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1.
Bacterial metal reduction is an important biogeochemical process in anaerobic environments. An understanding of electron transfer pathways from dissimilatory metal-reducing bacteria (DMRB) to solid phase metal (hydr)oxides is important for understanding metal redox cycling in soils and sediments, for utilizing DMRB in bioremedation, and for developing technologies such as microbial fuel cells. Here we hypothesize that the outer membrane cytochromes OmcA and MtrC from Shewanella oneidensis MR-1 are the only terminal reductases capable of direct electron transfer to a hematite working electrode. Cyclic voltammetry (CV) was used to study electron transfer between hematite electrodes and protein films, S. oneidensis MR-1 wild-type cell suspensions, and cytochrome deletion mutants. After controlling for hematite electrode dissolution at negative potential, the midpoint potentials of adsorbed OmcA and MtrC were measured (−201 mV and −163 mV vs. Ag/AgCl, respectively). Cell suspensions of wild-type MR-1, deletion mutants deficient in OmcA (ΔomcA), MtrC (ΔmtrC), and both OmcA and MtrC (ΔmtrC–ΔomcA) were also studied; voltammograms for ΔmtrC–ΔomcA were indistinguishable from the control. When the control was subtracted from the single deletion mutant voltammograms, redox peaks were consistent with the present cytochrome (i.e., ΔomcA consistent with MtrC and ΔmtrC consistent with OmcA). The results indicate that OmcA and MtrC are capable of direct electron exchange with hematite electrodes, consistent with a role as terminal reductases in the S. oneidensis MR-1 anaerobic respiratory pathway involving ferric minerals. There was no evidence for other terminal reductases operating under the conditions investigated. A Marcus-based approach to electron transfer kinetics indicated that the rate constant for electron transfer ket varies from 0.025 s−1 in the absence of a barrier to 63.5 s−1 with a 0.2 eV barrier.  相似文献   

2.
Electron transfer between redox active proteins and mineral oxides is important in a variety of natural as well as technological processes, including electron transfer from dissimilatory metal-reducing bacteria to minerals. One of the pathways that could trigger electron transfer between proteins and minerals is redox-linked conformation change. We present electrochemical evidence that mitochondrial cytochrome c (Mcc) undergoes significant conformation change upon interaction with hematite and indium-tin oxide (ITO) surfaces. The apparent adsorption-induced conformation change causes the protein to become more reducing, which makes it able to transfer electrons to the hematite conduction band. Although Mcc is not a protein thought to be involved in interaction with mineral surfaces, it shares (or can be conformed so as to share) some characteristics with multiheme outer-membrane cytochromes thought to be involved in the transfer of electrons from dissimilatory iron-reducing bacteria to ferric minerals during respiration. We present evidence that a 10.1 kDa monohoeme cytochrome isolated and purified from Acidiphilium cryptum, with properties similar to those of Mcc, also undergoes conformation change as a result of interaction with hematite surfaces.  相似文献   

