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1.
V-doped TiO2 nanoparticles(NPs) as dye adsorbents are synthesized by the co-precipitation method and characterized by X-ray powder diffraction, transmission electron microscope, N2 adsorption at 77 K, and X-ray photoelectron spectroscopy. The adsorption of methylene blue(MB) on the V-doped TiO2 NPs is studied in detail by varying the calcination temperature and V doping amount of the adsorbent, adsorbate concentration, adsorbent dosage, agitation rate, reaction temperature, and p H. The comparison of dye adsorption on V-doped TiO2 and parent TiO2 demonstrates that the adsorptive activity of TiO2 can be improved by V doping. The enhanced adsorptive performance can be attributed to the tremendous changes in texture, structure, and surface morphology of adsorbent. The adsorption kinetic analysis shows that the adsorption follows the pseudo-second order kinetics. The apparent activation energy for adsorption is calculated by Arrhenius formula to be 37.6 k J·mol-1, indicating that the adsorption is controlled by both of the diffusion and interfacial adsorption steps. The adsorption data are analyzed using Langmuir and Freundlich isotherms and the results indicate that the Langmuir model provides better correlation of the experimental data. The results conclusively show that the adsorption of MB is a spontaneous behavior and endothermic reaction with the ΔH value of 17.60 k J·mol-1. 相似文献
2.
《结构化学》2021,40(8)
The increasing carbon dioxide emissions have a huge impact on the global environment. Carbonation reaction of CaO is regarded as a potential method to capture carbon dioxide. The density functional theory calculations have been performed to investigate the adsorption of CO_2 on CaO(100) surface. This paper systematically studied the adsorption of CO_2 at different adsorption sites on CaO(100) surface and the influence of adsorption angle on adsorption energy. Based on the studying of adsorption sites, adsorption energy and electronic structure of the CO_2/CaO(100) systems, chemical adsorption mainly happens when CO_2 molecules are absorbed on the CaO(100) surfaces, but physical adsorption may also happen. The research found that CO_2 molecules reacted with surface O atom through C, forming monodentate surface carbonate species and tridentate carbonate. Among them, low-coordinated monodentate ligands have a higher stability than tridentate ligands due to the shorter C–OS bond length of monodentate ligands. 相似文献
3.
In this study the viewpoint is taken that the supported complexes react with active groups on the surface of the support to form new entities which may be called surface complexes.Various interactions between the support and the solute in solution of impregnation have been found,and these interactions may be divided into four calsses: (1) there is no noticeable chemical interaction between the dissolved coordination compound and the support,except the physical adsorption;(2) the metal ion of the complex is anchored on the surface through the surface group as a ligand forming a surface complex,or the support provides the central ion for the formation of a surface polynuciear complex through the bridging ligand of the complex;(3) the surface of the support provides the central ion for ligands dissociated from the complex or for the solvent molecules;(4) the metal hydroxide might be formed,when the acidity of the cation of the support is weaker than that of the metal ion of the complex in a aqueous solutio 相似文献
4.
ZHANG Jing DIAO Zhao-yu WANG Ze-xin 《高等学校化学研究》2006,22(4):488-492
The 5-parameter Morse potential(5-MP) of the interactions between Cl atoms and Ni surfaces was constructed. The adsorption and diffusion of Cl atoms on Ni low index-surfaces were investigated with 5-MP in detail. All the critical characteristics of the system, such as adsorption site, adsorption geometry, binding energy, eigenvalues for vibration, etc. were obtained. The calculated results show that chlorine atoms are likely to be adsorbed on the high symmetry- sites. Cl atoms locate on the four-fold hollow sites of the intact Ni(100) surface, while they tend to occupy threefold sites on the Ni( 111 ) surface. The four-fold hollow sites are the most stable adsorption sites on the Ni (110) surface for Cl, although the three-fold sites and the long-bridge sites are stable adsorption sites on the Ni(110) surface for the atoms of the first and second periods. For the Cl-Ni surface adsorption system, the surface binding energy of a Cl atom is relevant to the coarse degree of the cluster surface, and the binding energies have an order of Ni ( 111 ) 〈 Ni(100) 〈Ni(100). 相似文献
5.
