation(CAACO) reactor, an immobilized cell reactor using chemoautotrophs for the treatment of tannery wastewater. The treatment scheme comprised of anaerobic treatment, sand filtration, and CAACO reactor, which remove COD, BOD, TOC, VFA and sulphides respectively by 86%, 95%, 81%, 71% and 100%. Rice bran mesoporous activated carbon prepared indigenously and was used for immobilization of chemoautotrophs. The degradation of xenobiotic compounds by CAACO was confirmed through HPLC and FT-IR techniques.展开更多
文摘We analyze oxidative activity of DNA due to fluorescence of chromosomes inside cells, using flow cytometry method with nanometer spatial resolution. Statistics of fluorescence is presented in histogram as frequency distributions of flashes in the dependence on their intensity and in distributions of Shannon entropy, which was defined on the base of normalized distribution of information in original histogram for frequency of flashes. We show that overall sum of entropy, i.e. total entropy E , for any histogram is invariant and has identical trends of changes all values of E(r) = lnr at reduction of histogram’ rank r. This invariance reflects informational homeostasis of chromosomes activity in multi-scale networks of entropy inside all cells in various samples of blood for DNA inside neutrophils, lymphocytes, inside all leukocytes of human and inside chicken erythrocytes for various dyes, colors and various excitations of fluorescence. Informational homeostasis of oxidative activity of 3D DNA in the full set of chromosomes inside living cells exists for any Shannon-Weaver index of biodiversity of cells, at any state of health different beings. Regulation perturbations in information activity DNA provides informational adaptability and vitality of cells at homeostasis support. Noises of entropy, during regulation of informational homeostasis, depend on the states of health in real time. The main structural reconstructions of chromosomal correlations, corresponding to self-regulation of homeostasis, occur in the most large-scale networks of entropy, for rank r<32. We show that stability of homeostasis is supported by activity of all 46 chromosomes inside cells. Patterns, hidden switching and branching in sequences of averages of H?lder and central moments for noises in regulation of homeostasis define new opportunities in diagnostics of health and immunity. All people and all aerobic beings have one overall homeostatic level for countdown of information activity of DNA inside cells. We noted very bad and dangerous properties of artificial cells with other levels of informational homeostasis for all aerobic beings in foods, medical treatment and in biotechnologies.
基金Project(50974140) supported by the National Natural Science Foundation of ChinaProject(20090162110054) supported by Specialized Research Fund for the Doctoral Program of Higher Education of China
文摘The apparent sulfur oxidation activities of four pure thermophilic archaea, Acidianus brierleyi (JCM 8954), Metallosphaera sedula (YN 23), Acidianus manzaensis (YN 25) and Sulfolobus metallicus (YN 24) and their mixture in bioleaching chalcopyrite were compared, which were characterized indirectly by the evolution of the cells concentration, pH value and sulfate ions concentration in solution. The results show that the mixed culture contributed significantly to the raising of leaching rate, which suggests that the mixed culture had a higher sulfur oxidation activity than the pure culture. Meanwhile, the results also indicate that the changes of parameters characterizing the sulfur oxidation activity of thermophilic archaea are often influenced by many factors, so it is hard to reflect accurately the specific sulfur oxidation activities among the different sulfur-oxidizing microbes when bioleaching chalcopyrite at different conditions. Accordingly, an efficient method to characterize microbial sulfur oxidation activity appears to be desirable.
基金the National Key Research and Development Program of China(2022YFB3504503)the National Natural Science Foundation of China(52274355)the Gansu Province Science and Technology Major Special Project,China(22ZD6GD061).
文摘Precipitation is often used for the preparation of La(OH)_(3)with precipitants of liquid alkali and ammonia.To solve the problems of high cost and wastewater pollution caused by common precipitants,the active MgO synthesized by pyrolysis was used as the precipitant to prepare La(OH)_(3).The species distribution of LaCl_(3)and LaCl_(3)-MgCl_(2)mixed system solution was calculated,and the kinetic analysis of the precipi-tation process was carried out to confirm the key factors influencing the precipitation of La(OH)_(3).The results show that La(OH)_(3)with D_(50)of 5.57μm,a specific surface area of 25.70 m^(2)/g,a rod-like shape,and MgO content of 0.044 wt%,was successfully prepared by adding active MgO.The precipitation ratio of La reaches 99.92%.The La(OH)_(3)precipitation is controlled by the diffusion process.The activity of MgO has a significant influence on MgO content in the precipitate.The preparation of La(OH)_(3)by active MgO provides a potential way for an eco-friendly preparation method of rare earth.