3.
In order to understand the adsorption mechanism of metal atoms to semiconducting surfaces, we have studied, as a model system, the vapor phase adsorption of Ag, Au, and Cu on the (001) surface of molybdenite (MoS2) and the subsequent surface diffusion of these adsorbates. Our scanning tunneling microscopy (STM) images show that, depending on the type of metal atom that is adsorbed, islands of a characteristic size (2 nm for Ag, 8 to 10 nm for Cu, two distinct sizes of 2 nm and 8 to 10 nm for Au), shape (well rounded in the lateral extension) and thickness (one monolayer for Ag, 1 to 1.5 nm for Cu) are formed during the initial stages of deposition. Whole islands are observed to surface diffuse without loss of size or shape. Despite the relatively large size of the copper islands on molybdenite, these islands surface diffuse extensively, suggesting that the Cu-S interaction is weak. Surface diffusion is only hindered once individual islands start to coalesce. As copper islands accumulate, the size and shape of the original islands can still be recognized, supporting the conclusion that these characteristics are constant and that monolayer growth occurs by the aggregation of islands across the surface.The strength and the nature of the Ag-S(MoS2) bond were further investigated by using molecular orbital calculations, ultraviolet photoelectron spectroscopy (UPS) and scanning tunneling spectroscopy (STS). By applying quantum mechanical approaches using a two-dimensional periodic molybdenite slab and hexagonal MoS2 clusters of different sizes with metal atoms adsorbed to them, it is possible to calculate the electron transfer between the mineral surface and the metal atom as well as the adsorption energy as a function of surface coverage. In addition, we used the results from the quantum mechanical runs to derive empirical potentials that model the characteristics of the forces within the crystal, within the adsorbed islands, and the metal and mineral surface. The combination of quantum mechanical calculations and empirical force field calculations explain the electronic structure and the highest stability of Ag islands that have seven atoms in diameter, which exactly agrees with the size of experimentally observed islands. UPS results also suggest that a specific new state is formed (approximately 4.5 eV into the valence band) which may describe the Ag-S bond because it does not occur in pure silver or molybdenite.This study shows how the combination of microscopic (STM), spectroscopic (STS, UPS), compositional (X-ray photoelectron spectroscopy, XPS) and molecular modeling (quantum mechanical and empirical) techniques is a useful approach to understand the nature of the metal to sulfide bond. Further insights may be gained concerning the natural association of certain metals with sulfides.  相似文献   

4.
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5.
Evolutionary trees are derived based on nucleic acid and protein sequences and the methods of numerical taxonomy. From 5S ribosomal RNA sequences, molecules that participate in protein synthesis, the order of branching of many prokaryote species and the nuclear and organellar components of eukaryote species are inferred. All oxygen-evolving forms, including the chloroplasts and blue-green algae, are to be found on a single branch; the mitochondria are found with the Rhodospirillaceae, nonsulfur photosynthetic bacteria; and the eukaryote cytoplasmic components are found with the archae-bacteria, including Thermoplasma and Sulfolobus. This tree clearly supports the symbiotic origin of the eukaryote organelles. There is much redundant information available from c-type cytochromes, cytochromes c′, 4Fe-4S ferredoxins and 5.8S rRNA molecules. A gene duplication of ferredoxin, probably predating all of the species divergences, permitted us to infer an ancestral molecule that can be placed on the tree to give the base. The heterotrophic anaerobes have a sequence most resembling the ancestral sequence, suggesting that the ancestor may have been a heterotroph. Ten prokaryote species occur on both the c-type and the c′-type cytochrome trees. There is only one inconsistency in the topologies of the two trees, which may reflect a gene transfer among prokaryotes confirming that, for these genes of fundamental importance, gene transfer followed by acceptance is rare. The eukaryote trees derived from 5S and 5.8S rRNA suggest that the earliest eukaryotes were unicellular and that the multicellular forms of plants, animals, fungi and slime molds arose independently.  相似文献   

6.
The atomic and electronic structure of mineral surfaces affects many environmentally important processes such as adsorption phenomena. They are however rarely considered relevant to dissimilatory bacterial reduction of iron and manganese minerals. In this regard, surface area and thermodynamics are more commonly considered. Here we take a first step towards understanding the nature of the influence of mineral surface structure upon the rate of electron transfer from Shewanella oneidensis strain MR-1 outer membrane proteins to the mineral surface and the subsequent effect upon cell “activity.” Cell accumulation has been used as a proxy for cell activity at three iron oxide single crystal faces; hematite (001), magnetite (111) and magnetite (100). Clear differences in cell accumulation at, and release from the surfaces are observed, with significantly more cells accumulating at hematite (001) compared to either magnetite face whilst relatively more cells are released into the overlying aqueous phase from the two magnetite faces than hematite. Modeling of the electron transfer process to the different mineral surfaces from a decaheme (protoporphyrin rings containing a central hexacoordinate iron atom), outer membrane-bound cytochrome of S. oneidensis has been accomplished by employing both Marcus and ab initio density functional theories. The resultant model of electron transfer to the three oxide faces predicts that over the entire range of expected electron transfer distances the highest electron transfer rates occur at the hematite (001) surface, mirroring the observed cell accumulation data. Electron transfer rates to either of the two magnetite surfaces are slower, with magnetite (111) slower than hematite (001) by approximately two orders of magnitude. A lack of knowledge regarding the structural details of the heme-mineral interface, especially in regards to atomic distances and relative orientations of hemes and surface iron atoms and the conformation of the protein envelope, precludes a more thorough analysis. However, the results of the modeling concur with the empirical observation that mineral surface structure has a clear influence on mineral surface-associated cell activity. Thus surface structure effects must be accounted for in future studies of cell-mineral interactions.  相似文献   