RENLing-ling HEJing EvansD.G. DUANXue 《高等学校化学研究》2003,19(3):324-329
A hydrotalcite-like Mg2 /Al3 layered double hydroxide (LDH) material was prepared by means of amodified coprecipitation method involving a rapid mixing step followed by a separate aging process. LDH calcined at 500℃ , denoted as CLDH, was characterized by XRD, IR and BET surface area measurements.CLDH has a poor crystalline MgO-like structure with a high surface area and porosity. CLDH was used as asupport for the immobilization of penicillin G acylase(PGA). The effect of varying the immobilization conditions, such as pH, contact time and the ratio of enzyme to support, on the activity of the immobilized enzymein the hydrolysis of penicillin G has been studied. It was found that the activity of the immobilized enzyme decreased slightly with decreasing pH and reached a maximum after a contact time of 24 h. The activity of theimmobilized enzyme increased with increasing the ratio of enzyme to support. It was found that the adsorption of PGA inhibited the expected reaction of CLDH with an aqueous medium to regenerate a LDH phase. Itsoriginal activity(36%) after 15 cycles of reuse of the immobilized enzyme was retained, but no further loss in the activity was observed. 相似文献
6.
BINARY COMPETITIVE AND COOPERATIVE ADSORPTION OF AROMATIC COMPOUNDS ON POLYMERIC RESINS 总被引:1,自引:0,他引:1
The adsorption behaviors of 2-naphthalenesulfonic acid and aniline on a conventional macroporous resin Amberlite XAD4 and the other two newly-developed hypercrosslinked resins NDA101 and NDA100 were investigated in a single or binary batch system at 293 K and 313 K,respectively.All the adsorption isotherms of 2-naphthalenesulfonic acid and aniline on the test resins in both systems can fit well with the Langmuir equation,indicating that the adsorption is a favorable process.At the identical equilibrium concentration,the amount of aniline adsorbed on polymeric resins in the single system is higher than that in the binary system because of the competitive adsorption between 2-naphthalenesulfonic acid and aniline on the resin surface.However,the uptake amount of 2-naphthalenesulfonic acid in the binary system is markedly larger than that in the single system,which is presumably due to the cooperative effect arisen from the electrostatic interaction between 2-naphthalenesulfonic acid and aniline adsorbed on the resin surface.The simultaneous adsorption system was proven to be helpful for the selective adsorption toward 2-naphthalenesulfonic acid due to its larger selective index. 相似文献
7.
Cephalexin’s traces within pharmaceutical effluents have toxic impact toward ecological and human health.Low-cost activated carbon derived from Trapa natans husk was oxidized with hydrogen peroxide and nitric acid,and tested for their ability to remove cephalexin from aqueous solutions.Oxidization with H2O2 showed negative effect on the cephalexin sorption,whereas HNO3 oxidization improved the adsorption.The cephalexin adsorption isotherms on the native and HNO3 oxidized carbons correlated well with the Freundlich equation while their kinetics followed the pseudo-second order model.The removal of cephalexin by the native and HNO3 oxidized carbons was found to be most favored at low ionic strength and strong acidic conditions.Based on the thermal and FTIR analyses,the interaction mechanisms of the interaction between cephalexin and the carbons were proposed.Electrostatic attraction,hydrophobic interaction and chemical bonding with surface functional groups were demonstrated as primary mechanisms for cephalexin removal.The nitrogen functionalities on the carbon surface were considered to be an important factor affecting the adsorption process. 相似文献
8.