基金supported by the National Natural Science Foundation of China(21007033)the Fundamental Research Funds of Shandong University(2015JC017)~~
文摘An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide (GO) at -0.8 V, which shows unique electrocatalytic activity toward tetracycline (TTC) detection compared to the ERGO-12v (GO applied to a negative potential of-1.2 V), GO, chemically reduced GO (CRGO)-modified glassy carbon electrode (GC) and bare GC electrodes. The redox peaks of TTC on an ERGO-0.8v-modifled glass carbon electrode (GC/ERGO-0.8v) were within 0-0.5 V in a pH 3.0 buffer solution with the oxidation peak current correlating well with TTC concentration over a wide range from 0.1 to 160 mg/L Physical characterizations with Fourier transform infrared (FT-IR), Raman, and X-ray photoelectron spectroscopies (XPS) demonstrated that the oxygen-containing functional groups on GO diminished after the electrochemical reduction at -0.8 V, yet still existed in large amounts, and the defect density changed as new sp2 domains were formed. These changes demonstrated that this adjustment in the number of oxygen-containing groups might be the main factor affecting the electrocatalytic behavior of ERGO. Additionally, the defect density and sp2 domains also exert a profound influence on this behavior. A possible mechanism for the TTC redox reaction at the GC/ERGO-0.8v electrode is also presented. This work suggests that the electrochemical reduction is an effective method to establish new catalytic activities of GO by setting appropriate parameters.
文摘Bioleaching of sulfide minerals by bacteria, mainly Thiobacillus ferrooxidans(T.f.) and Thiobacillus thiooxidans, plays an important role in hydrometallurgy because of its economic and environmental attractions. The surveys of production process and the bacterial oxidation activity in the heap bioleaching were investigated. The results show that pH value is high, bacteria biomass and ferric concentration are low, generation time (above 7.13 h) is long in leachate, and less bacteria are adsorbed on the ores. The bacteria in the leachate exposing on the surface and connecting with mineral, have much faster oxidation rate of Fe(Ⅱ) and shorter generation time, compared with those which are in the reservoir for a long time. There is diversity for oxidation activity of Fe(Ⅱ), while there is no diversity for oxidation of sulfur. So it is advisable to add sulfuric acid to degrade pH value to 2.0, add nutrients and shorten recycling time of leachate, so as to enhance bacteria concentration of leachate and the leaching efficiency.
基金supported by the National Science Foundation of China(No.21074089)Tianjin Municipal Science and Technology Commission,China(No.09JCZDJC23300)
文摘For the first time,Au nanoparticles on graphene oxide(GO-AuNPs) were successfully fabricated without applying any additional reductants,just by the redox reaction between AuCl_4^(-1) and GO.Their structure was characterized by transmission electron microscopy and X-ray powder diffraction.The results show that flower-like AuNPs were successfully dispersed on GO surface.Importantly,they showed a high catalytic activity for the Suzuki-Miyaura coupling reaction in an aqueous medium.
基金the financial support from the Department of Atomic Energy–Board of Research in Nuclear Sciences(DAE-BRNS)(Grant No.2013/37P/1/BRNS),Mumbai,India
文摘Nanowire-shaped α-Mo O3 was synthesized on a large scale by hydrothermal route.Nanocrystalline α-Mo2 C phase was obtained by the carburization of α-Mo O3 nanowires with urea as a carbon source precursor.The phase purity and crystalline size of the synthesized materials were ascertained by using powder X-ray diffraction.The shape and morphology of synthesized materials were characterized by field-emission scanning electron microscopy(FE-SEM) and high resolution transmission electron microscopy(HR-TEM).The electrocatalytic activity of α-Mo2 C for I-/I3^-redox couple was investigated by the cyclic voltammetry.The synthesized α-Mo2 C was subsequently applied as counter electrode in dye-sensitized solar cells to replace the expensive platinum.