7.
黄铁矿表面及其与Au（HS）2^—溶液作用的STM研究   总被引：5，自引：0，他引：5  
张世柏  张平城 《矿物学报》1996,16(1):28-32,T001
本文用ＳＴＭ研究了黄铁矿和方铅矿表面的原子结构、纳米级微形貌、电子态分布及其吸附态的特点。ＳＴＭ电流图象揭示了表面缺陷与表面电子态之间的对应关系，硫化和的表面的化学反应活性可能是表现缺陷引起的局域导电性增强有关。ＳＴＭ观察进一步表明黄铁矿和方铅矿对金的硫氢配合物的吸附作用优先发生于扭折位和台阶边缘等高能部位，反映出吸附态的分布也是与表面电子态分布相对应的。这样就从微观领域考证了硫化物表面对化学活性  相似文献   

8.
The bioinorganic fraction of the dermal granules of Molpadia intermedia from a wide variety of habitats has been studied by chemical analysis, electron microscopy, X-ray diffraction, thermal analysis, visible and infrared spectroscopy and magnetic susceptibility. It was found to have many similarities to polynuclear iron(III) proteins. Silica was found to be an integral component of the granules. The proportions of the major elements, P and Si, were found to vary with habitat as well as the minor elements, Ca and Mg, whereas the Fe content remained relatively constant. Models are proposed for the microstructure of the granules and the processes of their growth.  相似文献   

9.
Lack of nutrients is a common challenge for enteric pathogens, like Shigella, when discharged in waters and soils by infected persons. These bacteria must evolve protective mechanisms to survive nutrient changing conditions. Many studies have demonstrated that bacterial starvation can affect cell morphology and surface properties such as lipopolysaccharide content. This study focuses on the morphological and physiological alterations of Shigella flexneri, a human pathogen, under nutrient starvation during 30 days. Our results showed that S. flexneri can survive under nutrient deficiency during 4 weeks. However, starved cells revealed several morphological changes indicating decrease of the size and change of the cell shape as observed by transmission electron microscopy. Furthermore, the outer membrane proteins and lipopolysaccharide profiles of starved cells revealed the disappearance, the appearance, and changes of the protein band levels. The survival and physiological adaptation of S. flexneri under nutrient limitation during 30 days may increase the risk of human and animal infections.  相似文献   

10.
不同剪切作用下CMC水溶液的微观结构研究   总被引：1，自引：0，他引：1  
针对聚合物钻井液重要组分之一的羧甲基纤维素钠盐(CMC),考虑钻井液在井底钻头与环空处所受的不同剪切作用,测试了其水溶液在相应近似剪切作用(分别为600,6 000 r/min)下的流变性,并结合冷冻干燥方法,利用扫描电子显微镜观测了这两种剪切作用后CMC水溶液相应的微观结构.结果表明高速剪切作用使CMC水溶液的空间网络骨架拉伸变细,甚至破坏,溶液黏度有所降低,流动性增大.这样,热量更容易通过这些网络骨架,使充填其中的小分子物质以热传导、对流传热等方式传递到钻屑表面,分解钻屑表面的水合物.水合物分解产生的气体和水则以分子扩散的形武向内向外进行传质,但会受到钻井液微观骨架结构和其中填充物质的阻碍.  相似文献   