The effect of metal ions with different valences on the retardation of soil-bentonite barrier materials and its mechanism 总被引:1,自引:0,他引:1
In this paper, with K+, Ca2+ and Fe3+ as the objects of study, retardation of soil-bentonite (SB) barrier materials for metal ions with different valences is investigated, and the adsorption mechanism, migration patterns and permeation behavior are explored so as to provide a theoretical basis for their application. The results show that the adsorption process for metal ions with different valences by SB barrier materials is fast, and the higher the valence, the greater the adsorption capacity. The fitting of the adsorption process conforms to pseudo-second-order adsorption kinetics and Langmuir-Freundlich adsorption equation, which explains that chemical adsorption is the dominating state and that the SB surface has certain heterogeneity. The permeability coefficient of K+, Ca2+ and Fe3+ in SB each has a maximum and the higher the valence, the sooner the maximum appears. Also the higher the valence, the more obvious the effect on SB retardation performance; and the sooner the ion breaks through the barrier wall completely, that is, the wall's retardation performance for higher valent ions may decline. 相似文献
9.
Adsorption separation of carbon dioxide,methane, and nitrogen on Hβ and Na-exchanged β-zeolite
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Xiaoliang Xu Xingxiang Zhao Linbing Sun Xiaoqin Liu 《天然气化学杂志》2008,17(4):391-396
Adsorption isotherms of carbon dioxide (CO2), methane (CH4), and nitrogen (N2) on Hβand sodium exchanged β-zeolite (Naβ) were volumetrically measured at 273 and 303 K. The results show that all isotherms were of Brunauer type I and well correlated with Langmuir-Freundlich model. After sodium ions exchange, the adsorption amounts of three adsorbates increased, while the increase magnitude of CO2 adsorption capacity was much higher than that of CH4 and N2. The selectivities of CO2 over CH4 and CO2 over N2 enhanced after sodium exchange. Also, the initial heat of adsorption data implied a stronger interaction of CO2 molecules with Na+ ions in Naβ . These results can be attributed to the larger electrostatic interaction of CO2 with extraframework cations in zeolites. However, Naβ showed a decrease in the selectivity of CH4 over N2, which can be ascribed to the moderate affinity of N2 with Naβ. The variation of isosteric heats of adsorption as a function of loading indicates that the adsorption of CO2 in Naβ presents an energetically heterogeneous profile. On the contrary, the adsorption of CH4 was found to be essentially homogeneous, which suggests the dispersion interaction between CH4 and lattice oxygen atoms, and such interaction does not depend on the exchangeable cations of zeolite. 相似文献
10.
The adsorption of asymmetrical triblock copolymers from a non-selective solvent on solid surface has been studied by using Scheutjens-Fleer mean-field theory and Monte Carlo simulation method on lattice model. The main aim of this paper is to provide detailed computer simulation data, taking A8-kB20Ak as a key example, to study the influence of the structure of copolymer on adsorption behavior and make a comparison between MC and SF results. The simulated results show that the size distribution of various configurations and density-profile are dependent on molecular structure and adsorption energy. The molecular structure will lead to diversity of adsorption behavior. This discrepancy between different structures would be enlarged for the surface coverage and adsorption amount with increasing of the adsorption energy. The surface coverage and the adsorption amount as well as the bound fraction will become larger as symmetry of the molecular structure becomes gradually worse. The adsorption layer becomes thicker with increasing of symmetry of the molecule when adsorption energy is smaller but it becomes thinner when adsorption energy is higher. It is shown that SF theory can reproduce the adsorption behavior of asymmetrical triblock copolymers. However, systematic discrepancy between the theory and simulation still exists.The approximations inherited in the mean-filed theory such as random mixing and the allowance of direct back folding may be responsible for those deviations. 相似文献
11.