基金Item Sponsored by National Natural Science Foundation of China(50764006,50574045)Yunnan Basic Applied Research Foundation of China(2006E0021M)
文摘To confirm sub-regular solution model valid for predicting the activity of component in binary oxide systems, seven systems in the whole concentration and twelve systems presenting saturation concentration have been studied. The total average relative errors of component 1 and 2 are 3.2 % and 4.1% respectively by application of the sub-regular solution model into the systems within the whole concentration. However, the total average relative errors are 16 % and 1088 % in the systems presenting saturation concentration. The results show that sub-regular solu- tion model is not good for predicting the systems presenting saturation concentration, especially for the systems con- taining acidic or neutral oxide. The reason may be that the influence of the two types of oxide on the configuration is greater in binary oxide systems. These oxides can be present in the form of complex anion partly, Si-O, Al-O, Ti-O and so on, for example (SiO4)4-. That is contrary to sub-regular solution model which is supposed that the oxide systems consist of cation and O2-. But compared with regular solution model and quasi-regular solution model, sub- regular solution model is closer to the characteristics of actual solution and the calculated results are superior.
基金supported by National Natural Science Foundation of China(No.81373274)Ph.D.Programs Foundation of Ministry of Education China(No.20120073110068)Shanghai Biomedical Supporting Funding(No.15431900600)
文摘6-Substituted 5,8-O-dimethyl-1,4-naphthoquinones(6-DMNQ),the promising anticancer scaffolds,were selectively generated by oxidative demethylation of 2-substituted 1,4,5,8-tetramethoxynaphthalenes with CAN in EtOAc/H2O in comparatively high yields.An interesting finding was that apart from the reported electron-withdrawing effects of substituents on position 2 of naphthalene ring,regioselective synthesis of 6-DMNQ was largely dependent on the steric effects in CAN-mediated oxidation.The selective cytotoxicities of 6-DMNQ from the in vitro cell-based assays were exhibited between the cancer cells and normal cells.Moreover,most of sulfur-containing 6-DMNQ derivatives displayed better anticancer activities than the corresponding oxygen-containing ones,which could provide an available strategy for the design of 6-DMNQ derivatives as potential anticancer agents.
文摘The catalytic activity of Perovskite-type mixed oxides (LaCoO3, PrCoO3 and SmCoO3) for the reduction of cyclohexanone to cyclohexanol with 2-propanol (Meerwein-PonndorfVerley reduction) has been studied. The data have been correlated with the surface electron donor properties of these mixed oxides
基金supported by Jilin Scientific and Technological Development Program(Nos.20220101054JC,20220201085GX)National Natural Science Foundation of China(Nos.22175074,52373182).
文摘Diradical polycyclic hydrocarbons(PHs)have unique open-shell structures and interesting physical prop-erties.However,owing to high reactivity of unpaired electrons,such open-shell organic diradicaloids are usually less stable than closed-shell systems,limiting their practical applications.In this study,we report P=O-attaching of diradical PHs as a new strategy to enhance their stability while maintaining diradi-cal properties.Three P=O-attached PHs containing the indeno[1,2-b]fluorene,fluoreno[3,2-b]fluorene and indeno[2,1-b]fluoreneπ-skeletons,respectively,were designed and synthesized.As theoretically and ex-perimentally proved,two of them have the relatively large diradical characters and open-shell singlet diradical nature.In comparison to their all-carbon analogues,the attached electron-withdrawing P=O groups endow them with much lower LUMO/HOMO energy levels but preserved magnetic activities and physical properties,such as thermally accessible triplet species and multi-redox ability.Moreover,the P=O groups effectively decrease their oxidation activities and thereby lead to their remarkably excellent ambient stabilities.Thus,this P=O-attaching strategy will be applicable to other diradical PH systems and may promote the generation of stable organic diradicaloids for radical chemistry and materials.
基金Project(5227010679)supported by the National Natural Science Foundation of China。
文摘The process of preparing anodic oxide film containing active sites and electroless nickel plating on highly active rare earth magnesium alloy was developed.The formation mechanism of electroless nickel plating on active anodic oxide film and the structure and properties of the composite coating were studied by several surface and electrochemical techniques.The results showed that Ag nanograins with an average size of 10 nm were embedded into the anodic oxide film with pores of 0.1−2μm.Ag nanoparticles provided a catalytic site for the deposition of Ni-B alloy,and the Ni crystal nucleus was first grown in horizontal mode and then in cylindrical mode.The corrosion potential of the composite coating increased by 1.37 V and the corrosion current reduced two orders of magnitude due to the subsequent deposition of Ni-P alloy.The high corrosion resistance was attributed to the misaligning of these micro defects in the three different layers and the amorphous structure of the Ni-P alloy in the outer layer.These findings provide a new idea for electroless nickel plating on anodic oxide film.