11.
Computer simulation of electron transfer at hematite surfaces   总被引：1，自引：0，他引：1  
Molecular dynamics simulations in combination with ab initio calculations were carried out to determine the rate of electron transfer at room temperature in bulk hematite (α-Fe2O3) and at two low-index surfaces, namely the (012) and (001) surfaces. The electron transfer reactions considered here involve the II/III valence interchange between nearest-neighbor iron atoms. Two electron transfer directions were investigated, namely the basal plane and c direction electron transfers. Electron transfer rates obtained in bulk hematite were in good agreement with ab initio electronic structure calculations thus validating the potential model. The surfaces were considered both in vacuum and in contact with an equilibrated aqueous solution. The reorganization energy is found to increase significantly at the first surface layer and this value is little affected by the presence of water. In addition, in the case of the (012) surface, the electronic coupling matrix element for the topmost basal plane transfer was calculated at the Hartree-Fock level and was found to be weak compared to the corresponding electron transfer in the bulk. Therefore, most surfaces show a decrease in the rate of electron transfer at the surface. However, where iron atoms involved in the electron transfer reaction are directly coordinated to water molecules, water lowers the free energy of activation to a great extent and provides a large driving force for electrons to diffuse toward the bulk thus opposing the intrinsic surface effect. The surfaces considered in this work show different electron transfer properties. Hematite has been shown to exhibit anisotropic conductivity and thus different surfaces will show different intra- and inter-layer rates depending on their orientation. Moreover, the calculations of electron transfers at the hydroxyl- and iron-terminated (001) surfaces revealed that surface termination has a significant effect on the electron transfer parameters in the vicinity of the surface. Finally, our findings indicate that undercoordinated terminal iron atoms could act as electron traps at the surface.  相似文献   

12.
Mining and metallurgical processing of gold and base metal ores can lead to the release of arsenic into the aqueous environment as a result of the weathering and leaching of As-bearing minerals during processing and following disposal. Arsenic in process solutions and mine drainage can be effectively stabilized through the precipitation of ferrihydrite. However, under anaerobic conditions imposed by burial and waste cover systems, ferrihydrite is susceptible to microbial reduction. This research, stimulated by the paucity of information and limited understanding of the microbial reduction of arsenical ferrihydrite, was conducted on synthetic adsorbed and co-precipitated arsenical 6-line ferrihydrite (Fe/As molar ratio of 10/1) using Shewanella sp. ANA-3 and Shewanella putrefaciens CN32 in a chemically defined medium containing 0.045 mM phosphate concentration. Both bacteria were equally effective in their reducing abilities around pH 7, resulting in initial rates of formation of dissolved As(III) of 0.10 μM/h for the adsorbed, and 0.08 μM/h for the co-precipitated arsenical 6-line ferrihydrite samples. The solid phases in the post-reduction samples were characterized by powder X-ray diffraction (XRD), micro-XRD, scanning electron microscopy (SEM), transmission electron microscopy (TEM), electron microprobe and X-ray absorption spectroscopy (XAS) techniques. The results indicate the formation of secondary phases such as a biogenic Fe(II)–As(III) compound, akaganeite, goethite, hematite and possibly magnetite during bacterial reduction experiments. Holes and bacterial imprints measuring about 1–2 μm were observed on the surfaces of the secondary phases formed after 1200 h of reduction. This study demonstrates the influence of Fe and As reducing bacteria on the release of significant concentrations of more mobile and toxic As(III) species from arsenical 6-line ferrihydrite, more readily from the adsorbed than from the co-precipitated ferrihydrite.  相似文献   