Mg‐Fe layered double hydroxide (LDH) with a Mg/Fe molar ratio of 3:1 was synthesized by using a coprecipitation method and the sorption removal of Pb(II) by the LDH sample from Pb(NO3)2 solution was investigated. It was found that Mg‐Fe LDH showed a good sorption ability for Pb(II) from Pb(NO3)2 solution, indicating that the use of LDH as a promising inorganic sorbent for the removal of heavy metal ions is possible. The sorption kinetics and the sorption isotherm of Pb(II) on the LDH sample obeyed the pseudo‐second order kinetic model and Aranovich‐Donohue equation, respectively. The sorption mechanism of Pb(II) on the LDH may be attributed to the surface‐induced precipitation and the chemical binding adsorption, and the removal ability arising from the surface‐induced precipitation is much higher than that from the chemical binding adsorption. 相似文献
12.
Baker's yeast was cross‐linked by glutaraldehyde and then modified by grafting with poly(amic acid), which was prepared via reaction of pyromellitic dianhydride (PMDA) and arginine at 50°C. The morphology of the pristine, cross‐linked, and modified biomass was observed by microscope. The presence of poly(amic acid) on the biomass surface was verified by X‐ray photoelectron spectroscopy (XPS) analyses. Due to the high density of the functional groups on the modified biomass surface, the metal adsorption capacity for nickel and lead increased significantly, especially when the carboxylic acid groups were converted into carboxylate ions using NaOH. The adsorption process for nickel and lead adsorption followed the pseudo‐second‐order kinetics. The metal adsorption data were fitted with the Langmuir and Freundlich isotherms with the former having a better fit. Using the Langmuir adsorption isotherm, the maximum uptakes for nickel and lead were found to be 0.848 and 0.980 mmol g?1 respectively which were about 15 and 11 times higher than the prisitine biomass. In the simulated wastewater containing 0.400 mmol l?1 of Ni2+ and Pb2+, the metal adsorption capacity of Ni2+ and Pb2+ reached 0.365 mmol l?1 and 0.390 mmol l?1, respectively. The metal ions loaded biomass was regenerated using Ethylene Diamine Tetraacetic Acid (EDTA) solution and used repeatedly over four cycles with little loss of uptake capacity. Copyright © 2007 John Wiley & Sons, Ltd. 相似文献
13.
SiO2‐PAN nanoparticles has been synthesized by reacting silica nanoparticles with 3‐aminopropyltriethoxysilane, formaldehyde and 1‐(2‐pyridylazo)‐2‐naphthol and characterized by FT‐IR and SEM which were used as new sorbent for the preconcentration of trace amount of Pb2+ from various samples. Conditions of the analysis such as preconcentration factor, effect of pH, sample volume, shaking time, elution conditions and effects of interfering ions for the recovery of analyte were investigated. The adsorption capacity of the nanometer SiO2‐PAN was found to be 168.34 μmol/g at optimum pH and the detection limit (3δ) was 0.63 µg/L. The extractant showed rapid kinetic sorption. The adsorption equilibrium of Pb2+ on the nanometer SiO2‐PAN was achieved within 15 min. Adsorbed Pb2+ was easily eluted with 6 mL of 4 mol·L?1 hydrochloric acid. The maximum preconcentration factor was 50. The method was applied to determine trace amounts of Pb2+ in different samples (water and food samples). 相似文献
14.
3‐Hydroxy‐N,N‐diethylaniline (HDEA) as a tertiary aromatic amine was introduced onto the surface of chloromethylated polysulfone (CMPSF) microfiltration membrane through modification reaction, resulting in the modified membrane PSF‐DEA. A redox surface‐initiating system (DEA/APS) was constituted by the bonded tertiary aromatic amine group DEA and ammonium persulfate (APS) in aqueous solution, and so, the free radicals formed on the membrane initiated sodium p‐styrenesulfonate (SSS) as an anionic monomer to produce graft polymerization, getting the grafting‐type composite microfiltration membrane, PSF‐g‐PSSS membrane. Subsequently, the adsorption property of PSF‐g‐PSSS membrane for three heavy metal ions, Pb2+, Zn2+, and Hg2+ ions, was fully examined, and the rejection performance of PSF‐g‐PSSS membrane towards the three heavy metal ions was emphatically evaluated via permeation experiments. The experimental results show that by the initiating of the surface‐initiating system of DEA/APS, the graft polymerization can smoothly be carried out under mild conditions. PSF‐g‐PSSS membrane as a functional microfiltration membrane has strong adsorption ability for heavy metal ions by right of strong electrostatic interaction (or ion exchange action) between the anionic sulfonate ions on the membrane and heavy metal ions. The order of adsorption capacity is Pb2+ > Zn2+ > Hg2+, and the adsorption capacity of Pb2+ ion gets up to 2.18 μmol/cm2. As the volume of permeation solutions, in which the concentrations of the three metal ions are 0.2 mmol/L, are in a range of 50 to 70 mL, the rejection rate of PSF‐g‐PSSS membrane for the three heavy metal ions can reach a level of 95%, displaying a fine rejection and removing performance towards heavy metal ions. 相似文献
15.