基金supported by the National Natural Science Foundation of China (21263015)the Education Department of Jiangxi Province (KJLD14005)the Natural Science Foundation of Jiangxi Province(20151BBE50006,20122BAB203009)~~
文摘Polycrystalline SnO2 fine powder consisting of nano-particles (SnO2-NP), SnO2 nano-sheets (SnO2-NS), and SnO2 containing both nano-rods and nano-particles (SnO2-NR+NP) were prepared and used for CO oxidation. SnO2-NS possesses a mesoporous structure and has a higher surface area, larger pore volume, and more active species than SnO2-NP, and shows improved activity. In contrast, although SnO2-NR+NP has only a slightly higher surface area and pore volume, and slightly more active surface oxygen species than SnO2-NP, it has more exposed active (110) facets, which is the reason for its improved oxidation activity. Water vapor has only a reversible and weak influence on SnO2-NS, therefore it is a potential catalyst for emission control processes.
基金supported by the 100 Talents Programme of the Chinese Academy of Sciencesthe National Basic Research Program of China(973 Program,2014CB932300,2012CB215500)the National Natural Science Foundation of China(21422108,51472232,51301160)~~
文摘Rechargeable Na-O2 batteries have attracted significant attention as energy storage devices owing to their theoretically high energy storage capacity and the natural abundance of sodium. However, practical applications of this type of battery still suffer from low specific capability, poor cycle sta- bility, instable electrolytes, and unstable polymer binders. Herein, we report a facile method of synthesizing binder free and flexible cathodes with C0304 nanowire arrays vertically grown onto carbon textiles. When employed as a cathode for Na-O2 batteries, this cathode exhibits superior performance, including a reduction of charge overpotential, high specific capacity (4687 mAh/g), and cycle stability up to 62 cycles. These enhanced performance can be attributed to the synergistic effect of the porosity and catalytic activity of the C0304 nanowire catalyst.
文摘Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization method. Through transmission electron microscopy, powder X-ray di raction, and X-ray photoelectron spectroscopy, the role of the carbon supports for the catalytic performances of Pd/C catalysts was examined in selective hydrogenation of acetylene. The results indicate that Pd/AC exhibited higher activity and selectivity than Pd/GO and Pd/rGO in the gas phase selective hydrogenation of acetylene. Thermal and chemical treatment of AC supports also have some effect on the catalytic performance of Pd/AC catalysts. The differences in the activity and selectivity of various Pd/C catalysts were partly attributed to the metal-support interaction.
基金supported by the National Natural Science Foundation of China (No. 21107101)the Fundamental Research Funds for the Central Universities of China (Ocean University of China)(No.201113005)
文摘The effects of chloride anion (Cl-) (up to 1.0 mol/L) on the decolorization of a model compound,azo dye Acid Orange 7 (AO7),by sulfate radical (SO4-) based-peroxydisulfate (PS) or peroxymonosulfate (PMS) oxidation under various activated conditions (UV 254 nm /PS,Thermal (70°C/PS,UV 254 nm /PMS,Co 2+ /PMS) were investigated.Methanol and NH4 + were used as quenching reagents to determine the contributions of active chlorine species (dichloride radical (Cl2-.) and hypochlorous acid (HClO)).The results indicated that the effects of Cl- on the reaction mechanism were different under various activated conditions.For UV/PS and Thermal/PS,the inhibition tendency became more clear as the Cl- concentration increased,probably due to the reaction between Cl- and SO4-.and the generation of Cl2-.or HClO.For UV/PMS,Cl- did not exhibit inhibition when the concentration was below 0.1 mol/L.As Cl- concentration reached to 1.0 mol/L,the decolorization rate of AO7 was,however,accelerated,possibly because PMS directly reacts with Cl- to form HClO.For Co2+ /PMS,Cl- exhibited a significant inhibiting effect even at low concentration ( 0.01 mol/L).When Cl- concentration exceeded 0.1 mol/L,the activation of PMS by Co 2+ was almost completely inhibited.Under this condition,HClO maybe played a major role in decolorization of AO7.The results implicated that chloride ion is an important factor in SO4-.-based degradation of organic contamination in chloride-containing water.