13.
Dissolved organic matter (DOM) has been shown to be an integral component in biogeochemical electron transfer reactions due to its demonstrated ability to facilitate redox reactions. While the role of DOM as a facilitator of electron transfer processes has been demonstrated, greater knowledge would lead to better understanding of the structural components responsible for redox behavior, such as quinones and nitrogen and sulfur (N/S) functional groups. This investigation uses direct scan voltammetry (DSV) coupled with fluorescence and NMR spectroscopy as well as thermochemolysis gas chromatography mass spectrometry (GC-MS) and X-ray photoelectron spectroscopy (XPS) to elucidate the organic moieties responsible for facilitating electron transfer reactions. We contrast electrochemical properties and structural details of three organic matter isolates from diverse sources; Great Dismal Swamp DOM (terrestrially derived, highly aromatic), Pony Lake DOM (microbially derived, highly aliphatic) and Toolik Lake (terrestrially derived, photochemically and microbially altered) with juglone (a redox-active model quinone). Aromatic and phenolic constituents were detected (by 13C NMR) and recovered (by thermochemolysis GC-MS) from all three fulvic acid samples, highlighting the ubiquity of these compounds and suggesting that the quinone-phenol redox couple is not limited to DOM derived from lignin precursors. The range of hydroxy-benzene and benzoic acid derivatives may explain the lack of a single pair of well-defined oxidation and reduction peaks in the DSV scans. The presence of a wide-range of hydroxylated benzoic acid isomers and other redox-active aromatic residues implies that native DOM possesses overlapping redox potentials analogous to their characteristic range of pKa values.  相似文献   

14.
We have used ex situ atomic force microscopy (AFM), scanning tunneling microscopy and spectroscopy (STM/STS) and X-ray photoelectron spectroscopy (XPS) to study the surfaces of natural arsenopyrite samples that were electrochemically polarized in 1 M HCl, or leached in acidic solutions containing ferric iron salts, and then reacted with aqueous gold (III) chloride at ambient temperatures. For arsenopyrite oxidized on a positive-going potential sweep, progressively increasing amounts of surface Fe(III)-O and As-O species, and of S/Fe and S/As ratios in a non-stoichiometric sulfidic layer were found. The products formed in the sweep to a potential of 0.6 V (Ag/AgCl) of the passivity region are shaped in about 100 nm protrusions of two sorts, which are arranged in micrometer-size separate areas, while they are largely mixed at higher, “transpassive” potentials. The quantities of surface alteration substances notably decrease after leaching in ferric chloride and ferric sulfate acidic solutions. Passivation of arsenopyrite was suggested to associate with the disordered, metal-deficient surface layer having moderate excess of sulfur rather than with the products of arsenopyrite oxidation. Exposure of arsenopyrite to 10−5-10−3 M (pH 2) solutions results in the deposition of 8-50 nm gold particles; only a small fraction of the gold is present as Au(I)-S species. The electrochemical oxidation at 0.6 V or ageing of arsenopyrite in air promotes the subsequent gold deposition; in contrast, the amount of Au deposited on arsenopyrite that was treated by leaching in ferric chloride and sulfate solutions was about 10 times smaller than with polished arsenopyrite samples. It has been concluded that reducing agents formed as intermediates of arsenopyrite decomposition facilitate the Au0 cementation although other factors related to the surface state of the arsenopyrite play a role as well. A decrease in the tunneling current magnitudes with decreasing the Au0 particle size has been revealed using STS. This effect along with the increase by 0.2-0.5 eV in the XPS Au 4f binding energies were tentatively ascribed to retarding the electron transitions by emerging electrostatic charge on gold nanoparticles (Coulomb blockade). Possible mechanisms for the effects, and their potential role in the deposition and hydrometallurgy of “invisible” gold are discussed.  相似文献   