In situ Magnesiothermal Synthesis of Mesoporous MgO/OMC Composite for Sensitive Detection of Lead Ions
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Yuzhen Li Shouzhu Li Chi Yang Qunhui Yuan Thomas Wagberg Guangzhi Hu 《Electroanalysis》2016,28(12):2939-2946
Mesoporous materials have exceptional properties for application owing to their ability to absorb and interact with guest species. A novel MgO/OMC composite with mesoporous structure was successfully synthesized via in situ magnesiothermic reduction. The structure was confirmed by N2 sorption isotherms, X‐ray diffraction pattern (XRD), transmission electron microscopy (TEM) and scanning electron microscopy (SEM). By using nafion and bismuth films as co‐modifiers, the MgO/OMC composite material shows high sensitivity of 0.113 μA ? L μg?1 and lower background current for electrochemical determination of lead ion (Pb2+) by using anodic stripping voltammetry. The high specific surface area and good mass transfer on the proposed mesoporous material, as well as the outstanding adsorption abilities of MgO to metal ions and the excellent conductivity of the carbon skeleton contribute to the enhanced electrochemical response of Pb2+. As the stripping response of Bi/MgO/OMC‐Nafion/PGE is highly linear (R2=0.998) over a Pb2+ concentration range of 2 to 300 μg/L, it was successfully used to analyse Pb2+ in real tap‐water samples with good recoveries. 相似文献
16.
AbstractAmino-functionalized mesoporous silica nanoparticles (AFMSN) were prepared based on the self-assembly process of the pre-fabricated template of anionic gemini surfactant. The perfect mass ration of the reactants for the synthesis of the AFMSN with high surface area and amino loading was optimized by orthogonal experiments. Adsorption capability of the optimized product for lead ion (Pb2+) was investigated in detail. Specially, the effects of the amino content, solution pH, adsorbent dosage, temperature, and interference of other metal ions on the removal efficiency of Pb2+ were studied. It is found that these factors can greatly affect the removal efficiency of Pb2+ and the prepared adsorbent exhibits the high adsorption selectivity for Pb2+. At an optimal condition, the AFMSN adsorbent presents an excellent adsorption capacity for Pb2+ up to 211.42?mg/g. The adsorption kinetics study revealed that the pseudo-second-order model could well describe the Pb2+ adsorption process, and the adsorption isotherm was fitted well with the Langmuir model. More importantly, the AFMSN adsorbent could be recycled 8 times and a high adsorption efficiency of Pb2+ could still be maintained. Therefore, the prepared AFMSN adsorbent may find practical application in removing Pb2+ from the polluted water. 相似文献
17.
Highly ordered amino‐functionalized hexagonal mesoporous silica (HMS‐NH2) had been synthesized successfully by co‐condensation. The resultant materials were characterized by means of XRD, TEM, FT‐IR, N2 ad‐desorption and 29Si NMR to confirm the ordered mesoporous structure and the functionalization of the amino groups. The sample was employed as a Pb2+ adsorbent in aqueous solutions at room temperature. Both Lagergren's first order kinetic model and Lagergren's second order kinetic model were used to describe the adsorption data. It was found that the pseudo second order model fitted the sorption kinetic data better than the pseudo first order model. According to the information analyzed from AAS, HMS‐NH2 had a Pb2+ adsorption amount of over 90.7 mg·g?1, showing a promising application for the treatment of wastewater containing Pb2+ ions. 相似文献
18.