基金financial support from the National Natural Science Foundation of China(grant no.21406052the Program for the Outstanding Young Talents of Hebei Province(grant no.BJ2014010)the Scientific Research Foundation for Selected Overseas Chinese Scholars,Ministry of Human Resources and Social Security of China(grant no.CG2015003002)
文摘The high-energy lithium/sulfur(Li/S) battery has become a very popular topic of research in recent years due to its high theoretical capacity of 1672 m Ah/g. However, the polysulfide shuttle effect remains of great concern with a great number of publications dedicated to its mitigation. In this contribution, a three-dimensional(3D) reduced graphene oxide/activated carbon(RGO/AC) film, synthesized by a simple hydrothermal method and convenient mechanical pressing, is sandwiched between the separator and the sulfur-based cathode, acting as a functional interlayer to capture and trap polysulfide species. Consequently, the Li/S cell with this interlayer shows an impressive initial discharge capacity of 1078 m Ah/g and a reversible capacity of 655 m Ah/g even after 100 cycles. The RGO/AC interlayer impedes the movement of polysulfide while providing unimpeded channels for lithium ion mass transfer. Therefore, the RGO/AC interlayer with a well-designed structure represents strong potential for high-performance Li/S batteries.
基金supported by the Natural Science Foundation of Hubei Province (No.2009CDA050)the New Century Excellent Talents in University (No. NCET-10-0137)the National Natural Science Foundation of China (No. 51072143)
文摘The microstructural evolution and oxidation resistance of multi-walled carbon nanotubes (MWCNTs) by di- rectly heating silicon powder and MWCNTs in a coke bed from 1000 to 1500 ~C are investigated with the aid of X-ray diffraction (XRD), scanning electron microscopy (SEM), high resolution transmission electron microscopy (HRTEM) and thermogravimetry-differential scanning calorimetry (TG-DSC). The results showed that the morphology and microstructure of MWCNTs did not change much after being treated from 1000 ~C to 1200 ~C. An obvious SiC coating was formed on the surface of MWCNTs from 1300 to 1400 ~C. Up to 1500 ~C, nearly all the MWCNTs transformed into SiC nanowires. The oxidation resistance of the treated MWCNTs was improved compared with as-received ones. Non-isothermal kinetics showed that the oxidation activation energy of the treated MWCNTs reached 208 kJ/mol, much higher than 264 k J/tool of as-received ones.
基金Project supported by the National key research and development program(2016YFC0204901)the National Natural Science Foundation of China(21576207)the introduction of talent and technology cooperation plan of Tianjin(14RCGFGX00849)
文摘MnO_x-CeO_2 catalysts were synthesized to investigate the active sites for NO oxidation by varying the calcination temperature. XRD and TEM results showed that cubic CeO_2 and amorphous MnO_x existed in MnO_x-CeO_2 catalysts. High temperature calcination caused the sintering of amorphous MnO_x and transforming to bulk crystalline Mn_2O_3, H_2-TPR and XPS results suggested the valence of Mn in MnO_x-CeO_2 was higher than pure MnO_x, and decreased with the increasing calcination temperature, The turnover frequency(TOF) was calculated based on the initial reducibility according to H_2-TPR quantitation and kinetic study. The TOF results indicated that the initial reducibility of amorphous MnO_x with high valence manganese ions was equivalent to the active sites for NO oxidation. It can be inferred that the amorphous MnO_x plays a key role in low-temperature NO oxidation.
文摘The wastewater discharged from tanneries lack biodegradability due to the presence of recalcitrant compounds at significant concentration. The focal theme of the present investigation was to use chemo-autotrophic activated carbon oxidation(CAACO) reactor, an immobilized cell reactor using chemoautotrophs for the treatment of tannery wastewater. The treatment scheme comprised of anaerobic treatment, sand filtration, and CAACO reactor, which remove COD, BOD, TOC, VFA and sulphides respectively by 86%, 95%, 81%, 71% and 100%. Rice bran mesoporous activated carbon prepared indigenously and was used for immobilization of chemoautotrophs. The degradation of xenobiotic compounds by CAACO was confirmed through HPLC and FT-IR techniques.