15.
Eight interplanetary dust particles (IDPs) exhibiting a wide range of H and N isotopic anomalies have been studied by transmission electron microscopy, x-ray absorption near-edge structure spectroscopy, and Fourier-transform infrared spectroscopy. These anomalies are believed to have originated during chemical reactions in a cold molecular cloud that was the precursor to the Solar System. The chemical and mineralogical studies reported here thus constitute direct studies of preserved molecular cloud materials. The H and N isotopic anomalies are hosted by different hydrocarbons that reside in the abundant carbonaceous matrix of the IDPs. Infrared measurements constrain the major deuterium (D) host in the D-enriched IDPs to thermally labile aliphatic hydrocarbon groups attached to macromolecular material. Much of the large variation observed in D/H in this suite of IDPs reflects the variable loss of this labile component during atmospheric entry heating. IDPs with elevated 15N/14N ratios contain N in the form of amine (-NH2) functional groups that are likely attached to other molecules such as aromatic hydrocarbons. The host of the N isotopic anomalies is not as readily lost during entry heating as the D-rich material. Infrared analysis shows that while the organic matter in primitive anhydrous IDPs is similar to that observed in acid residues of primitive chondritic meteorites, the measured aromatic:aliphatic ratio is markedly lower in the IDPs.  相似文献   

16.
Oxidative dissolution of natural rhodochrosite by the Mn(II) oxidizing bacterium Pseudomonas putida strain MnB1 was investigated based on batch and electrochemical experiments using natural rhodochrosite as the working electrode. Tafel curves and batch experiments revealed that bacterial exopolymers (EPS) significantly increased dissolution of natural rhodochrosite. The corrosion current significantly increased with reaction time for EPS treatment. However, the corrosion process was blocked in the presence of cells plus extra EPS due to formation of the passivation layer. Moreover, the scanning electron microscopy and the energy dispersive spectroscopy (SEM–EDS) results showed that the surface of the natural rhodochrosite was notably changed in the presence of EPS alone or/and bacterial cells. This study is helpful for understanding the role of EPS in bacterially oxidation of Mn(II). It also indicates that the Mn(II) oxidizing bacteria may exert their effects on Mn(II) cycle and other biological and biogeochemical processes much beyond their local ambient environment because of the catalytically dissolution of solid Mn(II) by EPS and the possible long distance transport of the detached EPS.  相似文献   

17.
页岩气储层孔隙系统表征方法研究进展   总被引：5，自引：0，他引：5       下载免费PDF全文
页岩气是以游离、吸附和溶解状态赋存于暗色泥页岩中的天然气,页岩的孔隙特征是决定页岩储层含气性的关键因 素。页岩孔隙结构复杂,一般以纳米孔隙占优势,用常规储层孔隙的表征方法难以解释美国的高产页岩气系统。因此,页 岩纳米孔隙的表征成为制约页岩气资源评价的关键因素。在综述目前国际上对页岩气储层孔隙表征方法的基础上,对比分 析其各自的适用范围和应用前景。页岩储层孔隙的主要表征方法有3种:(1)以微区分析为主的图像分析技术;(2)以压 汞法和气体等温吸附为主的流体注入技术;(3)以核磁共振、中子小角散射 计算机断层成像技术为代表的非流体注入技术。 图像分析能够直观、方便、快捷地获取孔隙形态等方面的特征;流体注入法在表征微孔隙的孔径分布、比表面积等方面具 有独到优势;非流体注入技术由于其原位、无损分析及粒子高穿透力的特点,使研究多种地质条件下的孔隙特性成为可能。 在目前的技术条件下,应明确各种表征技术的优势与限制,根据实际情况合理建立孔隙研究流程,综合利用多种技术手段 能在不同的尺度下有效表征页岩气储层孔隙。  相似文献   