《Arabian Journal of Chemistry》2014,7(3):277-286
Batch adsorption experiments were carried out, aiming to remove lead ions from aqueous solutions and water samples using powdered marble wastes (PMW) as an effective inorganic sorbent, which is cheap, widespread, and may represent an environmental problem. The main parameters (i.e., solution pH, sorbent and lead concentration, shaking time, and temperature) influencing the sorption process, were investigated. The results obtained showed that the sorption of Pb2+ ions onto PMW was fitted well with the linear Freundlich and Langmuir models over the concentration range studied. From the Dubinin–Radushkevick (D–R) isotherm model it was found that the adsorption was chemical in nature. Thermodynamic parameters viz. the change in Gibbs free energy change (ΔG°), enthalpy (ΔH°) and entropy (ΔS°) were also calculated. These parameters indicated that the adsorption process of Pb2+ ions on PMW was spontaneous and endothermic in nature. Under the optimum experimental conditions employed, the removal of about 100% of Pb2+ ions was attained. The procedure was successfully applied to remove lead ions from aqueous and different natural water samples. Moreover, the adsorption mechanism is suggested. 相似文献
19.
Microplastics, due to their surface properties, porosity and electrostatic interactions have a high affinity for cations sorption from the aqueous phase. As soil is a complex matrix, interactions between microplastics, soil constituents and heavy metals (HM) may modify the soil microenvironment for heavy metal mobilization/immobilization processes. In order to better understand the problem, three commonly found forms of microplastics in soil (fibers, fragments and microbeads) were mixed with Cu2+- or Pb2+-contaminated soil and incubated at 22 °C for 180 days. In soil samples pH and the content of water and acid exchangeable species of metals were analyzed. The results of this study showed that the presence of microplastics in HM-contaminated soil affected metal speciation, increasing the amount of easily exchangeable and potentially bioavailable forms of Cu2+ or Pb2+ in the tested soil. Soil pH also increased, confirming that microplastic particles affect soil properties relevant to the sorption/desorption process of metal cations. Overall, the smallest microplastic particles (≤1 mm), such as fibers or glitter microbeads, had a greater impact on the change in the sorption and desorption conditions of metals in tested soil than larger particles. The findings of our study show that microplastic form, shape and size should be considered as important factors that influence the soil properties and mobility of heavy metals in soil. 相似文献
20.
《Electroanalysis》2018,30(5):955-961
Herein, a sensitive electrochemical Pb2+ sensor was developed which based on DNA‐functionalized Au nanoparticles(AuNPs) and nanocomposite modified electrode. The DNA‐functionalized AuNPs includes two types of DNA, namely a Pb2+‐mediated DNAzyme comprising a biotin labeled‐enzyme DNA and a substrate strand DNA with a typical stem‐loop structure, and a ferrocene‐labeled linear signal DNA. Without Pb2+, the hairpin loop impeded biotin binding to avidin on the electrode. However,when the goal Pb2+ exists, the substratum strand was divided into two fragments that lead to the enzyme strand was substratumed on the electrode and biotin was admited by avidin, bringing about DNA‐functionalized AuNP(AuNPs) deposition on the electrode surface.The differential pulse voltammetry (DPV) was used to measure electrochemical response signals connect to signal DNA.For the amplification characters of the DNA‐functionalized AuNPs and nanocomposite, the electrochemical detection signal of Pb2+ was greatly improved and revealed high specificity. Under optimum conditions, the resultant biosensor bringed out a high sensitivity and selectivity for the determination of Pb2+. The proposed method was able to detect as low as picomolar Pb2+ concentrations. 相似文献