18.
In this study, we test the potential for passive cell wall biomineralization by determining the effects of non-metabolizing bacteria on the precipitation of uranyl, lead, and calcium phosphates from a range of over-saturated conditions. Experiments were performed using Gram-positive Bacillus subtilis and Gram-negative Shewanella oneidensis MR-1. After equilibration, the aqueous phases were sampled and the remaining metal and P concentrations were analyzed using inductively coupled plasma-optical emission spectroscopy (ICP-OES); the solid phases were collected and analyzed using X-ray diffractometry (XRD), transmission electron microscopy (TEM), and X-ray absorption spectroscopy (XAS).At the lower degrees of over-saturation studied, bacterial cells exerted no discernable effect on the mode of precipitation of the metal phosphates, with homogeneous precipitation occurring exclusively. However, at higher saturation states in the U system, we observed heterogeneous mineralization and extensive nucleation of hydrogen uranyl phosphate (HUP) mineralization throughout the fabric of the bacterial cell walls. This mineral nucleation effect was observed in both B. subtilis and S. oneidensis cells. In both cases, the biogenic mineral precipitates formed under the higher saturation state conditions were significantly smaller than those that formed in the abiotic controls.The cell wall nucleation effects that occurred in some of the U systems were not observed under any of the saturation state conditions studied in the Pb or Ca systems. The presence of B. subtilis significantly decreased the extent of precipitation in the U system, but had little effect in the Pb and Ca systems. At least part of this effect is due to higher solubility of the nanoscale HUP precipitate relative to macroscopic HUP. This study documents several effects of non-metabolizing bacterial cells on the nature and extent of metal phosphate precipitation. Each of these effects likely contributes to higher metal mobilities in geologic media, but the effects are not universal, and occur only with some elements and only under a subset of the conditions studied.  相似文献   

19.
A new organic–inorganic composite cation exchanger polyaniline Sn(IV) silicate has been synthesized. The physicochemical properties of this ion exchanger were determined using different analytical techniques including fourier transform infrared spectroscopy, simultaneous thermogravimetry–differential thermogravimetry analyses, X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray spectroscopy and elemental analysis studies. Ion exchange capacity and effect of heating temperature on ion exchange capacity were also carried out on this ion exchange material. Adsorption properties for different metal ions have been investigated and the results revealed that polyaniline Sn(IV) silicate had the highest adsorption capacity for Cd2+ ion. It’s selectivity was tested by achieving some important binary separations. Dependence of adsorption on contact time, temperature, pH of the solution and exchanger dose had been studied to achieve the optimum conditions. Adsorption kinetic study showed that the adsorption process followed the first order kinetics. Adsorption data were fitted to linearly transformed Langmuir isotherm with R 2 (correlation coefficient) >0.99. The maximum removal of Cd2+ was found at pH 9. The adsorption was fast and the equilibrium established within 40 min. Thermodynamic parameters viz- entropy change, enthalpy change and Gibb’s free energy change were also calculated.  相似文献   

20.
In this study, a series of RE3+:YVO4 catalysts were successful synthesized by environmentally friendly mild hydrothermal and supercritical hydrothermal techniques. The rare earth-doped YVO4 photocatalysts were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, photoluminescence spectroscopy. The X-ray diffraction analysis reveals that the as-prepared YVO4 crystals are of tetragonal phase. Further, the Fourier transform infrared spectroscopy result shows the absence of OH– molecules. The photoluminescence spectroscopy curves and UV–Vis spectra suggest that the band gap energy of YVO4 is shifted to lower energy level due to doping of Nd3+ and Er3+ ions. The catalytic activities of the as-prepared RE3+:YVO4 samples were tested for the photodegradation of amaranth aqueous dye solution under sunlight irradiation. Remarkably, the rare earth-doped YVO4 nanocrystal sample showed outstanding photocatalytic degradation activities than undoped YVO4 nanocrystal sample with good reusability. Under full spectrum irradiation, the as-prepared Nd3+-doped YVO4 nanocrystals exhibited about 83% degradation efficiency. The apparent rate constant k for as-prepared Nd3+-doped YVO4 nanocrystals with 50 mg of photocatalyst exhibits highest k value (0.32 min?1), which is 2.9% higher than pure YVO4 nanocrystals (0.11 min?1).  相似文献   

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